The 100 most-cited articles in Advanced Functional Materials, 2022

Abstract The oxygen evolution reaction (OER) generally exists in electrochemistry‐enabled applications that are coupled with cathodic reactions like hydrogen evolution, carbon dioxide reduction, ammonia synthesis, and electrocatalytic hydrogenation. The OER heavily impacts the overall energy efficiency of these devices because the sluggish OER kinetics result in a huge overpotential, thus, a large amount of efficient catalysts are needed. The benchmark iridium and ruthenium (Ir/Ru)‐based materials (mostly used in acid media) are, however, significantly limited by their scarcity. Non‐precious metal‐based catalysts (NPMCs) have emerged as the most promising alternatives; however, they tend to degrade quickly under the harsh operating conditions of typical OER devices. Another challenge is the unsatisfying performance of OER catalysts when integrated in real‐world devices. Herein, the OER active sites for three mainstream types of NPMCs including non‐precious transition metal oxides/(oxy)hydroxides, metal‐free carbon materials, and hybrid non‐precious metal and carbon composites are…

Abstract Electromagnetic (EM) functional materials play an increasingly important role in solving EM wave pollution in both modern military and civil fields. Graphene‐based materials are the most promising candidates in the applications of EM wave shielding and absorption owing to their remarkable structures and enhanced EM properties. Designing graphene‐based materials with elaborately controlled microstructures and optimized EM properties can effectively improve EM energy attenuation and conversion. Herein, the study begins with the EM attenuation mechanism, and multiscale design strategies of graphene‐based EM functional materials are outlined, including molecular‐scale, micro/nanoscale structure, macroscale structure, and integration of multiscale assembly design strategies. Applications in the EM wave shielding and absorption fields are reviewed, focusing on the latest advances in graphene‐based assemblies such as films, fabrics, and composites. Finally, the current challenges and future directions in this fast‐growing field are predicted.

Abstract With the enormous development of the electric vehicle market, fast charging battery technology is highly required. However, the slow kinetics and lithium plating under fast charging condition of traditional graphite anode hinder the fast charging capability of lithium‐ion batteries. To develop anode materials with rapid Li‐ions diffusion capability and fast reaction kinetics has received widely attentions. This review summarizes the current status in the exploration of fast charging anode materials, mainly including the critical challenge of achieving fast charging capability, the inherent structures and lithium storage mechanisms of various anode materials, as well as the recent progress to improve the rate performance involving morphology regulation, structure design, surface/interface modification, as well as forming multiphase systems. Finally, the challenges and future directions of developing fast charging Li‐ion batteries are highlighted.

Abstract Developing superelastic and superhydrophilic carbon aerogels with intriguing mechanical properties is urgently desired for achieving promising performances in highly compressive supercapacitors and strain sensors. Herein, based on synergistic hydrogen bonding, electrostatic interaction, and π–π interaction within regularly arranged layered porous structures, conductive carbon aerogels with cellulose nanofibrils (CNF), carbon nanotubes (CNT) and reduced graphene oxide (RGO) are developed via bidirectional freezing and subsequent annealing. Benefiting from the porous architecture and high surface roughness, CNF/CNT/RGO carbon aerogels exhibit ultralow density (2.64 mg cm –3 ) and superhydrophilicity (water contact angle ≈0° at 106 ms). The honeycomb‐like ordered porous structure can efficiently transfer stress in the entire microstructure, thereby endowing carbon aerogels with high compressibility and extraordinary fatigue resistance (10,000 cycles at 50% strain). These aerogels can be assembled into compressive solid‐state symmetric supercapacitors showing excellent area…

Abstract Ionic conductive hydrogels (ICHs) integrate the conductive performance and soft nature of tissue‐like materials to imitate the features of human skin with mechanical and sensory traits; thus, they are considered promising substitutes for conventional rigid metallic conductors when fabricating human‐motion sensors. However, the simultaneous incorporation of excellent stretchability, toughness, ionic conductivity, self‐healing, and adhesion via a simple method remains a grand challenge. Herein, a novel ICH platform is proposed by designing a phenylboronic acid‐ionic liquid (PBA‐IL) with multiple roles that simultaneously realize the highly mechanical, electrical, and versatile properties. This elaborately designed semi‐interpenetrating network ICH is fabricated via a facile one‐step approach by introducing cellulose nanofibrils (CNFs) into the PBA‐IL/acrylamide cross‐linked network. Ingeniously, the dynamic boronic ester bonds and physical interactions (hydrogen bonds and electrostatic interactions) of the cross‐linked network endow these hydrogels with remarkable…

Abstract High‐entropy (HE) oxides have become increasingly popular as electromagnetic wave‐absorbing materials owing to their customizable structure and unique HE effects. However, the weak loss property of single‐phase HE ceramics and the approaches implemented to improve them based on semi‐empirical rules severely limit their development. Herein, two biphasic HE oxides are prepared by simple sintering to realize accurate regulation of crystal phases and structural defects. It is verified that HE effects cause various defects that are beneficial for microwave dissipation within complex‐phase ceramics. In spinel/perovskite HE oxides, around the interface of spinel (111) and perovskite (110) planes, notable stress concentrations and lattice distortions are directly observed, inducing numerous point defects and stacking faults. Interestingly, besides the existing heterogeneous interface of rock salt (220)/spinel (220) plane and defects, rock salt/spinel HE oxides enabled synergistic effects via the precise regulation of components’ phase. Driven by structural defects and multi‐phases…

Abstract Vigorous development of 5G communication technologies can boost mobile networks yet bring in electromagnetic interferences and safety concerns in utilizing electronic devices. Particularly, 5G network can not only involve a low‐frequency band of n 78 (3.3–3.8 GHz) but also cover multi‐frequency bands of n 77 (3.3–4.2 GHz) and n 79 (4.4–5.0 GHz), displaying multiple electromagnetic radiations. Countless efforts have been devoted to investigating electromagnetic wave (EMW) absorbers with low‐ and multi‐band absorption properties. However, in terms of emerging materials and designs, few reports propose the mechanisms related to those properties. This perspective briefly reviews the impressive achievements of low‐ and multi‐frequency EMW absorbers and analyzes the design strategies that may enable low‐ and multi‐frequency absorption. Furthermore, the cutting‐edge mechanisms of corresponding electromagnetic responses, such as Snoek limit, quarter wavelength, and dielectric‐magnetic synergy effects are elaborated. Thus, this perspective can shed light on the new trends and…

Abstract 2D interfacial heterostructures have found an unassailable status in energy storage systems, particularly in supercapacitors citing the intriguing structural and electrochemical characteristics. Exactly a decade ago, MXene, a promising 2D transition metal carbide/nitride/carbonitride was found to possess excellent conductivity, hydrophilicity, laudable charge storage opportunities, and enriched surface functionalities conducive for supercapacitors with inherent challenging shortcomings. To substantially improve, assembled 2D/2D MXene heterostructures exhibit commendable performance backed by the fact of swift increase in research interest. In this review, state‐of‐the‐art research progress in material design and electrochemical performance of 2D/2D MXene heterostructures for supercapacitors are investigated. Discussion is initially on MXene fundamentals including synthesis and energy storage governing properties. Particularly, different preparation including electrostatic assembly, in situ growth, hydrothermal treatment, and objective specific strategies and its…

Abstract Polymeric metal‐organic framework (MOF)‐derived composites are promising functional materials because of their exceptional chemical homogeneity, designable components, and adjustable pore size. The modulation of oxygen and Mn vacancies via the introduction of heteroatoms and changes in the annealing temperature in MOFs‐derived composites can be a possible solution to investigate the polarization loss mechanism, which facilitates the improvement of electromagnetic loss capacity. Herein, the design of laminate‐stacked sphere‐shaped trimetallic CoNiMn‐MOFs is presented. The derived CoNi/MnO@C composites retain the original topography of the MOFs. The concentration of oxygen vacancies increases with the incorporation of heteroatoms, but decreases with annealing temperature, which prevails in the polarization loss mechanism rather than the contribution of Mn 2+ vacancies and heterogeneous interfaces. Therefore, the minimum reflection loss of the CoNi/MnO@C sample demonstrates −55.2 dB at 2.6 mm and the broad effective absorption bandwidth reaches 8.0 GHz at 2.1 mm. This work is…

Abstract Laser‐induced graphene (LIG) is a newly emerging 3D porous material produced when irradiating a laser beam on certain carbon materials. LIG exhibits high porosity, excellent electrical conductivity, and good mechanical flexibility. Predesigned LIG patterns can be directly fabricated on diverse carbon materials with controllable microstructure, surface property, electrical conductivity, chemical composition, and heteroatom doping. This selective, low‐cost, chemical‐free, and maskless patterning technology minimizes the usage of raw materials, diminishes the environmental impact, and enables a wide range of applications ranging from academia to industry. In this review, the recent developments in 3D porous LIG are comprehensively summarized. The mechanism of LIG formation is first introduced with a focus on laser‐material interactions and material transformations during laser irradiation. The effects of laser types, fabrication parameters, and lasing environment on LIG structures and properties are thoroughly discussed. The potentials of LIG for advanced applications…

Abstract Though visualizing perspiration constituents is crucial for physiological evaluation, inadequate material healing and unreliable power supply methods restrict its applications. Herein, a fully flexible self‐powered sweat sensor is fabricated from a cellulose‐based conductive hydrogel to address these issues. The hydrogel electrode is composed of a cellulose nanocomposite polymerized in situ with polyaniline and cross‐linked with polyvinyl alcohol/borax. The cellulose nanocomposites furnish the sweat sensor with tensile and electrical self‐healing efficiencies exceeding 95% within 10 s, a stretchability of 1530%, and conductivity of 0.6 S m−1. The sweat sensor quantitatively analyzes Na+, K+, and Ca2+ contents in perspiration, to sensitivities of 0.039, 0.082, and 0.069 mmol–1, respectively, in real time via triboelectric effect and wirelessly transmits the results to a user interface. This fabricated sweat sensor with high flexibility, stability, and analytical sensitivity and selectivity provides new opportunities for self‐powered health monitoring.

Abstract Coal features low‐cost and high carbon yield and is considered as a promising precursor for carbon anode of sodium‐ion batteries (SIBs) and sodium‐ion capacitors (SICs). Regulation of microcrystalline state and pore configuration of coal structure during thermal transformation is key to boost Na+ storage behavior. Herein, a facile strategy is reported to create abundant closed pores in anthracite‐derived carbon that greatly improves Na+ plateau storage. An altered thermal transformation pathway of chemical activation followed by high‐temperature carbonization is adopted to achieve the conversion of open nanopores and ordered carbon crystallite into closed pores surrounded by short‐range carbon structures. The optimized sample delivers a large reversible capacity of 308 mAh g–1 that is dominantly contributed by the low‐voltage plateau process. Experimental results reveal the enhanced pore‐filling mechanism in the developed closed pores. Benefitting from the improved plateau behavior, the constructed SIB delivers a high‐energy density of 231.2 Wh kg–1 with an average voltage…

Abstract Ion is one of the most common additives that can impart electrical conductivity to insulating hydrogels. The concurrent toughening effect of ions, however, is often neglected. This work reports the extreme toughening of hydrogels via the synergistic effect of cations and anions, without the need for specific structure design or adding other reinforcements. The strategy is to equilibrate a physical double network hydrogel consisting of both multivalent cation‐ and kosmotropic anion‐sensitive polymers in specific salt solutions that can induce cross‐linking and salting‐out simultaneously. Both effects are proven positive to boost the mechanical performance and electrical conductivity of the original weak gel, and result in a tough conductive gel with exceptional physical properties, achieving significant enhancements in fracture stress, fracture energy, and ionic conductivity by up to 530‐, 1100‐, and 4.9‐folds, respectively. The optimal fracture stress and toughness reach approximately 15 MPa and 39 kJ m –2 , exceeding most state‐of‐the‐art tough conductive hydrogels.…

Abstract Interfacial solar water evaporation, a promising way to address water shortages and water pollution, has attracted increasing attention. However, low evaporation rates limit its practical applications. Reducing evaporation enthalpy is one of the most efficient ways to improve the evaporation rate. In this study, micro‐meniscuses and microdroplets (MMDs) are found and observed on the surface of the polypyrrole nanoarrays on hydrophilic carbon cloth. The MMDs can reduce the evaporation enthalpy of the system, thus resulting in a high evaporation rate of 2.16 kg m −2 h −1 in pure water under 1 sun. Dynamic calculations imply that the evaporation rate of MMDs is approximately at least 1.7 times and 1.8 times that of a flat liquid film, respectively. Under 1 sun, the evaporators with MMDs enable stable evaporation in continuous 72 h in 10.0 wt% NaCl solution, simulated seawater, and actual wastewater, with an evaporation rate of 1.86, 1.99, and 1.82 kg m −2 h −1 , respectively. As far as it is known, these evaporation rates are the highest reported values for the 2D interfacial…

Abstract The development of a high‐performance electrocatalyst for oxygen evolution reaction (OER) is imperative but challenging. Here, a partial sulfidation route to construct Ni2Fe‐LDH/FeNi2S4 heterostructure on nickel foam (Ni2Fe‐LDH/FeNi2S4/NF) by adjusting the hydrothermal duration is reported. The heterostructures afford abundant hydroxide/sulfide interfaces that offer plentiful active sites, rapid charge and mass transfer, favorable adsorption energy to oxygenated species (OH− and OOH) evidenced by the density functional theory calculations, which synergistically boost the alkaline water oxidation. In the 1.0 m KOH solution, Ni2Fe‐LDH/FeNi2S4/NF exhibits an excellent OER catalytic activity with a much smaller overpotential (240 mV) to reach the current density of 100 mA cm−2 than single‐phase Ni2Fe‐LDH/NF (279 mV) or FeNi2S4/NF (271 mV). More impressively, 2000 cycles of cyclic voltammetry scan for water oxidation results in the formation of a sulfate layer over the catalyst. The corresponding post‐catalyst demonstrates better OER activity and durability than the initial one…

Abstract Oil fouling threatens the water flux stability of membranes for oil/water separation. Simple hydrophilic modification fights for an opportunity to prevent oil contamination but fails to eliminate severe water flux decline. In essence, a “single‐defense” mechanism is insufficient to build a potent barrier against accumulated cake layer under a filtration environment. This work reports a “double‐defense” design by integrating hydrophilic polymer brushes and hydrogel layer on oil/water separation membranes for desired anti‐oil‐fouling property, where a poly(vinylidene fluoride) porous membrane is first covered by a layer of poly(hydroxyethyl methylacrylate) hydrogel and then controllably grafted with poly(sulfobetaine) brushes. The spatially hierarchical structure establishes a highly covered “double‐defense” barrier for the membrane surface to efficiently repel oil adhesion and the formation of an accumulated cake layer. When separating various surfactant‐stabilized oil‐in‐water emulsions, the permeating flux displays a nearly zero decline throughout the whole filtration…

Abstract The single‐phase oxides with elemental complexity and compositional diversity, usually named high entropy oxides, feature homogeneously dispersed multi‐metallic elements in equiatomic concentration. The unusual properties of high entropy oxides endow their potential application in clean‐energy‐related electrocatalysis. However, the possible fundamental relationship between configuration entropy and the underlying catalytic mechanism is still not well understood and established. Herein, a high entropy perovskite cobaltate consisting of five equimolar metals in the B‐site (Mg, Mn, Fe, Co, and Ni) is employed as an electrocatalyst for oxygen evolution reaction (OER). The configuration entropy serves as an effective tool to promote the intrinsic activity of the Co reactive site and manipulate the OER mechanism. The high entropy cobaltate demonstrates a lower overpotential of 320 mV at a current density of 10 mA cm −2 , outperforming other counterparts. The X‐ray spectroscopies disclose the synergistic charge‐exchange effect among different cations and the formation of a new…

Abstract Photoelectrochemical water splitting based on nanostructured bismuth vanadate (BiVO4) can be a promising strategy to produce low‐cost and green H2 to replace fossil fuels and realize carbon neutrality. Herein, a simple chemical way to realize in situ carbon doping into BiVO4 crystalline structure is designed and obtained carbon‐doped BiVO4, namely C‐BiVO4, can improve the electronic conductivity of BiVO4. In addition, the introduction of the synthesized carbon quantum dots (CQDs) as a co‐catalyst, immobilizes CQDs onto the C‐BiVO4 nanosheet and acquires the optimized C‐BiVO4/CQDs heterogeneous structure, which not only boosts light absorption, but also enhances the separation and transfer of the photo‐generated charges. Stemming from the dual carbon actions, the as‐prepared C‐BiVO4/CQDs photoanode exhibits an excellent photocurrent density of 4.83 mA cm−2 at 1.23 V versus the RHE without the use of any hole scavengers. To assure the practical application of the sensitive photocatalyst, a polyaniline layer is electroplated onto the C‐BiVO4/CQDs catalyst as a conducting,…

Abstract This article provides a comprehensive overview of piezo‐ and ferro‐electric materials based on organic molecules and organic–inorganic hybrids for mechanical energy harvesting. Molecular (organic and organic–inorganic hybrid) piezo‐ and ferroelectric materials exhibit significant advantages over traditional materials due to their simple solution‐phase synthesis, light‐weight nature, thermal stability, mechanical flexibility, high Curie temperature, and attractive piezo‐ and ferroelectric properties. However, the design and understanding of piezo‐ and ferroelectricity in organic and organic–inorganic hybrid materials for piezoelectric energy harvesting applications is less well developed. This review describes the fundamental characterization of piezo‐ and ferroelectricity for a range of recently reported organic and organic–inorganic hybrid materials. The limits of traditional piezoelectric harvesting materials are outlined, followed by an overview of the piezo‐ and ferroelectric properties of organic and organic–inorganic hybrid materials, and their composites, for…

Abstract Flexible epidermic sensors made from conductive hydrogels are holding bright potential in personalized healthcare, multifunctional electronic skins, and human‐machine interfaces. However, it is still a great challenge to simultaneously realize conductive hydrogel‐based epidermic sensors with reliable self‐healing ability and remarkable sensing performances in high‐performance healthcare (especially electrophysiological signals) sensing for wearable human‐machine interaction, as well as accelerated wound healing for subsequent medical treatment together. Herein, a flexible healable high‐performance epidermic sensor is assembled from the facilely prepared antibacterial MXene hydrogel with efficiently accelerated wound healing for sensitively wearable human‐machine interaction. The as‐prepared hydrogel possesses enhanced mechanical performance, outstanding healable capability, reliable injectability, facile degradability, excellent biocompatibility, and robust antibacterial ability, which is capable of being assembled into a multifunctional epidermic sensor to sensitively…

Abstract Single‐atom catalysts (SACs) are widely investigated in Fenton‐like reactions for environmental remediation, wherein their catalytic performance can be further improved by coordination structure modulation, but the relevant report is rare. Herein, a series of atomically dispersed cobalt catalysts with diverse coordination numbers (denoted as CoN x , x represents nitrogen coordination number) are synthesized and their peroxymonosulfate (PMS) conversion performance is explored. The catalytic specific activity of CoN x is found to be dependent on coordination number of single atomic Co sites, where the lowest‐coordinated CoN 2 catalyst exhibits the highest specific activity in PMS activation, followed by under‐coordinated CoN 3 and normal CoN 4 . Experimental and theoretical results reveal that reducing coordination number can increase the electron density of single Co atom in CoN x , which governs the Fenton‐like performance of CoN x catalysts. Specifically, the entire Co–pyridinic NC motif serves as active centers for PMS conversion, where the single Co atom, and…

Abstract Developing low‐cost and highly efficient earth‐abundant oxygen evolution reaction (OER) electrocatalysts via an energy‐ and time‐saving method is of great significance to the generation of H 2 from electrochemical water splitting, which is highly desirable but still challenging. Herein, a one‐step route to in situ grow S‐doped FeOOH vertical nanosheets on iron foam (IF) in 20 min under room temperature is shown. This facile and ultrafast method effectively modifies the surface of the IF into an S‐doped FeOOH layer, and a full‐Fe electrode (S‐FeOOH/IF) is achieved. Systematic experiments and characterizations demonstrate that the redox reactivities for both of the iron and lattice oxygen in FeOOH are sufficiently activated, leading to the dramatically improved intrinsic OER activity. The as‐obtained S‐FeOOH/IF exhibits a fascinating OER performance with a low overpotential of 244 at 10 mA cm −2 . This work affords an efficient surface engineering strategy to drive commercial IF into cost‐efficient and robust earth‐abundant electrocatalysts for water oxidation, which has…

Abstract Hierarchical engineering of suitable dielectric‐magnetic multicomponents shows good performance for microwave absorbers, but still face bottlenecks. Herein, hierarchical double‐shelled nanotubes (DSNTs), in which the inner magnetic tubular subunits are assembled by magnetic‐heteroatomic components through cation‐exchange reactions, and the outer dielectric MnO2 nanosheets strengthen the synergistic interactions between confined heterogeneous interfaces are ingeniously designed and constructed. Hetero‐interfaces induced polarization is proposed to investigate the interfacial relaxation mechanism, and magnetic loss, closely related to the micrometer‐scale magnetic units, is mainly clarified by the magnetic interaction composed of magnetic coupling and magnetic diffraction; both of them are clearly confirmed by Lorentz off‐axis electron holography. The obtained hierarchical DSNTs demonstrate efficient microwave absorption with an optimal reflection loss of −54.7 dB and qualified absorption bandwidth of 9.5 GHz owing to desirable heterogeneous interfaces, multiple magnetic…

Abstract Electrochemical carbon dioxide reduction reaction (CO 2 RR) is an efficient strategy to relieve global environmental and energy issues by converting excess CO 2 from the atmosphere to value‐added products. Atomically dispersed metal‐nitrogen‐doped carbon (M‐N‐C) materials are superior catalysts for electrocatalytic CO 2 RR because of the 100% atomic utilization, unsaturated coordination configuration, relatively uniform active sites, and well‐defined and adjustable structure of active centers. However, the electrochemical CO 2 RR is a great challenge due to the process involving proton‐coupled multi‐electron transfer with a high energy barrier, which leads to unsatisfactory selectivity to the targeted product, especially for C2 products (e.g., C 2 H 4 and C 2 H 5 OH). Here, the authors systematically summarize effective means, including reasonable selection of isolated metal sites, regulation of the coordination environment of isolated metal atoms, and fabrication of dimetallic single‐atom sites for attaining optimal geometric and electronic structures of M‐N‐C materials…

Abstract Endowing artificial advanced materials and systems with biomimetic self‐regulatory intelligence is of paramount significance for the development of somatosensory soft robotics and adaptive optoelectronics. Herein, a bioinspired phototropic MXene‐reinforced soft tubular actuator is reported that exhibits omnidirectional self‐orienting ability and is capable of quickly sensing, continuously tracking, and adaptively interacting with incident light in all zenithal and azimuthal angles of 3D space. The novelty of the soft tubular actuator lies in three aspects: 1) the new polymerizable MXene nanomonomer shows high compatibility with liquid crystal elastomer (LCE) matrices and can be in situ photopolymerized into the polymer networks, thus enhancing the mechanical and photoactuation properties; 2) the distinct hollow and radially symmetrical structure facilitates the actuator with fast photoresponsiveness and phototropic performance through retarding the heat conduction along the radial direction; 3) the MXene‐LCE soft tubular actuator simultaneously integrates sensing,…

Abstract Among various advanced oxidation processes, coupled photocatalysis and heterogeneous Fenton‐like catalysis (known as photo‐Fenton‐like catalysis) to generate highly reactive species for environmental remediation has attracted wide interests. As an emerging metal‐free photocatalyst, graphitic carbon nitride (g‐C 3 N 4 , CN) has been recently recognized as a promising candidate to catalyze robustly heterogeneous photo‐Fenton‐like reactions for wastewater remediation. This review summarizes recent progress in fabricating various types of CN‐based catalysts for the photo‐Fenton‐like reaction process. Innovative engineering strategies on the CN matrix are outlined, ranging from morphology control, defect engineering, nonmetal atom doping, organic molecule doping to modification by metal‐containing species. The photo‐Fenton‐like catalytic activities of CN loaded with auxiliary sub‐nanoscale (e.g., quantum dots, organometallic molecules, metal cations, and single atom metals) and nanoscale metal‐based materials are critically evaluated. Hybridization of CN with bandgap‐matching…

Abstract Developing efficient and inexpensive electrocatalysts for the hydrogen evolution reaction (HER) is critical to the commercial viability of electrochemical clean energy technologies. Transition metal phosphides (TMPs), with the merits of abundant reserves, unique structure, tunable composition, and high electronic conductivity, are recognized as attractive HER catalytic materials. Nevertheless, the HER electrocatalytic activity of TMPs is still limited by various thorough issues and inherent performance bottlenecks. In this review, these issues are carefully sorted, and the corresponding reasonable explanations and solutions are elucidated on the basis of the HER catalytic activity origins of TMPs. Subsequently, highly targeted multiscale strategies to improve the HER performance of TMPs are comprehensively presented. Additionally, critical scientific issues for constructing high‐efficiency TMP‐based electrocatalysts are proposed. Finally, the HER reaction process, catalytic mechanism research, TMP‐based catalyst construction, and their application expansion are mentioned as…

Abstract Prussian blue analogs (PBAs) are promising cathode materials for sodium‐ion batteries (SIBs) due to their low‐cost, similar energy density comparable with that of LiFePO4 in lithium‐ion batteries, and long cycle life. Nevertheless, crystal water (≈10 wt%) in PBAs from aqueous synthesis environments can bring significant side effects in real SIBs, especially for calendar life and high temperature storage performance. Therefore, it is of great importance to eliminate crystal water in PBAs for future commercial applications. Herein, a facile heat‐treatment method is reported in order to remove water from Fe‐based PBAs. Although the heat‐treated sample can be easily rehydrated in air, it still exhibits a stable cycling performance over 2000 times under controlled charge cut‐off voltage. In situ synchrotron high‐temperature powder X‐ray diffraction demonstrates that the as‐prepared sample is maintained at a new trigonal phase after dehydration. Moreover, the redox reaction of low‐spin Fe2+/Fe3+ is activated and the high‐temperature storage performance of as‐prepared sample is…

Abstract The rapid development of portable flexible electronic devices means a multifunctional composite film with excellent thermal management capability, high electromagnetic interference (EMI) shielding, and a strong fire safety performance is urgently required. In this paper, inspired by a “brick–mortar” sandwich structure, phase change capsules (PCCs) and MXene nanosheets are prepared. Subsequently, a one‐step vacuum‐assisted filtration method is used to fabricate a multifunctional flexible PCC/MXene/polyvinyl alcohol (PMP) phase change composite film with high light‐to‐thermal conversion efficiency, Joule heating generation, fire safety, and EMI shielding effects. The superior preparation technology endows the film with multi‐source driven thermal management capabilities and excellent EMI shielding effectiveness values (43.13 dB). In addition, the PMP film exhibits good flexibility and high enthalpy (136.8 J g −1 ). Surprisingly, the PMP film's excellent fire safety properties improve its reliability and safety. In summary, the simple preparation technique and outstanding…

Abstract Aqueous zinc ion batteries (AZIBs) are receiving increasing attention for large‐scale energy storage systems owing to their appealing features with intrinsic safety, low cost, and scalability. Unfortunately, the water‐induced parasitic reactions and dendrite growth on the Zn anode severely impede the further development of AZIBs. Herein, a thiourea additive is introduced into ZnSO4 electrolyte to construct unique metal‐molecule interface for simultaneously regulating the Zn anode interface chemistry and the bulk electrolyte environment. Experimental results and theoretical calculations reveal that the formed metal‐molecule interface can not only serve as a corrosion inhibitor for alleviating the water‐induced side reactions, but also act as a Zn2+ ion regulator for promoting the homogenous Zn deposition, thus achieving a corrosion‐free and dendrite‐free Zn anode. Consequently, the Zn|Zn symmetric cell exhibits an extended lifespan of 1200 h at 1 mA cm–2, 1mAh cm–2, and a high cumulative capacity of 3000 mAh cm–2 at 10 mA cm–2. When paired with V2O5 cathode, the Zn|V2O5 full…

Abstract Hydrogen is an efficient, clean, and economical energy source, owing to its huge energy density. Electrochemical water splitting is a potential candidate for inexpensive and eco‐friendly hydrogen production. Recently, the development of 2D transition metal chalcogenides (TMDs) nanomaterials with a variety of physicochemical properties has shown their potential as eminent non‐noble metal‐based nanoscale electrocatalysts for hydrogen evolution. Nanostructuring such materials induces deep modification of their functionalities, compared to their bulk counterparts. High density of different types of exposed active sites is formed, and the small diffusion paths, which enhances the electron transfer in the 2D structures, can successfully aid the charge collection process in the electrocatalytic hydrogen evolution reactions. In this review, the key parameters to improve the catalyst performance of 2D TMDs in electrochemical hydrogen evolution reaction (HER) processes are discussed in detail and the most recent developments in the field are summarized, focusing on the improvement of…

Abstract Multifunctional fiber‐reinforced polymer (FRP) composites provide an ideal platform for next‐generation smart composites applications including structural health monitoring, electrical and thermal conductivity, energy storage and harvesting, and electromagnetic interference shielding without compromising their mechanical properties. Recent progress in carbon‐based nanomaterials such as graphene and carbon nanotubes (CNTs) has enabled the development of many novel multifunctional composites with excellent mechanical, electrical, and thermal properties. However, the effective incorporation of such carbon nanomaterials into FRP composites using scalable, high‐speed, and cost‐effective manufacturing without compromising their performance is challenging. This review summarizes the recent progress on graphene and CNT‐based FRP composites, their manufacturing techniques, and their applications in smart composites. Current technical challenges and future perspectives on smart FRP composites research to facilitate an essential step toward moving from research and development‐based…

Abstract Biobased resources are proposed as next‐generation materials for advanced application. Among them, silk fibroin, a protein‐based material generally obtained from Bombyx mori cocoons, is considered to play an increasing role in the development of a more sustainable generation of devices. In this review, the silk fibroin molecular structure and its original properties are presented, together with a wide overview of the available modifications and processing methods to reach custom structural and functional variations.

Abstract Over the past few decades, flexible sensors have been developed from the “electronic” level to the “iontronic” level, and gradually to the “ionic” level. Ionic flexible sensors (IFS) are one kind of advanced sensors that are based on the concept of ion migration. Compared to conventional electronic sensors, IFS can not only replicate the topological structures of human skin, but also are capable of achieving tactile perception functions similar to that of human skin, which provide effective tools and methods for narrowing the gap between conventional electronics and biological interfaces. In this review, the latest research and developments on several typical sensing mechanisms, compositions, structural design, and applications of IFS are comprehensively reviewed. Particularly, the development of novel ionic materials, structural designs, and biomimetic approaches has resulted in the development of a wide range of novel and exciting IFS, which can effectively sense pressure, strain, and humidity with high sensitivity and reliability, and exhibit self‐powered, self‐healing,…

Abstract Solar‐driven interfacial evaporation is an important approach for solving the issue of freshwater scarcity. However, the practical application of solar steam generation is hindered by high fabrication cost and environmental concerns regarding the petroleum‐based materials. Herein, lignocellulose (cellulose‐lignin composite) hydrogel (LCG) and lignin‐derived carbon (LC) are used as the substrate and photothermal material, respectively, to construct a fully lignocellulose‐based double‐layered hydrogel (LC@LCG) evaporator. Results indicate that LC has an ultrahigh specific surface area and full‐spectrum solar absorption of 98%. The presence of lignin can improve the hydrophilicity and maintain the capillary channels of the hydrogel, which tunes water into an intermediate state and reduces the vaporization enthalpy of water. Moreover, it ensures a high water transport rate in the hydrogel. Based on these advantages, the evaporation rate and photothermal conversion efficiency of hydrogel evaporator reach 1.84 kg m −2 h −1 under one sun and 86.5%, respectively. The…

Abstract Swelling is ubiquitous for conventional hydrogels but is not favorable for many situations, especially underwater applications. In this study, an anti‐swelling and mechanically robust polyacrylic acid (PAAc)/gelatin composite hydrogel is reported with a rapid gelation process (10 1 s) under mild conditions via the synergy of MXene‐activated initiation and zirconium ion (Zr 4+ )‐induced cross‐linking, without the requirement of external energy input. The MXene is found efficient to activate the chain initiation, while the Zr 4+ is prone indispensable for facilitating the cross‐linking of formed polymer chains. The resulting hydrogel exhibits integration of exceptional anti‐swelling properties and high mechanical performance at room temperature, thanks to the dense hydrogen bonds between PAAc and gelatin chains that enable an upper critical solution temperature above room temperature. Also, desirable electrical conductivity emerges in the hydrogel due to the simultaneous contribution of MXene and Zr 4+ , allowing stable electrical signal output of the gel upon deformation…

Abstract Nickel hydroxide (Ni(OH) 2 ) has been identified as one of the best promising electrocatalyst candidates for urea oxidation reaction (UOR) due to its flexible structures, wide compositions, and abundant 3d electrons under alkaline conditions. However, its layered structure with limited exposed edge sites severely hinders further improvement of the UOR activity. Herein, oxygen‐vacancy rich and vanadium doped Ni(OH) 2 (O vac ‐V‐Ni(OH) 2 ) catalysts are prepared and synergistically boost the urea electrooxidation. Vanadium doping contributes more exposed active sites, and simultaneously generates oxygen vacancies, switching the rate‐determining step of UOR from *COOH deprotonation to the N–H bond cleavage process and lowering the thermodynamic barrier by around 1.13 eV. The novel O vac ‐V‐Ni(OH) 2 demonstrates good electrocatalytic performances with a working potential of 1.47 V at a high current density of 100 mA cm −2 . Synergistic engineering of doping and oxygen vacancy is a promising strategy for designing efficient UOR electrocatalysts.

Abstract Organic ultralong room‐temperature phosphorescence (RTP) materials have promising applications in anti‐counterfeiting. To improve the encryption level, the exploration of organic materials with tunable solid‐state long persistent luminescence is in urgent need. Herein, a series of organic ultralong RTP polymeric systems are prepared by doping versatile indolocarbazole isomers into the poly(vinyl alcohol) (PVA) matrix. Notably, the doping film 11,12‐ICz@PVA exhibits excellent RTP property with an ultralong lifetime of 2.04 s and a high phosphorescence quantum yield of 44.1%. Theoretical calculations reveal that this excellent RTP property can be attributed to the strong electrostatic attraction resulting from the synergistic double hydrogen‐bond between the isomer 11,12‐ICz and PVA matrix. More impressively, color‐tunable and time‐dependent long persistent luminescence is successfully achieved through efficient phosphorescence energy transfer between the indolocarbazole isomers with ultralong blue RTP emissions and commercially available fluorescent dyes with emission colors…

Abstract High‐temperature dielectric polymers are in constant demand for the multitude of high‐power electronic devices employed in hybrid vehicles, grid‐connected photovoltaic and wind power generation, to name a few. There is still a lack, however, of dielectric polymers that can work at high temperature (> 150 °C). Herein, a series of all‐organic dielectric polymer composites have been fabricated by blending the n‐type molecular semiconductor 1,4,5,8‐naphthalenetetracarboxylic dianhydride (NTCDA) with polyetherimide (PEI). Electron traps are created by the introduction of trace amounts of n‐type small molecule semiconductor NTCDA into PEI, which effectively reduces the leakage current and improves the breakdown strength and energy storage properties of the composite at high temperature. Especially, excellent energy storage performance is achieved in 0.5 vol.% NTCDA/PEI at the high temperatures of 150 and 200 °C, e.g., ultrahigh discharge energy density of 5.1 J cm −3 at 150 °C and 3.2 J cm −3 at 200 °C with high discharge efficiency of 85–90%, which is superior to its…

Abstract Reduction of soluble hexavalent uranium (U(VI)) to sparingly soluble tetravalent uranium (U(IV)) with semiconductor photocatalysts is recognized as a novel, green, and simple U‐extraction method. Furthermore, effective charge separation and utilization are critical factors to achieve high‐efficiency U(VI) photoreduction. Herein, a UiO‐66‐based heterostructured photocatalyst (MnO x /UiO‐66/Ti 3 C 2 T x ) with spatially separated dual cocatalysts (MnO x nanoparticles and Ti 3 C 2 T x MXene nanosheets) is successfully developed for efficient U(VI) photoreduction without sacrificial agents. As co‐catalysts, MnO x nanoparticles favor the trapping of holes, while Ti 3 C 2 T x MXene nanosheets tend to collect electrons. Consequently, the photogenerated holes and electrons flow into and out of the photocatalyst, respectively, achieving efficient charge separation required by MnO x /UiO‐66/Ti 3 C 2 T x to remove U(VI). Impressively, the U(VI) removal ratio via MnO x /UiO‐66/Ti 3 C 2 T x reaches to 98.4% in the U(VI) solution after 60 min, with a photoreaction rate constant of 0.0948…

Abstract Massive bleeding and wound infection are the major problems often observed during severe trauma, and achieving rapid hemostasis in cases of high‐dose bleeding in arteries and viscera remains an acute clinical demand. Herein, a mussel‐ and barnacle cement proteins‐inspired dual‐bionic hydrogel is first proposed. Benefiting from abundant phenolic hydroxyl groups, a tough dissipative matrix, removal of interfacial water, as well as dynamic redox balance of phenol‐quinone, the multinetwork hydrogel achieves repeatable robust wet‐tissue adhesiveness (151.40 ± 1.50 kPa), a fast multimodal self‐healing ability, and excellent antibacterial property against both Gram‐positive/negative bacteria. For rabbit/pig models of cardiac penetration holes and femoral artery injuries, the dual‐bionic bioadhesive shows better hemostatic efficiency than commercial gauze due to the synergistic effect of strong wound sealing capability, excellent red blood cell capturing property, and activation of hemostatic barrier membrane. More interestingly, the hydrogel combined with commercial hemostatic…

Abstract Cuproptosis is a very newly recognized regulated cell death modality that is distinct from known death mechanisms and shows enormous prospect in cancer treatment. However, its efficacy is copper‐dependent and restricted by strictly regulated copper metabolism. Herein, a novel copper/iron hybrid hollow amorphous metal organic framework (HaMOF) is developed as an oxidative stress amplifier and copper/iron metabolic disrupter for synergistic cuproptosis/ferroptosis/apoptosis anticancer therapy. The HaMOF is fabricated from Cu2+, 3,3′‐dithiobis(propionohydrazide) and Fe3+ via an unsaturated coordination‐etching integration strategy, and then doxorubicin is loaded followed by surface decoration with hyaluronan. The obtained DOX@Fe/CuTH exhibits tumor microenvironment‐triggered catalytic therapeutic property, wherein it can amplify cellular oxidative stress by simultaneously boosting H2O2 production and depleting glutathione. Moreover, it can cause mitochondrial dysfunction and downregulate the expressions of copper transporter ATP7A and iron transporter FPN 1, thereby leading to…

Abstract Severe lower‐frequency (2–8 GHz) microwave pollution caused by the rapid development of 5th generation (5G) communication posts significance on cutting‐edge microwave absorbers. However, the intensely coupled wave‐impedance and microwave dissipating ability dramatically hinder their performance in the exact lower‐frequency range. The rationally designed heterostructure of hard/soft ferrite composite provides an efficient solution to address the issue. In this context, core‐shell structured hard/soft BaFe(12‐x)CoxO19@Fe3O4 with abundant heterointerface is created using facile spray‐drying and subsequent solvothermal approach, where hard magnetic BaFe(12‐x)CoxO19 serves as the core and soft magnetic Fe3O4 serves as the shell, respectively. The unique core‐shell integration contributes sufficient magnetic exchange coupling interaction for strong magnetic loss beyond Snoek's limitation, which considerably boosts a lower‐frequency microwave absorption. Accordingly, the minimum reflection loss (RLmin) of typical BaFe11.6Co0.4O19@Fe3O4 microcomposite reaches −48.9 dB at the…

Abstract MXenes (viz., transition metal carbides, carbonitrides, and nitrides) have emerged as a new subclass of 2D materials. Due to their outstanding physicochemical and biological properties, MXenes have gained much attention in the biomedical field in recent years, including drug delivery systems, regenerative medicine, and biosensing. Additionally, the incorporation of MXenes into hydrogels has garnered significant interest in biomedical engineering as an electroactive and mechanical nanoreinforcer capable of converting nonconductive scaffolds into excellent conductors of electricity with an impressive effect on mechanical properties for the engineering of electroactive organs and tissues such as cardiac, skeletal muscle, and nerve. However, many questions and problems remain unresolved that need to be answered to usher these 2D materials toward their true destiny. Thus, this review paper aims to provide an overview of the design and applications of MXene‐integrated composites for biomedical applications, including cardiac tissue engineering, wound healing, infection therapy,…

Abstract Over the past two decades, the unique features of ionic liquids (ILs) drive their exploration and exploitation in gel field and endow the gels with many excellent properties including thermal stability, antifreezing capability, mechanical strength, self‐healing, conductivity, and antibacterial performance. As promising functional materials, ionogels have attracted remarkable interest in various applications including flexible electronics, energy storage, and biomedical applications. This review aims to give a detailed overview of the recent advances in developing of IL‐based task‐specific ionogels. The effects of ILs on the ionogels’ formation and structure modification and their promotion on elevating these gel properties from the viewpoint of fundamental to the application are comprehensively discussed. The different interactions also discussed between ILs and other components in forming ionogels, such as hydrogen bond, electrostatic interaction, host–guest interaction, IL‐philic and IL‐phobic interaction, and introduced ILs’ dissolvability to biomass; and the unique…

Abstract The intrinsic zinc dendrite growth aggravated by the uneven electric field at the Zn anode surface and the water‐induced parasitic reactions have largely impeded rechargeable aqueous zinc‐ion batteries for the practical applications in large‐scale energy storage. Here, an effective strategy is proposed to manipulate Zn deposition and simultaneously prevent the generation of insulating by‐products (Zn4SO4(OH)6·xH2O) for improved plating/stripping on Zn anodes by the addition of a nontoxic electrolyte additive, β‐cyclodextrin (β‐CD). The simulation results indicate that β‐CD molecules prefer to adsorb horizontally on Zn (002) plane, regulating the diffusion pathways and deposition sites of Zn2+ for the preferred Zn deposition along (002) plane without dendrite formation and inhibiting the H2 generation and the formation of Zn4SO4(OH)6·xH2O by facilitating desolvation of [Zn(H2O)6]2+. Consequently, an ultra‐long stable cycling up to 1700 h at a high current density of 4 mA cm−2 can be achieved by the addition of β‐CD, 17 times that of the pure ZnSO4 electrolyte and the…

Abstract Aqueous Zn‐ion batteries have aroused much attention recently, yet challenges still exist in the lack of low‐cost, highly stable electrolytes to tackle the serious side reactions at Zn anode–electrolyte interface. Herein, a ZnSO 4 ‐based low‐cost aqueous electrolyte is demonstrated with a small amount of eco‐friendly silk peptide as an efficient additive. Compared with silk sericin and fibroin, silk peptide with abundant strong polar groups (COOH and NH 2 ) suppresses the side reactions. Namely, silk peptide regulates the solvation structure of Zn 2+ to decrease coordinated active H 2 O and SO 4 2− , and tends to anchor on Zn anode surface for the isolation of contact H 2 O/SO 4 2− as well as electrostatic shielding, demonstrating synergistic solvation and interface regulating effect. Consequently, the excellent cycle life (3000 h) and Coulombic efficiency (99.7%) of Zn anodes are revealed in 2 m ZnSO 4 electrolyte with only 5 mg mL −1 of silk peptide (≈0.49 USD L −1 ), promising practical applications of reversible zinc‐ion batteries.

Abstract Multiple relaxation behaviors are promising for broad frequency band and strong electromagnetic wave (EMW) absorption based on polarization‐controlled electromagnetic (EM) attenuation. However, rational selection of materials and structure manipulation through tunable substitution or phase control are challenging toward optimization of EMW absorption. Herein, bi‐metallic organic frameworks (B‐MOFs) with various morphologies are employed as EMW absorbers. Remarkably, the polar units can be enhanced by introducing Ni‐metal nodes into the Cu‐coordinated MOFs, rendering the B‐MOFs with self‐polarized properties and consecutive multifrequency EMW absorption behaviors. The maximum reflection loss of acetylene black (ACET) filled NiCu‐MOFs can reach –40.54 dB together with a wide bandwidth (<‐10 dB) of 5.87 GHz at a thickness of 2.5 mm. As a counterpart of the Ni/Cu/C derivatives, significantly increased broad band absorption (6.93 GHz) and multifrequency absorbing and polarization characteristics are also maintained in bimetal coexisting carbonized architectures as prepared by…

Abstract Vacancy engineering is an attractive approach to modulate the electronic structure of transition metal chalcogens. However, illustrating how anion vacancy can be engineered to tailor their electromagnetic (EM) parameters and electromagnetic wave (EMW) absorption, based on clear vacancy concentrations and/or various anion vacancies rather than semiempirical rules, is currently lacking but significantly desired. An anion‐doping‐induced vacancy engineering is pioneered, where the selective oxidation process upgrades the transformation from Co‐based precursor to S‐doped CoSe2 (System II) instead of Se‐doped CoS2 (System I) in the subsequent sulfuration/selenization, which results in vacancy level improvement and coexistence of sulfur vacancies (VS) and selenium vacancy (VSe). Thanks to the boosted dielectric polarization loss provided by the comparable coexistence of sulfur/selenium vacancies (VS/VSe = 0.52), S‐doped CoSe2 harvests a broad bandwidth of 9.25 GHz (8.75–18.00 GHz) at 2.42 mm. This feature almost simultaneously achieves 100% coverage for X‐, and Ku‐bands,…

Abstract Traditional microwaves absorption materials (MAMs) are applied in the form of coatings, generally inflexible, with high production costs and poor adaptability to applications in different locations. The diversification of application scenarios requires materials with multifunctionalities, but it is extremely challenging to integrate multifunctionalities within single material at present. Herein, a multifunctional CoNC@GN/PCL/TPU MAMs is synthesized. The CoNC@GN nano‐micro absorber has high‐efficiency microwave absorption ability. The electromagnetic microwave absorption performance is ultra‐light (4 wt.%), ultra‐thin (2.3 mm), and broadband (6.21 GHz), which is better than similar MAMs. Additionally, the samples have highly efficient electro‐thermal conversion properties, enabling controlled electrical heating performance and excellent self‐healing properties. More remarkably, the sample has an electrically driven shape memory effect that allows the material to target the absorption of multi‐angle incident electromagnetic waves. Therefore, CoNC@GN/PCL/TPU absorbers are the…

Abstract Separator modification has recently blossomed as an effective strategy to enable dendrite‐free Zn metal anodes. Nonetheless, the explored avenues are not conducive to mass production by far, and little attention is paid to the essence of separator regulation. Herein, a scalable Ti 3 C 2 T x MXene‐decorated Janus separator is designed by spray‐printing MXene nanosheets over one side of commercial glass fibre (GF). The thus‐derived MXene‐GF separator affords abundant surface polar groups, good electrolyte wettability, and high ionic conductivity, which is beneficial to homogenizing local current distribution and promoting Zn nucleation kinetics. It is noted that MXene‐GF displays adjustable dielectric constants with an optimized value of 53.5, offering a directional electrical field to expedite Zn‐ion flux and repel anions. Accordingly, dendrite‐free Zn anode equipped within symmetric cells can be achieved with MXene‐GF, enabling a stable cycling for 1180 h at 1 mA cm −2 and 1200 h at 5 mA cm −2 . More impressively, the assembled aqueous Zn‐ion battery full cell with Janus…

Abstract Owing to the sustainability, environmental friendliness, and structural diversity of biomass‐derived materials, extensive efforts have been devoted to use them as energy storage materials in high‐energy rechargeable batteries. A timely and comprehensive review from the structures to mechanisms will significantly widen this research field. Here, it starts with the operation mechanism of batteries, and it aims to summarize the latest advances for biomass‐derived carbon to achieve high‐energy battery materials, including activation carbon methods and the structural classification of biomass‐derived carbon materials from zero dimension, one dimension, two dimension, and three dimension. Each strategy starts with carefully selected examples and then moves to illustrate the underlying transport mechanism of electrons in the structure. In the end, challenges, strategies, and outlooks are pointed out for the future development of biomass‐derived carbon materials. Overall, this review will help researchers choose appropriate strategies to design biomass‐derived carbon materials,…

Abstract Efficient utilization of near‐infrared (NIR) light that takes a primary percentage of the solar spectrum is of great significance for practical applications of photocatalysis. However, development of singular NIR‐based photocatalysts still remains a grand challenge. Herein, a NIR‐based crystalline carbon nitride photocatalyst is proposed by using a molten‐salt assisted protocol with carbohydrazide as the oxygen‐containing precursor. Different from the doping strategy that always leads to structural damage and crystallinity decrease, structural oxygen arising from the special precursor itself is introduced into the framework of C3N4 with highly crystalline structure formed. The n→π* excitation is therefore activated with the absorption edge extended remarkably to 1400 nm. Theoretical calculations also reveal that the local internal electric field is simultaneously generated for promoting the charge separation/migration kinetics. Benefiting from structural oxygen incorporation and crystalline structure formation, the synthesized material shows a significantly enhanced…

Abstract Physical eutectogels are appealing materials for technological devices due to their superior ionic conductivity, thermal and electrochemical stability, non‐volatility, and low cost. Nevertheless, current physical eutectogels are suffering from weak mechanical strength and toughness. Here, taking advantage of the distribution difference of polyvinyl alcohol (PVA) in water and deep eutectic solvents (DESs), a simple and universal solvent‐replacement approach is proposed to regulate the spatiotemporal expression of intra/interpolymer interactions to prepare strong and tough physical eutectogels. The exchange of DESs with water can restrengthen the weakened interactions between PVA chains in water, enabling PVA to crystallize to construct a uniform and robust polymer network. Consequently, the resultant PVA eutectogel exhibits record‐high strength (20.2 MPa), toughness (62.7 MJ m –3 ), and tear‐resistance (tearing energy Σ42.4 kJ m –2 ), while possessing excellent stretchability (Σ550% strain), repairability, and adhesive performance. Furthermore, this strategy is proven to be…

Abstract As one of the fascinating high capacity cathodes, O3‐type layered oxides usually suffer from their intrinsic air sensitivity and sluggish kinetics originating from the spontaneous lattice Na extraction during air exposure and high tetrahedral site energy of Na + diffusion transition state. What is worse, the improvement on the two handicaps is hard to simultaneously realize because of the contradiction between Na containment suggested in air stability mechanism and enhanced Na diffusion mentioned in kinetics strategy. Herein, it is shown that a simple strategy of introducing proper Na vacancies into lattice can simultaneously realize a dual performance improvement. Na vacancies decrease the charge density on transitional metal ions and enhance the antioxidative capability of material, ensuring a stable lattice Na containment for Na 0.93 Li 0.12 Ni 0.25 Fe 0.15 Mn 0.48 O 2 when exposed to air. Additionally, more Na + diffusional sites and enlarged Na layer spacing are obtained and result in a significantly decreased energy barrier from ≈ 1000 to 300 meV and a high rate…

Abstract Nitrogen‐doped carbons are among the fastest‐growing class of materials used for oxygen electrocatalysis, namely, the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), thanks to their low cost, environmental friendliness, excellent electrical conductivity, and scalable synthesis. The perspective of replacing precious metal‐based electrocatalysts with nitrogen‐doped carbon is highly desirable for reducing costs in energy conversion and storage systems. In this review, the role of nitrogen and N‐induced structural defects on the enhanced performance of N‐doped carbon electrocatalysts toward the OER and the ORR as well as their applications for energy conversion and storage technologies is summarized. The synthesis of N‐doped carbon electrocatalysts and the characterization of their nitrogen functional groups and active sites for the conversion of oxygen are also reviewed. The electrocatalytic performance of the main types of N‐doped carbon materials for OER/ORR electrocatalysis are then discussed. Finally, major challenges and future opportunities of…

Abstract The modulation effect manifests an encouraging potential to enhance the performance of single‐atom catalysts; however, the in‐depth study about this effect for the isolated diatomic sites (DASs) remains a great challenge. Herein, a proximity electronic effect (PEE) of Ni/Co DASs is proposed that is anchored in N‐doped carbon (N‐C) substrate (NiCo DASs/N‐C) for synergistic promoting electrocatalytic oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). Benefiting from the PEE of adjacent Ni anchored by four nitrogen (Ni‐N 4 ) moiety, NiCo DASs/N‐C catalyst exhibits superior ORR and HER activity. In situ characterization results suggest Co anchored by four nitrogen (Co‐N 4 ) as main active site for O 2 adsorption‐activation process, which promotes the formation of key *OOH and the desorption of *OH intermediate to accelerate the multielectron reaction kinetics. Theoretical calculation reveals the adjacent Ni‐N 4 site as a modulator can effectively adjust the electronic localization of proximity Co‐N 4 site, promoting the *OH desorption and *H adsorption on…

Abstract Zinc ion hybrid supercapacitors (ZIHCs) with both high power density and high energy density have tremendous potential for energy storage applications such as hybrid electric vehicles and renewable energy storage. However, the large radius of hydrated Zn 2+ ions hampers their efficient storage in micropores with limited pore sizes, resulting in the limited gravimetric specific capacitance and inferior rate capability of ZIHCs. Therefore, it is critically important to understand to what extent pore size influences the storage of hydrated Zn 2+ ions in the pores with limited sizes. Herein, porous carbon nanosheets with different pore architectures are prepared using an ammonium chloride molten salt carbonization strategy. The influence of pore size on hydrated Zn 2+ ion storage in nanostructured carbon with divergent pore architectures is analyzed by electrochemical methods and molecular dynamic simulation. Micropores smaller than 6.0 Å obstruct the diffusion of hydrated Zn 2+ ions, while micropores larger than 7.5 Å exhibit a low diffusion energy barrier for the hydrated Zn…

Abstract Rechargeable aqueous Zn‐ion batteries (ZIBs) are always regarded as a promising energy storage device owing to their higher safety and durability. However, two problems have become the main trouble for the practical application of ZIBs such as the dendrite growth of Zn metal anode in electrolyte and the freezing of water solvent at low temperature. Herein, to overcome these challenges, a new strategy, multi‐component crosslinked hydrogel electrolyte, is proposed to inhibit Zn dendrites and realize low temperature environmental adaptability for ZIBs. Benefitting from the superior inhibition effect of the polyacrylamide and dimethyl sulfoxide (DMSO) on Zn dendrites, the coulombic efficiency of the symmetric cell of ≈99.5% is achieved during the Zn plating/stripping over 1 300 h, and the assembled full‐cell demonstrates the large specific capacity of 265.2 mAh g ‐1 and high cyclic stability with the capacity retention of 95.27% after 3 000 cycles. In addition, the full‐cell delivers stable operation at a wide temperature range, from 60 to −40 °C, due to the introduction of…

Abstract Green synthesis of urea under ambient conditions by electrochemical co‐reduction of N 2 and CO 2 gases using effective electrocatalyst essentially pushes the conventional two steps (N 2 + H 2 = NH 3 and NH 3 + CO 2 = CO(NH 2 ) 2 ) industrial process at high temperature and high pressure, to the brink. The single step electrochemical green urea synthesis process has hit a roadblock due to the lack of efficient and economically viable electrocatalyst with multiple active sites for dual reduction of N 2 and CO 2 gas molecules to urea. Herein, copper phthalocyanine nanotubes (CuPc NTs) having multiple active sites (such as metal center, Pyrrolic‐N3, Pyrrolic‐N2, and Pyridinic‐N1) as an efficient electrocatalyst which exhibits urea yield of 143.47 µg h –1 mg –1 cat and faradaic efficiency of 12.99% at –0.6 V versus reversible hydrogen electrode by co‐reduction of N 2 and CO 2 are reported. Theoretical calculation suggests that Pyridinic‐N1 and Cu centers are responsible to form CN bonds for urea by co‐reduction of N 2 to NN* and CO 2 to *CO, respectively. This study provides…

Abstract Since the first report of 3D printed biodegradable structures by stereolithography, vat photopolymerization has shown great potential in the fabrication of medical implants and devices. Despite its superior printing quality and manufacturing speed, the development of biodegradable devices by this technique remains challenging. This results from the conflicting viscosity requirements for the printing resins, i.e., low viscosity is required for high‐resolution 3D printing, whereas high viscosity is often needed to provide high mechanical strength. Recently emerging photopolymerization‐based 3D printing techniques, including heat‐assisted digital light processing (DLP) and volumetric printing, have brought new hope to the field. With its tolerance to high viscosity resins, heat‐assisted DLP enables the fabrication of complex, personalizes architectures from biodegradable photopolymers that are not printable by conventional printing techniques. On the other hand, volumetric printing, which abandons the layer‐by‐layer printing principle and thus circumvents the dependence on low…

Abstract The absorption frequency of conventional microwave absorbing materials (MAMs) is hardly tuned in operando, while such dynamic frequency regulation of MAMs is of great significance to meet the high demands of modern radars and intelligent electron devices. Here, an ingenious frequency‐tuning strategy by means of the pressure variations is developed by fabricating highly compressible carbon nanocoils/carbon foam (CNCs/CF) as a dynamically frequency‐tunable microwave absorber. Through adjusting the compression strain, the absorption bandwidth of CNCs/CF can be precisely tuned from S‐band (2−4 GHz) to Ku‐band (12−18 GHz). The adjustable effective absorption bandwidth is as wide as 15.4 GHz, which covers 96% of the entire microwave frequency. Under 10% compression strain, CNCs/CF shows an attractive bandwidth of 9.0 GHz and a strong reflection loss of −64.6 dB. Furthermore, the CNCs/CF also exhibit a good thermal insulation, strong hydrophobicity, and strain‐sensitive conductivity, endowing them with fascinating functions of heat insulation and self‐cleaning. The method of…

Abstract Herein, novel conductive composite hydrogels are developed with high stretchability, ultra‐softness, excellent conductivity, and good self‐healing ability. The hydrogels are formed in the water/glycerol binary solvent system, in which the polyaniline nanoparticles (PANI‐NPs) are incorporated into the poly(poly(ethylene glycol) methacrylate‐co‐acrylic acid) (P(PEG‐co‐AA)) scaffolds via the dynamically electrostatic interactions and hydrogen bonds. The PANI‐NPs serve as conductive fillers to assign conductivity to the hydrogel, while the enhanced interfacial interactions between the PANI‐NPs and P(PEG‐co‐AA) matrix endow the hydrogel with high stretchability (>1000%), low modulus (≈6 kPa), excellent elasticity (η = 0.07, energy loss coefficient at 500% strain), and fast self‐healing ability (93.3% after 10 mins). Particularly, the desirable anti‐freezing property is achieved by introducing a binary solvent system. The composite hydrogel‐based sensors are proposed, with the states‐independent properties, low detection limit (0.5% strain and 25 Pa), highly linear dependence,…

Abstract Unhealed wound after malignant skin tumor resection, characterized by full‐thickness cutaneous defects, large open cavities, and incomplete tumor tissue resection are the leading cause for long recovery times, poor prognoses, and high recurrence among patients. Herein, a hyaluronic acid (HA)‐based microneedle (MN) functionalized with biomineralized melanin nanoparticles is fabricated to concurrently administer tumor photothermal therapy (PTT) and promote skin tissue regeneration. Natural melanin nanoparticles derived from cuttlefish ink (CINP) possessing antioxidative and photothermal functionalities are employed to scavenge ROS and implement PTT. Further, CINPs are encapsulated within an amorphous silica shell that served as a source of bioactive to stimulate skin tissue regeneration. Due to the physical penetration characteristics of microneedles, the obtained CINP@SiO2‐HA MNs could exert photothermal eradication of the remaining subcutaneous tumor cells to avoid recurrence and inhibit Staphylococcus aureus infection in wound beds. Moreover, benefiting from ROS‐scavenging…

Abstract Given tunable hybridization structures in solid solutions, fascinating electromagnetic (EM) properties can be achieved for regulating EM wave (EMW) absorption. Herein, a novel metal–organic cooperative interactions method is proposed to manipulate the vacancy, interstitial, substitutional, and heterointerface structures in molybdenum disulfide (MoS2) solid solution simultaneously, thence meeting the synergistic polarization loss on various point and face sites. Assisted by the coordination between Cu2+ and polydopamine (PDA), the effect of Cu modification on MoS2 is highly improved, which further lead to polarization loss on S vacancy, interstitial Cu, substitutional N, and heterointerface between carbon and MoS2. Contributing to the synergetic effect among multiple polarizations, the Cu/C@MoS2 solid solution exhibit ultrahigh EMW absorption performance, of which EMA with twice PDA delivers the effective absorption bandwidth of 7.12 GHz and minimum reflection loss of −48.22 dB (2.5 mm). The energy attenuation of Cu/C@MoS2 improved almost 266.7% and 222.2% than C@MoS2 and…

Abstract Superamphiphobic coatings have wide application prospects in various fields, but suffer from low mechanical robustness. Although some strategies have been reported to solve the issue, it is still challenging for large‐scale preparation of robust superamphiphobic coatings via facile approaches. Here, a universal preparation method of mechanically robust superamphiphobic coatings by spraying a suspension containing silica nanoparticles decorated with perfluorodecyl polysiloxane and adhesive microparticles on various substrates have been reported. Phase separation of the adhesive avoids embedding of the nanoparticles in the adhesive by forming the nanoparticles@microparticles structure and meanwhile generates a reentrant tri‐tier hierachical micro‐/micro‐/nanostructure. Phase separation determines micromorphology, chemical composition, superamphiphobicity, and mechanical robustness of the coatings. Consequently, the coatings show excellent static and dynamic superamphiphobicity. Moreover, the coatings show excellent mechanical robustness because of the combined effects of the…

Abstract Passive radiative cooling technology provides a sustainable way of cooling by the combination of emitting heat to the cold universe and reflecting solar light without any energy input. However, the massive consumption of non‐degradable radiative cooling materials causes resource waste and environmental pollution. Meanwhile, the cooling efficiency can be easily affected by dirt contamination in outdoor environments. Here, by the combination of biomimetic hierarchical structure design and stereo‐complex crystals, a degradable and superhydrophobic (152°) stereo‐complex poly (lactic acid) aerogel with low thermal conductivity (37 mW m–1 K–1), high compression strength (0.1 MPa) and self‐cleaning ability via a simple water‐assisted thermally induced phase separation method is developed. The optimal aerogel has a high sunlight reflection (89%) and strong infrared emissivity (93%) that gets a temperature drop of 3.5 °C during the daytime and 5.8 °C during the nighttime. This aerogel opens an environmentally sustainable pathway to radiative cooling applications.

Abstract Solid oxide fuel cells (SOFCs) are efficient and fuel flexible electrochemical energy conversion devices that can power the future green society with regards to homes, cars, and even down to portable electronics. They do have the potential to become low cost, since no noble metals are used. Their broad commercialization, however, is hampered by the high operating temperatures of 700–900 ° C. Lowering the operating temperature of SOFCs is challenging as both the charge transport in the solid electrolyte and oxygen exchange reactions are thermally activated processes. Herein, the recent progress in the development of anode, electrolyte, and cathode materials to lower the operating temperature of SOFC below 600 ° C is summarized and the new opportunities, as well as challenges that remain to be solved, are discussed. The focus of this review is addressed to thin film SOFCs, sub‐micrometer SOFCs ( μ SOFCs) based on microelectromechanical systems, as well as devices based on proton‐conducting oxide electrolyte (protonic ceramic fuel cells), which are especially promising for…

Abstract Dual‐band electrochromism is a phenomenon where materials can independently regulate the transmittance of visible (VIS) and near‐infrared (NIR) light. Owing to their bistability, low energy consumption, and independent control over VIS and NIR regions, dual‐band electrochromic (EC) devices have been of great significance to fully harnessing VIS and NIR light and building an energy‐saving society. The past several years have witnessed the efforts put in developing novel EC materials to improve their dual‐band optical performance through altering their composition, structural, and physicochemical features, which determine the optical behavior of dual‐band EC devices. In this review, the concept, significance, working principle, and key influence factors of dual‐band electrochromism are briefly introduced. Next, the up‐to‐date progress of dual‐band EC materials including inorganic, organic, and composites materials are summarized, with a focus on material design, device fabrication, and performance optimization. Finally, the challenges and perspectives of dual‐band EC…

Abstract Frequent fire disasters have caused massive impacts to the environment, human beings, and the economy. MXene has recently been intensively researched as potential flame retardants to provide passive fire protection for other materials via its physical barrier and catalyzing carbonization effects. In parallel, MXene has also demonstrated a great promise for creating early fire warning sensors, which is an emerging field that has the potential to provide active fire response through its thermoelectric effect. This makes it possible to integrate passive fire retardancy and active fire warning into one MXene‐based fire protection system on demand. However, fulfilling these promises needs more research. Herein, an overview of passive flame‐retardant materials and next‐generation smart fire warning materials/sensors based on MXene and its derivatives is provided. This study reviews their conceptual design, characterization, modification principles, performances, applications, and mechanisms. A discussion of the challenges that need to be solved for their future practical…

Abstract Inspired by shape‐morphing organisms in nature, researchers have developed various hydrogels with stimuli‐responsive swelling, shrinking, bending, folding, origami, rolling, twisting, or locomotion. These smart hydrogels are usually created by patterning or 4D printing. The shape morphing of hydrogels allows the fabrication of helixing, twisting, and rolling microstructures, all of which are hard to reproduce directly by ordinary techniques. More importantly, under external stimuli (e.g., solvent, humidity, temperature, light, pH, and electric/magnetic fields), many hydrogels exhibit recoverable shape morphing and thus find promising applications in grippers, sensors, valves, soft robotics, etc. Since shape morphing determines the functions of hydrogels in a great number of cases, herein, recent advances of stimuli‐responsive hydrogels are summarized, with their types, shape‐morphing mechanisms, fabrication methods, shape‐morphing modes, and extensive applications covered. The conclusion and perspectives are also presented to guide the design and fabrication of functional…

Abstract Alkaline direct alcohol fuel cells (ADAFCs) represent an attractive alternative to hydrogen fuel cells for the more convenient storage, transportation, and lower cost of alcohols (e.g., methanol and ethanol) when compared with compressed hydrogen. However, the anode alcohol oxidation reaction (AOR) is generally plagued with high overpotential and sluggish kinetics, and often requires noble metal‐based electrocatalysts to accelerate the reaction kinetics. To this end, the development of efficient AOR electrocatalysts with high mass activity (MA), high durability, high Faradaic efficiency (FE), and low overpotential is central for realizing practical ADAFCs. Here, in this minireview, a brief introduction of the fundamental challenges associated with AOR in alkaline electrolyte, the key performance metrics, and the evaluation protocols for benchmarking AOR electrocatalysts are presented, followed by a summary of the recent advances in the noble‐metal based AOR electrocatalysts (e.g., Pt, Pd, and Rh) with an emphasis on the design criteria for improving the specific activity…

Abstract Nonprecious transition metal‐organic frameworks (MOFs) are one of the most promising precursors for developing electrocatalysts with high porosity and structural rigidity. This study reports the synthesis of high efficiency electrocatalysts based on S‐doped NiFeP. MOF‐derived S‐doped NiFeP structure is synthesized by a one‐step phosphorization process with using S‐doped MOFs as the precursor, which is more convenient and environment friendly, and also helps retain the samples’ framework. The oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) performance of the NiFeP catalysts can be improved after partially replacing P by S due to the tunable electronic structure. The optimized CCS‐NiFeP‐10 reaches a current density of 10 mA cm –2 for OER with an overpotential of 201 mV and outperforms most NiFe‐based catalysts. The S doping plays an important role in tuning the Δ G values for intermediates formation in Ni atoms to a suitable value and exhibits a pronouncedly improved the OER performance. CCS‐NiFeP‐20 sample presents excellent HER performance due to the…

Abstract The electrochemical performance of lithium‐sulfur (Li‐S) batteries is severely hindered by the sluggish sulfur redox kinetics and the shuttle effect of lithium polysulfides (LiPSs). Herein, an integrated composite catalyst consisting of Co nanoparticles and single‐atom (SA) Zn co‐implanted in nitrogen‐doped porous carbon nanosheets grafted with carbon nanotubes (Co/SA‐Zn@N‐C/CNTs) is rationally developed toward this challenge. Experimental and theoretical investigations indicate that the synergistically dual active sites of Co and atomic Zn‐N4 moieties with an optimal charge redistribution not only strongly confine the LiPSs but also effectively catalyze its conversion reactions by lowering the energy barrier from Li2S2 to Li2S while the N‐doped porous carbon‐grafted CNTs enables a large surface area for more active site exposure and provides a fast electron/ion pathway. Benefiting from synergies, Li‐S batteries equipped with the Co/SA‐Zn@N‐C/CNTs‐based sulfur cathode exhibit a high reversible capacity of 1302 mAh g−1 at 0.2 C and a low capacity fading rate of 0.033% per…

Abstract Carbon dots (CDs) present an enticing prospect for a variety of optical applications relying on their high photoluminescence (PL) quantum yield (QY). Herein, the synthesis, optical properties, structural characterizations, density‐functional theory (DFT) calculations, and potential applications of yellow‐emissive CDs (Y‐CDs) with ultra‐high PL QY are reported. Solvothermal treatment of citric acid and urea in toluene, followed by column chromatography, produces Y‐CDs exhibiting excitation‐independent PL emission at 553 nm with a high solution PL QY of 92%. A variety of optical and structural characterizations and DFT theoretical calculations are implemented to confirm the general structure and fluorescence origin of Y‐CDs, conjugated sp 2 ‐carbon domains (fused rings) with edge groups. Significantly, transparent Y‐CDs/acrylic resin films with strong solid‐state emissions are fabricated. The Y‐CD films exhibit a high fluorescence with PL QY of 98%, good PL stability (no PL variation under continuous irradiation for 180 h), and large Stokes shift (129 nm). The potential…

Abstract Optoelectronic synaptic devices, which combine the functions of photosensitivity and information processing, are essential for the development of artificial visual perception systems. Nevertheless, improving the paired pulse facilitation (PPF) index of optoelectronic synaptic devices, which is an urgent problem in the construction of high‐precision artificial visual perception systems, has received less attention so far. Herein, a light‐stimulated synaptic transistor (LSST) device with an ultra‐high PPF index ( ≈ 196%) is presented by introducing an ultra‐thin carrier regulator layer hexagonal boron nitride (h‐BN) into a classic graphene‐based hybrid transistor frame (graphene/CsPbBr 3 quantum dots). Crucially, analysis of the rate‐limiting effect of h‐BN on photogenerated carriers reveals the mechanism behind the LSST ultra‐high PPF index. Furthermore, a two‐layer artificial neural network connected by LSST devices demonstrate ≈ 91.5% recognition accuracy of handwritten digits. This work provides an effective method for constructing artificial visual perception systems…

Abstract Sluggish transport kinetics and rapid dendrite growth are considered the main obstacles that impair the performance of Zn metal batteries. This work has developed a unique strategy of dual‐interface engineering (DIE) to design the separator as efficient ions transport modulator. The dual function of spontaneous polarization effect and high zincophilicity of BaTiO 3 (BTO) is revealed by combining the theoretical and experimental studies. Benefiting from the decoration of BTO on glass fiber and well filling of the surface interspace, the DIE‐modified separator can not only effectively capture and accelerate Zn 2+ transport between the fiber–electrolyte interface, but also redistribute the ions transport into homogenization in the separator–anode interface. Therefore, the modified Zn anodes perform highly reversible Zn plating/stripping with ultrahigh cumulative capacity even up to 9500 mAh cm −2 at the high current density of 10 mA cm −2 . Meanwhile, the modified Zn‐MnO 2 battery can retain a specific capacity of 108 mAh g −1 after 1800 cycles at 1 A g −1 . Furthermore, the…

Abstract Metal‐organic frameworks (MOFs), an emerging class of porous organic‐inorganic hybrid materials, have shown great potential for water and wastewater treatment applications. However, pure MOF powders have limited practical applications in water treatment due to their insolubility, poor processability, brittleness, safety hazard from dust formation, and difficult separation from aqueous solutions. Thus, exploring potential MOFs composites with improved separation performance is of great importance. The marriage of MOFs with electrospun nanofiber with forethought into the final product's morphology, structure, and chemistry has opened up new opportunities for efficient wastewater treatment. The present review exhaustively summarizes the strategies to integrate MOFs into nanofibers via electrospinning to remove various pollutants (i.e., organic dyes, heavy metal ions, pharmaceuticals, personal care products, oily compounds, organic solvents, etc.) via adsorption, photodegradation, and membrane filtration. Besides, the most recent advances of electrospun MOF nanofibers for…

Abstract Direct seawater electrolysis is proposed as a potential low‐cost approach to green hydrogen production, taking advantage of the vastly available seawater and large‐scale offshore renewable energy being deployed. However, developing efficient, earth‐abundant electrocatalysts that can survive under harsh corrosive conditions for a long time is still a significant technical challenge. Herein, the fabrication of a self‐supported nickel‐iron phosphosulfide (NiFeSP) nanotube array electrode through a two‐step sulfurization/phosphorization approach is reported. The as‐obtained NiFeSP nanotubes comprise abundant NiFeS/NiFeP heterointerfaces and under‐coordinated metal sites, exhibiting outstanding activity and durability for the hydrogen and oxygen evolution reactions (HER and OER) in simulated alkaline‐seawater solution (KOH + NaCl), with an overpotential of 380 (HER) and 260 mV (OER) at 500 mA cm ‐2 and outstanding durability of 1000 h. Theoretical calculations support the observed outstanding performance, showing that the heterointerface and under‐coordinated metal sites…

Abstract Aqueous zinc metal batteries have garnered unprecedented attention owing to their high theoretical specific capacity, appropriate redox potential, and remarkable sustainability. Nevertheless, the intractable issues induced by the notorious Zn dendrite growth and serious interfacial side reactions significantly impede their large‐scale utilization. Inducing Zn to electrodeposit through parallel arrangement mode is critical to realizing dendrite‐free Zn metal anodes (ZMAs). To realize this purpose, a unique polymeric molecular design strategy through chemically grafting a thin polyanthraquinone (PAQ) overlayer on the Zn surface in the manner of spontaneous polymerization reaction of anthraquinone diazonium tetrafluoroborate (AQN 2 + BF 4 − ) is proposed firstly. Impressively, thus‐derived PAQ overlayer as an artificial protective layer can constrain the Zn 2+ ions 2D diffusion and homogenize the electric field and Zn 2+ ions concentration distribution, further guiding preferential growth along the Zn (002) plane. Assisted by the PAQ overlayer, the dendrite growth, H 2…

Abstract Conductive hydrogels have shown great promise in the field of sustainable power sources due to their unique features of sufficient flexibility, durability, and functional diversification. However, time‐ and energy‐consuming polymerization process and poor adaptability in extreme environments severely impede their practical application in such an emerging field. Herein, a facile and universal self‐catalytic system (AL‐Cu 2+ ) based on alkali lignin (AL) macromolecule has been designed to rapidly fabricate conductive and transparent organohydrogels in alkaline water–ethylene glycol (EG) binary solvent, which displays extreme environment applicability (‒40 to 60 °C), eligible stretchability (≈800% elongation), and robust self‐adhesion (≈31.4 kPa). Interestingly, the introduced EG accelerates the polymerization, endows extreme freezing/drying resistance, and improves self‐adhesion for the organohydrogels. The organohydrogel (water/EG = 2/3) that combines the above merits inspires the construction of triboelectric nanogenerator (O‐TENG) for mechanical energy harvesting and…

Abstract Artificial optoelectronic synapses with both electrical and light‐induced synaptic behaviors have recently been studied for applications in neuromorphic computing and artificial vision systems. However, the combination of visual perception and high‐performance information processing capabilities still faces challenges. In this work, the authors demonstrate a memristor based on 2D bismuth oxyiodide (BiOI) nanosheets that can exhibit bipolar resistive switching (RS) performance as well as electrical and light‐induced synaptic plasticity eminently suitable for low‐power optoelectronic synapses. The fabricated memristor exhibits high‐performance RS behaviors with a high ON/OFF ratio up to 10 5 , an ultralow SET voltage of ≈0.05 V which is one order of magnitude lower than that of most reported memristors based on 2D materials, and low power consumption. Furthermore, the memristor demonstrates not only electrical voltage‐driven long‐term potentiation, depression plasticity, and paired‐pulse facilitation, but also light‐induced short‐ and long‐term plasticity. Moreover, the…

Abstract Dual–single‐atom catalysts with synergistic effect of adjacent atomic metal sites show a great potential for oxygen reduction reaction (ORR). Herein, a dynamical synthetic strategy is demonstrated for the rational design of dual‐atom catalyst ((Zn, Cu)−NC) with non‐covalent Cu and Zn sites as nitrogen‐doped carbon as support. Owing to the non‐covalent interaction of Zn and Cu atomic pair sites, (Zn, Cu)−NC exhibits significant performances for ORR, surpassing the catalysts with individual Zn or Cu site. The theoretical calculations reveal that (Zn, Cu)−NC can highly activate the linear O2 molecule via the non‐covalent interaction between Zn and Cu pairs, providing the more effective overlap between the metal 3d orbitals and O 2p orbital. Therefore, the ORR activity is optimized with the improvement of the adsorption configuration and adsorption energy of O2. Further, both liquid and quasi‐solid zinc−air batteries with (Zn, Cu)−NC as air cathodes achieve remarkable energy density and stability. This research proposes a facile synthetic strategy to construct single‐atom…

Abstract Despite the substantial progress in cathode materials in the past few years, rechargeable zinc batteries (RZBs) are plagued by rapid performance degradation due to dendrite formation and notorious side reactions at the Zn anode side. Here, an optimized hydrated eutectic electrolyte (HEE) system containing methylsulfonylmethane, zinc perchlorate, and water, in which an organic ligand coordinated the solvation shell of Zn ions with water molecules constituting the eutectic network, is proposed. Compared to common aqueous solutions, this HEE system is proven effective in promoting the smooth Zn deposition and plating/stripping reversibility as well as suppressing side reactions. The vanadium‐based zinc batteries based on this new HEE exhibit exceptionally high‐capacity retention (≈100% retention even after 1600 cycles at a relatively small current density of 1000 mA g −1 ). This study offers a new type of electrolyte for RZBs and a deep understanding of the effect of Zn 2+ solvent sheath structure on the cycle reversibility.

Abstract Solar‐powered water evaporation is a straightforward, practical approach to use solar energy for water desalination. Solar absorbers made from photothermal materials capable of effectively confining heat and pumping water to the evaporation surface are essential for a high energy efficiency. However, separate designs of water transport routes and thermal insulating layers are required to simultaneously achieve desired water and thermal managements. This work reports an integrated design for efficient multifunctional capabilities through rational assembly of spectrally modified Ti3C2Tx (SM‐Ti3C2Tx) nanosheets and polyvinyl alcohol (PVA) into a multiscale 3D aerogel with a feather‐like microstructure. The aerogel contains longitudinal struts with transversely parallel ligaments developed at an angle of ≈60° from the struts, resembling the microstructure of down feathers in penguins and thus leading to excellent thermal insulation. The hydrophilic porous ligaments serve as upward water transport channels, pumping the water to the evaporation surface while confining it within…

Abstract Direct ink writing of liquid crystal elastomers (LCEs) offers a new opportunity to program geometries for a wide variety of shape transformation modes toward applications such as soft robotics. So far, most 3D‐printed LCEs are thermally actuated. Herein, a 3D‐printable photoresponsive gold nanorod (AuNR)/LCE composite ink is developed, allowing for photothermal actuation of the 3D‐printed structures with AuNR as low as 0.1 wt.%. It is shown that the printed filament has a superior photothermal response with 27% actuation strain upon irradiation to near‐infrared (NIR) light (808 nm) at 1.4 W cm −2 (corresponding to 160 °C) under optimal printing conditions. The 3D‐printed composite structures can be globally or locally actuated into different shapes by controlling the area exposed to the NIR laser. Taking advantage of the customized structures enabled by 3D printing and the ability to control locally exposed light, a light‐responsive soft robot is demonstrated that can climb on a ratchet surface with a maximum speed of 0.284 mm s −1 (on a flat surface) and 0.216 mm s −1 (on…

Abstract The rational fabrication of Pt‐free catalysts for driving the development of practical applications in alkaline water electrolysis and fuel cells is promising but challenging. Herein, a promising approach is outlined for the rational design of multimetallic catalysts comprising multiple active sites including Pd nanoclusters and Ru single atoms anchored at the defective sites of Ni(OH) 2 to simultaneously enhance hydrogen evolution reactions (HER) and ethanol oxidation reactions (EOR). Remarkably, Pd 12 Ru 3 /Ni(OH) 2 /C exhibits a remarkably reduced HER overpotential (16.1 mV@10 mA cm −2 with a Tafel slope of 21.8 mV dec −1 ) as compared to commercial 20 wt.% Pt/C (26.0 mV@10 mA cm −2 , 32.5 mV dec −1 ). More importantly, Pd 12 Ru 3 /Ni(OH) 2 /C possesses a self‐optimized overpotential to 12.5 mV@10 mA cm −2 after 20 000 cycles stability test while a significantly decreased performance for commercial 20wt.% Pt/C (64.5 mV@10 mA cm −2 after 5000 cycles). The mass activity of Pd 12 Ru 3 /Ni(OH) 2 /C for the EOR is up to 3.724 A mg PdRu −1 , ≈20 times higher than that of…

Abstract With the aggravation of global warming and extreme weather, cooling demand has witnessed a continuous increase and is expected to increase tenfold by 2050. Radiative sky cooling (RSC) without any pollution and energy consumption has drawn worldwide attention in the past few years. Large‐scale and scalable porous cooling materials have greatly advanced the progress of this technology. Herein, a critical review on porous cooling materials with the goal of advancing their commercial applications is presented. The detailed design principles of daytime radiative cooling are first discussed to clarify the critical factors of porous structures for great cooling performance. What follows are detailed discussions on porous cooling materials from pore‐forming methods. Subsequently, the recent progress of the promising particle‐embedding porous structures, mainly including white and colorful coolers for various applications, is outlined. Additionally, some special cooling materials are highlighted to further broaden the applications of RSC technology. Last but not the least, the…

Abstract Transition metal carbides/nitrides (MXenes) with metallic electrical conductivity and excellent processability attract increasing attention for assembling multifunctional macrostructures. However, the challenges, involving poor mechanical strength, inferior oxidation stability, and limited scalable manufacturing, impede their wide applications. Herein, the large‐area, high‐strength, ultra‐flexible hybrid films are developed through the multiple physical and chemical cross‐linking of MXene/cellulose films facilitated by graphene oxide. The MXene‐based films manifest significantly improved hydrophobicity, water/solvent resistance, and oxidation stability, and meanwhile, maintain excellent conductivity and electromagnetic interference shielding performance. The X‐band surface‐specific shielding effectiveness (SE) of 18,837.5 dB cm2 g−1 and an SE over 60 dB in an ultra‐broadband frequency range are achieved, comparable to the best shields ever reported. Furthermore, the wearable films demonstrate excellent photothermal antibacterial and electrothermal deicing applications.…

Abstract Platinum (Pt)‐based electrocatalysts are the benchmark catalysts for hydrogen evolution reaction (HER); however, they are limited by the scarcity and high price. Introducing an adequate substrate to disperse and anchor Pt‐based species is a feasible pathway to improve the utilization efficiency. Herein, a quick and continuous spray drying route is proposed to fabricate 3D crumpled Ti3C2Tx MXene loaded with sub‐nanometer platinum clusters (Pt/MXene). The 3D crumpled structure inhibits the restacking of layered MXene nanosheets and guarantees the fully exposure of Pt clusters. The as‐prepared catalyst exhibits excellent HER performances comparable to commercial Pt/C, including a low overpotential of 34 mV to reach a current density of 10 mA cm−2, a superior mass activity (1847 mA mgPt−1), a small Tafel slope (29.7 mV dec−1), and a high turnover frequency (10.66 H2 s−1). The improved activity of Pt/MXene can be attributed to the charge transfer from Pt clusters to MXene, which weakens the hydrogen adsorption, as evidenced by the density functional theory calculations. The…

Abstract Wearable sensors have drawn considerable interest for healthcare applications due to their low cost, flexibility, lightweight, and biocompatibility. Gold nanomaterials possess excellent properties such as high conductivity/flexibility, facile surface functionalization, biocompatibility, wide electrochemical sensing window, and extraordinary optical response, making them excellent candidates for wearable sensors. By implementing gold nanomaterials such as gold nanoparticles (AuNPs) and gold nanowires (AuNWs), great efforts are devoted to fabricate wearable sensors with rational designs for healthcare applications. This review focuses on recent advances in gold nanomaterials‐implemented wearable sensors, particularly the fabrication method, the working mechanism, and the performance of these wearable sensors in healthcare‐related applications. Wearable sensors including strain/pressure sensors, humidity/gas sensors, electrochemical sensors, and colorimetric sensors are discussed and highlighted. Meanwhile, future prospects and challenges are also discussed on the development…

Abstract Photocatalytic hydrogen peroxide (H 2 O 2 ) production from dioxygen and water is regarded as a promising technology since it can achieve sustainable and green solar‐to‐chemical energy conversion. Herein, oxygen and potassium dual‐heteroatom incorporated polymeric carbon nitride (O/KCN) is rationally designed for H 2 O 2 generation with an ultrahigh rate of 309.44 µM h −1 mg −1 , which surpasses that of other C 3 N 4 ‐based photocatalysts. The enhanced performance can be ascribed to the effective light absorption, fast charge transfer/separation, strong oxygen adsorption, and highly selective two‐electron oxygen reduction reaction (ORR). Density functional theory calculations further confirm that the obtained O/KCN is more favorable than others for electrons migrating from β spin‐orbital to π* orbitals of O 2 molecule, thus optimizing O 2 molecule activation to promote the formation of intermediate species *OOH and decrease the energy barrier of H 2 O 2 production. This work not only provides in‐depth insights for the photocatalytic H 2 O 2 generation mechanism, but also…

Abstract Advancing the development of electrocatalytic CO 2 reduction reaction (CO 2 RR) to address the environmental issues caused by excessive consumption of fossil fuels requires rational design of remarkable electrocatalysts, where the identification of active sites and further understanding of structure–performance relationship are the bases. However, the notable dynamic evolution often appears on the catalysts, with typical examples of Cu‐based catalysts, under operating conditions, causing great difficulty in identifying the real active sites and further understanding the correlations between structure and catalytic property. In this context, understanding the dynamic evolution process of catalytically active sites during CO 2 RR is of particular importance, which inspires to organize the present review. Herein, the fundamental principles of dynamic evolution in CO 2 RR including thermodynamics and kinetics aspects, followed by the introduction of operando techniques employed to probe the evolution under operating conditions are first highlighted. The dynamic evolution…

Abstract Scintillators with high light yield, low detection limit, large X‐ray attenuation efficiency as well as stable and nontoxic compositions are of great importance for radiation detection applications. Here, 0D (C 8 H 20 N) 2 Cu 2 Br 4 single crystals are obtained and show blue emission peaking at 468 nm with a near‐unity photoluminescence quantum yield of 99.7%, a large Stokes shift of 148 nm (i.e., negligible self‐absorption), and a good environmental stability along with strong X‐ray absorption capability. Moreover, a high light yield of up to ≈ 91 300 photons/MeV and a low detection limit of 52.1 nGy air s −1 are realized, which is more than one hundred times lower than the dose rate of 5.5 µGy air s −1 required for X‐ray medical diagnostics. (C 8 H 20 N) 2 Cu 2 Br 4 ceramic wafer scintillation screen is fabricated by a cold pressing sintering process, and the clear contrast images of opaque metal box and electronic component with a spatial resolution of 9.54 lp mm −1 are realized. This study not only designs a new lead‐free metal halide scintillator, but also develops a…

Abstract Impressive short‐circuit current density and fill factor have been achieved simultaneously in single‐junction organic solar cells (OSCs) with the emergence of high‐performance non‐fullerene acceptors. However, the power conversion efficiencies (PCEs) of OSCs still lag behind those of inorganic and perovskite solar cells, mainly due to the modest open‐circuit voltage ( V OC ) imposed by relatively large energy loss ( E loss ). Generally, E loss in solar cells can be divided into three parts. Among them, Δ E 1 is inevitable for all photovoltaic cells and depends on the optical bandgap of solar cells, while radiative recombination energy loss, Δ E 2 , in OSCs can approach the negligible value via finely matching donor with acceptor material in the blend. The relatively large non‐radiative recombination energy loss, Δ E 3 , becomes the main barrier to further reduce E loss and thus enhance PCE in non‐fullerene acceptor‐based OSCs. In this review, the recent studies and achievements about Δ E 3 in non‐fullerene acceptor‐based OSCs have been summarized from the aspects of…

Abstract Heteroatom doping engineering is desirable in tuning crystal structures and electrical properties, which is considered an opportunity to further develop microwave absorption materials. However, the competition mechanism and priority among doped atoms have not been revealed, which are insufficient to guide the most reasonable dielectric coupling model and design high‐performance absorbers. In this work, based on in situ N and O, ex situ S is introduced through external thermal driving, leading to fierce competition among anions. Specifically, S atoms replace pyrrole N, drive out lattice O, and create O vacancies, bringing more extensive local charge redistribution and stronger electron interaction, thus activating the defect‐induced polarization (3–6 times higher than conduction loss) in the middle/high‐frequency region. Therefore, the effective absorption bandwidth (EAB) of 9.03 GHz and the minimum reflection loss ( RL min ) of −64.05 dB at a filling rate of 10 wt.% are obtained, which improves the record of carbon absorbers as reported. Through macro‐designs, i.e.,…

Abstract Interfacial coupling strategy has allured extensive attention for the possibility to endow active electrode materials with superior performance. However, the design of strong coupling engineering with interfacial evolution during electrochemical processes is very challenging. Herein, inspired by the powerful robotic arms and density functional theory calculations, multiple functional groups identified with intense affinity to V atom are successfully grafted on carbon nanotubes (CNTs), thereby in situ building robust interfacial bonds (VOC and VC) to tightly anchor VS 4 particles. The largely decreased band gaps and energy barriers show the fortified conductivity of VS 4 ‐CNT heterostructure. Besides, the spacial confinement effect induced by interfacial linkages substantively enhances the mechanical properties to inhibit structural collapse, and restrains the dissolution of polysulfides as verified by molecular dynamics simulations, thus prolonging life span. Excellent energy density of 105.5 Wh kg –1 can be delivered after assembling full sodium‐ion capacitors…

Abstract Sluggish charge kinetics in photocatalysts and slow hole transfer in oxidation half‐reaction severely limit the photocatalytic activity of hydrogen evolution. ZnIn 2 S 4 with an asymmetrical layered structure of [S–In]–[S–In–S]–[Zn–S] unit cell is a promising material offering asymmetrical crystal polarization to overcome the limitation; however, the polarization‐induced internal electric field by this material remains largely unexplored. Herein, the polarization‐induced internal electric field of ZnIn 2 S 4 by engineering the polarity intensity in microscopic units is demonstrated for the first time. Specifically, ultrathin ZnIn 2 S 4 nanosheets are employed to establish a Ni 12 P 5 /ZnIn 2 S 4 ‐O (NP/ZIS‐O) system with powerful bulk and interface cascade electric field by the oxygen doping and ohmic junction. Enabled by such a design, the photogenerated electrons can rapidly migrate to NP active sites, suppressing the photogenerated electron‐hole pair recombination on ZIS‐O. To further overcome the inefficient hole transfer in oxidation half‐reaction, the preferential…

Abstract High strength, toughness, and conductivity are among the most sought‐after properties of flexible electronics. However, existing engineering materials find it difficult to achieve both excellent mechanical properties and high conductivity. To address this challenge, this study proposes a facile yet versatile strategy for preparing super‐tough conductive organo‐hydrogels via freeze‐casting assisted solution substitution (FASS). This FASS strategy enables the formation of organo‐hydrogels in one step with exquisite hierarchical anisotropic structures coupled with synergistic strengthening and toughening effects across multiple length scales. As an exemplary material, the prepared polyvinyl alcohol (PVA) organo‐hydrogel with solvent content up to 87 wt% exhibits a combination of high strength (6.5 MPa), high stretchability (1710% in strain), ultra‐high toughness (58.9 MJ m−3), as well as high ionic conductivity up to 6.5 S m−1 with excellent strain sensitivity. The exceptional combination of mechanical properties and conductivity makes the PVA organo‐hydrogel a promising…

Abstract The high‐throughput scalable production of inexpensive and efficient electrode materials at high current densities demanded by industry is a huge challenge for large‐scale implementation of energy storage technologies. Here, inspired by theoretical calculations that a FeS 2 /TiO 2 heterostructure with built‐in electric field (BEF) can reduce the reaction energy barrier and enhance charge transport, the scalable production of cheap FeS 2 /TiO 2 heterostructure is fabricated by utilizing natural ilmenite as precursor, exhibiting excellent electrochemical performances for sodium‐ion capacitors (SICs) anode. Assembling it with activated carbon (AC) cathode for SICs delivers high energy density (73.7 Wh kg −1 ) and high power density (10 kW kg −1 ) as well as outstanding cycle lifespan. Impressively, the method breaks through the traditional preparation approach by using natural minerals instead of high‐purity chemical raw materials as precursors for constructing heterojunctions, and price of the mineral is nearly five orders of magnitude lower than that of commercial chemical…