The 100 most-cited articles in Advanced Functional Materials, 2023

Abstract Growth in intermittent renewable sources including solar and wind has sparked increasing interest in electrical energy storage. Grid‐scale energy storage integrated with renewable sources has significant advantages in energy regulation and grid security. Aqueous zinc‐ion batteries (AZIBs) have emerged as a practically attractive option for electrical storage because of environmentally benign aqueous‐based electrolytes, high theoretical capacity of Zn anode, and significant global reserves of Zn. However, application of AZIBs at the grid‐scale is restricted by drawbacks in cathode material(s). Herein, a comprehensive summary of the features and storage mechanisms of the latest cathode materials is provided. The fundamental problems and corresponding in‐depth causes for cathode materials is critically reviewed. It is also assess practical challenges, appraise their translation to commerce and industry, and systematically summarize and discuss the potential solutions reported in recent works. It is established necessary design strategies for Zn anodes and electrolytes that are…

Abstract The Tauc plot is a method originally developed to derive the optical gap of amorphous semiconductors such as amorphous germanium or silicon. By measuring the absorption coefficient α ( hν ) and plotting versus photon energy hν , a value for the optical gap ( Tauc gap ) is determined. In this way non‐direct optical transitions between approximately parabolic bands can be examined. In the last decades, a modification of this method for (poly‐) crystalline semiconductors has become popular to study direct and indirect interband transitions. For this purpose, ( ahν ) n ( n = , 2) is plotted against hν to determine a value of the electronic bandgap . Due to the ease of performing UV–vis measurements, this method has nowadays become a standard to analyze various (poly‐) crystalline solids, regardless of their different electronic structure. Although this leads partially to widely varying values of the respective bandgap of nominally identical materials, there is still no study that critically questions which peculiarities in the electronic structure prevent a use of the Tauc plot…

Abstract Metamaterial absorbers have been widely studied and continuously concerned owing to their excellent resonance features of ultra‐thin thickness, light‐weight, and high absorbance. Their applications, however, are typically restricted by the intrinsic dispersion of materials and strong resonant features of patterned arrays (mainly referring to narrow absorption bandwidth). It is, therefore essential to reassert the principles of building broadband metamaterial absorbers (BMAs). Herein, the research progress of BMAs from principles, design strategies, tunable properties to functional applications are comprehensively and deeply summarized. Physical principles behind broadband absorption are briefly discussed, typical design strategies in realizing broadband absorption are further emphasized, such as top‐down lithography, bottom‐up self‐assembly, and emerging 3D printing technology. Diversified active components choices, including optical response, temperature response, electrical response, magnetic response, mechanical response, and multi‐parameter responses, are reviewed in…

Abstract Supercapacitors can harvest electrical energy from intermittent sources and transfer it quickly, but their specific energy must be raised if they are applied to efficiently power wearable and flexible electronics, as well as larger equipment. However, the remaining big gap between the lab research and practical applications seriously hinders the further progress of advanced supercapacitors, especially for electrode materials. Consequently, from a commercial/usable perspective, a clear guideline from lab research to commercialization is highly desired for bringing advanced supercapacitors from basic research into reality. This review focuses on the key factors of advanced supercapacitors from lab research to commercialization and summarizes recent progress in the field of supercapacitors as well as outlines key perspectives for future research. First, the several energy storage mechanisms are illustrated for building better supercapacitors. Then, the up‐to‐date key achievements and progresses of smart methods toward high‐energy supercapacitors and effective strategies for…

Abstract Recently, the need for miniaturization and high integration have steered a strong technical wave in developing (micro‐)electronic devices. However, excessive amounts of heat may be generated during operation/charging, severely affecting device performance and leading to life/property loss. Benefiting from their low density, easy processing and low manufacturing cost, thermally conductive polymer composites have become a research hotspot to mitigate the disadvantage of excessive heat, with potential applications in 5G communication, electronic packaging and energy transmission. By far, the reported thermal conductivity coefficient (λ) of thermally conductive polymer composite is far from expectation. Deeper understanding of heat transfer mechanism is desired for developing next generation thermally conductive composites. This review holistically scopes current advances in this field, while giving special attention to critical factors that affect thermal conductivity in polymer composites as well as the thermal conduction mechanisms on how to enhance the λ value. This review…

Abstract Metal–organic frameworks (MOFs) show captivating performances in many large‐scale applications including gas adsorption and separation, heat reallocation, water production, or remediation which can overcome important drawbacks of the conventionally used porous materials in the industry. This raises, therefore, the commercial interest in MOFs which brings the necessity to decrease the cost of their production, calling for the synthesis optimization from small‐scale to large‐scale. However, the commercial availability, yet very limited, is highly dependent on their production cost. Thus, to promote the commercial development and availability of MOFs, many steps can be taken. In this work, the state‐of‐art of the large‐scale production of MOFs can be first outlined, before discussing the criteria of greener MOF synthesis processes. Besides, a critical evaluation of the available synthesis routes for large‐scale production can be given, taking into consideration their cost, environmental impact, safety, and feasibility. Moreover, since there are strong limitations to the use in…

Abstract The rapid development of additive manufacturing has fueled a revolution in various research fields and industrial applications. Among the myriad of advanced 3D printing techniques, two‐photon polymerization lithography (TPL) uniquely offers a significant advantage in nanoscale print resolution, and has been widely employed in diverse fields, for example, life sciences, materials sciences, mechanics, and microfluidics. More recently, by virtue of the optical transparency of most of the resins used, TPL is finding new applications in optics and photonics, with nanometer to millimeter feature dimensions. It enables the minimization of optical elements and systems, and exploration of light‐matter interactions with new degrees of freedom, never possible before. To review the recent progress in the TPL related optical research, it starts with the fundamentals of TPL and material formulation, then discusses novel fabrication methods, and a wide range of optical applications. These applications notably include diffractive, topological, quantum, and color optics. With a panoramic…

Abstract Aqueous zinc ion batteries (AZIBs) with high safety, low cost, and eco‐friendliness advantages show great potential in large‐scale energy storage systems. However, their practical application is hindered by low Columbic efficiency and unstable zinc anode resulting from the side reactions and deterioration of zinc dendrites. Herein, tripropylene glycol (TG) is chosen as a dual‐functional organic electrolyte additive to improve the reversibility of AZIBs significantly. Importantly, ab initio molecular dynamics theoretical simulations and experiments such as in situ electrochemical impedance spectroscopy, and synchrotron radiation‐based in situ Fourier transform infrared spectroscopy confirm that TG participates in the solvation sheath of Zn 2+ , regulating overpotential and inhibiting side reactions; meanwhile, TG inhibits the deterioration of dendrites and modifies the direction of zinc deposition by constructing an adsorbed layer on the zinc anode. Consequently, a Zn‐MnO 2 full cell with TG electrolyte exhibited a specific capacity of 124.48 mAh g ‐1 after 1000 cycles at a…

Abstract The rational design of magnetic composites has great potential for electromagnetic (EM) absorption, particularly in the low‐frequency range of 2–8 GHz. However, the scalable synthesis of such magnetic absorbers with both high magnetic content and good dispersity remains challenging. In this study, a confined diffusion strategy is proposed to fabricate functional magnetic‐carbon hollow microspheres. Driven by the ferromagnetic enhanced Kirkendall diffusion effect, the in situ alloying of FeCo nanoparticles is tightly confined in carbon shells, effectively inhibiting magnetic agglomeration. Moreover, the core–shell FeCo–carbon nano‐units further assemble into dispersive microscale magnetic‐carbon Janus bulges on both the inner and outer surfaces of the hollow microsphere. The optimized hollow FeCo@C microspheres exhibit excellent low‐frequency EM wave absorption performance: the minimum reflection loss ( RL min ) is −35.9 dB, and the absorption bandwidth covers almost the entire C‐band. Systematic investigation reveals that the large size of the magnetic‐carbon integration,…

Abstract As one of the most electrochemical energy storage devices, lithium‐ion batteries (LIBs) remain the workhorse of the energy market due to their unparalleled advantages. Remarkably, Si‐based materials play a pivotal role in LIBs anodes owing to ultrahigh theoretical capacity of Si and rich natural resources. However, bulk silicon materials are difficult to meet the current commercial demand because of their low conductivity, sluggish reaction kinetics, and huge volume expansion. The construction of porous structures has been acknowledged as an effective way to solve the above issues. Herein, the delicate design of porous Si‐based anode materials including synthetic strategies, the engineering of surface morphology and micro/nano‐structure, and the regulation of different compositions, as well as their applications in LIBs is systematically summarized. Particularly, the fine engineering of different pore parameters for Si‐based materials is on focus. Importantly, the relationship between thick electrodes and tortuosity/porosity, and the structural effect between pores and…

Abstract Electrochemical reduction of nitrate to ammonia (NO3RR) holds a great promise for attaining both NH3 electrosynthesis and wastewater purification. Herein, single‐atom Bi alloyed Pd metallene (Bi1Pd) is reported as a highly effective NO3RR catalyst, showing a near 100% NH3‐Faradaic efficiency with the corresponding NH3 yield of 33.8 mg h−1 cm−2 at −0.6 V versus RHE, surpassing those of almost all ever reported NO3RR catalysts. In‐depth theoretical and operando spectroscopic investigations unveil that single‐atom Bi electronically couples with its neighboring Pd atoms to synergistically activate NO3− and destabilize *NO on Bi1Pd, leading to the reduced energy barrier of the potential‐determining step (*NO→*NOH) and enhanced protonation energetics of NO3−‐to‐NH3 pathway.

Abstract Ammonia as an irreplaceable chemical has been widely demanded to keep the sustainable development of the modern society. However, its industrial production consumes huge energy and releases extraordinary green‐house gases, leading to various environmental issues. To achieve the green production of ammonia is a great challenge that has been extensively pursued recently. In the review, a most promising strategy, electrochemical nitrate reduction reaction (e‐NO3RR) for the purpose is comprehensively investigated to give a full understanding of its development and mechanism and provide guidance for future directions. Particularly, the development of electrocatalysts is focused to realize the high ammonia yield rate and Faraday efficiency for industrial applications. The recent‐developed catalysts, including noble metallic materials, alloys, metal compounds, single‐metal‐atom catalysts, and metal‐free materials, are systematically discussed to review the effects of various factors on the catalytic performance in e‐NO3RR. Accordingly, the strategies, including defects…

Abstract Given the merits of affordable cost, superior low‐temperature performance, and advanced safe properties, sodium‐ion batteries (SIBs) have exhibited great development potential in large scale energy storage applications. Among various emerging carbonaceous anode materials applied for SIBs, hard carbon (HC) has recently gained significant attention regarding their relatively low cost, wide availability, and optimal overall performance. However, the insufficient initial Coulombic efficiency (ICE) of HC is the main bottlenecks, which is inevitably hindering their further commercial applications. Herein, an in‐depth holistic exposition about the reasons causing the unsatisfied ICE and the recent advances on effective improvement strategies are comprehensively summarized in this review, which have been divided into two aspects including the intrinsic property (degree of graphitization, pore structure, defect, et al.) and the extrinsic factor (electrolyte, electrode materials, et al.). In addition, future prospects and perspectives on HC to enable practical application in SIBs are…

Abstract Ammonia is not only an important feedstock for chemical industry but also a carbon‐free energy carrier and a safe storage media for hydrogen. Due to the advantages compared to Haber–Bosch process, electrochemical NO 3 − ‐to‐NH 3 conversion via nitrate reduction reaction (NO 3 − RR) received attention. Recently, “green hydrogen” generated from water electrolysis shows promise to become the energy for future but limited by the safety of storage and transportation. This review proposes electrochemical NO 3 − ‐to‐NH 3 conversion can store renewable electric energy and “green hydrogen” into NH 3 , which is a potential solution for solving the puzzle of “green hydrogen” storage and transportation. Moreover, the theoretical insights of NO 3 − RR and electrocatalyst design are discussed. Finally, the challenges and opportunities in this field are elucidated. This review provides a novel perspective for NO 3 − RR and accelerates the development of effective electrocatalysts for NO 3 − ‐to‐NH 3 conversion.

Abstract Organogels are an important class of gels, and are comparable to hydrogels owing to their properties as liquid‐infused soft materials. Despite the extensive choice of liquid media and compatible networks that can provide a broader range of properties, relatively few studies are reported in this area. This review presents the applicability of organogels concerning their choice of components, unique properties, and applications. Their distinctive features compared to other gels are discussed, including multi‐stimuli responses, affinity to a broad range of substances, thermal and environmental stability, electronic and ionic conductivity, and actuation. The active role of solvents is highlighted in the versatility of organogel properties. To differentiate between organogels and other gels, these are classified as gels filled with different organic liquids, including highly polar organic solvents and binary solvent systems. Most promising applications of organogels as sophisticated multifunctional materials are discussed in light of their unique features.

Abstract Halide perovskites, in the form of thin films and colloidal nanocrystals, have recently taken semiconductor optoelectronics research by storm, and have emerged as promising candidates for high‐performance solar cells, light‐emitting diodes (LEDs), lasers, photodetectors, and radiation detectors. The impressive optical and optoelectronic properties, along with the rapid increase in efficiencies of solar cells and LEDs, have greatly attracted researchers across many disciplines. However, most advances made so far in terms of preparation (colloidal nanocrystals and thin films), and the devices with highest efficiencies are based on Pb‐based halide perovskites, which have raised concerns over their commercialization due to the toxicity of Pb. This has triggered the search for lower‐toxicity Pb‐free halide perovskites and has led to significant progress in the last few years. In this roadmap review, researchers of different expertise have joined together to summarize the latest progress, outstanding challenges, and future directions of Pb‐free halide perovskite thin films and…

Abstract As the dominant means of energy storage technology today, the widespread deployment of lithium‐ion batteries (LIBs) would inevitably generate countless spent batteries at their end of life. From the perspectives of environmental protection and resource sustainability, recycling is a necessary strategy to manage end‐of‐life LIBs. Compared with traditional hydrometallurgical and pyrometallurgical recycling methods, the emerging direct recycling technology, rejuvenating spent electrode materials via a non‐destructive way, has attracted rising attention due to its energy efficient processes along with increased economic return and reduced CO 2 footprint. This review investigates the state‐of‐the‐art direct recycling technologies based on effective relithiation through solid‐state, aqueous, eutectic solution and ionic liquid mediums and thoroughly discusses the underlying regeneration mechanism of each method regarding different battery chemistries. It is concluded that direct regeneration can be a more energy‐efficient, cost‐effective, and sustainable way to recycle spent LIBs…

Abstract Supercapacitors offer superior energy storage capabilities than traditional capacitors, making them useful for applications such as electric vehicles and rapid large‐scale energy storage. The energy storage performance of these devices relies on electrical double‐layer capacitance and/or pseudocapacitance from rapid reversible redox reactions. Metal–organic frameworks (MOFs) have recently emerged as a new class of electrode materials with promising supercapacitor performances and capacitances that exceed those of traditional materials. However, the comparison of the supercapacitor performance of a porous carbon and a state‐of‐the‐art MOF highlights a number of challenges for MOF supercapacitors, including low potential windows, limited cycle lifetimes, and poor rate performances. It is proposed that the well‐defined and tuneable chemical structures of MOFs present a number of avenues for improving supercapacitor performance. Recent experimental and theoretical work on charging mechanisms in MOF‐based supercapacitors is also discussed, and it is found that there is a need…

Abstract Ionogels, composed of ionic liquids and supporting networks, possess a plethora of exceptional properties, including nonvolatility, remarkable thermal and electrochemical stability, elevated mechanical strength, as well as outstanding ionic conductivity. Based on these extraordinary characteristics, ionogels have found extensive applications in diverse fields encompassing functional materials, sensors, soft electronics, solid electrolytes, and biomedicine. In recent years, ionogels have witnessed significant advancements and emerged as a highly popular subject matter. Consequently, this review provides a comprehensive overview of the latest progress made in the realm of ionogels. The preparation methods of ionogels are initially introduced following a concise introduction. Subsequently, the properties of ionogels, encompassing mechanical properties, high and low temperature resistance, ionic conductivity, stimuli‐response properties, self‐healing properties, recyclability and their structure‐property relationships, are comprehensively discussed. Moreover, recent…

Abstract Harnessing the physiochemical properties and enzymatic activities of nanozymes will provide new insights for disease theranostics. Herein, a novel carbon dot (C‐dot) superoxide dismutase (SOD) nanozyme that exhibits red fluorescence with emission wavelength of 683 nm and shows high SOD‐like activity of >4000 U mg −1 is reported, which presents the great potential for imaging the biodistribution of nanozyme itself in vivo and ameliorating acute lung injury. Through surface modifications, the mechanism of C‐dot SOD nanozyme activity is revealed to be relied on their surface functional groups which bind with superoxide radicals, promote the electron transfer between C‐dots and superoxide radicals, and finally accelerate the dismutation of superoxide radicals. The absolute quantum yield of ≈14% of red fluorescence C‐dot nanozyme endow it bioimaging in vitro and in vivo. Moreover, the C‐dot nanozyme effectively enters the cells, accumulates at mitochondria, and protects living cells from oxidative damage by scavenging reactive oxygen species (ROS) and reducing the levels of…

Abstract For mass production of hydrogen fuel by electrochemical water splitting, seawater is preferred because of its abundant reserves on Earth. However, the current seawater electrolysis technology is seriously hindered by the low selectivity and poor stability of oxygen evolution reaction (OER) at anode due to undesirable chloride electrochemistry and severe corrosion in practical application. Herein, based on the “work function optimization” concept, vein‐like Cr‐doping CoxP is rationally designed as a highly‐efficient OER electrocatalyst for direct seawater electrolysis, achieving current densities of 20 and 100 mA cm–2 at overpotentials of 268 and 325 mV, respectively, together with high OER selectivity and long‐term stability. Experimental data and theoretical calculations reveal that the regulation of the electronic structure of CoxP induced by Cr doping strongly alleviates the work function of CoxP, which not only accelerates the electron transfer between the catalyst surface and the absorbates but also lowers the energy barriers of water dissociation and rate‐determining…

Abstract Surface chemistry and interlayer engineering determines the electrical properties of 2D MXene. However, it remains challenging to regulate the surface and interfacial chemistry of MXene simultaneously. Herein, simultaneous modulation of Ti 3 C 2 T x MXene surface termination and layer spacing by alkali treatment are achieved. The electrical and electromagnetic properties of Ti 3 C 2 T x are investigated in detail with respect to KOH and ammonia concentration dependence. A high concentration of KOH caused the Ti 3 C 2 T x layer spacing to expand to 13.7 Å and the surface O/F ratio to increase to 33.84. Because of its weaker ionization effect, ammonia provides finer tuning compared to the drastic intercalation of KOH with a thorough sweeping of the F‐containing groups. Ti 3 C 2 T x is enriched with conductive ‐OH termination after ammonia treatment, which achieves an effective balance with the increased interlayer resistance. Therefore, NH 3 H 2 O‐Ti 3 C 2 T x achieves broad‐band impedance matching and exhibits an efficient microwave loss of −49.1 dB at a low thickness of 1.7…

Abstract Dielectric capacitors with high power densities are crucial for pulsed electronic devices and clean energy technologies. However, their breakdown strengths ( E b ) strongly limit their power densities. Herein, by modifying the interfacial polarization by adjusting the difference in activation energies (Δϕ) between the grain and grain boundary phases, the significant enhancement of E b in the (1‐ x )(0.94Na 0.5 Bi 0.5 TiO 3 ‐0.06BaTiO 3 )‐ x Ca 0.7 La 0.2 TiO 3 (NBT‐BT‐ x CLT, x = 0, 0.18, 0.23, 0.28, 0.33, 0.38, and 0.43) ceramics is achieved. The results indicate that adding CLT introduces a super‐paraelectric state, refines grain size, and, most importantly, decreases the Δϕ value. When Δϕ is tuned close to zero in the specific NBT‐BT‐0.38CLT sample, a significant boost in E b value of 64 kV mm −1 is obtained. As a result, the recoverable energy storage density of the ceramics reaches an unprecedented giant value of 15.1 J cm −3 together with a high efficiency of 82.4%, as well as ultrafast discharge rate of 32 ns, and high thermal and frequency stability. The results…

Abstract Constructing MOF‐on‐MOF heterojunction with elaborate charge transfer mechanism and interface is a promising strategy for improving the photocatalytic properties of MOFs. Herein, a Step‐scheme (S‐scheme) MIL‐125‐NH2@CoFe Prussian blue analogue (PBA) heterojunction is reported for the first time. The MOF‐on‐MOF heterostructure exhibits a sandwich‐like morphology with hollow CoFe PBA nanocages selectively assembled on the top‐down surfaces of MIL‐125‐NH2 nanocakes. Experimental findings and theoretical simulation results reveal the formation of internal electric field via interfacial TiOCo bonds at the heterojunction, providing driving force and atomic transportation highway for accelerating the S‐scheme charge transfer and enhancing the redox performance. Contributed further by the hollow sandwich‐like structures with increased active site exposure, the designed MOF‐on‐MOF heterojunction exhibits significantly enhanced photocatalytic activity for degradation of various organic pollutants. This study provides insights toward the rational design of semiconducting MOF‐based…

Abstract Shape memory polymers (SMPs) are one of the primary directions in the development of modern high‐tech new materials, which are integrated with sensing, actuation, information processing, and autonomous deformation. Here, multifunctional shape memory polymers are focused and a detailed introduction to the characteristics of self‐deformation, self‐sensing, self‐healing, and self‐learning is provided. Integrating with other functional materials to form shape memory polymer composites (SMPC), designing and controlling the material structure and organization at the microscale, thereby achieving more precise and controllable shape memory effects and expanding the potential of material applications. Ultimately, it is shown that SMPs and their composites have a wide range of fascinating applications in the fields of robotics, smart clothing, smart textiles, biomedical devices, and wearable technology. SMPs will thus continue to play a significant role in future deeper exploration.

Abstract Oxygen evolution reaction (OER) remains a bottleneck for electrocatalytic water‐splitting to generate hydrogen. However, the traditional adsorbed evolution mechanism (AEM) possesses sluggish reaction kinetics due to the scaling relationship, while lattice oxygen mechanism (LOM) triggers an unstable structure due to the escaping of lattice oxygen. Herein, a proof‐of‐concept Fe‐Co(OH) 2 /Fe 2 O 3 heterostructure is put forward, where Fe‐Co(OH) 2 following AEM can complete rapidly deprotonation process while Fe 2 O 3 following LOM can trigger O─O coupling step. Combining the theoretical and experimental investigation confirmed that the redistributed space‐charge of Fe‐Co(OH) 2 /Fe 2 O 3 junction can optimize synergistically adsorbed and lattice oxygen, the coupling mechanism of AEM and LOM can facilitate synchronously the OER activity and stability. As a result, the Fe‐Co(OH) 2 /Fe 2 O 3 heterostructure shows excellent OER performance with low overpotential of only 219 and 249 mV to reach a current density of 10 and 100 mA cm −2 . Specifically, the Fe‐Co(OH) 2 /Fe 2 O 3…

Abstract Tactile sensing technology is crucial for soft grippers. Soft grippers equipped with intelligent tactile sensing systems based on various sensors can interact safely with the unstructured environments and obtain precise properties of objects (e.g., size and shape). It is essential to develop state‐of‐the‐art sensing technologies for soft grippers to handle different grasping tasks. In this review, the development of tactile sensing techniques for robotic hands is first introduced. Then, the principles and structures of different types of sensors normally adopted in soft grippers, including capacitive tactile sensors, piezoresistive tactile sensors, piezoelectric tactile sensors, fiber Bragg grating (FBG) sensors, vision‐based tactile sensors, triboelectric tactile sensors, and other advanced sensors developed recently are briefly presented. Furthermore, sensing modalities and methodologies for soft grippers are also described in aspects of force measurement, perception of object properties, slip detection, and fusion of perception. The application scenarios of soft grippers…

Abstract Lithium‐ion batteries with their portability, high energy density, and reusability are frequently used in today's world. Under extreme conditions, lithium‐ion batteries leak, burn, and even explode. Therefore, improving the safety of lithium‐ion batteries has become a focus of attention. Researchers believe using a solid electrolyte instead of a liquid one can solve the lithium battery safety issue. Due to the low price, good processability and high safety of the solid polymer electrolytes, increasing attention have been paid to them. However, polymer electrolytes can also decompose and burn under extreme conditions. Moreover, lithium dendrites are formed continuously due to the uneven charge distribution on the surface of the lithium metal anode. A short circuit caused by a lithium dendrite can cause the battery to thermal runaway. As a result, the safety of polymer solid‐state batteries remains a challenge. In this review, the thermal runaway mechanism of the batteries is summarized, and the batteries abuse test standard is introduced. In addition, the recent works on the…

Abstract Aqueous zinc‐ion batteries (ZIBs) with metallic Zn anodes have emerged as promising candidates for large‐scale energy storage systems due to their inherent safety and competitive capacity. However, challenges of Zn anodes, including dendrite growth and side reactions, impede the commercialization of ZIBs. The regulation of the Zn/electrolyte interphase is a feasible method to achieve high‐performance ZIBs with prolonged lifespan and high reversibility. Considering the as‐made artificial interphase is the result of a combination of protection materials, protection mechanisms, and construction techniques, this review comprehensively summarizes the recent progress of interphase modulation and provides a systematic guideline for constructing ideal artificial layers. In addition to revealing the entanglement relationship between the failure behaviors of Zn anodes and timely concluding the emerging protection mechanisms for stable Zn/electrolyte interphase, this review also evaluates the constructing techniques in regard of commercialization, including engineering workflow,…

Abstract Vanadium‐based intercalation materials have attracted considerable attention for aqueous zinc‐ion batteries (ZIBs). However, the sluggish interlaminar diffusion of zinc ions due to the strong electrostatic interaction, severely restricts their practical application. Herein, oxygen vacancy‐enriched V 2 O 5 structures (Zn 0.125 V 2 O 5 ·0.95H 2 O nanoflowers, O v ‐ZVO) with expanded interlamellar space and excellent structural stability are prepared for superior ZIBs. In situ electron paramagnetic resonance (EPR) and X‐ray diffraction (XRD) characterization revealed that numerous oxygen vacancies are generated at a relatively low reaction temperature because of partially escaped lattice water. In situ spectroscopy and density functional theory (DFT) calculations unraveled that the existence of oxygen vacancies lowered Zn 2+ diffusion barriers in O v ‐ZVO and weakened the interaction between Zn and O atoms, thus contributing to excellent electrochemical performance. The Zn||O v ‐ZVO battery displayed a remarkable capacity of 402 mAh g −1 at 0.1 A g −1 and impressive energy…

Abstract Developing low‐cost and high‐efficient bifunctional catalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is greatly significant for water electrolysis. Here, Ni 3 N‐CeO 2 /NF heterostructure is synthesized on the nickel foam, and it exhibits excellent HER and OER performance. As a result, the water electrolyzer based on Ni 3 N‐CeO 2 /NF bifunctional catalyst only needs 1.515 V@10 mA cm −2 , significantly better than that of Pt/C||IrO 2 catalysts. In situ characterizations unveil that CeO 2 plays completely different roles in HER and OER processes. In situ infrared spectroscopy and density functional theory calculations indicate that the introduction of CeO 2 can optimizes the structure of interface water, and the synergistic effect of Ni 3 N and CeO 2 improve the HER activity significantly, while the in situ Raman spectra reveal that CeO 2 accelerates the reconstruction of O V (oxygen vacancy)‐rich NiOOH for boosting OER. This study clearly unlocks the different catalytic mechanisms of CeO 2 for boosting the HER and OER activity of Ni 3 N for…

Abstract Rechargeable sodium‐ion batteries (SIBs) are emerging as a viable alternative to lithium‐ion battery (LIB) technology, as their raw materials are economical, geographically abundant (unlike lithium), and less toxic. The matured LIB technology contributes significantly to digital civilization, from mobile electronic devices to zero electric‐vehicle emissions. However, with the increasing reliance on renewable energy sources and the anticipated integration of high‐energy‐density batteries into the grid, concerns have arisen regarding the sustainability of lithium due to its limited availability and consequent price escalations. In this context, SIBs have gained attention as a potential energy storage alternative, benefiting from the abundance of sodium and sharing electrochemical characteristics similar to LIBs. Furthermore, high‐entropy chemistry has emerged as a new paradigm, promising to enhance energy density and accelerate advancements in battery technology to meet the growing energy demands. This review uncovers the fundamentals, current progress, and the views on the…

Abstract High‐performance elastomers are expected to possess excellent healing and recycling ability, damage resistance in conjunction with high strength and toughness. Herein, a dual dynamic crosslinking strategy is implemented by multiple hydrogen and disulfide bonds to obtain a novel amorphous and transparent polyurethane/nanocellulose elastomer with excellent self‐healing, self‐reinforcing and toughening performance. First, hydrogen bonds are introduced in TEMPO‐oxidized cellulose nanofibers (TCNF) by modification with 2‐ureido‐4[1H]‐pyrimidone (UTCNF), while disulfide bonds (SS) are introduced in the polyurethane (PU) main chain, leading to the formation of dual dynamic cross‐linking networks. The PU‐SS‐UTCNF elastomer can fully self‐heal within 4.0 h at 50 °C. Surprisingly, for the first time, the PU‐SS‐UTCNF elastomer also self‐strengthens and self‐toughens after multiple hot‐pressing, with tensile strength and toughness that increase by up to 401% and 257% compared to original elastomer samples, up to 50.0 MPa and 132.5 MJ m ‐3 . The self‐strength and self‐toughening effects…

Abstract The large‐scale deployment of aqueous Zn‐ion batteries is hindered by Zn anode instability including surface corrosion, hydrogen gas evolution, and irregular Zn deposition. To tackle these challenges, a polyhydroxylated organic molecular additive, trehalose, is incorporated to refine the solvation structure and promote planar Zn deposition. Within solvation structure regions involving trehalose, the hydroxy groups participate in the reconstruction of hydrogen bond networks, which increases the overpotential for water decomposition reaction. Moreover, at the Zn metal–molecule interface, the chemisorption of trehalose onto the surface of the zinc anode enhances corrosion resistance and facilitates the deposition of zinc in a planar manner. The optimized electrolyte significantly improves Zn striping/plating reversibility and maintains stable potentials over 1600 h at 5 mA cm −2 with a cutoff capacity of 1 mA h cm −2 in symmetric cells. When combined with the MnO 2 cathode, the assembled coin cell retains ≈89% of its capacity after 1000 cycles. This organic molecule additive,…

Abstract Core–shell nanostructures have received widespread attention because of their potential usage in various technological and scientific fields. However, they still face significant challenges in terms of fabrication of core–shell nanostructure libraries on a controlled, and even programmed scale. This study proposes a general approach to systematically fabricate core–shell nanohybrids using liquid‐metal Ga alloys as reconfigurable templates, and the initiation of a local galvanic replacement reaction is demonstrated utilizing an ultrasonic system. Under ultrasonic agitation, the hydrated gallium oxides generated on the liquid metal droplets, simultaneously delaminated themselves from the interfaces. Subsequently, single‐metal or bimetallic components are deposited on fresh smooth Ga‐based alloys via galvanic reactions to form unique core–shell metal/metal nanohybrids. Controlled and quantitative regulation of the diversity of the non‐homogeneous nanoparticle shell layer composition is achieved. The obtained core–shell nanostructures are used as efficient microwave absorbers…

Abstract The practicality of aqueous zinc ion batteries (AZIBs) for large‐scale energy storage is hindered by challenges associated with zinc anodes. In this study, a low‐cost and multi‐function electrolyte additive, cetyltrimethyl ammonium bromide (CTAB), is presented to address these issues. CTAB adsorbs onto the zinc anode surface, regulating Zn2+ deposition orientation and inhibiting dendrite formation. It also modifies the solvation structure of Zn2+ to reduce water reactivity and minimize side reactions. Additionally, CTAB optimizes key physicochemical parameters of the electrolyte, enhancing the stability of the electrode/electrolyte interface and promoting reversibility in AZIBs. Theoretical simulations combined with operando synchrotron radiation‐based in situ Fourier transform infrared spectra and in situ electrochemical impedance spectra further confirm the modified Zn2+ coordination environment and the adsorption effect of CTAB cations at the anode/electrolyte interface. As a result, the assembled Zn‐MnO2 battery demonstrates a remarkable specific capacity of 126.56 mAh…

Abstract Aqueous zinc‐ion batteries (ZIBs) are considered as the promising candidate of flexible energy storage devices due to their high safety, eco‐friendliness, and low‐cost. However, conventional flexible aqueous ZIBs undergo severe capacity loss at bending and subzero temperature states. Herein, an anti‐freezing hydrogel electrolyte based on zinc tetrafluoroborate (Zn(BF 4 ) 2 ) and polyacrylamide (PAM) is developed. Owing to the strong electronegativity of F atoms, BF 4 − anions interact with water molecules by OH···F to replace the OH···O between water molecules in Zn(BF 4 ) 2 ‐PAM hydrogel electrolyte, inhibiting the formation of ice crystal lattice in hydrogel electrolyte at low‐temperature. Therefore, the Zn(BF 4 ) 2 ‐PAM hydrogel remains unfrozen state, good flexibility, and high ionic conductivity even at −70 °C, which ensures that they can act as the electrolytes of anti‐freezing flexible ZIBs. As a proof of concept, anti‐freezing flexible ZIBs with all‐in‐one integrated configuration are assembled based on Zn(BF 4 ) 2 ‐PAM hydrogel. They display enhanced…

Abstract Poly(vinylidene fluoride) (PVDF)‐based polymers demonstrate great potential for applications in flexible and wearable electronics but show low piezoelectric coefficients (e.g., − d 33 < 30 pC N −1 ). The effective improvement for the piezoelectricity of PVDF is achieved by manipulating its semicrystalline structures. However, there is still a debate about which component is the primary contributor to piezoelectricity. Therefore, current methods to improve the piezoelectricity of PVDF can be classified into modulations of the amorphous phase, the crystalline region, and the crystalline–amorphous interface. Here, the basic principles and measurements of piezoelectric coefficients for soft polymers are first discussed. Then, three different categories of structural modulations are reviewed. In each category, the physical understanding and strategies to improve the piezoelectric performance of PVDF are discussed. In particular, the crucial role of the oriented amorphous fraction at the crystalline–amorphous interface in determining the piezoelectricity of PVDF is emphasized. At…

Abstract Conductive hydrogels (CHs) for flexible bioelectronic devices have raised great attention due to their tunable mechanical performances, adhesion, anti‐swelling, and biocompatibility. This review summarizes the current development of conductive hydrogel‐based flexible bioelectronic devices in the aspect of classifications and applications. Firstly, the conductive hydrogels are classified into two kinds according to the types of conductivity: ionic conductive hydrogels and electronic conductive hydrogels (hydrogel based on pure conductive materials, introducing conductive micro/nano‐materials). Secondly, the applications of conductive hydrogels for bioelectronic device, like wearable devices (strain sensor, body fluid detector, serviced in extreme environment), tissue engineering (skin, heart, nerve, muscle), and other applications (bionic robot, cancer treatment), are highly illustrated. Finally, a depth outlook is given, which aims to promote the development of this field in the future.

Abstract It is an urgent need that defect repair can develop from simple device fixation to living tissue reconstruction, from short life function replacement to permanent regeneration repair. At present, bone transplantation has become the second largest transplantation surgery after blood transfusion, and artificial bone transplantation generates great hope for the repair and treatment of bone defect. In order to repair bone defect, artificial bone must have good biological properties and sufficient mechanical properties, and it should also have the shape matching to bone defect site and the connected porous structure. For structures and properties requirements of artificial bone, in this review three major challenges faced by artificial bone transplantation are systemtically analyzed and current methods and strategies to address these issues are discussed: 1) the need for developing a type of bone scaffold material with both biological and mechanical properties, 2) the need for realizing the controllable fabrication of individual shape and multistage pore structure of bone…

Abstract MXene aerogels have shown great potential for many important functional applications, in particular electromagnetic interference (EMI) shielding. However, it has been a grand challenge to create mechanically hyperelastic, air‐stable, and durable MXene aerogels for enabling effective EMI protection at low concentrations due to the difficulties in achieving tailorable porous structures, excellent mechanical elasticity, and desired antioxidation capabilities of MXene in air. Here, a facile strategy for fabricating MXene composite aerogels by co‐assembling MXene and cellulose nanofibers during freeze‐drying followed by surface encapsulation with fire‐retardant thermoplastic polyurethane (TPU) is reported. Because of the maximum utilization of pore structures of MXene, and conductive loss enhanced by multiple internal reflections, as‐prepared aerogel with 3.14 wt% of MXene exhibits an exceptionally high EMI shielding effectiveness of 93.5 dB, and an ultra‐high MXene utilization efficiency of 2977.71 dB g g−1, tripling the values in previous works. Owing to the presence of…

Abstract Wound with drug‐resistant bacterial infections has become a serious challenge for the healthcare system, and designing wound dressing to self‐adapt to the need of different stage of wound healing remains challenging. Herein, self‐adaptive wound dressings with multiple stimuli‐responsiveness and antibacterial activity are developed. Specifically, MoS 2 carrying a reactive oxygen species (ROS) responsive nitric oxide (NO) release precursor L‐arginine (MSPA) is designed and incorporated into carboxymethyl chitosan/ poly( N‐isopropylacrylamide) based cryogels (CMCS/PNIPAM) with multiple responsiveness (pH, near infrared (NIR), and temperature) to form self‐adaptive antibacterial cryogels that adapt to the therapeutic needs of different stages in infected wound healing. In response to the slightly acidic environment of bacterial infection, the cryogels assist the bacterial capture capacity through acid‐triggered protonation behavior, and effectively enhance the photodynamic antibacterial efficiency. Controllable on‐demand delivery of ROS, NO, and remote management of infected…

Abstract Polydimethylsiloxanes (PDMS) foam as one of next‐generation polymer foam materials shows poor surface adhesion and limited functionality, which greatly restricts its potential applications. Fabrication of advanced PDMS foam materials with multiple functionalities remains a critical challenge. In this study, unprecedented self‐adhesive PDMS foam materials are reported with worm‐like rough structure and reactive groups for fabricating multifunctional PDMS foam nanocomposites decorated with MXene/cellulose nanofiber (MXene/CNF) interconnected network by a facile silicone foaming and dip‐coating strategy followed by silane surface modification. Interestingly, such self‐adhesive PDMS foam produces strong interfacial adhesion with the hybrid MXene/CNF nano‐coatings. Consequently, the optimized PDMS foam nanocomposites have excellent surface super‐hydrophobicity (water contact angle of ≈159 o ), tunable electrical conductivity (from 10 −8 to 10 S m −1 ), stable compressive cyclic reliability in both wide‐temperature range (from −20 to 200 o C) and complex environments (acid,…

Abstract Electrooxidation of 5‐hydroxymethylfurfural (HMF) into 2,5‐furandicarboxylic acid (FDCA) is a highly promising approach for producing value‐added chemicals from biomass. However, developing highly efficient electrocatalysts for HMF oxidation (HMFOR) with high current density in large‐scale productions remains a challenge. Herein, it is demonstrated that the Mn‐doped NiS nanosheet electrocatalysts grown directly on 3D graphite felt (GF) substrates can efficiently perform electrooxidation of HMF into FDCA at industrial‐level current density (500 mA cm −2 ) in the H‐cell. The Mn 0.2 NiS/GF exhibits excellent HMFOR performance with high selectivity (98.3%), yield (97.6%), faradaic efficiency (94.2%), and robust stability (10 cycles). Especially, FDCA production rate up to 4.56 g h −1 can be achieved, superior to those reported in HMFOR literatures. Furthermore, by scaling up the Mn 0.2 NiS/GF electrode area and assembling it in a continuous‐flow electrolyzer, high FDCA production rate of 44.32 g h −1 is achieved. The high activity of Mn 0.2 NiS/GF for HMFOR can be attributed to…

Abstract Recent advances in ordered porous materials, including metal‐organic (MOF) and covalent organic frameworks (COF), are set to revolutionize the strategies used for wastewater treatment. This is attributed to the large surface area, high crystallinity, structural tunability, thermal and chemical stability, and well‐defined structures of MOF and COF. Despite the distinctive properties exhibited by the single system (either MOF or COF), the combination of COF and MOF, as a hybrid construct, offers a remarkable opportunity to achieve superior functionality and performance. The favorable features of COF–MOF hybrids in different wastewater treatment sectors have opened new venues for effective environmental remediation. This review presents the state‐of‐the‐art design, synthesis, and application of COF–MOF hybrids. The synthesis principles, including MOF‐first, COF‐first, and post‐synthetic linkage of pre‐synthesized COFs and MOFs are summarized. The potential of these novel materials is evaluated by considering contaminant sensing, adsorptive removal, and catalytic…

Abstract Very recently, MXene‐based wearable hydrogels have emerged as promising candidates for epidermal sensors due to their tissue‐like softness and unique electrical and mechanical properties. However, it remains a challenge to achieve MXene‐based hydrogels with reliable sensing performance and prolonged service life, because MXene inevitably oxidizes in water‐containing system of the hydrogels. Herein, catechol‐functionalized poly(vinyl alcohol) (PVA‐CA)‐based hydrogels is proposed to inhibit the oxidation of MXene, leading to rapid self‐healing and superior strain sensing behaviors. Sufficient interaction of hydrophobic catechol groups with the MXene surface reduces the oxidation‐accessible sites in the MXene for reaction with water and eventually suppresses the oxidation of MXene in the hydrogel. Furthermore, the PVA‐CA‐MXene hydrogel is demonstrated for use as a strain sensor for real‐time motion monitoring, such as detecting subtle human motions and handwriting. The signals of PVA‐CA‐MXene hydrogel sensor can be accurately classified using deep learning models.

Abstract Breathable, flexible, and highly sensitive pressure sensors have drawn increasing attention due to their potential in wearable electronics for body‐motion monitoring, human‐machine interfaces, etc. However, current pressure sensors are usually assembled with polymer substrates or encapsulation layers, thus causing discomfort during wearing (i.e., low air/vapor permeability, mechanical mismatch) and restricting their applications. A breathable and flexible pressure sensor is reported with nonwoven fabrics as both the electrode (printed with MXene interdigitated electrode) and sensing (coated with MXene/silver nanowires) layers via a scalable screen‐printing approach. Benefiting from the multi‐layered porous structure, the sensor demonstrates good air permeability with high sensitivity (770.86–1434.89 kPa −1 ), a wide sensing range (0–100 kPa), fast response/recovery time (70/81 ms), and low detection limit (≈1 Pa). Particularly, this sensor can detect full‐scale human motion (i.e., small‐scale pulse beating and large‐scale walking/running) with high sensitivity, excellent…

Abstract The S‐scheme heterojunctions have great potential for photocatalytic carbon dioxide reduction due to their unique carrier migration pathways, superior carrier separation efficiencies, and high redox capacities. However, the precise process of the oriented powerful electron transport remains a great challenge. Herein, an InOCd bond‐modulated S‐scheme heterojunction of In 2 O 3 /CdSe‐DETA is synthesized by a simple microwave‐assisted hydrothermal method for the accelerated photogenerated electron transfer. Meanwhile, the oxygen vacancies (Vo) of In 2 O 3 have an electron capture effect. Consequently, thanks to the synergistic effect of this In‐Vo‐In‐O‐Cd structural units at the interface, electrons are extracted and rapidly transferred to the surface‐active sites, which improves the electronic coupling of CO 2 . This finding precisely adjusts the electron transfer pathway and shortens the electron transfer distance. The synergistic effect of this chemical bond established in the S‐scheme heterostructure with oxygen vacancies in In 2 O 3 (Vo‐In 2 O 3 ) provides new insights…

Abstract Constructing an efficient alkaline hydrogen evolution reaction (HER) catalyst with low platinum (Pt) consumption is crucial for the cost reduction of energy devices, such as electrolyzers. Herein, nanoflower‐like carbon‐encapsulated CoNiPt alloy catalysts with composition segregation are designed by pyrolyzing morphology‐controlled and Pt‐proportion‐tuned metal–organic frameworks (MOFs). The optimized catalyst containing 15% CoNiPt NFs (15%: Pt mass percentage, NFs: nanoflowers) exhibits outstanding alkaline HER performance with a low overpotential of 25 mV at a current density of 10 mA cm −2 , far outperforming those of commercial Pt/C (47 mV) and the most advanced catalysts. Such superior activity originates from an integration of segregation alloy and Co‐O hybridization. The nanoflower‐like hierarchical structure guarantees the full exposure of segregation alloy sites. Density functional theory calculations suggest that the segregation alloy components not only promote water dissociation but also facilitate the hydrogen adsorption process, synergistically accelerating…

Abstract Flexible conductive materials with intrinsic structural characteristics are currently in the spotlight of both fundamental science and advanced technological applications due to their functional preponderances such as the remarkable conductivity, excellent mechanical properties, and tunable physical and chemical properties, and so on. Typically, conductive hydrogel fibers (CHFs) are promising candidates owing to their unique characteristics including light weight, high length‐to‐diameter ratio, high deformability, and so on. Herein, a comprehensive overview of the cutting‐edge advances the CHFs involving the architectural features, function characteristics, fabrication strategies, applications, and perspectives in flexible electronics are provided. The fundamental design principles and fabrication strategies are systematically introduced including the discontinuous fabrication (the capillary polymerization and the draw spinning) and the continuous fabrication (the wet spinning, the microfluidic spinning, 3D printing, and the electrospinning). In addition, their potential…

Abstract As a chemical product with rapidly expanding demand in the field of modern energy and environmental applications, hydrogen peroxide (H 2 O 2 ) has garnered widespread attention. However, the existing industrial production of H 2 O 2 is plagued by high energy consumption, harmful waste emission, and severe safety issues, making it difficult to satisfy the environmental/economic production concept. Artificial photosynthesis offers a viable strategy for green and sustainable H 2 O 2 production since it uses sunlight as an energy source to initiate the reaction of oxygen and water to produce H 2 O 2 . Among various photocatalysts, covalent organic frameworks (COFs), featuring highly ordered skeletons and well‐defined active sites, have emerged as promising photocatalysts for H 2 O 2 production. This review presents the nascent and burgeoning area of photocatalytic H 2 O 2 production based on COFs. First, a brief overview of photocatalytic technology is provided, followed by a detailed introduction to the principles and evaluation of the photocatalytic H 2 O 2 generation.…

Abstract Multi‐resonance thermally activated delayed fluorescence (MR‐TADF) emitters have drawn considerable attention because of their remarkable optoelectronic properties of high emission efficiency and narrow emission profile, and represent an active subject of cutting‐edge research in the organic electroluminescence (EL). However, the slow reverse intersystem crossing (RISC) rate of MR‐TADF emitter caused by the large energy gap (Δ E ST ) and small spin‐orbit coupling (SOC) matrix elements between the singlet and triplet excited states limits their further development in organic EL devices. Currently, innovative molecular design strategies have been developed including heavy atom integration, π‐extended MR framework and metal perturbation, and so on to improve the RISC process of MR‐TADF emitters for high‐performance EL devices. Here, an overview is presented on the recent progress of MR‐TADF emitters with fast RISC rate ( > 10 −5 s −1 ), with particular attention to the molecular design, optoelectronic properties, and device performance of organic light‐emitting diodes (OLEDs),…

Abstract Sophisticated sensing and actuation capabilities of many living organisms in nature have inspired scientists to develop biomimetic somatosensory soft robots. Herein, the design and fabrication of homogeneous and highly conductive hydrogels for bioinspired somatosensory soft actuators are reported. The conductive hydrogels are synthesized by in situ copolymerization of conductive surface‐functionalized MXene/Poly(3,4‐ethylenedioxythiophene)/poly(styrenesulfonate) ink with thermoresponsive poly(N‐isopropylacrylamide) hydrogels. The resulting hydrogels are found to exhibit high conductivity (11.76 S m−1), strain sensitivity (GF of 9.93), broad working strain range (≈560% strain), and high stability after over 300 loading–unloading cycles at 100% strain. Importantly, shape‐programmable somatosensory hydrogel actuators with rapid response, light‐driven remote control, and self‐sensing capability are developed by chemically integrating the conductive hydrogels with a structurally colored polymer. As the proof‐of‐concept illustration, structurally colored hydrogel actuators are…

Abstract Incorporating zero‐energy‐input cooling technology into personal thermal management (PTM) systems is a promising solution for preventing heat‐related illnesses while reducing energy consumption. Although concepts for passive radiative cooling materials are proposed, achieving subambient cooling performance while providing good wearing comfort remains a challenge. Here, a moisture‐wicking nonwoven metafabric is reported that assembles radiative cooling and evaporative heat dissipation to achieve high‐performance thermal and moisture comfort management. This metafabric demonstrates excellent spectral‐selectivity (sunlight reflection of ≈92%, atmospheric window thermal emissivity of ≈97%) and Janus wettability through large‐scale electrospinning and hierarchical design, and also inherits superior elasticity, air/moisture permeability of nonwoven fabric. Subambient temperature drops of ≈6.5 °C (≈750 W m −2 solar intensity) for stand‐alone metafabric are observed. Thanks to the moisture‐wicking effect (water evaporation rate of 0.31 g h −1 and water transport index of 1220%) of…

Abstract With the increase of environmental pollution and depletion of fossil fuel resources, the utilization of renewable biomass resources for developing functional materials or fine chemicals is of great value and has attracted considerable attention. Nanocellulose, as a well‐known renewable nanomaterial, is regarded as a promising nano building block for advanced functional materials owing to its unique structure and properties, as well as natural abundance. Typically, its high mechanical strength, structural flexibility, reinforcing capabilities, and tunable self‐assembly behavior makes it highly attractive to fabricate flexible materials for various applications. Herein, the recent progress in the design, properties, and applications of advanced flexible materials from nanocellulose is comprehensively summarized. The preparation and properties of nanocellulose are first briefly introduced and discuss its merits in fabricating flexible materials. Then, various advanced flexible materials from nanocellulose are introduced, and the critical role of nanocellulose in constructing…

Abstract Phase change materials (PCMs) are a class of thermo‐responsive materials that can be utilized to trigger a phase transition which gives them thermal energy storage capacity. Any material with a high heat of fusion is referred to as a PCM that is able to provide cutting‐edge thermal storage. PCMs are commercially used in many applications like textile industry, coating, and cold storage typically for heat control. These intriguing substances have recently been rediscovered and employed in a broad range of life science applications, including biological, human body, biomedical, pharmaceutical, food, and agricultural applications. Benefiting from the changes in physicochemical properties during the phase transition makes PCMs also functional for barcoding, detection, and storage. Paraffin wax and polyethylene glycol are the most commonly studied PCMs due to their low toxicity, biocompatibility, high thermal stability, high latent enthalpy, relatively wide transition temperature range, and ease of chemical modification. Current challenges in employing PCMs for life science…

Abstract Metal–organic frameworks (MOFs) are highly versatile materials that have been identified as promising candidates for membrane‐based gas separation applications due to their uniformly narrow pore windows and virtually unlimited structural and chemical features. Defect engineering of MOFs has opened new opportunities for manipulating MOF structures, providing a simple yet efficient approach for enhancing membrane separation. However, the utilization of this strategy to tailor membrane microstructures and enhance separation performance is still in its infancy. Thus, this summary aims to provide a guideline for tailoring defective MOF‐based membranes. Recent developments in defect engineering of MOF‐based membranes will be discussed, including the synthesis strategies for defective MOFs, the effects of defects on the gas adsorption properties, gas transport mechanisms, and recently reported defective MOF‐based membranes. Furthermore, the emerging challenges and future prospects will be outlined. Overall, defect engineering offers an exciting opportunity to improve the…

Abstract Capacitive deionization (CDI) is an emerging water desalination technology for removing different ionic species from water, which is based on electric charge compensation by these charged species. CDI is becoming popular because it is more energy‐efficient and cost‐effective than other technologies, such as reverse osmosis and distillation, specifically in dealing with brackish water having low or moderate salt concentrations. Over the past decade, the CDI research field has witnessed significant advances in the used electrode materials, cell architectures, and associated mechanisms for desalination applications. This review article first discusses ion storage/removal mechanisms in carbon and Faradaic materials aided by advanced in situ analysis techniques and computations. It then summarizes research progress toward electrode materials in terms of structure, surface chemistry, and composition. More still, it discusses CDI cell architectures by highlighting their different cell design concepts. Finally, current challenges and future research directions are summarized to…

Abstract Conducting polymer hydrogels are widely used as strain sensors in light of their distinct skin‐like softness, strain sensitivity, and environmental adaptiveness in the fields of wearable devices, soft robots, and human‐machine interface. However, the mechanical and electrical properties of existing conducting polymer hydrogels, especially fatigue‐resistance and sensing robustness during long‐term application, are unsatisfactory, which severely hamper their practical utilities. Herein, a strategy to fabricate conducting polymer hydrogels with anisotropic structures and mechanics is presented through a combined freeze‐casting and salting‐out process. The as‐fabricated conducting polymer hydrogels exhibit high fatigue threshold (>300 J m −2 ), low Young's modulus (≈100 kPa), as well as long‐term strain sensing robustness (over 10 000 cycles). Such superior performance enables their application as strain sensors to monitor the real‐time movement of underwater robotics. The design and fabrication strategy for conducting polymer hydrogels reported in this study may open up an…

Abstract Multifunctional films with integrated temperature adjustment, electromagnetic interference (EMI) shielding, and thermal camouflage are remarkably desirable for wearable products. Herein, a novel Janus‐type multifunctional ultra‐flexible film is fabricated via continuous electrospinning followed by spraying. Interestingly, in the polyvinyl alcohol (PVA)/phase change capsules (PCC) layer (P 1 ), the PCC is strung on PVA fibers to form a stable “candied haws stick” structure that obviates slipping or falling off. The film with sufficient melting enthalpy (141.4 J g −1 ) guarantees its thermoregulation capability. Simultaneously, its high mid‐IR emissivity (90.15%) endows the film with radiative cooling properties (reducing temperature by 10.13 °C). Mechanical strength is significantly improved by superimposing a polylactic acid (PLA) layer (P 2 ) on its surface. By spraying a thin MXene layer on the PLA surface of P 2 P 1 film, the obtained (MXene/P 2 P 1 ) MP 2 P 1 film is endowed with satisfactory low‐voltage heating, photo‐thermal and superior thermal camouflage…

Abstract Aqueous Zn ion batteries (ZIBs) are one of the most promising battery chemistries for grid‐scale renewable energy storage. However, their application is limited by issues such as Zn dendrite formation and undesirable side reactions that can occur in the presence of excess free water molecules and ions. In this study, a nanocellulose‐carboxymethylcellulose (CMC) hydrogel electrolyte is demonstrated that features stable cycling performance and high Zn 2+ conductivity (26 mS cm −1 ), which is attributed to the material's strong mechanical strength (≈70 MPa) and water‐bonding ability. With this electrolyte, the Zn‐metal anode shows exceptional cycling stability at an ultra‐high rate, with the ability to sustain a current density as high as 80 mA cm −2 for more than 3500 cycles and a cumulative capacity of 17.6 Ah cm −2 (40 mA cm −2 ). Additionally, side reactions, such as hydrogen evolution and surface passivation, are substantially reduced due to the strong water‐bonding capacity of the CMC. Full Zn||MnO 2 batteries fabricated with this electrolyte demonstrate excellent…

Abstract The conductive hydrogels always suffered from high internal friction, large hysteresis, and low capability of accurately predicting physical deformation, which seriously restricted their application in smart wearable devices. To address these problems, solvent molecules are directionally inserted into the polymer molecule chains via bridge effect to effectively reduce the molecular internal friction. Moreover, swelling is also combined to eliminate the temporary entanglements in the hydrogel system. The cooperation between the bridge and swollen effect endows the prepared polyacrylamide (PAM)/laponite/H3BO3/ethylene glycol (Eg) organohydrogel (PLBOH) ultralow hysteresis (1.38%, ε = 100%), ultrafast response (≈10 ms), and high linearity in the whole‐strain‐range (R2 = 0.996) with a great sensitivity (GF = 2.68 at the strain range of 0–750%). Meanwhile, the prepared PL10B30OH exhibits long‐term stability, excellent stretchability, and low dissipated energy. Furthermore, the assembled triboelectric nanogenerator (TENG) displays an outstanding energy harvesting performance with…

Abstract Vulnerable robustness of superhydrophobic materials have mightily hindered their practical applications. Herein, a controllable and effective strategy is demonstrated for constructing robust superhydrophobicity with aqueous hydrophobic interaction driving self‐assembly (HIDS), using polydopamine (PDA) as the binder and SiO2 particles as the nano‐sized structures to enable low‐adhesive property. The proposed strategy realizes the rapid interfacial assembly of PDA by manipulating the wetting properties of SiO2@PDA core‐shell particles with hydrophobic modifier. The polyurethane (PU) sponges are facilely rendered superhydrophobic with remarkable robustness, stemming from the excellent adherence of HIDS enhanced covalent interaction between PDA and PU. Coated sponge possesses ultralong‐term stability during the oil‐water separation, the separation efficiency can be maintained at 98.8% even after 1000 cycle separations and strikingly, superhydrophobicity is still retained after 100 cycle abrasion with ultrahigh loading pressure of 49 kPa. Versatilely, the coatings can be…

Abstract Solar steam generation has become one of the most promising strategies to relieve the freshwater crisis. Whereas, the construction of a solar‐thermal water evaporation structure that can operate continuously under sunlight to generate clean water with high efficiency, good stability, and high salt‐rejecting capability is quite crucial but challengeable. Enlightened by the water transport and transpiration process in trees, an advanced nanofibrous aerogel evaporator is fabricated with multifunctional capabilities through decoration of functional component onto an aerogel skeleton. The rational integration of hierarchical structure and functional constituents, results in outstanding solar‐vapor conversion efficiency of 96.1% and a fast evaporation rate about 2.33 kg m −2 h −1 under 1 sun. Additionally, the evaporator exhibits remarkably outdoor evaporation and highly effective salt‐resistant performances. Significantly, the evaporator can monitor salt precipitation in its inner pores in real time. This study demonstrates an eco‐friendly and economic solution for sustainable…

Abstract Oil–water separation membranes easily fail to oil foulants with low surface energy and high viscosity, which severely limits these membranes’ applications in treating oily wastewater. Herein, an oil–water separation membrane by bioinspired bubble‐mediated antifouling strategy is fabricated via growing hierarchical cobalt phosphide arrays on stainless steel mesh. The as‐prepared membrane is superhydrophilic/superaerophobic and electrocatalytic for hydrogen evolution under water, which helps to rapidly generate and release abundant microbubbles surrounding the oil‐fouled region on the membrane. These microbubbles can spontaneously coalesce with the oil foulants to increase their buoyancy and warp their interface tension by morphing the oil shape. And this spontaneous coalescence also increases the kinetic energy of oil foulants resulting from the decreased bubbles’ interface energy and potential energy. The synergy of the warped interface tension, increased buoyancy, and kinetic energy drives the efficiently dynamic antifouling of this membrane. This dynamic antifouling even…

Abstract Composites‐based photocatalysis relies on the interfacial electron transfer between the metallic cocatalyst and photosensitizer (the semiconductor) to realize spatial separation of charge carriers. Herein, an ingenious heterojunction between Co‐CN single atom catalysts (SACs) and g‐C3N4 is constructed for heterogeneous photo‐Fenton‐like reactions. Driven by built‐in electric field across the heterojunctions, the separation and migration of the photogenerated charge carriers is promoted, leading to the fast electron transfer from the g‐C3N4 to the Co‐CN SACs. Theoretical calculations and transient absorption spectroscopy reveal the modulated charge transfer and trapping in the SA‐Co‐CN/g‐C3N4 heterostructure, resulting in the remarkably enhanced generation of reactive oxygen species via peroxymonosulfate activation under light irradiation. This ingenious SA‐Co‐CN/g‐C3N4/PMS/vis system is efficient for the oxidation of various antibiotics with high removal efficiency (>98%), a wide operating pH range (pH 3–11) and excellent stability in long‐term operation. This study…

Abstract Recent research on wood‐based solar evaporators has made great progress and significant breakthroughs have been made in using lignin as a photothermal material; however, the intensity change mechanism regarding the conjugate structure of lignin is almost never mentioned. This study innovatively proposes a mechanism to explain the changes in conjugate intensity that occur before and after lignin dissolution and fabricates a lignin/wood‐based solar evaporator (LWE) using an all‐wood‐based material that is salt‐tolerant and has long‐term serviceability. Lignin in the evaporator serves not only as a photothermal material for converting light energy into heat energy but also as a reinforcement for the evaporator's structural strength. Adding lignin changes the original structure of balsa wood, increasing the proportion of intermediate water in the LWE, thereby lowering the enthalpy of water evaporation. The optimized LWE with an enhanced desalination capability, dye removal property, and high stability exhibits full‐spectrum solar absorption of about 83.6%, a photothermal…

Abstract In this study, graphene oxide (GO) and polyacrylamide/polyacrylic acid (PAM/PAA) are used to prepare hydrogels with photothermal conversion properties for highly efficient uranium extraction from seawater. Zwitterionic 2‐methacryloyloxy ethyl phosphorylcholine (MPC) is introduced in the PAM/PAA/GO hydrogel to obtain PAM/PAA/GO/MPC (PAGM), exhibiting good antibacterial properties. PAGM demonstrates efficient and specific adsorption of uranium (VI) (U(VI)). Under light conditions, the adsorption capacity of PAGM reaches 196.12 mg g −1 (pH = 8, t = 600 min, C 0 = 99.8 mg L −1 , m/v = 0.5 g L −1 ). The adsorption capacity is only 160.29 mg g −1 under dark conditions (pH = 8, t = 600 min, C 0 = 99.8 mg L −1 , m/v = 0.5 g L −1 ). The adsorption capacity of light is 22.5% higher than that of dark. The adsorption process is fitted using the Langmuir and pseudo‐second‐order models. Furthermore, PAGM exhibits good repeatability and stability after five adsorption–desorption cycles. PAGM exhibits a U(VI) adsorption capacity of 6.1 mg g −1 after storage for one month in natural…

Abstract Aqueous zinc‐ion batteries feature high safety, low cost, and relatively high energy density; however, their cycle life is hindered by severe Zn dendrite formation and water‐induced parasitic reactions. Herein, a porous polyaniline (PANI) interfacial layer is developed on the surface of Zn metal anode to regulate the transport and deposition of Zn 2+ , achieving an ultra‐stable and highly reversible Zn anode. Specifically, the abundant polar groups (NH and N) in PANI have a strong attraction to H 2 O, which can trap and immobilize H 2 O molecules around Zn 2+ . Moreover, the protective layer regulates ion flux and deposition behavior of Zn 2+ through the ion confinement effect. Consequently, the Zn@PANI anode exhibits improved reversible plating/stripping behavior with a low nucleation overpotential (37.9 mV) at 2.0 mA cm ‐2 compared to that of bare Zn anode. The MnO 2 //Zn@PANI cell demonstrates a high capacity retention of 94.3% after 1000 cycles at 1.0 A g −1 . This study lays the foundation for accessible interface engineering and in‐depth mechanistic analysis of Zn…

Abstract High‐quality backlit display puts forward urgent demand for color‐converting materials. Recently, metal halide perovskites (MHPs) with full spectral tunability, high photoluminescence quantum yields (PLQYs), and high color purity have found potential application in wide‐color‐gamut display. Regrettably, naked MHPs suffer from long‐term instable issue and cannot pass harsh stability tests. Herein, amorphous‐glass‐protected green/red CsPbX3 quantum dots (QDs) are prepared by elaborately optimizing glass structure, perovskite concentration, and in situ crystallization. PLQYs of green CsPbBr3@glass and red CsPbBr1.5I1.5@glass reach 94% and 78%, respectively, which are the highest ones of CsPbX3@glass composites reported so far and comparable to colloidal counterparts. Benefited from complete isolation of QDs from external environment by glass network, CsPbX3@glass can endure harsh commercial standard aging tests of 85 °C/85%RH and blue‐light‐irradiation, which are applied to construct white light‐emitting diodes (wLEDs) with high external quantum efficiency of 13.8% and…

Abstract Advanced sensation and actuation abilities of various living organisms in nature have inspired researchers to design bioinspired self‐sensing soft actuators. However, the majority of conventional soft actuators primarily possess actuation capabilities while lacking a real‐time sensing signal feedback. Here, a promising strategy is reported to develop highly stretchable and conductive hydrogels for bioinspired self‐sensing soft actuators, which integrate actuation and strain‐sensing functions into a single materials system. The conductive hydrogels are designed and fabricated by in situ copolymerization of amino‐functionalized MXene‐encapsulated liquid metal nanodroplets (LM@A‐MXene) and poly( N ‐isopropylacrylamide) hydrogels with controllable activated nanogels as nano‐cross‐linkers. The resulting hydrogel presents a compacted conducting network and highly porous microstructure, giving rise to robust integration of high conductivity, excellent strain sensitivity, broad stretchability, high stability, and fast response speed. Interestingly, the gradient network structure,…

Abstract Flexible triboelectric nanogenerators (TENGs) with multifunctional sensing capabilities offer an elegant solution to address the growing energy supply challenges for wearable smart electronics. Herein, a highly stretchable and durable electrode for wearable TENG is developed using ZIF‐8 as a reinforcing nanofiller in a hydrogel with LiCl electrolyte. ZIF‐8 nanocrystals improve the hydrogel's mechanical properties by forming hydrogen bonds with copolymer chains, resulting in 2.7 times greater stretchability than pure hydrogel. The hydrogel electrode is encapsulated by microstructured silicone layers that act as triboelectric materials and prevent water loss from the hydrogel. Optimized ZIF‐8‐based hydrogel electrodes enhance the output performance of TENG through the dynamic balance of electric double layers (EDLs) during contact electrification. Thus, the as‐fabricated TENG delivers an excellent power density of 3.47 Wm – 2 , which is 3.2 times higher than pure hydrogel‐based TENG. The developed TENG can scavenge biomechanical energy even at subzero temperatures to power…

Abstract In recent years, metal‐organic frameworks, especially MOF‐based derivatives, have been regarded as one of the best candidate electrode materials for the next generation of advanced materials, due to high porosity, large surface area, modifiable functional groups as well as controllable chemical composition. This review presents the corresponding synthesis methods, structural design, and electrochemical performance of MOF‐derived materials, including metal oxides, metal sulfides, metal phosphides, and carbon materials, in high‐performance lithium‐ion batteries. Subsequently, the problems that exist in the current application of MOF‐based derivatives as electrodes in lithium‐ion batteries are discussed along with possible and feasible solutions. At last, some reasonable pathways and strategies for the design of MOF derivatives are also suggested.

Abstract The excited‐state tuning of luminescent metal–organic compounds has made great progress in the fields of optical imaging, photocatalysis, photodynamic therapy, light‐emitting devices, sensors, and so on. Although metal–organic compounds with high luminescence efficiency can be realized via enhanced molecular rigidity and heavy‐atom effect, their corresponding luminescence lifetimes are still limited on the order of a nanosecond to a millisecond, owing to the inherent competition between luminous efficiency and lifetime. Therefore, the advanced applications (i.e., persistent afterglow imaging, information security, anti‐counterfeiting, and smart materials, among others) related with long persistent luminescence (LPL, typically with the excited‐state lifetime larger than millisecond) are seriously hindered. This review gives a timely and systematic summary of metal–organic compounds for realizing room‐temperature phosphorescence (RTP)‐type and thermally activated delayed fluorescence (TADF)‐type LPL during last few years. Particularly, based on the perspectives of time,…

Abstract In response to the need of sustainable development, there is an increasing demand for electrical energy storage, leading to a stimulated pursuit of advanced batteries. Aqueous zinc ion batteries (AZIBs) have attracted much attention due to their low cost, high safety, and environmental friendliness. Despite the great efforts made by researchers in designing and developing high‐performance AZIBs, several challenges remain. Particularly for Zn anode, the growth of zinc dendrites and occurance of various side reactions significantly hinder the advancement of AZIBs. This review article aims to discuss the principles of AZIBs, the electrolyte's structure and properties, the challenges faced by AZIBs anodesm and the strategies to improve battery performance through electrolyte modification in a systematic manner. In conclusion, potential future directions aimed at enhancing the stability of zinc anodes and cathodes by electrolyte modification strategies are proposed to ensure that research efforts are geared toward achieving realistic performance targets for commercializing AZIBs.

Abstract Dielectric polarization and magnetic resonance associated with intrinsic constituent and extrinsic structure are two kinds of fundamental attenuation mechanisms for microwave absorbers, but remain extremely challenging in revealing the composition‐morphology‐performance correlation. Herein, hierarchical MXene/metal‐organic framework derivatives with coherent boundaries and magnetic units below critical grain size are constructed to realize synergistic dielectric–magnetic enhancement by phase‐evolution engineering and dynamic magnetic resonance. Specifically, phase‐evolution induced inseparable interfaces, diverse incompatible phases, and defects/vacancies contribute to dielectric polarization, while closely distributed magnetic units simultaneously realize nanoscale multi‐domain coupling and long‐range magnetic interaction. As results, the hierarchical derivatives promise an exceptional reflection loss of −59.5 dB and an effective absorption bandwidth of 6.1 GHz. Both experimental results and theoretical calculations indicate that phase‐evolution engineering and dynamic…

Abstract Benefiting from inherent lightweight, flexibility, and good adaptability to human body, functional textiles are attracting tremendous attention to cope with wearable issues in sustainable applications around human beings. In this feature article, a comprehensive and thoughtful review is proposed regarding research activities of functional textiles with smart properties. Specifically, a brief exposition of highlighting the significance and rising demands of novel textiles throughout the human society is begun. Next, a systematic review is provided about the fabrication of functional textiles from 1D spinning, 2D modification, and 3D construction, their diverse functionality as well as sustainable applications, showing a clear picture of evolved textiles to the readers. How to engineer the compositions, structures, and properties of functional textiles is elaborated to achieve different smart properties. All these tunable, upgraded, and versatile properties make the developed textiles well suited for extensive applications ranging from environmental monitoring or freshwater…

Abstract Wearable strain sensors with the ability of detecting physiological activities play an important role in personalized healthcare. Electrospun fibers have become a popular building block for wearable strain sensors due to their excellent mechanical properties, breathability, and light weight. In this review, the structure and preparation process of electrospun fibers and the conductive layer are systematically introduced. The impact of materials and structures of electrospun fibers on the wearable strain sensors with a following discussion of sensing performance optimization strategies is outlined. Furthermore, the applications of electrospun fiber‐based wearable strain sensors in biomonitoring, motion detection, and human‐machine interaction are presented. Finally, the challenges and promising future directions for the community of wearable strain sensors based on electrospun fibers are pointed out.

Abstract Electrochemical reduction of nitrate to ammonia (NO3RR) has been recognized as an appealing approach to realize both sustainable NH3 production and waste nitrate removal. Herein, from the perspective of Lewis acid‐base interaction, a single‐atom Fe‐doped V2O5 (Fe‐V2O5) catalyst enriched is designed with Lewis acid sites, which present the maximum NH3‐Faradaic efficiency of 97.1% with the corresponding NH3 yield of 12.5 mg h−1 cm−2 at –0.7 V versus RHE. Mechanistic studies based on theoretical calculations and operando spectroscopic characterizations identify the creation of Lewis acid Fe‐V pairs on Fe‐V2O5, which can synergetically activate the NO3−, promote the hydrogenation energetics, and restrain the hydrogen evolution, leading to the enhanced NO3RR activity and selectivity.

Abstract The electrochemical performance of aqueous zinc metal batteries (AZMBs) is highly dependent on the electric double layer (EDL) properties at Zn electrode/electrolyte interface. Herein, a novel reconfigured EDL is constructed via a double‐charged theanine (TN) additive for super‐stable and deep‐rechargeable AZMBs. Experiments and theoretical computations unravel that the positively charged TN not only serves as preferential anchor to form a water‐poor Helmholtz plane onto the Zn anode, but also its anionic end could coordinate with Zn2+ to tailor the solvation structure in the diffusion layer and further reconstruct the inner H‐bonds networks, thus effectively guiding uniform Zn deposition and suppressing the water‐induced side reactions. Consequently, the Zn//Zn cells acquire outstanding cycling stabilities of nearly 800 h at a high depth of discharge of 80%. Moreover, the Zn//VOX full cells deliver substantial capacity retention (94.12% after 1400 cycles at 2 A g−1) under practical conditions. Importantly, the designed 2.7 Ah Zn//VOX pouch cell harvests a recorded energy…

Abstract Rechargeable aqueous zinc‐ion batteries (AZIBs) are recognized as one of the most competitive next generation energy storage systems due to the high theoretical capacity (820 mAh g −1 ), abundant reserves, low expense, and environmental friendliness. However, in comparison to that monovalent ion secondary battery, the multivalent ion rechargeable battery faces larger metal ion sizes and higher charge/discharge number in the electrochemical reaction process, thereby suffering from larger steric resistance and the electrostatic repulsion in the intercalation–deintercalation process. At present, a great deal of research has shown that the guest ion pre‐embedded host structured cathodes can effectively alleviate the above problems and improve the comprehensive performance of aqueous zinc ion battery. In this review, the development of vanadium oxide ion‐intercalated cathode materials in AZIBs is reviewed, mainly including M X V 2 O 5 ∙nH 2 O, M X V 3 O 8 ∙nH 2 O, M X V 6 O 13 ∙nH 2 O, M X V 6 O 16 ∙nH 2 O, and M X V 10 O 25 ∙nH 2 O type materials. The reaction mechanisms and…

Metal-organic framework (MOF) materials are gaining significant interest in biomedical research, owing to their high porosity, crystallinity, and structural and compositional diversity. Their versatile hybrid organic/inorganic chemistry endows MOFs with the capacity to retain organic (drug) molecules, metals, and gases, to effectively channel electrons and photons, to survive harsh physiological conditions such as low pH, and even to protect sensitive biomolecules. Extensive preclinical research has been carried out with MOFs to treat several pathologies and, recently, their integration with other biomedical materials such as stents and implants has demonstrated promising performance in regenerative medicine. However, there remains a significant gap between MOF preclinical research and translation into clinically and societally relevant medicinal products. Here, we outline the intrinsic features of MOFs and discuss how these are suited to specific biomedical applications like detoxification, drug and gas delivery, or as (combination) therapy platforms. We furthermore describe…

Abstract Separator modification is an efficient strategy to handle with the challenges of lithium metal batteries but its success is primarily subject to the modification of the materials. Herein, a cationic covalent organic framework (COF) composed of positively charged organic units and weakly bonded fluoride ions (F − ) is introduced to modify the commercial polypropylene separator (COF−F@PP). It is found that the organic unit has abundant nanopores to homogenize the lithium ions (Li + ) flux and can interact with electrolyte solvent molecules to form a desolvation structure of Li + . Meanwhile, the F − within the nanopores is proved to assist in building a robust LiF−riched solid electrolyte interphase to avoid the side reactions between lithium anode and electrolyte. Hence, the COF−F@PP delivers feasible practicality for the outstanding cycling stability, high Coulombic efficiency, and superior rate capability of Li//LFP coin cell at 5 C, low N/P ratio (2.19) full cell, and pouch cell at 1 C.

Abstract Gait analysis provides a convenient strategy for the diagnosis and rehabilitation assessment of diseases of skeletal, muscular, and neurological systems. However, challenges remain in current gait recognition methods due to the drawbacks of complex systems, high cost, affecting natural gait, and one‐size‐fits‐all model. Here, a highly integrated gait recognition system composed of a self‐powered multi‐point body motion sensing network (SMN) based on full textile structure is demonstrated. By combining of newly developed energy harvesting technology of triboelectric nanogenerator (TENG) and traditional textile manufacturing process, SMN not only ensures high pressure response sensitivity up to 1.5 V kPa −1 , but also is endowed with several good properties, such as full flexibility, excellent breathability (165 mm s −1 ), and good moisture permeability (318 g m −2 h −1 ). By using machine learning to analyze periodic signals and dynamic parameters of limbs swing, the gait recognition system exhibits a high accuracy of 96.7% of five pathological gaits. In addition, a…

Abstract When skin trauma occurs, rapid achievement of the post‐wound closure is required to prevent microbial invasion, inhibit scar formation and promote wound healing. To develop a wound dressing for accelerating post‐wound‐closure and wound healing, a thermo‐responsive and tissue‐adhesive hydrogel with interpenetrating polymer networks (IPN) is fabricated based on N ‐dimethylbisacrylamide (NIPAM) and glutaraldehyde (GTA) cross‐linked hyaluronic acid (HA). Results not only confirm the thermo‐stimulated self‐contraction and tissue adhesiveness of the HA‐based IPN (PNI‐HA), which effectively aids wound closure via mechanical stretch, but also verify the hemocompatibility and cytocompatibility of PNI‐HA that tend to accelerate wound healing. In vivo, a mouse model of total skin defect demonstrates that PNI‐HA acting as hydrogel sealant significantly achieves the sutureless post‐wound‐closure at the early stage of wound healing, and then promotes wound healing by reducing inflammatory cells infiltration, promoting angiogenesis as well as reducing collagen deposition. These results…

Abstract Global reliance on fossil fuel combustion for energy production has contributed to the rising concentration of atmospheric CO 2 , creating significant global climate challenges. In this regard, direct air capture (DAC) of CO 2 from the atmosphere has emerged as one of the most promising strategies to counteract the harmful effects on the environment, and the further development and commercialization of this technology will play a pivotal role in achieving the goal of net‐zero emissions by 2050. Among various DAC adsorbents, metal–organic frameworks (MOFs) show great potential due to their high porosity and ability to reversibly adsorb CO 2 at low concentrations. However, the adsorption efficiency and cost‐effectiveness of these materials must be improved to be widely deployed as DAC sorbents. To that end, this perspective provides a critical discussion on several types of benchmark MOFs that have demonstrated high CO 2 capture capacities, including an assessment of their stability, CO 2 capture mechanism, capture‐release cycling behavior, and scale‐up synthesis. It then…

Abstract Optimization of components and micromorphology regulation are shown to be effective in boosting electromagnetic wave absorption (EMWA). One approach to achieve this enhancement is by utilizing the polarization effects of heterogeneous interfaces. Herein, NiSe 2 ‐CoSe 2 @C@MoSe 2 composites derived from NiCo‐MOF‐74 are fabricated via a facile selenization reaction and subsequent hydrothermal method. By varying the mass ratios of NiSe 2 ‐CoSe 2 @C and MoSe 2 , a series of NiSe 2 ‐CoSe 2 @C@MoSe 2 composites with hierarchical flower‐like core–shell structures are obtained. The EMWA properties of the composites display a trend of initially increasing and then decreasing with the increasing content of MoSe 2 . Interestingly, when the mass ratio of NiSe 2 ‐CoSe 2 @C and MoSe 2 is 3:2, the minimum reflection loss (RL) value is −50.10 dB and an effective absorption bandwidth (RL< −10 dB) value can reach 4.80 GHz (13.20–18.00 GHz). The remarkable EMWA capability can be ascribed to the synergy effects of conductive loss, polarization loss, and suitable impedance matching. This work…

Abstract Electrocatalytic glycerol oxidation reaction (GOR) is an effective way to convert biomass byproduct to high value‐added chemicals, which; however, suffers from the low oxidation activity and conversion ratio of the presently available catalysts. Herein, the NiCo 2 O 4 /NF bimetallic oxide nanoarray is controllably fabricated by Ni substituting for octahedral Co 3+ in Co 3 O 4 , which exhibits excellent GOR catalytic activity at elevated current densities ( E 300 = 1.42 V, E 600 = 1.62 V) and overall Faradaic efficiency of 97.5% at 1.42 V (FE formic acid = 89.9% and FE glycolic acid = 7.62%). The high performance is attributed to the structure evolution including the rapid generation of Ni III ‐OOH and Co III ‐OOH active species, the optimized intermediates adsorption, and the accelerated electron transfer owing to the Ni introduction, which are evidenced by the operando spectroscopy measurements and density functional theory calculations, respectively. The GOR/hydrogen evolution coupled two‐electrode electrolytic cell voltage is ≈299 mV lower than that of the water…

Abstract Multiple‐resonance (MR) thermal activated delayed fluorescence (TADF) emitters have attracted increasing attention in organic electroluminescence devices, owing to their superior quantum efficiency and narrowband emission for high color purity. However, MR‐TADF materials often suffer from severe aggregation‐caused quenching (ACQ) and efficiency roll‐off problems due to their rigid planar structures and the lack of sufficient charge‐transfer (CT) characters with inefficient reverse intersystem crossing (RISC). Herein, by attaching electron‐rich triphenylamine (TPA) with twisted spatial conformation to the MR framework, two efficient narrowband MR‐TADF emitters, namely BNCz‐pTPA and BNCz‐mTPA, are developed. The TPA substituent endows the new emitters with aggregation‐induced emission enhancement (AIEE) for ACQ suppression. The unprecedented AIEE‐MR‐TADF emitters exhibit CT character in high‐lying triplet excited states for faster RISC, while the locally‐excited (LE) character of the first singlet excited state is retained for narrowband emission with high emission…

Abstract The development of a multi‐functional solar‐driven interfacial evaporation (SDIE) system remains a significant challenge for its large‐scale applications. By taking advantage of high surface area, excellent young's moduli, anchoring/coupling capability, large absorption surface, strong absorption in the broadband solar spectrum, and efficient photothermal conversion efficiencies of 2D emerging materials (Xenes, Mxenes, etc.), hybrid SDIEs are developed to increase the use of solar energy beyond water production. This work aims to offer a systematic review of the recent advancement in 2D emerging materials except for graphene and their significant role in hybrid SDIEs to stimulate both fundamental and applied research on utilizing the underutilized auxiliary energy sources for future integrated water, energy, and environmental systems. For this purpose, first, the most recent progress in 2D photothermal materials is discussed, mainly including emerging Xenes, MXenes, and TMDs‐inspired hybrid SDIEs. Second, structural optimization strategies and modulation of the intrinsic…

Abstract The advancements in high‐performance flexible energy storage devices are crucial to realize the integration and multifunctionality of wearable devices. Transition metal selenides (TMSes), possess high theoretical capacity and electrical conductivity, which hold great promise for energy storage applications. This review provides a succinct summary of the progress of TMSes as high‐performance electrode materials for supercapacitor applications. First, the energy storage mechanism of TMSes and the effective strategies for achieving high‐performance TMSes are discussed. Subsequently, the recent process of TMSes‐based supercapacitors and other multifunctional applications is summarized. This paper aims to provide the superiority of TMSes as electrode materials and their recent advances for energy devices, to promote the development of high‐performance TMSes electrode materials in the fields of energy storage.

Abstract Hyaluronic acid (HA) is an attractive anionic polysaccharide polymer with inherent pharmacological properties and versatile chemical groups for modification. Due to their water retention ability, biocompatibility, biodegradation, cluster of differentiation‐44 targeting, and highly designable capacity, HA hydrogels have been an emerging biomaterial, showing tailoring performance in terms of chemical modifications and hydrogel forms. Various preparation technologies have been developed for the fabrication of the tailoring HA hydrogels with unique structures and functions. They have been utilized in diverse biomedical applications like drug delivery and tissue engineering scaffolds. Herein, this review comprehensively summarizes the HA derivatives with different molecule weights and functional modifications. Then the various fabrication methods to obtain tailoring hydrogels in the forms of nanogel, nanofiber, microparticle, microneedle patch, injectable hydrogel, and scaffold are reviewed as well. The emphasis is focused on the shining biomedical applications of these…

Abstract High‐performance thermal insulating aerogels are attractive candidates for thermal protection in extreme environments. However, inorganic aerogels’ brittleness and poor machinability limit their applications, while organic aerogels suffer from severe strength degradation and structural collapse at high temperatures. Herein, for the first time, a thermo‐responsive self‐ceramifiable aerogel is demonstrated with exceptional strengthening and thermal insulation at high temperatures. This aerogel exhibits excellent toughness and processability like polymers under normal conditions but spontaneously transforms into high‐strength semi‐crystalline hard ceramics upon exposure to high temperatures. After prolonged thermal attack at 800 °C, the strength of the aerogels does not decrease but significantly increases several‐fold (from 0.739 to 2.726 MPa). The self‐ceramization behavior and mechanism of the aerogel are illustrated in detail. The unique self‐ceramifiable capacity enables aerogels to provide fire resistance, high‐strength support, and excellent thermal insulation at…

Abstract The rational design of Ti 3 C 2 T x MXene‐derived TiO 2 ‐based photocatalysts with broad light absorption and efficient charge separation has recently attracted considerable attention for antibiotic degradation. However, the complementary effects of each component, especially oxygen vacancies (OVs) and high work function O‐terminated Ti 3 C 2 (O‐Ti 3 C 2 ), in affecting light absorption and photocatalytic activity remain controversial. In this study, Ti 3 C 2 T x ‐derived TiO 2 /Ti 3 C 2 T x photocatalysts are regulated by alkalization in the controlled KOH solution and calcination in different heating atmospheres to reveal the contribution of OVs, Ti 3+ , carbon species, and high work function titanium carbide. Carbon species and rich OVs co‐exist in TiO 2 /O‐Ti 3 C 2 (OV/C‐TT‐1K(N 2 )) which exhibit superior photocatalytic performance in tetracycline hydrochloride degradation with a kinetic constant of 0.0217 min −1 . Combined with experimental and DFT computational results, the broadened visible light response and desirable redox properties are caused by OVs and carbon…

Abstract NaF‐rich electrode–electrolyte interphases play crucial roles in determining the cycling stability of sodium metal batteries (SMBs) because of their electronic insulation and mechanical stability. In this work, perfluorobenzene (PFB) is proposed as the additive to contribute the formation of NaF‐rich solid electrolyte interphases (SEI). PFB at the periphery of the solvation layer can pull out a part of the EC with the lowest solvation energy by Van der Waals forces, thus allowing more to participate in the Na + solvation layer and form an anion‐aggregated solvation sheath, thus promoting the decomposition of to produce NaF. In addition, PFB has a higher highest occupied molecular orbital and lower lowest unoccupied molecular orbital energy level, which also preferentially decomposes to produce NaF at both electrodes. Benefiting from the intensified NaF ratio in SEI, the Na||Na symmetric cells with such an electrolyte achieves a superior cycling life over 350 h at 1 mA cm −2 , and the Na||Na 3 V 2 (PO 4 ) 2 O 2 F batteries also realize ultrahigh cycling performance with…

Abstract Hard carbon (HC) is widely regarded as the most promising anode material for sodium‐ion batteries (SIBs). For improving the sodium storage capacity of HC anode, current research primarily focuses on the high‐voltage slope region. Actually, increasing the storage capability in the low‐voltage plateau region is more important for enhancing the energy density of full cells. Therefore, in this study, HC anode with rich closed pore structure is designed and constructed with the help of carbon dots (CDs), and it is demonstrated that the presence of closed pore structure can provide more sodium storage sites in the plateau region, resulting in an obvious increase of sodium storage capacity. Moreover, the pore‐filling and intercalation mechanism for sodium storage in plateau region is revealed by in situ Raman spectroscopy and ex situ transmission electron microscopy (TEM). It is worth noting that the increase in capacity induced by closed pore‐filling is not accompanied by a decrease in initial coulombic efficiency (ICE), due to the fact that the introduction of closed pores does…

Abstract It is widely believed that excess/residual lead iodide (PbI 2 ) can affect the performance of perovskite solar cells . Moderate PbI 2 can enhance efficiency by passivating defects, while extremely active PbI 2 leads to non‐negligible hysteresis effects and reduces device stability. Although several efforts are made to investigate the role of excess PbI 2 , its impact is still underestimated. Recent advances further demonstrate the extraordinary potential of modifying excess PbI 2 ; however, a comprehensive study is required to obtain a deeper understanding. Herein, the important breakthroughs regarding excess PbI 2 are reviewed and the mechanism of excess PbI 2 in terms of efficiency and stability is rethought. In addition, the origins, verification, and regulation of residual PbI 2 are summarized.

Abstract Neuromorphic visual system with image perception, memory, and preprocessing functions is expected to simulate basic features of the human retina. Organic optoelectronic synaptic transistors emulating biological synapses may be promising candidates for constructing neural morphological visual system. However, the sensing wavelength range of organic optoelectronic synaptic transistors usually limits their potential in artificial multispectral visual perception. Here, retina‐inspired optoelectronic synaptic transistors that present broadband responses covering ultraviolet, visible, and near‐infrared regions are demonstrated, which leverage the wide‐range photoresponsive charge trapping layer and the heterostructure formed between PbS quantum dots and organic semiconductor. Simplified neuromorphic visual arrays are developed to simulate comprehensive image perception, memory, and preprocessing functions. Benefitting from the flexibility of the charge trapping and organic semiconductor layers, a flexible neuromorphic visual array can be fabricated, having an ultralow power…

Abstract It is a great challenge to design active and durable oxygen evolution reaction (OER) electrocatalysts for proton exchange membrane (PEM) electrolyzer due to the high dissolution of electrocatalysts in acidic solution. Herein, the Nd‐doped RuO2 (Nd0.1RuOx) is developed for enhanced oxygen evolution in 0.5 m H2SO4 solution with an overpotential of 211 mV to achieve 10 mA cm−2. The theoretical calculation reveals that the improved activity of Nd0.1RuOx is due to the moderate decrease of d‐band center energy, which balances the adsorption and desorption of oxygen intermediates. Moreover, the formation of more high valence state Ru4+ in Nd0.1RuOx is beneficial to the chemical stability of Ru species during the OER process, indicating that the introduction of Nd can effectively suppress the dissolution of Ru in acidic electrolytes. In addition, the PEM electrolyzer using Nd0.1RuOx/CC as the anode can be operated at 10 mA cm−2 stably for 50 h. This study sheds new light on the design of the OER catalysts in acid by engineering the electronic structure of RuO2.

Abstract Adsorption‐photocatalysis technology based on covalent organic frameworks (COFs) offers an alternative method for advancing the field of uranium extraction from seawater. When determining the photocatalytic activity of COFs, the binding energy of excitons ( E b ) functions is the decisive factor. Nevertheless, the majority of reported COFs have a large E b , which seriously restricts their application in the field of photocatalysis. Using a practical π‐skeleton engineering strategy, the current study synthesizes three donor‐acceptor olefin‐linked COFs containing amidoxime units in an effort to minimize E b . Theoretical and experimental results reveal that the construction of planar and continuous π ‐electron delocalization channels can significantly reduce E b and promote the separation of electron‐hole pairs, thereby enhancing the photocatalytic activities. Moreover, the E b of the TTh‐COF‐AO with a planar π ‐skeleton donor is significantly reduced, and exhibits a substantially smaller E b (38.4 meV). Under visible light irradiation, a high photo‐enhanced uranium…