The 100 most-cited articles in Advanced Functional Materials, 2024

Abstract The trends of miniaturization, lightweight, and high integration in electronics have brought serious issues in heat dissipation and electromagnetic compatibility and also limited the simultaneous use of thermally conductive and microwave absorption materials. Therefore, it is imperative to design materials that possess those dual functions. In this work, one‐pot method is used to anchor zeolitic imidazolate framework ZIF‐67 coated with polydopamine (PDA) on boron nitride (BN) to obtain BN@ZIF‐67@PDA. The pyrolysis product BN@Co‐C@C is used as heterostructured thermally conductive/microwave absorption fillers and blended with polyethylene terephthalate (PET) to prepare BN@Co‐C@C/PET composites. When the mass ratio of BN to ZIF‐67@PDA is 7.5:1 and the mass fraction of BN 7.5 @Co‐C@C is 45 wt%, the BN 7.5 @Co‐C@C/PET composites exhibit excellent thermal conductivities and microwave absorption performances. The thermal conductivity coefficient is 5.37 W m −1 K −1 , which is 35.8 times higher than that of PET (0.15 W m −1 K −1 ), and also higher than that of 45 wt% (BN 7.5…

Abstract Recent developments have introduced a groundbreaking form of collinear magnetism known as “altermagnetism”. This emerging magnetic phase is characterized by robust time‐reversal symmetry breaking, antiparallel magnetic order, and alternating spin‐splitting band structures, yet it exhibits vanishing net magnetization constrained by symmetry. Altermagnetism uniquely integrates traits previously considered mutually exclusive to conventional collinear ferromagnetism and antiferromagnetism, thereby facilitating phenomena and functionalities previously not achievable within these traditional categories of magnetism. Initially proposed theoretically, the existence of the altermagnetic phase has since been corroborated by a range of experimental studies, which have confirmed its unique properties and potential for applications. This review explores the rapidly expanding research on altermagnets, emphasizing the novel physical phenomena they manifest, methodologies for inducing altermagnetism, and promising altermagnetic materials. The goal of this review is to furnish readers with…

Abstract The demand for low‐frequency microwave absorption materials is becoming more and more urgent. Novel shape anisotropy chain‐like CoNi is fabricated using polyvinylpyrrolidone as a shape‐directing agent via solvothermal method, which is then mixed with polydimethylsiloxane (PDMS) to prepare corresponding multifunctional chain‐like CoNi/PDMS composite films. Shape anisotropy and strong magnetic coupling effect of chain‐like CoNi enhance natural resonance and magnetic loss capability. The minimum reflection loss (RL min ) is −50.5 dB and low‐frequency effective absorption bandwidth (EAB) is 1.04 GHz (2.64–3.68 GHz) at 3.9 mm for chain‐like CoNi. The corresponding 18 vol% chain‐like CoNi/PDMS composite films present optimal low‐frequency microwave absorption performance with RL min of −56.7 dB and low‐frequency EAB of 1.04 GHz (2.96–4.00 GHz) at 4.1 mm, which is far superior to 18 vol% spherical CoNi/PDMS composite films with RL min of −9.5 dB. Meantime, the in‐plane and inter‐plane thermal conductivity coefficients of 18 vol% chain‐like CoNi/PDMS composite films are 2.05 and…

Abstract Defect engineering is an emerging technology for tailoring nanomaterials' characteristics and catalytic performance in various applications. Recently, defect‐engineered nanoparticles have emerged as highly researched materials in catalytic applications because of their exceptional redox reaction capabilities and physicochemical and optical properties. The properties of nanomaterials can be readily adjusted by controlling the nature and concentration of defects within the nanoparticles, avoiding the need for intricate design strategies. This review investigates defect engineering in nanocatalysts, including the design, fabrication, and applications. Initially, the various categories and strategies of nanomaterial defects and their impacts on the nanocatalysts' electronic and surface properties, catalytic activity, selectivity, and stability are summarized. Then, the catalytic processes and their uses, including gas sensing, hydrogen (H 2 ) evolutions, water splitting, reductions of carbon dioxide (CO 2 ) and nitrogen to value‐aided products, pollutant degradation, and…

Abstract Rational manipulation of composition and microstructure design is recognized as an effective pathway to realize multifunctional high‐performance microwave absorber. In this work, necklace‐like hollow polyacrylonitrile (PAN)/carbon nanofibers are designed and constructed through a simple continuous electrospinning‐carbonization‐etching route. Specifically, by varying the carbonization temperature, the ratio of PAN to carbon content of necklace‐like hollow PAN/carbon nanofibers can be effectively regulated, resulting in tunable electromagnetic parameters and conductive loss capacities. After that, the hollow structure is further introduced to improve the feature of lightweight, impedance‐matching characteristics, and interfacial polarization loss ability. Accordingly, the necklace‐like hollow PAN/carbon nanofibers exhibited a frequency bandwidth of 6.60 GHz and a minimum reflection loss of −44.73 dB at 1.76 mm. Both the experimental and theoretical simulation results indicated that the obtained necklace‐like hollow PAN/carbon nanofibers possessed the high chemical stability…

Abstract Urea oxidation reaction (UOR) has garnered significant attention in recent years as a promising and sustainable clean‐energy technology. Urea‐containing wastewater poses severe threats to the environment and human health. Numerous studies hence focus on developing UOR as a viable process for simultaneously remediating wastewater and converting it into energy. Moreover, UOR, which has a thermodynamic potential of 0.37 V (vs reversible hydrogen electrode, RHE), shows great promise in replacing the energy‐intensive oxygen evolution reaction (OER; 1.23 V vs RHE). The versatility and stability of urea, particularly at ambient temperatures, make it an attractive alternative to hydrogen in fuel cells. Since UOR entails a complex intermediate adsorption/desorption process, many studies are devoted to designing cost‐effective and efficient catalysts. Notably, transition metal‐based materials with regulated d orbitals have demonstrated significant potential for the UOR process. However, comprehensive reviews focusing on transition metal‐based catalysts remain scarce. In light of…

Abstract Understanding of fundamental mechanism and kinetics of the oxygen evolution reaction (OER) is pivotal for designing efficient OER electrocatalysts owing to its key role in electrochemical energy conversion devices. In the past few years, the lattice oxygen oxidation mechanism (LOM) arising from the anodic redox chemistry has attracted significant attention as it involves a direct O─O coupling and thus bypasses thermodynamic limitations in the traditional adsorbate evolution mechanism (AEM). Transition metal‐based oxyhydroxides are generally acknowledged as the real catalytic phase in alkaline media. In particular, their low‐dimensional layered structures offer sufficient structural flexibility to trigger the LOM. Herein, a comprehensive overview is provided for recent advances in anion redox from LOM‐based electrocatalysts. Based on analyses of electronic structure of electrocatalysts and LOM, a strategy is proposed to activate LOM. Possible identification techniques for corroboration of the oxygen redox are also reviewed. In addition, the structural reconstruction process…

Abstract Hard carbon (HC) materials with rich closed pore structures and nano‐scaled soft carbon coating layer have emerged as promising anode in sodium‐ion batteries (SIBs). However, it still remains a tremendous challenge to precisely regulate closed pore structures and soft carbon coating thicknesses for achieving excellent electrochemical performance in SIBs at low‐voltage platforms. Herein, PCHC‐10 with abundant and suitable‐sized closed pore size (0.45 nm) and nano‐scaled soft carbon coating layer has been accurately designed by chemical crosslink reaction between the pre‐oxidized phenolic resin and a small addition of pitch to form ester‐based bond. As anode, PCHC‐10 delivered large reversible capacity of 359.8 mAh g −1 within 0.001–2.5 V, and high capacity of 242.8 mAh g −1 in low voltage platforms (≤0.15 V). Besides, PCHC‐10 anode exhibits 91.4% capacity retention for 100 cycles, and Na 3 V 2 (PO 4 ) 3 //PCHC‐10 full cell has superior rate performance and high energy density of 231.2 Wh kg −1 . Furthermore, the detailed electrochemical storage behaviors and theoretical…

Abstract Anion defect engineering is proven to be an efficient approach to reconstruct the electronic configuration of carbon‐based magnetoelectric materials for targeted modulation of electromagnetic (EM) performance. However, traditional mono‐anionic doping suffers from low defect concentration and lacks diverse polarization mechanisms. In this work, multi‐anions (N/S/F) stepwise‐doped carbon/Fe 3 C magnetoelectric composites are elaborately constructed, wherein the predesigned N defects serve as activated sites for anomalously adopting S anions (Step I) and subsequent F anions (Step II) in non‐marginal areas of the carbon layer. It is found that S prefers to replace pyrrolic N defects while F tends to form dangling bonds with the C site adjacent to the pyridinic N. Intriguingly, besides the inherent polarized resonance of N defect at ≈15 GHz, customized S and F defects induce new polarization resonances at ≈10 GHz and ≈15+ GHz, respectively. Under a typical multi‐polarization effect with the synergetic magnetic response, the carbon/Fe 3 C composites with N/S/F defects harvest the…

Abstract Covalent organic frameworks (COFs) attract significant attention due to their ordered, crystalline, porous, metal‐free, and predictable structures. These unique characteristics offer great opportunities for the diffusion and transmission of photogenerated charges during photocatalysis. Currently, a considerable number of COFs are used as metal‐free organic semiconductor photocatalysts. This review aims to understand the relationships between the structure and photocatalysis performance of COFs and provides in‐depth insight into the synthetic strategy to improve photocatalysis performance. Subsequently, the review focuses on the structural motif of COFs in sustainable photocatalytic hydrogen evolution, carbon dioxide reduction, hydrogen peroxide generation, and organic compound transformations. Last, in conjunction with the significant progress achieved and the challenges yet to be overcome, a candid discussion is undertaken regarding the challenges and opportunities in the field of COF photocatalysis, accompanied by the presentation of potential research avenues and future…

Abstract Photocatalytic uranium extraction from seawater is an ideal strategy to obtain uranium resources. Herein, the cyano‐functionalized graphitic carbon nitride (g‐C 3 N 4 ‐CN) with an isosite structure of adsorption and photoreduction for U(VI) is successfully prepared to achieve efficient photocatalytic uranium extraction from seawater. As the key of the isosite structure, the cyano group not only dramatically promotes the separation of photogenerated charges of g‐C 3 N 4 ‐CN and enriched electrons around it, but also greatly improves the adsorption capacity and selectivity for U(VI) over g‐C 3 N 4 ‐CN by complexing with U(VI). Therefore, g‐C 3 N 4 ‐CN exhibits efficient and stable photocatalytic U(VI) reduction performance, with a saturated uranium extraction capacity of 2644.3 mg g −1 , significantly higher than most reported g‐C 3 N 4 ‐based photocatalysts. Moreover, it also performs well in solar light‐driven uranium extraction from actual seawater. Briefly, this work illustrates the importance of constructing the isosite structure of adsorption and photoreduction for…

Abstract Research on organic–inorganic hybrid materials (OIHMs) has experienced explosive growth in the past decades. The diversity of organic components allows for the introduction of various spatial scales, functional groups, and polarities, while inorganic components provide higher hardness, heat resistance, and stability, their flexible combination facilitates the formation of diverse structures. Furthermore, simple and cost‐effective synthesis methods, such as room temperature solution processes and mechanochemical techniques, enable precise control over the materials' properties at different scales, thus achieving adjustable structure–performance relationships. This review will discuss the recent research progress of OIHMs within the field of optoelectronics and related optoelectronic device applications. According to the dimension of inorganic components and the nature of organic–inorganic interface, this review divides OIHMs into four structural categories. The ongoing research has revealed diverse applications for OIHMs in the fields of solar cells, light‐emitting devices,…

Abstract Silicon (Si), stands out for its abundant resources, eco‐friendliness, affordability, high capacity, and low operating potential, making it a prime candidate for high‐energy‐density lithium‐ion batteries (LIBs). Notably, the breakthrough use of nanostructured Si (nSi) has paved the way for the commercialization of Si anodes. Despite this, challenges like high processing costs, severe side reactions, and low volumetric energy density have impeded widespread industrial adoption. Micron‐scale Si (µSi) has always faced setbacks compared to nSi due to its greater volume expansion. However, recent years have witnessed a resurgence of interest in µSi‐based anodes. Capitalizing on its inherent advantages, including low cost and high tap density, µSi has once again captured the attention of both academic and industrial communities. This review begins by contrasting the strengths and weaknesses of µSi and nSi, then outline potential solutions to enhance µSi performance, covering aspects like structural regulation, composite anodes, binder design, and electrolyte exploration.…

Abstract The development of nanocomposite microwave absorbers is a critical strategy for tackling electromagnetic pollution. However, challenges persist regarding material stability and achieving broadband absorption. Herein, a novel multi−scale design approach for metamaterial absorbers is proposed. First, a series of bimetallic (cobalt and copper) semiconductive metal–organic framework (SC−MOF) crystals with atomically resolved structures are successfully prepared to serve as building blocks for metamaterials. By simply adjusting the concentration ratio of the two ions, the controllable preparation of crystal morphology can be achieved. This enables to precisely tune the absorption peak and bandwidth range of the SC−MOF, resulting in excellent EMW absorption performance (effective absorption bandwidth: 6.16 GHz, minimum reflection loss: −61 dB). Based on this, printable inks are further constructed by encapsulating the SC−MOF in polydimethylsiloxane and 3D‐printed multi−layered metamaterial absorbers based on woodpile porous architecture. The metamaterial absorber demonstrates a…

Abstract Real‐time monitoring of respiration plays a very important role in human health assessment, especially in monitoring and analyzing respiration during exercise and sleep. However, traditional humidity sensors still have problems in flexibility, sensitivity, and durability, so there is an urgent need to develop humidity sensors with high sensitivity, stretchability, and environmental resistance as respiratory monitoring applications. Here, based on the double network hydrogel structure of polyvinyl alcohol and polyacrylamide, a highly sensitive, highly stretchable, and environmentally stable organic hydrogel humidity sensor has been manufactured by using the synergistic effect of lithium chloride and MXene. The hydrogel humidity sensor shows rapid response in the humidity range of 40–85% RH, and has a high sensitivity of −103.4%/% RH. In addition, it exhibits more than 3000% mechanical strain and excellent environmental resistance, which is attributed to the chemical cross‐linking in the hydrogel network and the synergistic effect of multiple hydroxyl groups in glycerol…

Abstract Piezocatalysis and piezo‐photocatalysis technology is a continuously developing catalytic technology based on the piezoelectric effect of catalysts, which breaks the barrier between mechanical and chemical energy. The piezoelectric polarization field formed by the mechanical deformation of piezoelectric materials is proven to effectively manipulate band structures, improve the separation of electron‐hole pairs and enhance the catalytic activity, thus alleviating energy crises and environmental issues. Herein, this review first introduces the technology of piezocatalysis and piezo‐photocatalysis, comprehensively summarizes the synthesis methods of piezo(photo)catalysis materials, and analyzes and discusses the measures to optimize the performance of piezo(photo)catalysts. The following systematically summarizes the characteristics and development of the current main piezo(photo)catalytic systems, and discusses the application of first principles calculations in piezo(photo)catalysis in combination with practical researches. Subsequently, the main application progress of…

Abstract Heterostructured (HS) materials, characterized by heterogeneous zones with differences in mechanical or physical properties, represent a revolutionary advancement in material science. During deformation, hetero‐deformation‐induced (HDI) stress forms due to the synergistic interactions between soft and hard zones, leading to remarkable HDI strengthening and strain hardening. This mechanism significantly enhances their performance, surpassing that of traditional homogeneous materials. This review delves into the classification, preparation techniques, fundamental deformation mechanisms, and research methods of HS materials. It outlines the preparation methods of various HS materials, emphasizing their unique characteristics and applications. The review elaborates on the fundamental deformation mechanisms of HS materials, focusing on non‐uniform plastic deformation behavior and HDI strain hardening. Furthermore, it explores the application of heterogeneous design concepts in materials, analyzing their microstructure tuning mechanisms and mechanical properties. This review aims…

Abstract Rechargeable aqueous zinc (Zn) batteries are a promising candidate for large‐scale energy storage, but the noncompact and dendritic Zn deposition, water‐induced parasitic reaction, and narrow operating temperature range severely hinder their practical application. Here, it is demonstrated that these challenges can be conquered by introducing low‐cost acetamide (Ace) into aqueous electrolytes. The non‐sacrificial Ace molecules with both donor and acceptor groups can disrupt the original H‐bonded network of water, replace the solvating‐H 2 O in Zn 2+ ‐solvation sheath, form dynamic adsorption on Zn, and create an H 2 O‐poor electrical double‐layer. Consequently, the presence of Ace suppresses water erosion on Zn, homogenizes Zn nucleation/growth, reduces water reactivity, and depresses the freezing point of electrolyte. The formulated Ace‐containing electrolyte features a wide temperature range from −20 to 60 °C and enables highly compact and dendrite‐free Zn electrodeposition even at 25 mAh cm −2 using a non‐pressure electrolytic cell. Moreover, the Ace‐containing…

Abstract Antibacterial photodynamic therapy (aPDT) and antibacterial sonodynamic therapy (aSDT) utilize sensitizers (photosensitizers/sonosensitizers) to produce reactive oxygen species (ROS) for antibacterial treatment under the stimulation of light/ultrasound, which have the characteristics of broad‐spectrum antibacterial properties, low drug‐resistance, and effective targeting of infected tissues. Nanomaterials in aPDT/aSDT are primarily used as nano‐sensitizers or nano‐carriers of sensitizers. They enhance the stability and permeability of sensitizers, improve targeting of sensitizers, strengthen photodynamic/sonodynamic properties of sensitizers (modification of sensitizers absorption efficiency and light/ultrasonic response stress by modulation of nanoparticle shape, size, and structure). Also, they improve modifiability of sensitizers (controlling the release rate and time of the sensitizer as needed to optimize the therapeutic effect), enhance programmability and multifunctionality of sensitizers (flexible application of nanotechnology for designing sensitizers with multiple…

Abstract Defects and microstructures have been utilized to effectively modulate electromagnetic (EM) wave absorption for mitigating electromagnetic pollution and stealth issues. However, precisely feasibly tailoring them still remains challenging. Here, by using a multilevel hollow cobalt sulfide embedded in a heteroatomic sulfur (S) ‐doped carbon aerogel, a preferential reaction strategy of modulating point defects and hollow microstructures via controllable S atoms migration is proposed to improve the EM wave absorption. S atoms contribute to the creation of hollow structures via Kirkendall effects, as well as inducing point defects in the carbon lattice through doping. More significantly, the mechanisms prioritizing the formation of hollow structures over defects have been discovered, with low‐velocity atomic migration primarily modulating the microstructure for interfacial polarization and impedance matching, and high‐velocity atom migration focused on introducing defects to achieve polarization and conductive loss. The resulting aerogel exhibits an exceptionally maximum…

Abstract Photocatalytic conversion of CO2 to methane faces challenges due to the stability of CO2, unpredictable intermediates, and complex electron transfer steps. Herein, a spatial In2S3/In2O3 heterojunction with abundant S vacancies (ISIO(VS)) is obtained through facile Polyvinylpyrrolidone (PVP) treatment to reach a methane yield of 16.52 µmol·g−1·h−1 with a selectivity of 95.93%, which is the highest among reported In2S3 and In2O3 based catalysts. The work function (Wf), differential charge density, and Kelvin Probe Force Microscopy (KPFM) results confirm that S vacancies strengthen the built‐in electric field (BEF) of In2S3/In2O3 (ISIO) heterojunctions, improving carrier separation. Density functional theory (DFT) calculations reveal that S vacancies induce electron redistribution, facilitating adsorption and activation of CO2 and *CO intermediate, thus promoting hydrogenation to yield *CHO. The reaction pathway of photocatalytic CO2 reduction is revealed by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and Gibbs free energy (ΔG). The S vacancies…

Abstract The development of nanomaterials is crucial to upgrading of modern industry. MXene nanosheets have attracted significant attention due to their superb resistance to permeation, diverse surface chemical properties, impressive mechanical properties, and metal‐like electrical and thermal conductivity, etc., providing unique advantages in various technical fields. When MXene nanosheets are combined with polymers to form functional coatings, their applications span multiple fields, including anticorrosion, wear resistance, flame‐retardancy, electromagnetic interference (EMI) shielding, and de‐icing. This review, in conjunction with MXene's barrier property, lubricity, thermal stability, conductivity, and photothermal conversion property, discusses in detail the various applications of MXene‐based polymer coatings. Additionally, it examines the dispersion and interaction of MXene within polymer coatings and the role of functionalized MXene in polymers. Finally, based on the current research status and emerging needs, the development challenges and future research opportunities of…

Abstract The preparation of core–shell structured nanoparticles using the galvanic replacement reaction of liquid metals is a simple and efficient method. However, precise modulation of the core and shell components to regulate the microwave absorption performance still needs to be further explored. In this study, various types of indium/oxide core–shell nanoparticles are prepared based on a competitive galvanic reaction of gallium‐indium liquid metals. The prepared indium/oxide core–shell structured nanoparticles exhibit superior electromagnetic (EM) wave absorption properties with a minimum reflection loss (RL) of −40.25 dB at 1.7 mm and the widest effective absorption band of 6.12 GHz at 2.1 mm. The superior wave‐absorbing properties originate from the dielectric losses of the interfacial and dipole polarizations. In addition, an externally applied magnetic field improves the polarization loss and microwave dissipation to achieve a minimum RL of −45.65 dB at 2.4 mm. The liquid‐metal‐assisted competitive galvanic reaction strategies extend the variety of core–shell structured…

Abstract The integration of bio‐inspired hierarchical design into synthetic carbon materials holds promise for developing lightweight, high‐performance structural materials. Hierarchical and heterogeneous nanoscale units are crucial to load bearing and mechanical functionality yet receives limited attention for difficulties in accurate regulation. Herein, one kind of multilayered heterogeneous have proposed pyrocarbon based composite constructed through chemical vapor deposition method with nanoscale graphene orderliness regulation. Sequential construction from orientational graphene sheets to nondirective isotropic networks is achieved through controlling the size and morphology of pyrolysis intermediates with moderate oxidation, being expected to facilitate load transfer and structural stability through dynamically adjustment in heterogeneous interfacial sliding. The resulting multilayer heterogeneous phases exhibit impressive strengthening and toughening mechanisms dominated by microstructural multiscale coupling, which provides new solutions for developing structural composites…

Abstract The lithium‐sulfur (Li‐S) battery stands as a strong contender for the next‐generation energy storage system, characterized by abundant sulfur resources, environmental sustainability, and high specific capacity. However, its energy density remains constrained by factors such as low sulfur loading and fraction in the cathode, excessive electrolyte, and an excess of anode. These mild conditions significantly limit the energy density of Li‐S batteries, making them less competitive. To achieve higher energy density, harsh operation conditions are necessary, but these remain challenging to implement, even in a lab‐scale production. In this comprehensive review, the emphasis will be on recent advancements in Li‐S batteries, specifically in the realm of designing high sulfur loading, high sulfur fraction, lean electrolyte, and low limited negative electrode Li‐S batteries. A visualizable model that illustrates the relationship between cell energy density and various cell parameters, underscoring the importance of exploring Li‐S batteries under extreme operating conditions for…

Abstract Persistent oxidative stress and bacterial infection are significant challenges that impede diabetic wound healing. By combining diagnosis and treatment, pH variation on the wound tissue can be monitored in real time, and precise treatment can be carried out promptly to promote diabetic wound healing. In this study, a lipoic acid‐modified chitosa (LAMC) hydrogel is constructed via an amidation reaction, and ceria oxide‐molybdenum disulfide nanoparticles with a polydopamine layer (C@M@P), along with carbon quantum dots (CDs) synthesized by a hydrothermal method, are loaded into the hydrogel, thus developing a diagnostic and therapeutic hydrogel (LAMC/CD‐C@M@P). By incorporating CDs, the hydrogel exhibits high sensitivity and reversibility to pH under ultraviolet light. Furthermore, the images of hydrogels can be collected using smartphones and converted into wound pH signals, providing a means for early detection of bacterial infection. Notably, the LAMC/CD‐C@M@P hydrogel exhibits excellent photothermal antibacterial capability against Staphylococcus aureus and Escherichia…

Abstract Promoting advanced functional films that integrate protective behaviors for synergetic radar, infrared (IR), and visible light is confronted with extreme challenges. The effective integration of shielding capacity and IR camouflage into single‐component carbon films remains an enormous challenge because of limited conductivity and high IR absorption. In this work, carbon nanotube (CNT) films with excellent electromagnetic interference (EMI) shielding, switchable IR camouflage, and energy conversion are obtained via a (FCCVD) method and subsequent defect engineering strategies induced by temperature (Strategy I) and N/S co‐doping (Strategy II). Wherein the effect on the electronic configuration as well as multi‐spectra performance is deeply explored. Ascribing to the synergistic effects of strategies, defective CNT films present superior EMI shielding effectiveness (SE) with a high absorption effectiveness ratio of 86.9%, and a large span of emissivity (0.479), which provides the necessary condition for various application scenarios. Under the applied electric field…

Abstract Aqueous zinc ion batteries hold promise as alternative systems to lithium‐based batteries. However, practical development faces critical challenges due to parasitic side reactions and dendrite growth in zinc anodes. While introducing electrolyte additives is promising, monofunctional additives offer limited protection to the zinc anode from a single aspect. Herein, a disodium succinate additive is presented to establish a hydrophobic and zincophilic dual electric layer structure on the Zn surface, regulate the solvation structure of Zn 2+ , and act as a pH buffer during cycling. As a result, the symmetrical cell with an electrolyte containing 0.2 m SADS shows a durable life of over 2200 h, and the Zn||MnO 2 full cell still maintains an 80% capacity retention after 1000 cycles. In addition, SADS both show wide applicability in the match with NVO and I 2 cathode. This work provides a low‐cost and multifunctional electrolyte additive, facilitating the development of high‐performance aqueous zinc ion batteries.

Abstract As wearable sensors advance rapidly, demands for multifunctional conductive soft materials are ever higher, including high stretchability, resilience, adhesiveness and stability, simultaneously in one material, for stable long‐term use. Nanocomposite hydrogels incorporating conductive two‐dimensional (2D) nanofillers, such as MXene‐composited gels, emerge as promising candidates. Yet, fulfilling all above requirements, particularly large stretchability with low hysteresis, remains a challenge, owing to the easy oxidation and weak interactions of MXene nanosheets with polymer chains. Herein, an interfacial engineering strategy is proposed, where tannic acid (TA) with high‐density hydroxyl groups is introduced to encapsulate MXene into a stable TA@MXene nano‐motif and meanwhile increase the hydrogen‐bonding interactions between TA@MXene and polymer network. By incorporating TA@MXene into poly(hydroxyethyl acrylate) (PHEA) network in a glycerol/water binary solvent, the obtained organohydrogel exhibits integrated properties of high stretchability (>500%) with low hysteresis…

Abstract The sustainable production of hydrogen utilizing solar energy is a pivotal strategy for reducing reliance on fossil fuels. ZnIn 2 S 4 (ZIS), as a typical metal sulfide semiconductor, has received extensive attention in photocatalysis. Although the introduction of sulfur (S) vacancies in ZIS to enhance photocatalytic hydrogen production by creating defect energy levels has been explored, detailed studies on the control and modulation of S‐vacancies in ZIS are sparce. This study demonstrates that while moderate levels of S‐vacancies can enhance hydrogen evolution, excessive vacancies may hinder the process, underscoring the importance of S‐vacancy modulation. Guided by theoretical calculations, We have designed and synthesized ZIS with modulated S‐vacancies to realize favorable hydrogen adsorption‐free energy and integrated in a Schottky‐heterojunction with MXene co‐catalysts for enhanced hydrogen evolution. The optimized hydrogen evolution performance of ZnIn 2 S 4 /MXene (ZMX) reaches 14.82 mmol g −1 h −1 under visible light irradiation, surpassing many reported ZnIn 2 S 4…

Abstract Hydrogel adhesives exhibit great potential in various biomedical fields such as tissue sealing and soft robotics. However, the high‐water content and defective network structures of these hydrogel adhesives result in low intrinsic mechanical strength, severely impeding their application. In this study, it is reported that the strong hydrogel adhesive strength can be achieved when a balance is established between adhesive forces and cohesive forces. Based on this principle, a new double network (DN) design is created to combine an adhesive polyvinyl alcohol (PVA) as the first network with a flexible sodium alginate (SA) as the second network. A delicate balance is achieved between cohesion and adhesion by adjusting the ratio between the first rigid adhesive network and the second flexible network. As a result, this balanced DN hydrogel adhesive exhibits a strong tissue adhesion strength, approximately three times higher than that in the non‐balance situation.

Abstract The construction of lightweight yet robust, durable magnetic transition metal carbides and/or nitride (MXene) aerogels is highly desired for assembling high‐performance, multifunctional architectures. However, the fabrication and application of magnetic MXene aerogels is severely restricted by their inferior mechanical strength and poor water/oxygen resistance. Here, sustainable cellulose nanofibrils (CNFs) are employed for assisting in the physical and chemical dual cross‐linking to strongly bind the MXenes and MOF‐derived magnetic nanoparticles. The dual‐crosslinked magnetic MXene aerogels (D‐MMAs) achieve a density as low as 12 mg cm −3 , and acquire a significantly improved mechanical strength of up to 1311% over physically crosslinked ones, as well as remarkably improved hydrophobicity, and oxidation stability. Furthermore, the multifunctional integration of efficient and tunable electromagnetic wave (EMW) absorption, remarkable photothermal conversion, thermal insulation, prominent oil‐water separation, thin/thick oil and dye absorption capability, and the remote…

Abstract In recent years, the penetration rate of lithium iron phosphate batteries in the energy storage field has surged, underscoring the pressing need to recycle retired LiFePO 4 (LFP) batteries within the framework of low carbon and sustainable development. This review first introduces the economic benefits of regenerating LFP power batteries and the development history of LFP, to establish the necessity of LFP recycling. Then, the entire life cycle process and failure mechanism of LFP are outlined. The focus is on highlighting the advantages of direct recycling technology for LFP materials. Directly regenerating LFP materials is a very promising solution. Directly regenerating spent LFP (S‐LFP) materials can not only protect the environment and save resources, but also directly add lithium atoms to the vacancies of missing lithium atoms to repair S‐LFP materials. At the same time, simply supplementing lithium to repair S‐LFP simplifies the recovery process and improves economic benefits. The status of various direct recycling methods is then reviewed in terms of the…

Abstract Soft robots have recently attracted increasing interest due to their advantages in durability, flexibility, and deformability, which enable them to adapt to unstructured environments and perform various complex tasks. Perception is crucial for soft robots. To better mimic biological systems, sensors need to be integrated into soft robotic systems to obtain both proprioceptive and external perception for effective usage. This review summarizes the latest advancements in flexible sensing feedback technologies for soft robotic applications. It begins with an introduction to the development of various flexible sensors for soft robots, followed by an in‐depth exploration of smart materials and advanced manufacturing methods. A detailed description of flexible sensing modalities and methodologies is also included in the review to illustrate the continuous breakthrough of the technology. In addition, the applications of soft robots based on these advanced sensing technologies are concluded as well. The challenges of flexible sensing technologies for soft robots and promising…

Abstract The multiscale structural engineering strategy presents a powerful method for tailoring the structural attributes of materials at various levels, enabling the flexible control and manipulation of their electromagnetic properties. Nonetheless, orchestrating the multiscale architecture of polymer‐derived carbon aerogels specifically for microwave absorption poses significant challenges. Herein, aramid‐derived hard carbon nanofiber aerogel microspheres (CNFAMs) featuring a hierarchical skin‐core structure are fabricated through a wet‐spinning technique, combined with reprotonation‐mediated self‐assembly and carbonization processes. The presence of large‐scale voids between neighboring microspheres and the microscale porosity within the microspheres themselves improves impedance matching and promotes microwave reflection and scattering. The distinct graphitic domains and defects serve as pivotal elements for conduction and polarization losses, significantly impacting microwave attenuation. By meticulously tailoring the macroscale dimensions, microscale porous architecture, and…

Abstract Hard carbon (HC) has been widely regarded as the most promising anode material for sodium‐ion batteries (SIBs) due to its decent capacity and low cost. However, the poor initial Coulombic efficiency (ICE) of HC seriously hinders its practical application in SIBs. Herein, pyridinic N‐doped hard carbon polyhedra with easily accessible carbonyl groups and in situ coupled carbon nanotubes are rationally synthesized via a facile pretreated zeolitic imidazolate framework (ZIFs)‐carbonization strategy. The comprehensive ex/in situ techniques combined with theoretical calculations reveal that the synergy of pyridinic‐N and carbonyl groups promoted by the pretreatment and carbonization process would not only optimize the Na+ adsorption energy but also accelerate the desorption of Na+, significantly suppressing the irreversible capacity loss. As a result, the as‐synthesized hard carbon polyhedra as an anode can deliver an unprecedented high ICE of 98% with a large reversible capacity of 389.4 mAh g−1 at 0.03 A g−1. This work may provide an effective strategy for the structural design…

Abstract Quasi‐solid aqueous zinc ion batteries (AZIBs) based on flexible hydrogel electrolytes are promising substitutions of lithium‐ion batteries owing to their intrinsic safety, low cost, eco‐friendliness and wearability. However, it remains a challenge to lower the freezing point without sacrificing the fundamental advantages of hydrogel electrolytes such as conductivity and mechanical properties. Herein, an all‐around hydrogel electrolyte is constructed through a convenient energy dissipation strategy via the rapid and reversible intramolecular/intermolecular ligand exchanges between Zn 2+ and alterdentate ligands. The as‐obtained hydrogel exhibits excellent mechanical properties, fatigue resistance, high Zn‐ion conductivity (38.2 mS cm −1 ), good adhesion (19.1 kPa), and ultra‐low freezing point (−97 °C). Due to the alterdentate ligands help to improve the zinc ion solvation structure and guide uniform Zn deposition, the Zn||Zn symmetric cells show stable plating/stripping behavior and long‐term cycle stability. The Zn||V 2 O 5 full cells exhibit large capacity of 230.6 mAh g…

Abstract The use of materials from renewable sources instead of fossil fuels is a crucial step forward in the industrial transition toward sustainability. Among polysaccharides, alginate stands out as a versatile and eco‐friendly candidate due to its ability to form functional complexes with cations. This review provides an up‐to‐date and comprehensive description of alginate complexation with specific cations, focusing on how interaction forces can be harnessed to tailor the physicochemical properties of cation‐alginate‐based functional materials. Methodologies and approaches for the development and multiscale characterization of these materials are introduced and discussed. Alginate complexes with mono‐, di‐, tri‐, and tetravalent cations (namely Ag + , Mg 2+ , Ca 2+ , Sr 2+ , Ba 2+ , Mn 2+ , Co 2+ , Ni 2+ , Cu 2+ , Zn 2+ , Cd 2+ , Pb 2+ , UO 2 2+ , Cr 3+ , Fe 3+ , Al 3+ , Ga 3+ , Y 3+ , La 3+ , Ce 3+ , Nd 3+ , Eu 3+ , Tb 3+ , Gd 3+ , Zr 4+ , Th 4+ ) are reviewed. Each cation is discussed individually, highlighting how it can uniquely influence the material properties thereby…

Abstract Electrocatalytic nitrate reduction reaction (NO 3 RR) driven by renewable energy is a promising technology for the removal of nitrate‐containing wastewater. However, the sluggish kinetics resulted from the complex proton‐coupled electron transfer and various intermediates remain the key barriers for large‐scale application of NO 3 RR. Herein, a tactic is reported to raise rate of NO 3 RR and increase selectivity to N 2 using bimetal catalyst: Co is inclined to act on the key steps needed in NO 3 RR process, rate‐determining step (RDS: *NO 3 to *NO 2 , the asterisk means intermediates) and the subsequent *N hydrogenation as well as Fe exhibits the efficient activity for the selectivity‐ determining step (SDS: *NO to *N then to N 2 ) via a relay catalysis mechanism. A removal efficiency of 78.5% and an ultra‐long cycle stability of 60 cycles (12 h per cycle) are achieved on FeCo alloy confined with nitrogen‐doped porous carbon nanofibers (FeCo‐NPCNFs). DFT calculations unveil that the introduction of Co active site not only regulates the d‐band center of FeCo alloy, optimizes…

Abstract High mechanical strength, excellent toughness, low hysteresis, and robust resilience are of great importance for stretchable conductive hydrogels (CHs) to heighten their reliabilities for self‐powered sensing applications. However, it still remains challenging to simultaneously obtain the mutually exclusive performances. Herein, an intrinsically conductive and adhesive hydrogel is fabricated by one‐step radical polymerization of acrylamide (AAm), three hydroxy groups together clustered‐N‐[tris(hydroxymethyl)methyl]acrylamide (THMA), and cationic 1‐Butyl‐3‐Vinylimidazolium Bromide (ILs) dissolved in core‐shell structurally dispersed PEDOT:PSS (PP) solution. Owing to abundant clustered hydrogen bonds, electrostatic interactions between PILs chains and anionic PSS shells, and polymer chain entanglements, the CHs feature superior mechanical properties with a high tensile strength (0.25 MPa), fracture strain (1015%), fracture toughness (1.22 MJ m ‐3 ), fracture energy of 36.5 kJ m ‐2 and extremely low hysteresis (5%), and display excellent resilience and fatigue resistance. As a…

Abstract Conductive hydrogels are gaining significant attention as promising candidates for the fabrication materials for flexible electronics. Nevertheless, improving the tensile properties, hysteresis, durability, adhesion, and electrochemical properties of these hydrogels remains challenging. This work reports the development of a novel semi‐interpenetrating network poly(ionic liquid) hydrogel named PATV, via the in situ polymerization of acrylamide, N ‐[Tris(hydroxymethyl)methyl] acrylamide, and 1‐vinyl‐3‐butylimidazolium tetrafluoroborate. The density functional theory calculations reveal that the poly(ionic liquid) in the hydrogel network acts as physical cross–linking points to construct hydrogen‐bond networks. Furthermore, the hydrogen‐bond networks dissipate energy efficiently and quickly, and thus stress concentration and hysteresis are avoided. The prepared hydrogel has a low hysteresis (9%), high tensile properties (900%), fast response (180 ms), high sensitivity (gauge factor = 10.4, pressure sensitivity = 0.14 kPa −1 ), and wide sensing range (tensile range: 1–600%,…

Abstract Organic room‐temperature phosphorescence (RTP) materials are actively explored as attractive candidates for optoelectronic and bioelectronics applications given their unique long‐lived excited‐state features and inherent merits of low‐cost, appreciable functionality, and good biocompatibility. In recent years, many efforts in molecular design and aggregation modulation are devoted to achiev efficient RTP from organics, among which an emerging strategy focuses on confining chromophores within polymer matrices. Polymers possess intertwined chains making them a good platform to restrain the nonradiative decays and quenching, allowing the triplet excitons to survive a long time enough for emission at room temperature. Progress relating to polymer‐based organic RTP materials is highlighted as a new creative subject in the field. This review outlines recent advancements in polymer‐based organic RTP materials. The fundamental mechanism of organic RTP is first presented. Thereafter, design considerations and strategies to construct polymer‐based organic RTP materials are summarized…

Abstract The “Nobel Prize in Chemistry 2023” is awarded to Moungi G. Bawendi, Louis E. Brus, and Alexey I. Yekimov for discovering and synthesizing Quantum Dots (QDs). Colloidal QDs possess fascinating size‐, morphological‐, composition‐, and assembly‐tunable electronic and optical properties, which makes them star materials for various optoelectronic applications, especially as luminescent materials for next‐generation wide color gamut ultra‐high‐definition displays. Perovskite QDs (PQDs) have gained widespread attention in recent years. In less than ten years, research on perovskite‐related materials and devices has basically been perfected in terms of quantum yield and external quantum efficiency (EQE). However, on the eve of its industrial application, some key technical indicators and technical processes need to be met and resolved. The development and transformation of QD materials and then focuses on the progress of luminescence linewidth and EQE of the PQD light‐emitting diode. Finally, several application avenues are reviewed for PQDs, and some challenges and opportunities…

Abstract Chronic diabetic wound repair is a global medical challenge. Developing a hydrogel dressing to effectively promote angiogenesis and detect wound state in diabetic wound management is an unmet medical requirement. Herein, a facile and efficient strategy to prepare self‐healing hydrogel with enhanced angiogenesis and real‐time monitoring for diabetic wounds is presented, by cross‐linking carboxymethyl cellulose (CMC) with precoordinated europium‐ethylenediaminetetraacetic acid (Eu‐EDTA) complexes. Benefiting from the dynamic and reversible coordination interaction formation, the hydrogel exhibits remarkable injectability and self‐healing properties, thus forming efficient coverage in irregular and deep wounds with minimally invasive procedures. Furthermore, the fluorescence of the hydrogel changes linearly with pH value in the range of 4.5–7.5 and enables real‐time pH measurement to monitor the wound state. More importantly, the hydrogel can effectively promote the proliferation and migration of endothelial cells and enhance tube formation ability, demonstrating great…

Abstract Electrochemical (EC) analysis has emerged as a high‐sensitivity, reliable, cost‐effective, and rapidly evolving technique that has garnered significant attention across diverse domains. Furthermore, EC‐based techniques hold great potential for miniaturization and integration. The integration of EC techniques with diverse mode/signal (such as light, magnetic, and thermal signals, etc.) provides unique opportunities for biosensors to acquire more information through a single sensing platform. By coupling multiple signals or processing them logically, the detection accuracy can be further improved, and the probability of false positives or negatives can be minimized. In this review, a thorough analysis of multi‐ mode/signal sensors in the field of EC sensing is conducted, along with their integration with various sensing techniques (e.g., fluorescence, photothermal, colorimetry, microfluidic, etc.). The aim is to delve into the latest advances, potential applications, as well as challenges in multi‐mode/signal biosensors, where the utilization of multiple sensing modalities…

Abstract Energy‐efficient building materials are eye‐catching for reducing indoor energy consumption via eliminating electromagnetic interference and pollution, controlling the thermal transfer, and promoting sunlight harvesting and providing a comfortable living environment. To realize broadband microwave shielding, the elaborate control of microstructures has showed great potential and research direction. By composition regulation and structure design with various dimension, the synergistic effects including conductive networks, interfacial polarization, magnetic coupling, dipole polarization, and dielectric‐magnetic synergy, can significantly improve electromagnetic (EM) shielding capacity. Thermal management including thermal conversion, thermal storage, thermal radiation, and thermal conduction has enormous potential in enhancing the sustainability and energy efficiency for future buildings. Smart windows are able to switch optical transmittance and colors, which is contributed to saving building energy. Herein, in this review, the recent progress of broadband shielding,…

Abstract Metamaterials (MMs), which include phononic crystals (PCs) as a particular type, exhibit anomalous wave propagation properties through artificial design of topologies or lattice forms of unit‐cells. Recent advancements in MMs signify an ascendant research trend, providing promising design ideas and means for unprecedented wave propagation properties. The imperative for on‐demand, real‐time active control of wave propagation underscores the significance of tunable manipulation of acoustic/elastic waves, promoting the design and development of tunable MMs. Furthermore, the versatility of intelligent materials and their ongoing development and innovation contribute significantly to the emergence of diverse intelligent MMs. This comprehensive survey provides an overview of recent advancements and current research trends in the interdisciplinary field of intelligent MMs with electro‐/magneto‐mechanical couplings. The primary objective of the review is to emphasize significant progress in agile manipulation of acoustic/elastic waves in electro‐/magneto‐mechanical coupled MMs,…

Abstract Flexible pressure sensors with broad linearity range and excellent sensor‐to‐sensor uniformity have attracted unprecedented attention in the electronic skins, human–machine interfaces, and environmental monitoring. However, challenges including poor sensor‐to‐sensor uniformity owing to the randomness of the used nanomaterials or porous structures and saturated response that leads to a restricted linearity range because of structural stiffening have been yet addressed. Herein, a novel dielectric layer based on beetle‐inspired gradient slant structures (GSS) is proposed to endow capacitive pressure sensors with extensive linearity range and excellent sensor‐to‐sensor uniformity. The excellent compressibility of the GSS due to the bending deformation of the slant pillars significantly enhances sensor sensitivity. The broad linearity range comes from the compensation of contact area during sequential contact of the GSS dielectric layer from tall to low slant pillars with electrodes. The high sensor‐to‐sensor uniformity is ascribed to the excellent batch‐to‐batch consistency of…

Abstract Biomimetic electronic skins (e‐skins) are widely used in wearables, smart prosthesis and soft robotics. However, multimodal e‐skins, especially those based on hydrogels, face multiple challenges for practical applications, involving multi‐sensing signal mutual interference, low breathability and stretchability. Here, a breathable and stretchable multimodal e‐skin with a multilayer film microstructure is developed to achieve self‐calibrated sensing of any two of three stimuli: strain, temperature, and humidity, with minimal crosstalk. Hydrogel fibers with different shapes are designed for strain and temperature sensing modules, and the hydrogel film is developed as a humidity sensing module. The multimodal e‐skin exhibits impressive sensing performance, including a low strain detection limit (0.03%), strain linearity (R 2 = 0.990), high‐temperature sensitivity (1.77%/°C), and a wide humidity detection range (33–98% RH). Interestingly, due to the directional anisotropy in strain sensitivity of different shaped fibers, the e‐skin realizes self‐calibrated detection of strain…

Abstract The huge consumption of alkali during biomass‐derived porous carbon production leads to pollution and high carbon‐emission. This study employs the concept of Fenton chemistry to achieve hierarchical porous biomass carbon materials with a remarkably high specific surface area of 3440 m 2 g −1 with double activation efficiency compared to traditional activation process. The optimized carbon electrode demonstrates exceptional specific capacitance of 425.2 F g −1 at a current density of 0.1 A g −1 and great rate performance (286.1 F g −1 at 100 A g −1 ) in 6 m KOH electrolyte. The enabled supercapacitor demonstrates remarkable cycling stability, retaining up to 99.74% of its initial capacitance after undergoing 20 000 charge–discharge cycles. In addition, the electrolyte ion distribution in different pore structures is simulated using Molecular Dynamics, which confirms that the structure is conducive to the rapid diffusion of ions, thus matching the excellent electrochemical properties. The assembled symmetric supercapacitors achieve a maximum energy density of 42.1 Wh kg −1…

Abstract Silicon‐based anode has high theoretical capacity but suffers from poor electrical conductivity, large volume expansion, and unstable solid electrolyte interphase (SEI). Adding carbon nanotubes (CNTs) and carbon coatings are both very effective methods for addressing the above issues. The intrinsic sp 2 covalent structure endows CNTs with excellent electrical conductivity, mechanical strength, and chemical stability, which makes them suitable for various energy storage applications, such as in lithium‐ion batteries (LIBs). Apart from the conductive network, CNTs can serve as current collectors, mechanical probes, and mechanical frameworks, and they have potential in the construction of next‐generation battery architectures. Carbon coatings are mixed ionic‐electronic conductors with good chemical stability that provide mechanical support and mitigate the volume expansion of Si‐based materials. This review outlines the advances in CNTs and carbon coatings as conductive networks in Si‐based anodes, as well as insights into their future development. It provides an in‐depth…

Abstract Oxygen vacancy engineering is a promising strategy to enhance the electrocatalytic activities in conventional metal oxide electrocatalysts. However, the utilization of oxygen vacancies in high‐entropy oxides remains unknown, primarily due to the challenges associated with facile introduction of the oxygen vacancies and explanation of their roles in complex high‐entropy systems. Herein, the facile introduction of oxygen vacancies into high‐entropy oxides is realized and the unique high entropy‐driven role of oxygen vacancies for oxygen evolution reaction (OER) process is revealed. A low‐temperature surface carbonization–decarbonization approach is developed to introduce and regulate the oxygen vacancies in high‐entropy spinel oxides (HEOs). The oxygen vacancies in HEOs can both facilitate pre‐oxidation process for faster OH − adsorption and induce the unique bridge site pathway for easier deprotonation, distinctive in conventional oxides where oxygen vacancies favor * OH adsorption yet hinder the deprotonation. Consequently, the as‐prepared high‐entropy spinel oxides with…

Abstract Electrochemical reduction of nitrate (NO3RR) holds great promise for environmentally friendly ammonia production. Tandem catalysis is a promising strategy for boosting the NO3RR and inhibiting side effects, but it is still challenged by lacking well‐designed catalysts to drive this catalytic process. Herein, the study develops the CuCo branched nanowires (CuCo NW) catalyst, which efficiently converts NO3 − to NH3 on Co (111) and Cu (111) crystal facets through a tandem catalysis mechanism. The in situ grown CuCo NW on Cu foam demonstrates a remarkable Faraday efficiency of 90.3% at 1.0 A cm−2 and maintains stable operation for 200 h at 100 and 200 mA cm−2 in a flow reactor. Density functional theory calculations suggest that the initial absorption and subsequent deoxygenation of *NO3 on Co (111) leading to the formation of *NO2, followed by its transfer to Cu (111) and further conversion to *NH3, establish an optimal pathway by managing rate‐determining steps on individual surfaces for NO3RR. To showcase the practical application of the catalyst, the study further develops…

Abstract Solar‐driven synthesis of hydrogen peroxide (H2O2) through photocatalysis stands out as a promising avenue for sustainable energy generation, marked by environmental friendliness and industrial feasibility. However, the inherent limitations of carbon nitride (CN) in photocatalytic H2O2 production significantly impede their performance. Herein, a novel 0D/2D carbon dots‐modified CN nanosheet heterojunction (CDsMCN) is introduced, synthesized through a hydrothermal‐calcination tandem strategy induced by CDs derived from melamine. This innovative technique enhances the n→π* electronic transition in CDsMCN, accelerating the separation efficiency of electron‐hole pairs, boosting oxygen adsorption, and promoting a highly selective 2e− ORR. Comparative to pristine CN, CDs10MCN exhibited a remarkable tenfold increase in H2O2 production, reaching an impressive 1.48 mmol L−1. Furthermore, CDs10MCN demonstrates exceptional stability, maintaining its catalytic efficiency at the initial level over four consecutive cycles. The notable achievement of a molar selectivity of H2O2 ≈80% at an…

Abstract The proton exchange membrane water electrolysis system has long been considered a promising technique for the generation of hydrogen owing to its high electrolytic efficiency, reliability, and quick response to renewable energy sources. At present, noble metals and their oxides (e.g., Pt, IrO 2 , and RuO 2 ) are widely used as high active electrocatalysts for accelerating the conversion efficiency of the water electrolysis process, especially in acidic media. Nevertheless, the scarcity and instability seriously impede their large‐scale application in practice. In the past years, metal‐organic frameworks (MOFs) have proven to be an ideal platform for designing efficient and cost‐effective electrodes due to their unique physicochemical properties. In this review, the fundamental catalytic mechanisms of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in acidic media are discussed first. Then, design strategies and advanced characterizations for MOF‐based water‐splitting catalysts are summarized. Finally, the recent research advances of MOF‐based…

Abstract Currently, microbial infections have posed an arduous challenge to global public health, whereas the rise of antibiotic resistance is rendering traditional antibiotic therapies futile, prompting the development of new antimicrobial technologies. Photoactive nanomaterials have thus garnered a thriving interest for disinfection owing to their superior antibacterial efficaciousness, favorable biosafety, and rapidness and spatiotemporal precision in excreting bactericidal actions. The review summarizes recent advances and emerging trends in the design, nanoengineering, and bioapplications of photoactive antimicrobials. It commences by elaborating fundamental theories on bacterial resistance, and antibacterial mechanisms of nanomaterials and phototherapy. Subsequently, the regulation of the antibacterial effectiveness of photoactive nanomaterials is comprehensively discussed, centering on criteria and strategies for tuning photoabsorption spectra, photothermal conversion, and photocatalytic efficiency, alongside tactics for enabling synergistic therapies. This is followed by…

Abstract TiO 2 photocatalysis has gained attention as a cost‐effective way of degrading contaminants. However, it relies on UV excitation and experiences rapid carrier recombination. To address these drawbacks, novel xylan‐based carbon dots@hydrogenated TiO 2 (CDs@TiO 2‐x ) composited by direct Z‐scheme heterojunction is fabricated as a visible light‐driven photocatalytic material, which broadens the range of light absorption to visible light and suppresses the recombination of photogenerated carriers. The spindle‐shaped CDs@TiO 2‐x has C/N/O/S groups, positive charges, and oxygen vacancies on its surface, and can degrade 89% of methylene blue and 87% of methyl orange within 90 min, and 99% of rhodamine B within 60 min in visible light. It also eradicates 99.9% of E. coli in 2 h and 97.1% of S. aureus in 2.5 h. These performances surpass CDs and TiO 2‐x , and exhibit advantages in similar composite materials. The degradation pathways of dyes and the specific antibacterial processes induced by ROS are thoroughly investigated through LC‐MS testing and related enzyme activity assays.…

Abstract Photocatalytic nitrogen reduction represents a viable technology for green ammonia synthesis under mild conditions. However, the performance of the photocatalysts is typically limited by high charge carrier recombination and low adsorption and activation of nitrogen molecules. Herein, Bi/Bi 2 Sn 2 O 7 (Bi/BSO) heterojunction nanocomposites are prepared via a one‐step hydrothermal method, where NaOH etching of oxygen vacancies in the Bi─O bonds of Bi 2 Sn 2 O 7 (BSO) is exploited for the in situ formation of metallic Bi and hence Schottky junctions with the semiconducting BSO. This leads to a high separation rate of photogenerated charge carriers. Consequently, compared to the pure‐phase BSO, the Bi/BSO heterostructures exhibit markedly enhanced ammonia production, reaching an optimum rate of 284.5 µmol g −1 h −1 , where the rectifying contact between the semiconducting BSO and metallic Bi facilitates directional BSO to Bi electron transfer, leading to enrichment of photogenerated electrons at the active sites of metallic Bi. First‐principles calculations confirm the…

Abstract The rapid, energy‐efficient, scalable preparation of high‐strength, flexible, multifunctional nanostructured aerogels is highly desired yet challenging. Here, an ambient‐pressure‐dried (APD) strategy is developed involving self‐foaming, dip‐coating, and graphene oxide (GO)‐assisted multiple cross‐linking treatments for the prompt, large‐area preparation of polyurea/transition metal carbides/nitrides (MXenes) aerogels. The APD MXene‐based aerogels showcase low density, remarkable mechanical strength, and ultraflexiblity involving stretchability, good conductivity, hydrophobicity, and high resistance to various solvents. Synergies of robust, elastic cell walls and porous structure contribute to high‐efficiency absorption of high‐frequency, high‐speed mechanical shock waves for the aerogels, significantly transcendinging the biomasses, plastics, elastomers, ceramics, and metals. In addition to the excellent microwave shielding performance of over 40 dB in ultrabroadband frequencies of 4–40 GHz, the oxidation stability is elevated for APD MXene aerogels, consequently yielding…

Rechargeable lithium-ion batteries (LIBs), commercially pioneered by SONY 33 years ago, have emerged as the preferred power source for portable electric devices, electric vehicles (EVs), and LIBs-based grid storage systems.This preference is attributed to their exceptional characteristics, including high electromotive force, lightweight design, and impressive energy density.LIBs are now even being explored for potential use in electric flight applications.Over several decades, significant progress has been made in developing mature electrode materials and cell architectures, such as olivine LiFePO 4 , layered oxides, Li-rich Mnbased materials, and graphite anodes.Generally, there remains an urgent need to continuously reduce costs, enhance safety measures, and increase energy density associated with LIBs.This demand is particularly crucial in the EVs market, where lower costs and greater energy density are required to extend the travel distance.Thus far, Li(Ni,Mn,Co)O 2 (NMC) and Li(Ni,Mn,Co)O 2 (NCA) compounds have been extensively studied and identified as promising cathode…

Abstract Inverted perovskite solar cells (IPSCs) have attracted unprecedented attention due to their negligible hysteresis, long‐term operational stability, low temperature, and cost‐effective fabrication process, as well as wide applications. The power conversion efficiency (PCE) of IPSCs has skyrocketed from 3.9% in 2013 to certified 26.1% in 2023, which is over the certified 25.8% of regular counterpart, benefiting from the emergence of a great number of organic hole‐transporting materials (HTM). This review provides an overview of the recent development of organic hole‐transporting materials in the efficiency and stability of IPSCs, including organic small molecules and conjugated conductive polymers. The effective strategies for the charge‐transport layer and perovskite films of IPSCs are also discussed. Finally, the prospective for further development of IPSCs is outlined, including developing novel hole‐transporting materials and fabricating techniques to meet the requirements of commercial application.

Abstract The use of all‐solid‐state lithium metal batteries (ASSLMBs) has garnered significant attention as a promising solution for advanced energy storage systems. By employing non‐flammable solid electrolytes in ASSLMBs, their safety profile is enhanced, and the use of lithium metal as the anode allows for higher energy density compared to traditional lithium‐ion batteries. To fully realize the potential of ASSLMBs, solid‐state electrolytes (SSEs) must meet several requirements. These include high ionic conductivity and Li+ transference number, smooth interfacial contact between SSEs and electrodes, low manufacturing cost, excellent electrochemical stability, and effective suppression of dendrite formation. This paper delves into the essential requirements of SSEs to enable the successful implementation of ASSLMBs. Additionally, the representative state‐of‐the‐art examples of SSEs developed in the past 5 years, showcasing the latest advancements in SSE materials and highlighting their unique properties are discussed. Finally, the paper provides an outlook on achieving balanced…

Abstract Stimuli‐responsive polymers have received increasing attention for various applications due to their ability to adapt physical and chemical properties in response to external environmental stimuli. In this regard, poly(N‐isopropylacrylamide) (PNIPAM) is the most extensively studied stimuli‐responsive polymer and, consequently has been prominently featured in (bio)‐sensor development, adaptive coating technology, drug delivery, wound healing, tissue regeneration, artificial actuator design, sensor technology, responsive coatings, and soft robotics. This success can be mainly attributed to the accessible and versatile nature of the PNIPAM platform, thus allowing the synthesis of a wide variety of copolymer architectures, topologies and compositions. Within this review, the structural and compositional features of PNIPAM‐based materials in sensor and biosensor applications are discussed with a focus on the literature from 2016 until now. The reader is provided with the current state of the art regarding PNIPAM‐based sensor development and their molecular design. Finally, the…

Abstract The proactive exploration of electrocatalytic conversion for renewable energy valorization is of tremendous significance in addressing the issues of fossil energy exhaustion, among which the critical challenge of electrocatalysis lies in the rational design of efficient electrocatalysts that are rich in the earth. Among electrocatalysts, the design of heterostructured materials exhibits immense potential for the optimization of noble metals and elaboration of non‐precious metal electrocatalysts with durability. In this review, a systematic overview of modern advances in heterostructured electrocatalysts for a range of energy conversion reactions is described, and special interfacial design brings additional functional effects. Subsequently, various synthesis methods and characterization techniques for heterostructured electrocatalysts are also summarized. The innovative classification of heterostructures in methods of interfacial junction, crystal structure, structural morphology, and properties of the components is presented in this review. Finally, the possible challenges…

Abstract Photocatalytic hydrogen evolution reaction (HER) is a very promising and sustainable technology, yet precisely exploring effective HER photocatalysts remains a critical challenge due to the rapid charge recombination. In this work, a brand‐new S‐scheme heterojunction is successfully designed and constructed by in situ growth of twinned Zn0.5Cd0.5S Solid Solution (CZS) on a novel fluorenone‐based covalent triazine framework (FOCTF). The S‐scheme heterojunctions is identified via in situ irradiation XPS, and electron spin resonance, which can greatly improve the photocatalytic HER rate and stability. Under illumination, the highest photocatalytic HER rate of well‐designed CZS‐FOCTF is 247.62 mmolg−1h−1, 3.83 times as high as that of pure CZS. Experimental and theoretical investigations corroborate that the new FOCTF has a well‐matched staggered band alignment and work function difference with CZS. The as‐fabricated CZS‐FOCTF S‐scheme heterojunction can establish a favorable internal electric field, which accelerates the directional S‐scheme charge migration, thereby enhancing…

Abstract Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) is a widely used lithium (Li) salt that is extensively studied in the field of electrolytes for Li‐ion batteries (LIBs) to improve their performance. A thorough understanding of its underlying mechanisms in LIBs is crucial for gaining deeper insights into its future development. This paper provides an extensive review of the role of LiTFSI in enhancing battery performance, including its benefits for negative electrode protection, the facilitation of fast charging capabilities, and the promotion of battery operation across a wide temperature range. It also highlights the specific drawbacks of LiTFSI in the electrolyte domain and examines potential solutions. By leveraging the unique properties of LiTFSI, the strategies for its effective utilization in current research are outlined. Finally, the paper discusses the lack of research into the mechanism of LiTFSI in interface protection, particularly the evolution mechanisms of multi‐component Li salts at the positive and negative electrode interfaces, and it reasonably…

Abstract Rechargeable aqueous zinc‐ion batteries (ZIBs) with low cost and high safety arouse most promises as next‐generation energy storage configurations. Yet the heterogeneous electric field distributions and interfacial side reactions are considered stumbling roadblocks toward the commercialization of ZIBs. Here, these challenges via cationic electrostatic shielding and anionic preferential adsorption by sodium gluconate (SG) additive are addressed. The polar functional groups (─COO − ) of SG anions preferentially anchor to the Zn anode, which can alter Zn 2+ migration pathways and restrain side reactions. Moreover, as per the smaller effective reduction potential, the separated cations (Na + ) from SG serve as a dynamic armor to provide strong electrostatic shielding effect for uniform Zn 2+ deposition on the [002] crystal plane, radically eliminating Zn dendrite growth and promoting anti‐corrosion behaviors of Zn. Consequently, the Zn//Zn symmetric cell with modified electrolyte confers a lifespan of up to 600 h at a high 80% depth of discharge. Furthermore, even under a…

Abstract Ti, V, Cr, Mn, Co, and Cu, have been investigated as a third dopant in NiFe sulfide for enhanced oxygen evolution reaction (OER)/oxygen reduction reaction (ORR). The effects of dopant on surface electronic structure, conductivity, and thermodynamic barrier of reaction are addressed and discussed. For the OER, X‐ray photoelectron spectroscopy analysis shows that electron transferring from the Ni to the dopants enhances the catalytic performance of the sulfide. Cu doped NiFe sulfide exhibits the best OER performance. For the ORR, density functional theory calculation indicates that Ti, V, Mn, Co, and Cu upshift the d‐band center (ɛ d ), while Cr downshifts the ɛ d . Among the dopants, V leads to optimized electronic structure modification, giving optimized adsorption energy of *O on the Ni, the lowest rate determining step ΔG 1 , and the best ORR activity. By considering E 10 ‐E 1/2 together with the maximum current density of the OER and limited diffusion current density of the ORR, NiFeVS exhibits the best OER/ORR bifunctionality. The performance of NiFeVS as a cathodic…

Abstract Owing to zinc dendrites and parasitic reactions, aqueous Zn‐metal batteries often suffer from poor reversibility and cyclability. Electrolyte additives present a promising strategy to improve Zn anode stability. However, the ever‐evolving perspectives and mechanisms, paradoxically, complicate battery design, causing a scenario where any electrolyte additive seems to be effective. Herein, it is taken ionic liquid (IL) additives as an example and detailed explored the impact of three typical IL anions, namely OTF − , TFA − , and BF 4 − . It is identified that the primary determinant of electrolyte additives as their electrical double layer (EDL) structures and their subsequent solid‐electrolyte interface (SEI) composition. An advantageous EDL structure, akin to an ion‐shield, can reduce the absorption of H 2 O molecules, which further enrich the SEI with zincophilic and hydrophobic components, thereby mitigating parasitic reactions and Zn dendrite formation. As a result, the Zn||Zn cell with optimal [EMIM]OTF additives demonstrates an exceptional cycling life under…

Abstract Transition metal sulfides as anode materials for sodium‐ion batteries (SIBs) have the advantage of high capacity. However, their cycle‐life and rate performance at ultra‐high current density is still a thorny issue that limit the applicability of these materials. In this paper, the carbon‐embedded heterojunction with sulfur‐vacancies regulated by ultrafine bimetallic sulfides (vacancy‐CoS 2 /FeS 2 @C) with robust interfacial C‐S‐Co/Fe chemical bonds is successfully synthesized and explored as an anode material for sodium‐ion battery. By changing the ratio of two metal cations, the concentration of anion sulfur vacancies can be in‐situ adjusted without additional post‐treatment. The as‐prepared vacancy‐CoS 2 /FeS 2 @C anode material offers ultrahigh rate performance (285.1 mAh g −1 at 200 A g −1 ), and excellent long‐cycle stability (389.2 mAh g −1 at 40 A g −1 after 10000 cycles), outperforming all reported transition metal sulfides‐based anode materials for SIBs. Both in‐situ and ex‐situ characterizations provide strong evidence for the evolution mechanism of the phases…

Abstract Rapid capacity fading and structural collapse, along with other deep‐rooted challenges in the high‐voltage region, are insufficient to meet the requirements for commercial applications of O3‐type layered cathodes. Hereby, rare earth metal (RE) within the IIIB group are utilized as the robust dopants for O3‐NaNi 1/3 Fe 1/3 Mn 1/3 O 2 (NFM) to achieve the purpose of reconstructing the crystal lattice and regulating the interlayer structure. The inactive RE 3+ acts as a pillar, reinforces the TMO 6 octahedron, and broadens the Na + diffusion layer in the configuration of O‐Na‐O‐TM (RE)‐O‐Na‐O, giving rise to the enhanced crystal stability and accelerating the transmission of sodium ions. More impressively, the scandium incorporation is working as a “vitamin” that improves Ni/Fe redox reversibility, alleviating the irreversible P3‐O3’‐P3’ phase transformation and further restraining the disordered Fe migration into the neighboring Na layer, which is firmly validated by in situ X‐ray diffraction coupled with the synchrotron X‐ray absorption spectroscopy. Consequently, the…

Abstract High mechanical strength, toughness, and fatigue resistance are essential to improve the reliability of conductive hydrogels for self‐powered sensing. However, achieving mutually exclusive properties simultaneously remains challenging. Hence, a novel directed interlocking strategy based on topological network structure and mechanical training is proposed to construct tough hydrogels by optimizing the network structure and modulating the orientation of molecular chains. Combining Zn 2+ crosslinked cellulose nanofibers (CNFs) and a polyacrylamide‐poly(vinyl alcohol) double‐network, the unique interlocked‐network structure exhibits an enhanced toughening effect due to hydrogen bonding and metal‐ligand interactions. The aligned nanocrystalline domains achieved by training further contribute to an increase in the toughness and fatigue thresholds. This innovative approach synergistically enhances the mechanical properties of the nano‐conductive hydrogel, achieving a maximum tensile strength of 4.98 MPa and a toughness of 48 MJ m −3 . Notably, the CNFs template with anchored…

Abstract Aqueous zinc‐ion batteries are promising for next‐generation energy storage systems. However, the zinc dendrite growth, corrosion, and hydrogen evolution reaction at the electrochemical interface severely impede their further development. Herein, a Zn2+‐rich and H2O‐poor Helmholtz plane is constructed to regulate the electrochemical interface between the zinc anode and the electrolyte. Electrochemical and in situ spectroscopy characterizations reveal that the designed electric double layer with abundant Zn2+ coordination sites and less H2O content can facilitate rapid electron transfer, homogenize Zn2+ deposition, and alleviate the side reactions induced by active H2O. Benefiting from the high reversibility and stability of zinc anode, the Zn||Zn symmetric cell can be cycled over 1000 h at 1 mA cm−2 and the Zn||NH4V4O10 full cell can maintain a capacity of 85.23% for 1000 cycles at 3 A g−1. This work aims at Helmholtz plane reconfiguration and provides a realizable strategy in interface construction for other similar systems.

Abstract The capacitive properties of supercapacitors highly rely on the reasonable design of high‐performance electrode materials. Herein, a synergetic strategy of pre‐oxidation and pre‐carbonization is proposed to prepare coal tar pitch (CTP) based porous carbon. The formation mechanism of porous carbon is revealed. Pre‐oxidation increases the heteroatom content and promotes the decomposition of polycyclic aromatic hydrocarbons into small molecules, which is more conducive to improving the subsequent activation and enhancing the microporous specific surface area. Also, the autoclave pre‐carbonization promotes the polymerization of the precursors and increases the carbon yield. Benefiting from the synergistic effect of pre‐oxidation and pre‐carbonation, the obtained carbon exhibits a superior specific capacitance of 365 F g −1 . Meanwhile, ZnCl 2 is used as a hydrogen‐bonding acceptor to synthesize ZnCl 2 ‐EG/PVA deep eutectic solvent (DES) gel, and it is applicable to acidic, neutral, and alkaline electrolytes. The capacitor assembled with the prepared porous carbon and DES gel…

Abstract Diabetic wounds are difficult to heal, and the key to wound healing is exudate management and effective disinfection. Inspired by the asymmetric wettability of Janus‐structured lotus leaves, herein the study has presented the design of a biomimetic asymmetric Janus membrane that integrates unidirectional biofluid drainage and photothermal‐enhanced evaporation/sterilization capabilities for accelerating diabetic wound healing. This Janus membrane is prepared by electrospinning polyacrylonitrile (PAN) nanofiber membrane containing polydopamine (PDA) on the surface of polypropylene (PP) nonwoven membrane. Such PP/PANx%PDA Janus membrane enables antigravity “pumping” of the water from the hydrophobic PP layer to the hydrophilic PANx%PDA layer within 22 s through contact points on the Janus interface. The incorporation of 30 wt% PDA in PAN imparts high photoabsorption and photothermal responsiveness, facilitating continuous volatilization of the exudate, achieving twice the displacement of water, and causing irreversible damage to bacteria. As a result, it effectively alleviates…

Abstract The development of efficient photocatalysts is a mainstay for the advancement of photocatalytic technology. Heterojunction photocatalysts can overcome the inherent limitations of single photocatalysts, integrating the advantages of each component, and achieving efficient separation of photogenerated charges, making them a research focus in the field of photocatalysis. The role of point defects in photocatalytic reactions is diverse and can significantly influence the performance of photocatalysts. This review comprehensively summarizes the latest advancements in point defect engineering for the modulation of heterojunction photocatalysts. First, the types of point defects and their impact on photocatalytic processes are introduced. Subsequently, the common types of heterojunction photocatalysts are presented. Then, in accordance with recent research progress, the regulatory mechanisms of point defects within heterojunction photocatalysts are outlined, with a particular focus on their functions on surface/interfacial properties and photogenerated charge transfer processes.…

Abstract The creation of functional hydrogels with robust load‐bearing capacity adaptable to complex tissue regeneration remains challenging. Silk fibroin (SF) is a natural biomaterial with excellent mechanical strength and cell adhesion capacity, possessing tremendous potential to solve the aforementioned dilemma. The excellent biodegradability and biocompatibility and the molecular structure with multiple modifiable moieties provide opportunities for the injectability and multifunctionality of hydrogels. Furthermore, the incorporation of other polymers or active ingredients can improve the basic properties, confer biological activities and pharmacological effects, and provide the prerequisites for hydrogels to fulfill specific requirements. Therefore, SF‐based hydrogels are widely applied in tissue repair and regeneration, especially in bone, skin, nerve, liver, myocardium, and cornea, which have effectively addressed the challenges of scaffolds' lack of cell adhesion sites, excessive degradation, as well as the lack of efficient, long‐lasting antimicrobial properties. This review…

Abstract Rechargeable aqueous zinc‐ion batteries (AZIBs) are one of the most promising post‐lithium battery technologies due to their low cost, high safety, and environmental friendliness. However, their practical development is hindered by the issues of Zn metal anodes, including dendrite growth, passivation, hydrogen evolution and other side reactions. Herein, to circumvent these issues, a facile and universal alloy electrodeposition strategy is proposed to construct a 3D structured ternary Zn alloy artificial interphase layer on Zn foil as an anode for high‐performance AZIBs. The density functional theory (DFT) theoretical calculations, in situ optical visualization and spectroscopic results validate that the zincophilic Zn─Sn─Bi@Zn ternary alloy anode with lower migration energy barrier and weak hydrogen adsorption sites can promote the uniform Zn deposition and suppress hydrogen evolution reactions. The Zn─Sn─Bi@Zn//NH 4 V 4 O 10 full cell demonstrates a high specific capacity 110.4 mAh g −1 even after 10 000 cycles at 5.0 A g −1 . Notably, the full cell with a high NH 4 V 4 O…

Abstract Ultra‐wideband microwave absorbing (MA) materials covering the low‐frequency range (2–6 GHz) are highly desirable in civil and military fields. These materials can be fabricated based on the design of electromagnetic meta‐structure. Herein, a structural‐functional‐integrated ultra‐wideband SiO 2 fiber reinforced cyanate ester (CE) MA composite based on an in situ‐grown graphene meta‐nanointerface layer (GrMI) (SiO 2f /GrMI/CE) is reported. The relationship between the periodic structure of the graphene nano‐interface layer and the MA performance is discussed through experiments and simulations. The results show that SiO 2f /GrMI/CE with a thickness of 8.78 mm exhibits an effective absorption bandwidth of 15.46 GHz (2.54–18 GHz). Remarkably, the reflection loss remains basically unchanged upon increasing the incident angle from 5° to 50°. Additionally, GrMI is an effective load‐bearing constituent, which increases the interfacial shear stress between SiO 2f and the CE by ≈210% and contributes to achieving composites with an ultra‐high flexural strength (552.7 MPa). The…

Abstract Diabetic foot ulcers (DFUs), a serious and increasingly common chronic issue among diabetics, often do not respond well to generalized treatment strategies. Hypoxia and the overexpression of reactive oxygen species (ROS), resulting in inflammatory dysregulation and subsequent imbalance in macrophage phenotypes, are critical factors contributing to the prolonged non‐healing of DFU wounds. These two issues often interact in a continuous, problematic cycle. Presently, there is a lack of comprehensive strategies aimed at addressing both of these factors simultaneously to interrupt this detrimental cycle. Herein, an immunomodulatory hydrogel (PHG2) is developed for reshaping the hostile DFU microenvironment. The engineered PHG2 not only removes excess internally‐produced ROS but also generates O 2 , with its efficiency further boosted by local hyperthermia (42.5 °C) activated by near‐infrared light. Through both in vitro and in vivo studies, along with transcriptomic assessment, it is confirmed that PHG2 disrupts the detrimental feedback loop between ROS and inflammation while…

Abstract Electrolyte regulation in Zn‐based aqueous batteries (ZABs) has been extensively reported, and a broad range of strategies has been proposed. However, there is currently a lack of systematic summaries and a comprehensive understanding of the impact of hydrogen bond (H‐bond) networks on electrolyte performance. This work presents the electrolyte structure model, encompassing solvation structure, electrolyte/Zn anode interface, and H‐bond network. Through emphasizing and summarizing the reconstruction, strengthening, and breaking of the H‐bond network within the electrolyte structure, various specific regulation strategies are identified, such as high Gutmann donor number solvent, organic co‐solvent, molecular crowding additives, structure‐breaking ions, and solid‐state design. A critical appraisal is then provided on the key performance metrics influenced by these regulation methods, including Coulomb efficiency, voltage hysteresis, freezing point, and lifespan. This work is expected to illustrate electrolyte structure design to improve the comprehensive performance of ZABs.…

Abstract For the development of electrolyte additives as an effective strategy to improve the performance of zinc‐ion batteries (ZIBs), most researchers focus on the functional groups but overlook the crucial molecular configuration. Herein, six stereoisomers of 2,3,4,5‐tetrahydroxyvaleraldehyde with identical groups but various spatial arrangements are studied as the electrolyte additive in ZIBs. Based on the experimental analysis and theoretical calculations, the adsorption with Zn (002) plane is found to be an important dominant for the stereoisomer to enhance the Zn anode performance. Among these stereoisomers, D‐Arabinose with preferential and strongest chemisorption effect modifies the anode/electrolyte interface most effectively, leading to the highest stability and reversibility of the Zn anode. The adsorbed D‐Arabinose shows multifunctional effects at the interface, which not only regulates the Zn 2+ solvation structure and reconfigures the hydrogen bond framework, but also facilitates uniform Zn 2+ deposition by promoting 3D Zn 2+ diffusion and homogenizing the electric…

Abstract The effectuation of pH‐universal electrocatalysis is highly attractive but still challenging for the hydrogen evolution reaction (HER). It appeals for not only the facilitated electron transport but also the kinetical proton mass transfer. In this study, a via‐hole Ru/MoO 2 confined heterostructure is profiled as a metal‐support platform for the electron/mass transfer‐boosted pH‐universal HER studies. It is indicated that the as‐formed Ru─O─Mo bridge can modulate the electronic transport at the interface, and the proton adsorption and transfer are kinetically derived by the intensified metallic Ru─Ru bond. Resultantly, the Ru/MoO 2 heterostructure stably attains the Pt‐beyond HER activity with an ultralow overpotential of 9.2 mV at 10 mA cm −2 in 1 m KOH, and also achieves the competitive HER activity and stability in the acidic/neutral electrolytes. Both the experimental and computational results reveal the accelerated HER kinetics is attributable to the intensive mass transfer through the interfacial Ru→MoO 2 hydrogen spillover effect. This work opens up the opportunities…

Abstract Water‐based secondary batteries with multivalent metals anode provide a promising option for energy storage with low cost and high security. However, the electrochemical performance of aqueous Zinc ion batteries (AZIBs) is mainly restricted by problems such as poor reversibility and hydrogen evolution. Herein, an “amphoteric polymer strategy” with buffer‐adsorption mechanism for AZIBs is proposed by introducing poly‐L‐Glutamic Acid (PGA) into the electrolyte. Amphoteric polymer enriched functional carboxyl and amino groups confer high compatibility of the Zn metal anodes as well as the relative stability of the bulk electrolyte pH simultaneously. Partial PGA molecules distributed in bulk electrolyte dynamically dissociate to stabilize pH and correspondingly slow down the generation of inert components, while others specifically adsorbed on zinc foil can relieve electrochemical corrosion and induce dendrite‐free uniform Zn deposition. Consequently, long‐term cycling stability (>1650 h) and high levels of reversibility (Coulombic efficiency>99.5%) of Zn anode are harvested in…

Abstract Hydrogel‐based sensing devices show potential in wearable electronics. However, most hydrogels are mechanically weak, bringing functional stability problems in real usage environment that may interact with occasionally external forces. There are demands to develop robust hydrogel‐based devices with good performances. Here, a highly sensitive temperature sensor with robust, ionic conductive, and double cross‐linked polyacrylamide‐sodium alginate hydrogel is developed. It is found that ions with larger radius show higher sensitivity to temperature changes (e.g., Ba 2+ ) in the hydrogel, because ion movement is dependent with ion sizes. The sensor shows advantages of fast response (2.02 s of 40 °C temperature difference), wide sensing range (22–100 °C), and high robustness (withstanding 2000 cyclic compression and 175 N m −1 for 180° anti‐peeling test). The wearable sensor can effectively distinguish the temperatures of various body parts (0.9 °C temperature difference) and monitor respiration (0.5 °C temperature difference) in real‐time. A wearable 5×5 sensing array is…

Abstract Electromagnetic interference (EMI) shielding composites with both thermal response/management functions and message transfer/encryption behavior are ideal for use in fields such as aerospace, construction engineering, and military equipment. In this work, a self‐cross‐linking supramolecular solid–solid phase change polyethylene glycol (ScPEG) coating is prepared based on multiple hydrogen bonds, which is used for encapsulating glass fiber fabric (GFF) modified with silver nanowires (AgNWs). The solid–solid phase change coating is obtained through the hydrolysis‐condensation of PEG with a reactive silanol end group. Polyethylene glycol molecular chains can store and release heat by switching between the crystalline and amorphous state. The silanol groups can form supramolecular networks through the physical cross‐linking of multiple hydrogen bonds, resulting in an excellent thermal stability. In particular, hydrogen bonds between ScPEG and AgNW‐modified GFF (A‐GFF) enhance interfacial interactions, and the resulting robust structure enables an efficient stress transfer.…

Abstract The electrochemical reduction of nitrate to ammonia (NO3RR) has emerged as a promising but challenging orientation in sustainable development. Cu is one of the most effective NO3RR catalysts. However, the accumulation of NO2− on their surface has erected bars to the further improvement of NO3RR efficiency. Herein, Cu‐based electrocatalyst with low‐coordinated Cu atoms (Cu‐LC) is synthesized via the instantaneous ablation and rapid cooling of the Cu target by pulse laser and proposed as a new NO3RR electrocatalyst, which exhibits enhanced NO3RR activity with NH3 selectivity of 97.01%, yield rate of 0.624 mmol h−1 cm−2 at −0.8 V versus RHE and long‐term durability, superior to most reported Cu‐based catalysts. The introduction of low‐coordinated Cu sites upshifts the Cu d‐band center to near the Fermi Level, enhancing the adsorption of key intermediates (*NO2, *NO) in NO3RR, and also effectively regulating the generation of *NO2 and hydrogenation process, inhibiting the accumulation of NO2− on the Cu‐LC surface, thus achieving efficient NH3 production. Furthermore, when…

Abstract Highly luminescent carbon dots (CDs) have garnered significant attention and are increasingly utilized in various fields. Despite its importance, there has been a lack of comprehensive reviews focusing specifically on highly luminescent CDs. It is aimed here to fill that gap by exploring CDs with high photoluminescence quantum yield (PLQY), starting with an examination of the luminescent mechanisms underlying highly luminescent CDs. The selection of synthetic raw materials and preparation methods along with the research progress are reviewed and the information on highly luminescent CDs across various luminescent bands is then statistically summarized in several tables. Subsequently, the structural features, synthesis methods, and purification strategies that lead to high PLQY in CDs are summarized based on analyzing collected examples of highly luminescent CDs. Furthermore, the highly luminescent‐based multifunctional applications of CDs in bioimaging, light‐emitting diodes, luminescent solar concentrators, and lasers are introduced. Finally, the current research landscape…

Abstract The exploitation of highly activity oxygen evolution reaction (OER) electrocatalysts is critical for the application of electrocatalytic water splitting. Triggering the lattice oxygen mechanism (LOM) is expected to provide a promising pathway to overcome the sluggish OER kinetics, however, effectively enhancing the involvement of lattice oxygen remains challenging. In this study, the fabrication of B, Fe co‐doped CoP (B, Fe─CoP) nanofibers is reported, which serve as highly efficient OER electrocatalyst through phosphorization and boronation treatment of Fe‐doped Co 3 O 4 nanofibers. Experimental results combined with theoretical calculations reveal that simultaneous incorporation of both B and Fe can more effectively trigger the participation of lattice oxygen in CoFe oxyhydroxides reconstructed from B, Fe─CoP nanofibers compared to incorporating only B or Fe. Therefore, the optimized B, Fe─CoP nanofibers exhibit superb OER activity with low overpotentials of 361 and 376 mV at 1000 mA cm −2 in alkaline freshwater and alkaline natural seawater, respectively. The present…

Abstract Electrocatalytic reduction of NO 2 − to NH 3 (NO 2 RR) presents a fascinating approach for simultaneously migrating NO 2 − pollutants and producing valuable NH 3 . In this study, single‐atom Rh‐alloyed copper (CuRh 1 ) is explored as a highly active and selective catalyst toward the NO 2 RR. Combined theoretical calculations and in situ FTIR/EPR spectroscopic experiments uncover the synergistic effect of Rh 1 and Cu to promote the NO 2 RR energetics of CuRh 1 through a tandem catalysis pathway, in which Rh 1 activates the preliminary adsorption and hydrogenation of NO 2 − (NO 2 − → *NO 2 → *NOOH → *NO), while the generated *NO on Rh 1 is then transferred on Cu substrate which promotes the rate‐determining step of *NO → *NHO toward the NH 3 synthesis. As a result, CuRh 1 equipped in a flow cell presents an unprecedented NH 3 yield rate of 2191.6 µmol h −1 cm −2 and NH 3 ‐Faradaic efficiency of 98.9% at a high current density of 322.5 mA cm −2 , as well as long‐term stability for 100 h electrolysis.

Abstract Materials with target load plateaus offer the potential for developing innovative vibration suppression and isolation systems for applications such as satellite platforms, submarines, and electric vehicles. However, implementing these materials can pose significant challenges. In this study, stair‐stepping mechanical metamaterials with programmable load plateaus are presented, which are created via a three‐level (unit, module, and 3D object) construction strategy. The strategy inspired by the inverse design concept achieves tunability in the number and properties of load plateaus within the force–displacement profiles of the metamaterials. This approach even yields appealing stair‐stepping response patterns, as validated by experiments and finite element simulations. Promisingly, programming the unit from its initial configuration to a “zero stiffness” configuration enables these metamaterials excellent vibration isolation performance. Furthermore, two reversible methods are proposed for switching among various unit configurations, namely shape memory programming and…

Abstract Tactile sensors have garnered considerable interest for their capacity to detect and quantify tactile information. The incorporation of microstructural designs into flexible tactile sensors has emerged as a potent strategy to augment their sensitivity to pressure variations, thereby enhancing their linearity, response spectrum, and mechanical robustness. This review underscores the imperative for progress in microstructured flexible tactile sensors. Subsequently, the discourse transitions to the prevalent materials employed in the fabrication of sensor electrodes, encapsulation layers, and active sensing mediums, elucidating their merits and limitations. In‐depth discussions are devoted to tactile sensors adorned with microstructures, including but not limited to, micropyramids, microhemispheres, micropillars, microporous configurations, microcracks, topological interconnections, multilevel constructs, random roughness, biomimetic microstructures inspired by flora and fauna, accompanied by exemplar studies from each category. Moreover, the utility of flexible tactile…

Abstract Seawater electrolysis is a sustainable technology for producing hydrogen that would neither cause global freshwater shortages nor create carbon emissions. However, this technology is severely hampered by the insufficient stability and the competition from the chlorine evolution reaction (ClER) in actual application. Herein, a metal–organic framework (MOF)‐on‐MOF heterojunction (Ni‐BDC/NH 2 ‐MIL‐88B(Fe)) denoted as (Ni‐BDC/NM88B(Fe)) is synthesized as an effective oxygen evolution reaction (OER) electrocatalyst for high‐performance seawater electrolysis, which exhibits a long stability of 200 h and low overpotentials of 232 and 299 mV at 100 mA cm −2 in alkaline freshwater and seawater solution, respectively. The exceptional performance is attributed to the rapid self‐reconstruction of Ni‐BDC/NM88B(Fe) to produce NiFeOOH protective layer, thereby avoiding ClER‐induced dissolution. Moreover, the interface interaction between Ni‐BDC and NM88B(Fe) could form the Ni─O─Fe bonds in Ni‐BDC/NM88B(Fe) to promote the electron transfer and lower the energy barrier of the…

Abstract Anode‐free sodium metal batteries (AFSMBs) as one new battery configuration, have attracted more attention in recent years and considered as the promising next‐generation energy storage systems, owing to the advantages of high theoretical energy density, high safety, cost‐saving, and simplified fabrication process. The practical application of AFSMBs, however, is impeded by their poor cycle life arising from the low coulombic efficiency (CE), the growth of metal dendrite, and unstable solid electrolyte interphase (SEI). Recently, some works are reported to dissolve the above‐mentioned issues. In this review, it provides a comprehensive summary of AFSMBs including their origin, mechanism, advantages, challenges, strategies, and perspectives. First, the intrinsic issues of conventional sodium metal batteries are summarized as safety concerns and manufacturing difficulty, which is the background of promoting AFSMBs’ birth. Subsequently, the mechanism, construction requirement, advantages, and challenges of AFSMBs are discussed. Furthermore, the strategies for improving AFSMBs…

Abstract 2D materials, with outstanding optical, thermal, and electric properties, are emerging as promising candidates for fabricating high‐performance photodetectors. Recently, impressive progresses have been made in this area and some challenges are remaining to improve the properties of photodetectors. As one important part in the mainstream photodetection mechanisms, photothermoelectric (PTE) effect is showing unique priorities in fabricating advanced photodetectors, especially broadband detection operating in the mid‐infrared and terahertz spectral regime. Here, recent progress on PTE photodetectors based on layered 2D materials is reviewed. The physical mechanism of PTE effect is first discussed and then the optical and thermoelectric properties of various 2D materials are analyzed. Furthermore, strategies to improve the photodetection performance of PTE detectors are summarized in two major categories including enhanced photothermal conversion and thermoelectric conversion processes. Finally, the challenges and prospects for future research in 2D thermoelectric materials and…

Abstract Hydrogels are made tough to resist crack propagation. However, for seamless integration into devices and machines, it necessitates robustness against cyclic loads. Central to this objective is enhancing fatigue resistance, an indispensable attribute facilitating the optimal performance of hydrogels within a multitude of biological contexts, spanning various plant and animal tissues, as well as diverse biomedical and engineering areas. In this review, recent research concerning the fatigue behavior of hydrogels, presenting a comprehensive consolidation of the inherent mechanisms that underpin diverse strategies aimed at fortifying fatigue resistance, is summarized. A critical facet in the architectural blueprint of fatigue‐resistant hydrogels is emphasized, involving the imposition of spatial constraints upon the main chains at the crack tips, thereby effectuating a protracted delay in their fracture initiation during prolonged cyclic loading. The integration of multiscale mechanisms encompassing networks, interactions, media, and structures stands as a pivotal factor in the…

Abstract The miniaturization trend of future electrical and electronic systems tender higher demands for high‐temperature resistant dielectric capacitors. The exponential increase in leakage current of dielectric polymers under high temperatures and strong electric fields is a pivotal bottleneck constraining the application of capacitors. Herein, a design is described where various animated quantum dots (A‐QDs), serving as crosslinkers, are introduced into the polyimide (PI) matrix to regulate the excitation and transport of carriers. Using fluorescence lifetime imaging (FLIM) and Kelvin probe force microscopy (KPFM), it is demonstrated that the intrinsic quantum confinement effect of quantum dots (QDs) significantly enhances carrier immobilization. Moreover, the dynamic stability of the covalently bonded network at elevated temperatures has proven to be effective in reducing dielectric loss, while enhancing the electrical insulation properties of the hybrid films. Therefore, at 200 °C, the optimal hybrid film exhibits an exceptional discharged energy density of 5.8 J cm −3 with an…

Abstract Multifunctionalization of electromagnetic wave absorbing materials (EMWAMs) presents a promising avenue for their application in complex scenarios. However, the effective integration of multiple supplementary functions into EMWAMs continues to pose a significant challenge. Herein, a novel nanofiber elastomer (NFE) incorporating multicomponent inorganic FeS 2 /S,N co‐doped carbon nanofibers (NFs) and organic component (Ecoflex) are designed and synthesized. The sulfur doping ratios and species can be effectively modulated via controlling the amount of sulfur and sulfurization temperature. The optimized FeS 2 /S,N co‐doped carbon NFs/Ecoflex NFE not only exerted an excellent impedance matching characteristic, but also displays boosted conductive loss and polarization loss capacities. Amongst, the designed NFE achieved an ultra‐wide effective absorption bandwidth (EAB) of 7.40 GHz and minimum reflection loss (RL min ) of −21.82 dB at the thin matching thickness (≈2.00 mm). Furthermore, FeS 2 /S,N co‐doped carbon NFs/Ecoflex NFE simultaneously presents greatly improved…

Abstract Transition bimetallic sulfides show significant promise for energy‐related applications because of their plentiful active sites and synergistic redox activity. However, limited pore size and low‐conductivity issues hinder their application. The structure of NiCo–S with rich sulfur vacancies is first predicted by density functional theory (DFT) calculations. Different sulfur vacancy concentrations are modeled by DFT calculations, and the results confirm that sulfur vacancies enhance the conductivity of the electrode material and are more beneficial for the adsorption of OH * species. It is verified by the differential charge density that the electric field formed on the surface of the electrode can lead to strong interfacial interactions by electron aggregation, which promotes electron/ion transfer kinetics. Furthermore, NiCo–S nanosheets are prepared on carbon cloth enriched with different concentrations of sulfur vacancies (denoted as NiCo‐Sv‐x, with x representing the concentration of sulfur vacancies) by sulfide etching NiCo‐MOF and annealing under H 2 /Ar atmosphere.…

Abstract Developing highly effective transition metal‐based bifunctional electrocatalysts remains a tremendously challenging task for large‐scale overall water splitting. Herein, a multiheterostructured Mo‐doped Ni2P/FexP electrocatalyst on NiFe foam with P vacancy (denoted as Mo─Ni2P/FexP‐V/NFF) is developed to serve as an efficient dual‐pH electrocatalyst. Due to the synergistic effect of multiple strategies (heteroatom doping, heterointerface, and P vacancy), the Mo─Ni2P/FexP‐V/NFF possesses remarkable hydrogen evolution reaction (HER) catalytic activity in alkaline/acidic and excellent oxygen evolution reaction (OER) in alkaline media, along with encouraging durability. The mechanisms of improved electrocatalytic activity combining multicharacterizations and density functional theory (DFT) calculations are elucidated. Specifically, X‐ray absorption fine structure experimental analysis confirms that the Mo doping can optimize the electronic structure of electrocatalyst. In situ Raman spectroscopy demonstrates that the evolved oxyhydroxides are the real active substances for the…