The 100 most-cited articles in Advanced Materials, 2024

Interfacial layers (ILs) are prerequisites to form the selective charge transport for high-performance organic photovoltaics (OPVs) but mostly result in considerable parasitic absorption loss. Trimming the ILs down to a mono-molecular level via the self-assembled monolayer is an effective strategy to mitigate parasitic absorption loss. However, such a strategy suffers from inferior electrical contact with low surface coverage on rough surfaces and poor producibility. To address these issues, here, the self-assembled interlayer (SAI) strategy is developed, which involves a thin layer of 2-6 nm to form a full coverage on the substrate via both covalent and van der Waals bonds by using a self-assembled molecule of 2-(9H-carbazol-9-yl) (2PACz). Via the facile spin coating without further rinsing and annealing process, it not only optimizes the electrical and optical properties of OPVs, which enables a world-record efficiency of 20.17% (19.79% certified) but also simplifies the tedious processing procedure. Moreover, the SAI strategy is especially useful in improving the absorbing…

In the last decade, interfacial solar steam generation (ISSG), powered by natural sunlight garnered significant attention due to its great potential for low-cost and environmentally friendly clean water production in alignment with the global decarbonization efforts. This review aims to share the knowledge and engage with a broader readership about the current progress of ISSG technology and the facing challenges to promote further advancements toward practical applications. The first part of this review assesses the current strategies for enhancing the energy efficiency of ISSG systems, including optimizing light absorption, reducing energy losses, harvesting additional energy, and lowering evaporation enthalpy. Subsequently, the current challenges faced by ISSG technologies, notably salt accumulation and bio-fouling issues in practical applications, are elucidated and contemporary methods are discussed to overcome these challenges. In the end, potential applications of ISSG, ranging from initial seawater desalination and industrial wastewater purification to power generation,…

Abstract The advancement of thin, lightweight, and high‐power electronic devices has increasingly exacerbated issues related to electromagnetic interference and heat accumulation. To address these challenges, a spray‐drying‐sintering process is employed to assemble chain‐like CoNi and flake boron nitride (BN) into hydrangea‐like CoNi@BN heterostructure fillers. These fillers are then composited with polydimethylsiloxane (PDMS) to develop CoNi@BN/PDMS composites, which integrate low‐frequency microwave absorption and thermal conductivity. When the volume fraction of CoNi@BN is 44 vol% and the mass ratio of CoNi to BN is 3:1, the CoNi@BN/PDMS composites exhibit optimal performance in both low‐frequency microwave absorption and thermal conductivity. These composites achieve a minimum reflection loss of −49.9 dB and a low‐frequency effective absorption bandwidth of 2.40 GHz (3.92–6.32 GHz) at a thickness of 4.4 mm, fully covering the n79 band (4.4–5.0 GHz) for 5G communications. Meanwhile, the in‐plane thermal conductivity ( λ ∥ ) of the CoNi@BN/PDMS composites is 7.31 W m −1 K −1 ,…

Abstract Photocatalytic hydrogen peroxide (H2O2) synthesis from water and O2 is an economical, eco‐friendly, and sustainable route for H2O2 production. However, single‐component photocatalysts are subjected to limited light‐harvesting range, fast carrier recombination, and weak redox power. To promote photogenerated carrier separation and enhance redox abilities, an organic/inorganic S‐scheme photocatalyst is fabricated by in situ growing In2S3 nanosheets on a covalent organic framwork (COF) substrate for efficient H2O2 production in pure water. Interestingly, compared to unitary COF and In2S3, the COF/In2S3 S‐scheme photocatalysts exhibit significantly larger light‐harvesting range and stronger visible‐light absorption. Partial density of state calculation, X‐ray photoelectron spectroscopy, and femtosecond transient absorption spectroscopy reveal that the coordination between In2S3 and COF induces the formation of mid‐gap hybrid energy levels, leading to smaller energy gaps and broadened absorption. Combining electron spin resonance spectroscopy, radical‐trapping experiments, and…

Modern human civilization deeply relies on the rapid advancement of cutting-edge electronic systems that have revolutionized communication, education, aviation, and entertainment. However, the electromagnetic interference (EMI) generated by digital systems poses a significant threat to the society, potentially leading to a future crisis. While numerous efforts are made to develop nanotechnological shielding systems to mitigate the detrimental effects of EMI, there is limited focus on creating absorption-dominant shielding solutions. Achieving absorption-dominant EMI shields requires careful structural design engineering, starting from the smallest components and considering the most effective electromagnetic wave attenuating factors. This review offers a comprehensive overview of shielding structures, emphasizing the critical elements of absorption-dominant shielding design, shielding mechanisms, limitations of both traditional and nanotechnological EMI shields, and common misconceptions about the foundational principles of EMI shielding science. This systematic review serves as a…

In the era of information, characterized by an exponential growth in data volume and an escalating level of data abstraction, there has been a substantial focus on brain-like chips, which are known for their robust processing power and energy-efficient operation. Memristors are widely acknowledged as the optimal electronic devices for the realization of neuromorphic computing, due to their innate ability to emulate the interconnection and information transfer processes witnessed among neurons. This review paper focuses on memristor-based neuromorphic chips, which provide an extensive description of the working principle and characteristic features of memristors, along with their applications in the realm of neuromorphic chips. Subsequently, a thorough discussion of the memristor array, which serves as the pivotal component of the neuromorphic chip, as well as an examination of the present mainstream neural networks, is delved. Furthermore, the design of the neuromorphic chip is categorized into three crucial sections, including synapse-neuron cores, networks on chip (NoC), and…

In the past decade, with the rapid development of wearable electronics, medical health monitoring, the Internet of Things, and flexible intelligent robots, flexible pressure sensors have received unprecedented attention. As a very important kind of electronic component for information transmission and collection, flexible pressure sensors have gained a wide application prospect in the fields of aerospace, biomedical and health monitoring, electronic skin, and human-machine interface. In recent years, MXene has attracted extensive attention because of its unique 2D layered structure, high conductivity, rich surface terminal groups, and hydrophilicity, which has brought a new breakthrough for flexible sensing. Thus, it has become a revolutionary pressure-sensitive material with great potential. In this work, the recent advances of MXene-based flexible pressure sensors are reviewed from the aspects of sensing type, sensing mechanism, material selection, structural design, preparation strategy, and sensing application. The methods and strategies to improve the performance of MXene-based…

Abstract The excessive enrichment of nitrate in the environment can be converted into ammonia (NH 3 ) through electrochemical processes, offering significant implications for modern agriculture and the potential to reduce the burden of the Haber–Bosch (HB) process while achieving environmentally friendly NH 3 production. Emerging research on electrocatalytic nitrate reduction (eNitRR) to NH 3 has gained considerable momentum in recent years for efficient NH 3 synthesis. However, existing reviews on nitrate reduction have primarily focused on limited aspects, often lacking a comprehensive summary of catalysts, reaction systems, reaction mechanisms, and detection methods employed in nitrate reduction. This review aims to provide a timely and comprehensive analysis of the eNitRR field by integrating existing research progress and identifying current challenges. This review offers a comprehensive overview of the research progress achieved using various materials in electrochemical nitrate reduction, elucidates the underlying theoretical mechanism behind eNitRR, and discusses effective…

Abstract The interaction between oxygen species and metal sites of various orbitals exhibits intimate correlation with the oxygen reduction reaction (ORR) kinetics. Herein, a new approach for boosting the inherent ORR activity of atomically dispersed Fe−N−C matrix is represented by implanting Fe atomic clusters nearby. The as‐prepared catalyst delivers excellent ORR activity with half‐wave potentials of 0.78 and 0.90 V in acidic and alkaline solutions, respectively. The decent ORR activity can also be validated from the high‐performance rechargeable Zn–air battery. The experiments and density functional theory calculations reveal that the electron spin‐state of monodispersed Fe active sites is transferred from the low spin (LS, t 2g 6 e g 0 ) to the medium spin (MS, t 2g 5 e g 1 ) due to the involvement of Fe atomic clusters, leading to the spin electron filling in σ∗ orbit, by which it favors OH − desorption and in turn boosts the reaction kinetics of the rate‐determining step. This work paves a solid way for rational design of high‐performance Fe‐based single atom catalysts…

Lithium-ion batteries (LIBs), in which lithium ions function as charge carriers, are considered the most competitive energy storage devices due to their high energy and power density. However, battery materials, especially with high capacity undergo side reactions and changes that result in capacity decay and safety issues. A deep understanding of the reactions that cause changes in the battery's internal components and the mechanisms of those reactions is needed to build safer and better batteries. This review focuses on the processes of battery failures, with voltage and temperature as the underlying factors. Voltage-induced failures result from anode interfacial reactions, current collector corrosion, cathode interfacial reactions, overcharge, and over-discharge, while temperature-induced failure mechanisms include SEI decomposition, separator damage, and interfacial reactions between electrodes and electrolytes. The review also presents protective strategies for controlling these reactions. As a result, the reader is offered a comprehensive overview of the safety features and…

With the commercialization of first-generation flexible mobiles and displays in the late 2010s, humanity has stepped into the age of flexible electronics. Inevitably, soft multifunctional sensors, as essential components of next-generation flexible electronics, have attracted tremendous research interest like never before. This review is dedicated to offering an overview of the latest emerging trends in soft multifunctional sensors and their accordant future research and development (R&D) directions for the coming decade. First, key characteristics and the predominant target stimuli for soft multifunctional sensors are highlighted. Second, important selection criteria for soft multifunctional sensors are introduced. Next, emerging materials/structures and trends for soft multifunctional sensors are identified. Specifically, the future R&D directions of these sensors are envisaged based on their emerging trends, namely i) decoupling of multiple stimuli, ii) data processing, iii) skin conformability, and iv) energy sources. Finally, the challenges and potential opportunities for these…

The repair and functional reconstruction of bone defects resulting from severe trauma, surgical resection, degenerative disease, and congenital malformation pose significant clinical challenges. Bone tissue engineering (BTE) holds immense potential in treating these severe bone defects, without incurring prevalent complications associated with conventional autologous or allogeneic bone grafts. 3D printing technology enables control over architectural structures at multiple length scales and has been extensively employed to process biomimetic scaffolds for BTE. In contrast to inert and functional bone grafts, next-generation smart scaffolds possess a remarkable ability to mimic the dynamic nature of native extracellular matrix (ECM), thereby facilitating bone repair and regeneration. Additionally, they can generate tailored and controllable therapeutic effects, such as antibacterial or antitumor properties, in response to exogenous and/or endogenous stimuli. This review provides a comprehensive assessment of the progress of 3D-printed smart scaffolds for BTE applications. It begins…

Abstract Aqueous zinc‐ion batteries (AZIBs) have experienced a rapid surge in popularity, as evident from the extensive research with over 30 000 articles published in the past 5 years. Previous studies on AZIBs have showcased impressive long‐cycle stability at high current densities, achieving thousands or tens of thousands of cycles. However, the practical stability of AZIBs at low current densities (<1C) is restricted to merely 50–100 cycles due to intensified cathode dissolution. This genuine limitation poses a considerable challenge to their transition from the laboratory to the industry. In this study, leveraging density functional theory (DFT) calculations, an artificial interphase that achieves both hydrophobicity and restriction of the outward penetration of dissolved vanadium cations, thereby shifting the reaction equilibrium and suppressing the vanadium dissolution following Le Chatelier's principle, is described. The approach has resulted in one of the best cycling stabilities to date, with no noticeable capacity fading after more than 200 cycles (≈720 h) at 200 mA g −1…

In recent years, there has been widespread adoption of machine learning (ML) technologies to unravel intricate relationships among diverse parameters in various additive manufacturing (AM) techniques. These ML models excel at recognizing complex patterns from extensive, well-curated datasets, thereby unveiling latent knowledge crucial for informed decision-making during the AM process. The collaborative synergy between ML and AM holds the potential to revolutionize the design and production of AM-printed parts. This review delves into the challenges and opportunities emerging at the intersection of these two dynamic fields. It provides a comprehensive analysis of the publication landscape for ML-related research in the field of AM, explores common ML applications in AM research (such as quality control, process optimization, design optimization, microstructure analysis, and material formulation), and concludes by presenting an outlook that underscores the utilization of advanced ML models, the development of emerging sensors, and ML applications in emerging AM-related fields.…

Abstract [4‐(3,6‐dimethyl‐9H‐carbazol‐9yl)butyl]phosphonic acid (Me‐4PACz) self‐assembled molecules (SAM) are an effective method to solve the problem of the buried interface of NiO x in inverted perovskite solar cells (PSCs). However, the Me‐4PACz end group (carbazole core) cannot forcefully passivate defects at the bottom of the perovskite film. Here, a Co‐SAM strategy is employed to modify the buried interface of PSCs. Me‐4PACz is doped with phosphorylcholine chloride (PC) to form a Co‐SAM to improve the monolayer coverage and reduce leakage current. The phosphate group and chloride ions (Cl − ) in PC can inhibit NiO x surface defects. Meantime, the quaternary ammonium ions and Cl − in PC can fill organic cations and halogen vacancies in the perovskite film to enable defects passivation. Moreover, Co‐SAM can promote the growth of perovskite crystals, collaboratively solve the problem of buried defects, suppress nonradiative recombination, accelerate carrier transmission, and relieve the residual stress of the perovskite film. Consequently, the Co‐SAM modified devices show power…

Perovskite (PVSK) photovoltaic (PV) devices are undergoing rapid development and have reached a certified power conversion efficiency (PCE) of 26.1% at the cell level. Tremendous efforts in material and device engineering have also increased moisture, heat, and light-related stability. Moreover, the solution-process nature makes the fabrication process of perovskite photovoltaic devices feasible and compatible with some mature high-volume manufacturing techniques. All these features render perovskite solar modules (PSMs) suitable for terawatt-scale energy production with a low levelized cost of electricity (LCOE). In this review, the current status of perovskite solar cells (PSCs) and modules and their potential applications are first introduced. Then critical challenges are identified in their commercialization and propose the corresponding solutions, including developing strategies to realize high-quality films over a large area to further improve power conversion efficiency and stability to meet the commercial demands. Finally, some potential development directions and issues…

Photocatalytic solar hydrogen generation, encompassing both overall water splitting and organic reforming, presents a promising avenue for green hydrogen production. This technology holds the potential for reduced capital costs in comparison to competing methods like photovoltaic-electrocatalysis and photoelectrocatalysis, owing to its simplicity and fewer auxiliary components. However, the current solar-to-hydrogen efficiency of photocatalytic solar hydrogen production has predominantly remained low at ≈1-2% or lower, mainly due to curtailed access to the entire solar spectrum, thus impeding practical application of photocatalytic solar hydrogen production. This review offers an integrated, multidisciplinary perspective on photocatalytic solar hydrogen production. Specifically, the review presents the existing approaches in photocatalyst and system designs aimed at significantly boosting the solar-to-hydrogen efficiency, while also considering factors of cost and scalability of each approach. In-depth discussions extending beyond the efficacy of material and system design…

Abstract Increasing closed pore volume in hard carbon is considered to be the most effective way to enhance the electrochemical performance in sodium‐ion batteries. However, there is a lack of systematic insights into the formation mechanisms of closed pores at molecular level. In this study, a regulation strategy of closed pores via adjustment of the content of free radicals is reported. Sufficient free radicals are exposed by part delignification of bamboo, which is related to the formation of well‐developed carbon layers and rich closed pores. In addition, excessive free radicals from nearly total delignification lead to more reactive sites during pyrolysis, which competes for limited precursor debris to form smaller microcrystals and therefore compact the material. The optimal sample delivers a large closed pore volume of 0.203 cm 3 g −1 , which leads to a high reversible capacity of 350 mAh g −1 at 20 mA g −1 and enhanced Na + transfer kinetics. This work provides insights into the formation mechanisms of closed pores at molecular level, enabling rational design of hard carbon…

High-sensitive metasurface-based sensors are essential for effective substance detection and insightful bio-interaction studies, which compress light in subwavelength volumes to enhance light-matter interactions. However, current methods to improve sensing performance always focus on optimizing near-field response of individual meta-atom, and fingerprint recognition for bio-substances necessitates several pixelated metasurfaces to establish a quasi-continuous spectrum. Here, a novel sensing strategy is proposed to achieve Terahertz (THz) refractive sensing, and fingerprint recognition based on surface waves (SWs). Leveraging the long-range transmission, strong confinement, and interface sensitivity of SWs, a metasurface-supporting SWs excitation and propagation is experimentally verified to achieve sensing integrations. Through wide-band information collection of SWs, the proposed sensor not only facilitates refractive sensing up to 215.5°/RIU, but also enables the simultaneous resolution of multiple fingerprint information within a continuous spectrum. By covering 5 µm thickness of…

Abstract Urea electrosynthesis from co–electrolysis of NO 3 − and CO 2 (UENC) offers a promising technology for achieving sustainable and efficient urea production. Herein, a diatomic alloy catalyst (CuPd 1 Rh 1 –DAA), with mutually isolated Pd and Rh atoms alloyed on Cu substrate, is theoretically designed and experimentally confirmed to be a highly active and selective UENC catalyst. Combining theoretical computations and operando spectroscopic characterizations reveals the synergistic effect of Pd 1 –Cu and Rh 1 –Cu active sites to promote the UENC via a tandem catalysis mechanism, where Pd 1 –Cu site triggers the early C–N coupling and promotes *CO 2 NO 2 –to–*CO 2 NH steps, while Rh 1 –Cu site facilitates the subsequent protonation step of *CO 2 NH 2 to *COOHNH 2 toward the urea formation. Impressively, CuPd 1 Rh 1 –DAA assembled in a flow cell presents the highest urea Faradaic efficiency of 72.1% and urea yield rate of 53.2 mmol h −1 g cat −1 at −0.5 V versus RHE, representing nearly the highest performance among all reported UENC catalysts.

Radiative cooling (RC) is a carbon-neutral cooling technology that utilizes thermal radiation to dissipate heat from the Earth's surface to the cold outer space. Research in the field of RC has garnered increasing interest from both academia and industry due to its potential to drive sustainable economic and environmental benefits to human society by reducing energy consumption and greenhouse gas emissions from conventional cooling systems. Materials innovation is the key to fully exploit the potential of RC. This review aims to elucidate the materials development with a focus on the design strategy including their intrinsic properties, structural formations, and performance improvement. The main types of RC materials, i.e., static-homogeneous, static-composite, dynamic, and multifunctional materials, are systematically overviewed. Future trends, possible challenges, and potential solutions are presented with perspectives in the concluding part, aiming to provide a roadmap for the future development of advanced RC materials.

The global energy crisis and environmental concerns are driving research into renewable energy and sustainable energy conversion and storage technologies. Solar energy, as an ideal sustainable resource, has significant potential to contribute to the goal of net-zero carbon emissions if effectively harnessed and converted into a reliable and storable form of energy. Photocatalysts have the potential to convert sunlight into chemical energy carriers. In this respect, covalent organic frameworks (COFs) have shown great promise due to their tunable structure on different length scales, high surface areas, and beneficial optical properties such as broad visible light absorption. This review offers a comprehensive overview of the key developments in COF-based photocatalysts for various applications, including water splitting, hydrogen peroxide generation, organic transformations, and carbon dioxide and nitrogen reduction. The underlying mechanisms, essential principles for material design, and structure-function relationships of COFs in various photocatalytic applications are discussed.…

Nanomedicines are extensively explored for cancer therapy. By delivering drug molecules more efficiently to pathological sites and by attenuating their accumulation in healthy organs and tissues, nanomedicine formulations aim to improve the balance between drug efficacy and toxicity. More than 20 cancer nanomedicines are approved for clinical use, and hundreds of formulations are in (pre)clinical development. Over the years, several key pitfalls have been identified as bottlenecks in nanomedicine tumor targeting and translation. These go beyond materials- and production-related issues, and particularly also encompass biological barriers and pathophysiological heterogeneity. In this manuscript, the author describes the most important principles, progress, and products in nanomedicine tumor targeting, delineates key current problems and challenges, and discusses the most promising future prospects to create clinical impact.

Electromagnetic interference (EMI) shielding materials with low electromagnetic (EM) waves reflection characteristics are ideal materials for blocking EM radiation and pollution. Materials with low reflectivity must be constructed using materials with excellent EM waves absorption properties. However, materials simultaneously possessing both low reflectivity and excellent EMI shielding performance remain scarce, consequently, multilayer structures need to be developed. Poly(p-phenylene-2,6-benzobisoxazole) nanofibers (PNF) are prepared by deprotonation. PNF are combined with MXene and heterostructure MXene@Ni prepared by in-situ growth; MXene@Ni/PNF acts as an EM absorption layer while MXene/PNF acts as an EM reflective layer. Finally, (MXene@Ni/PNF)-(MXene/PNF) aerogels are prepared by layer-by-layer freeze-drying based on the layered modular design concept. Experimental characterizations revealed that (MXene@Ni/PNF)-(MXene/PNF) aerogels enable the efficient absorption-reflection-reabsorption of EM waves, effectively eliminating EMI. When the mass ratio of MXene to Ni in MXene@Ni…

Organic solar cells, as a cutting-edge sustainable renewable energy technology, possess a myriad of potential applications, while the bottleneck problem of less than 20% efficiency limits the further development. Simultaneously achieving an ordered molecular arrangement, appropriate crystalline domain size, and reduced nonradiative recombination poses a significant challenge and is pivotal for overcoming efficiency limitations. This study employs a dual strategy involving the development of a novel acceptor and ternary blending to address this challenge. A novel non-fullerene acceptor, SMA, characterized by a highly ordered arrangement and high lowest unoccupied molecular orbital energy level, is synthesized. By incorporating SMA as a guest acceptor in the PM6:BTP-eC9 system, it is observed that SMA staggered the liquid-solid transition of donor and acceptor, facilitating acceptor crystallization and ordering while maintaining a suitable domain size. Furthermore, SMA optimized the vertical morphology and reduced bimolecular recombination. As a result, the ternary device achieved a…

Abstract Real‐time continuous monitoring of non‐cognitive markers is crucial for the early detection and management of chronic conditions. Current diagnostic methods are often invasive and not suitable for at‐home monitoring. An elastic, adhesive, and biodegradable hydrogel‐based wearable sensor with superior accuracy and durability for monitoring real‐time human health is developed. Employing a supramolecular engineering strategy, a pseudo‐slide‐ring hydrogel is synthesized by combining polyacrylamide (pAAm), β‐cyclodextrin (β‐CD), and poly 2‐(acryloyloxy)ethyltrimethylammonium chloride (AETAc) bio ionic liquid (Bio‐IL). This novel approach decouples conflicting mechano–chemical effects arising from different molecular building blocks and provides a balance of mechanical toughness (1.1 × 10 6 Jm −3 ), flexibility, conductivity (≈0.29 S m −1 ), and tissue adhesion (≈27 kPa), along with rapid self‐healing and remarkable stretchability (≈3000%). Unlike traditional hydrogels, the one‐pot synthesis avoids chemical crosslinkers and metallic nanofillers, reducing cytotoxicity. While the…

Abstract Heterointerface engineering, which plays a pivotal role in developing advanced microwave‐absorbing materials, is employed to design zeolitic imidazolate framework (ZIF)–MXene nanocomposites. The ZIF–MXene composites are prepared by electrostatic self‐assembly of negatively charged titanium carbide MXene flakes and positively charged Co‐containing ZIF nanomaterials. This approach effectively creates abundant Mott–Schottky heterointerfaces exhibiting a robust built‐in electric field (BIEF) effect, as evidenced by experimental and theoretical analyses, leading to a notable attenuation of electromagnetic energy. Systematic manipulation of the BIEF‐exhibiting heterointerface, achieved through topological modulation of the ZIF, proficiently alters charge separation, facilitates electron migration, and ultimately enhances polarization relaxation loss, resulting in exceptional electromagnetic wave absorption performance (reflection loss RLmin = −47.35 dB and effective absorption bandwidth fE = 6.32 GHz). The present study demonstrates an innovative model system for elucidating the…

Biomass assumes an increasingly vital role in the realm of renewable energy and sustainable development due to its abundant availability, renewability, and minimal environmental impact. Within this context, 5-hydroxymethylfurfural (HMF), derived from sugar dehydration, stands out as a critical bio-derived product. It serves as a pivotal multifunctional platform compound, integral in synthesizing various vital chemicals, including furan-based polymers, fine chemicals, and biofuels. The high reactivity of HMF, attributed to its highly active aldehyde, hydroxyl, and furan ring, underscores the challenge of selectively regulating its conversion to obtain the desired products. This review highlights the research progress on efficient catalytic systems for HMF synthesis, oxidation, reduction, and etherification. Additionally, it outlines the techno-economic analysis (TEA) and prospective research directions for the production of furan-based chemicals. Despite significant progress in catalysis research, and certain process routes demonstrating substantial economics, with key indicators…

Extracellular vesicles (EVs) are promising next-generation therapeutics and drug delivery systems due to demonstrated safety and efficacy in preclinical models and early-stage clinical trials. There is an urgent need to address the immunogenicity of EVs (beyond the apparent lack of immunotoxicity) to advance clinical development. To date, few studies have assessed unintended immunological recognition of EVs. An in-depth understanding of EV-induced immunogenicity and clearance is necessary to develop effective therapeutic strategies, including approaches to mitigate immunological recognition when undesired. This article summarizes various factors involved in the potential immunogenicity of EVs and strategies to reduce immunological recognition for improved therapeutic benefit.

4D (bio-)printing endows 3D printed (bio-)materials with multiple functionalities and dynamic properties. 4D printed materials have been recently used in biomedical engineering for the design and fabrication of biomedical devices, such as stents, occluders, microneedles, smart 3D-cell engineered microenvironments, drug delivery systems, wound closures, and implantable medical devices. However, the success of 4D printing relies on the rational design of 4D printed objects, the selection of smart materials, and the availability of appropriate types of external (multi-)stimuli. Here, this work first highlights the different types of smart materials, external stimuli, and design strategies used in 4D (bio-)printing. Then, it presents a critical review of the biomedical applications of 4D printing and discusses the future directions of biomedical research in this exciting area, including in vivo tissue regeneration studies, the implementation of multiple materials with reversible shape memory behaviors, the creation of fast shape-transformation responses, the ability to operate at the…

Aqueous zinc-iodine batteries (AZIBs) are highly appealing for energy requirements owing to their safety, cost-effectiveness, and scalability. However, the inadequate redox kinetics and severe shuttling effect of polyiodide ions impede their commercial viability. Herein, several Zn-MOF-derived porous carbon materials are designed, and the further preparation of iron-doped porous carbon (Fe-N-C, M9) with varied Fe doping contents is optimized based on a facile self-assembly/carbonization approach. M9, with atomic Fe coordinated to nitrogen atoms, is employed as an efficient cathode host for AZIBs. Functional modifications of porous carbon hosts involving the doping species and levels are investigated. The adsorption tests, in situ Raman spectroscopy, and in situ UV-vis results demonstrate the adsorption capability and charge-discharge mechanism for the iodine species. Furthermore, experimental findings and theoretical analyses have proven that the redox conversion of iodine is enhanced through a physicochemical confinement effect. This study offers basic principles for the strategic…

Wearable epidermic electronics assembled from conductive hydrogels are attracting various research attention for their seamless integration with human body for conformally real-time health monitoring, clinical diagnostics and medical treatment, and human-interactive sensing. Nevertheless, it remains a tremendous challenge to simultaneously achieve conformally bioadhesive epidermic electronics with remarkable self-adhesiveness, reliable ultraviolet (UV) protection ability, and admirable sensing performance for high-fidelity epidermal electrophysiological signals monitoring, along with timely photothermal therapeutic performances after medical diagnostic sensing, as well as efficient antibacterial activity and reliable hemostatic effect for potential medical therapy. Herein, a conformally bioadhesive hydrogel-based epidermic sensor, featuring superior self-adhesiveness and excellent UV-protection performance, is developed by dexterously assembling conducting MXene nanosheets network with biological hydrogel polymer network for conformally stably attaching onto human skin for…

Abstract Intractable infected microenvironments caused by drug‐resistant bacteria stalls the normal course of wound healing. Sono‐piezodynamic therapy (SPT) is harnessed to combat pathogenic bacteria, but the superabundant reactive oxygen species (ROS) generated during SPT inevitably provoke severe inflammatory response, hindering tissue regeneration. Consequently, an intelligent nanocatalytic membrane composed of poly(lactic‐co‐glycolic acid) (PLGA) and black phosphorus /V 2 C MXene bio‐heterojunctions (2D 2 ‐bioHJs) is devised. Under ultrasonication, 2D 2 ‐bioHJs effectively eliminate drug‐resistant bacteria by disrupting metabolism and electron transport chain (ETC). When ultrasonication ceases, they enable the elimination of SPT‐generated ROS. The 2D 2 ‐bioHJs act as a “lever” that effectively achieves a balance between ROS generation and annihilation, delivering both antibacterial and anti‐inflammatory properties to the engineered membrane. More importantly, in vivo assays corroborate that the nanocatalytic membranes transform the stalled chronic wound environment into a…

Abstract The intelligent construction of non‐noble metal materials that exhibit reversible oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) with bifunctional electrocatalytic performance is greatly coveted in the realm of zinc‐air batteries (ZABs). Herein, a crafted structure‐amorphous MnO 2 lamellae encapsulated covalent triazine polymer‐derived N, S, P co‐doped carbon sphere (A‐MnO 2 /NSPC) is designed using a self‐doped pyrolysis coupled with an in situ encapsulation strategy. The customized A‐MnO 2 /NSPC‐2 demonstrates a superior bifunctional electrocatalytic performance, confirmed by a small Δ E index of 0.64 V for ORR/OER. Experimental investigations, along with density functional theory calculations validate that predesigned amorphous MnO 2 surface defects and abundant heteroatom catalytic active sites collectively enhance the oxygen electrocatalytic performance. Impressively, the A‐MnO 2 /NSPC‐based rechargeable liquid ZABs show a large open‐circuit potential of 1.54 V, an ultrahigh peak power density of 181 mW cm −2 , an enormous capacity of 816 mAh g −1…

Abstract Zinc–iodine batteries have the potential to offer high energy‐density aqueous energy storage, but their lifetime is limited by the rampant dendrite growth and the concurrent parasite side reactions on the Zn anode, as well as the shuttling of polyiodides. Herein, a cation‐conduction dominated hydrogel electrolyte is designed to holistically enhance the stability of both zinc anode and iodine cathode. In this hydrogel electrolyte, anions are covalently anchored on hydrogel chains, and the major mobile ions in the electrolyte are restricted to be Zn 2+ . Specifically, such a cation‐conductive electrolyte results in a high zinc ion transference number (0.81) within the hydrogel and guides epitaxial Zn nucleation. Furthermore, the optimized Zn 2+ solvation structure and the reconstructed hydrogen bond networks on hydrogel chains contribute to the reduced desolvation barrier and suppressed corrosion side reactions. On the iodine cathode side, the electrostatic repulsion between negative sulfonate groups and polyiodides hinders the loss of the iodine active material. This…

Abstract Covalent organic frameworks (COFs) as a new type of photocatalysts have shown unique advantages in visible‐light‐driven hydrogen evolution, while the reported overall water‐splitting systems are still very rare among various COF‐based photocatalysts. Herein, two COFs are integrated to construct a type of organic S‐scheme heterojunction for improved overall water splitting. In this system, TpBpy‐COF and COF‐316 serve as H 2 ‐ and O 2 ‐evolving components, respectively, which are combined through π–π interaction between conjugated aromatic rings. By introducing ultra‐small Pt nanoparticles (NPs) into the pores of the TpBpy‐COF nanosheets (NS), the resultant COF‐316/Pt@TpBpy‐COF NS heterostructure achieves extremely high H 2 and O 2 evolution rates of 220.4 and 110.2 µmol g −1 h −1 , respectively, under visible light irradiation ( λ ≥ 420 nm). The results of transient absorption spectra (TAS) and photoelectronic measurements indicate that the organic heterojunction interface notably facilitates the separation and transfer of photogenerated electron‐hole pairs. Further,…

Abstract Despite of urgent needs for highly stable and efficient electrochemical water‐splitting devices, it remains extremely challenging to acquire highly stable oxygen evolution reaction (OER) electrocatalysts under harsh industrial conditions. Here, a successful in situ synthesis of FeCoNiMnCr high‐entropy alloy (HEA) and high‐entropy oxide (HEO) heterocatalysts via a Cr‐induced spontaneous reconstruction strategy is reported, and it is demonstrated that they deliver excellent ultrastable OER electrocatalytic performance with a low overpotential of 320 mV at 500 mA cm −2 and a negligible activity loss after maintaining at 100 mA cm −2 for 240 h. Remarkably, the heterocatalyst holds outstanding long‐term stability under harsh industrial condition of 6 m KOH and 85 °C at a current density of as high as 500 mA cm −2 over 500 h. Density functional theory calculations reveal that the formation of the HEA‐HEO heterostructure can provide electroactive sites possessing robust valence states to guarantee long‐term stable OER process, leading to the enhancement of electroactivity. The…

Sodium-ion batteries (SIBs) have undergone rapid development as a complementary technology to lithium-ion batteries due to abundant sodium resources. However, the extended charging time and low energy density pose a significant challenge to the widespread use of SIBs in electric vehicles. To overcome this hurdle, there is considerable focus on developing fast-charging anode materials with rapid Na⁺ diffusion and superior reaction kinetics. Here, the key factors that limit the fast charging of anode materials are examined, which provides a comprehensive overview of the major advances and fast-charging characteristics across various anode materials. Specifically, it systematically dissects considerations to enhance the rate performance of anode materials, encompassing aspects such as porous engineering, electrolyte desolvation strategies, electrode/electrolyte interphase, electronic conductivity/ion diffusivity, and pseudocapacitive ion storage. Finally, the direction and prospects for developing fast-charging anode materials of SIBs are also proposed, aiming to provide a valuable…

Water is the source of life and civilization, but water icing causes catastrophic damage to human life and diverse industrial processes. Currently, superhydrophobic surfaces (inspired by the lotus effect) aided anti-icing attracts intensive attention due to their energy-free property. Here, recent advances in anti-icing by design and functionalization of superhydrophobic surfaces are reviewed. The mechanisms and advantages of conventional, macrostructured, and photothermal superhydrophobic surfaces are introduced in turn. Conventional superhydrophobic surfaces, as well as macrostructured ones, easily lose the icephobic property under extreme conditions, while photothermal superhydrophobic surfaces strongly rely on solar illumination. To address the above issues, a potentially smart strategy is found by developing macrostructured photothermal storage superhydrophobic (MPSS) surfaces, which integrate the functions of macrostructured superhydrophobic materials, photothermal materials, and phase change materials (PCMs), and are expected to achieve all-day anti-icing in various fields.…

Cuproptosis is a novel copper-dependent programmed cell death. The efficacy of cuproptosis is highly dependent on intracellular copper accumulation and counteracted by a high level of glutathione (GSH) in tumor cells. Here, this work develops a self-amplified cuproptosis nanoparticles (Cel-Cu NP) using celastrol (Cel), a natural product isolated from medical plant. In Cel-Cu NP, Cel serves as a versatile copper ionophore, exhibiting an ideal coordination capacity toward copper ions without compromising the cuproptosis induction. Notably, Cel can simultaneously scavenge GSH content to amplify cuproptosis. Moreover, this self-amplified cuproptosis further activates immunogenic cell death (ICD) to elicit robust immune response. Combining with immune checkpoint blockade, Cel-Cu NP effectively eradicates metastatic tumors in a mouse lung metastasis model. This study provides an efficient nanomedicine by inducing self-amplified cuproptosis for robust immunotherapy.

Wearable and implantable active medical devices (WIMDs) are transformative solutions for improving healthcare, offering continuous health monitoring, early disease detection, targeted treatments, personalized medicine, and connected health capabilities. Commercialized WIMDs use primary or rechargeable batteries to power their sensing, actuation, stimulation, and communication functions, and periodic battery replacements of implanted active medical devices pose major risks of surgical infections or inconvenience to users. Addressing the energy source challenge is critical for meeting the growing demand of the WIMD market that is reaching valuations in the tens of billions of dollars. This review critically assesses the recent advances in energy harvesting and storage technologies that can potentially eliminate the need for battery replacements. With a key focus on advanced materials that can enable energy harvesters to meet the energy needs of WIMDs, this review examines the crucial roles of advanced materials in improving the efficiencies of energy harvesters, wireless charging, and…

Diverse and adaptable modes of complex motion observed at different scales in living creatures are challenging to reproduce in robotic systems. Achieving dexterous movement in conventional robots can be difficult due to the many limitations of applying rigid materials. Robots based on soft materials are inherently deformable, compliant, adaptable, and adjustable, making soft robotics conducive to creating machines with complicated actuation and motion gaits. This review examines the mechanisms and modalities of actuation deformation in materials that respond to various stimuli. Then, strategies based on composite materials are considered to build toward actuators that combine multiple actuation modes for sophisticated movements. Examples across literature illustrate the development of soft actuators as free-moving, entirely soft-bodied robots with multiple locomotion gaits via careful manipulation of external stimuli. The review further highlights how the application of soft functional materials into robots with rigid components further enhances their locomotive abilities. Finally,…

Abstract Solar fuel synthesis is intriguing because solar energy is abundant and this method compensates for its intermittency. However, most photocatalysts can only absorb UV‐to‐visible light, while near‐infrared (NIR) light remains unexploited. Surprisingly, the charge transfer between ZnO and CuInS2 quantum dots (QDs) can transform a NIR‐inactive ZnO into a NIR‐active composite. This strong response is attributed to the increased concentration of free charge carriers in the p‐type semiconductor at the interface after the charge migration between ZnO and CuInS2, enhancing the localized surface plasmon resonance (LSPR) effect and the NIR response of CuInS2. As a paradigm, this ZnO/CuInS2 heterojunction is used for H2O2 production coupled with glycerin oxidation and demonstrates supreme performance, corroborating the importance of NIR response and efficient charge transfer. Mechanistic studies through contact potential difference (CPD), Hall effect test, and finite element method (FEM) calculation allow for the direct correlation between the NIR response and charge transfer. This…

Abstract Ensuring high catalytic activity and durability at low iridium (Ir)usage is still a big challenge for the development of electrocatalysts toward oxygen evolution reaction (OER) in proton exchange membrane water electrolysis (PEMWE). Here, a rapid liquid‐reduction combined with surface galvanic replacement strategy is reported to synthesize the sub 2 nm high‐entropy alloy (HEA) nanoparticles featured with Ir‐rich IrRuNiMo medium‐entropy oxide shell (Ir‐MEO) and a IrRuCoNiMo HEA core (HEA@Ir‐MEO). Advanced spectroscopies reveal that the Ir‐rich MEO shell inhibits the severe structural evolution of transition metals upon the OER, thus guaranteeing the structural stability. In situ differential electrochemical mass spectrometry, activation energy analysis and theoretical calculations unveil that the OER on HEA@Ir‐MEO follows an adsorbate evolution mechanism pathway, where the energy barrier of rate‐determining step is substantially lowered. The optimized catalyst delivers the excellent performance (1.85 V/3.0 A cm −2 @80 °C), long‐term stability (>500 h@1.0 Acm −2 ), and low…

Abstract Modulating the electronic structure of catalysts to effectively couple the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is essential for developing high‐efficiency anion exchange membrane water electrolyzer (AEMWE). Herein, a coral‐like nanoarray composed of nanosheets through the synergistic layering effect of cobalt and the 1D guiding of vanadium is synthesized, which promotes extensive contact between the active sites and electrolyte. The HER and OER activities can be enhanced by modulating the electronic structure through nitridation and phosphorization, respectively, enhancing the strength of metal‐H bond to optimize hydrogen adsorption and facilitating the proton transfer to improve the transformation of oxygen‐containing intermediates. Resultantly, the AEMWE achieves a current density of 500 mA cm –2 at 1.76 V for 1000 h in 1.0 M KOH at 70 °C. The energy consumption is 4.21 kWh Nm –3 with the producing hydrogen cost of $0.93 per kg H 2 . Operando synchrotron radiation and Bode phase angle analyses reveal that during the high‐energy consumed…

Wireless and wearable sensors attract considerable interest in personalized healthcare by providing a unique approach for remote, noncontact, and continuous monitoring of various health-related signals without interference with daily life. Recent advances in wireless technologies and wearable sensors have promoted practical applications due to their significantly improved characteristics, such as reduction in size and thickness, enhancement in flexibility and stretchability, and improved conformability to the human body. Currently, most researches focus on active materials and structural designs for wearable sensors, with just a few exceptions reflecting on the technologies for wireless data transmission. This review provides a comprehensive overview of the state-of-the-art wireless technologies and related studies on empowering wearable sensors. The emerging functional nanomaterials utilized for designing unique wireless modules are highlighted, which include metals, carbons, and MXenes. Additionally, the review outlines the system-level integration of wireless modules with…

Abstract By manipulating their asymmetric electronic spin states, the unique electronic structures and unsaturated coordination environments of single atoms can be effectively harnessed to control their magnetic properties. In this research, the first investigation is presented into the regulation of magnetic properties through the electronic spin states of single atoms. Magnetic single‐atom one‐dimensional materials, M‐N‐C/ZrO2 (M = Fe, Co, Ni), with varying electronic spin states, are design and synthesize based on the electronic orbital structure model. The SAs 3d electron spin structure of the composite M‐N‐C modulates the magneto physical properties and triggers a unique natural resonance loss, which achieves a controllable tuning of the effective absorption band under low‐frequency conditions. The minimum reflection loss (RLmin) of M‐N‐C can reach ‐69.71 dB, and the effective absorption bandwidth (EAB) ratio is as high as 91% (2–18 GHz). The current work provides a path toward achieving controllable modulation of low‐frequency electromagnetic wave bands by exploring the…

Abstract Single‐atom catalysts (SACs) have been increasingly explored in lithium–sulfur (Li–S) batteries to address the issues of severe polysulfide shuttle effects and sluggish redox kinetics. However, the structure‐activity relationship between single‐atom coordination structures and the performance of Li–S batteries remain unclear. In this study, a P, S co‐coordination asymmetric configuration of single atoms is designed to enhance the catalytic activity of Co central atoms and promote d‐p orbital hybridization between Co and S atoms, thereby limiting polysulfides and accelerating the bidirectional redox process of sulfur. The well‐designed SACs enable Li–S batteries to demonstrate an ultralow capacity fading rate of 0.027% per cycle after 2000 cycles at a high rate of 5 C. Furthermore, they display excellent rate performance with a capacity of 619 mAh g −1 at an ultrahigh rate of 10 C due to the efficient catalysis of CoSA‐N 3 PS. Importantly, the assembled pouch cell still retains a high discharge capacity of 660 mAh g −1 after 100 cycles at 0.2 C and provides a high areal…

Abstract The resistance of gels and elastomers increases significantly with tensile strain, which reduces conductive stability and restricts their use in stable and reliable electronics. Here, highly conductive tough hydrogels composed of silver nanowires (AgNWs), liquid metal (LM), and poly(vinyl alcohol) (PVA) are fabricated. The stretch‐induced orientations of AgNWs, deformable LM, and PVA nanocrystalline create conductive pathways, enhancing the mechanical properties of the hydrogels, including increased ultimate fracture stress (13‐33 MPa), strain (3000–5300%), and toughness (390.9–765.1 MJ m −3 ). Notably, the electrical conductivity of the hydrogels is significantly improved from 4.05 × 10 −3 to 24 S m −1 when stretched to 4200% strain, representing a 6000‐fold enhancement. The incorporation of PVA nanocrystalline, deformable LM, and AgNWs effectively mitigates stress concentration at the crack tip, thereby conferring crack propagation insensitivity and fatigue resistance to the hydrogels. Moreover, the hydrogels are designed with a reversible crosslinking network, allowing…

Triboelectric nanogenerator (TENG) manifests distinct advantages such as multiple structural selectivity, diverse selection of materials, environmental adaptability, low cost, and remarkable conversion efficiency, which becomes a promising technology for micro-nano energy harvesting and self-powered sensing. Tribo-dielectric materials are the fundamental and core components for high-performance TENGs. In particular, the charge generation, dissipation, storage, migration of the dielectrics, and dynamic equilibrium behaviors determine the overall performance. Herein, a comprehensive summary is presented to elucidate the dielectric charge transport mechanism and tribo-dielectric material modification principle toward high-performance TENGs. The contact electrification and charge transport mechanism of dielectric materials is started first, followed by introducing the basic principle and dielectric materials of TENGs. Subsequently, modification mechanisms and strategies for high-performance tribo-dielectric materials are highlighted regarding physical/chemical, surface/bulk, dielectric…

Burn wounds often bring high risks of delayed healing process and even death. Reactive oxygen species (ROS) play a crucial role in burn wound repair. However, the dynamic process in wound healing requires both the generation of ROS to inhibit bacteria and the subsequent reduction of ROS levels to initiate and promote tissue regeneration, which calls for a more intelligent ROS regulation dressing system. Hence, a dual-layered hydrogel (Dual-Gel) tailored to the process of burn wound repair is designed: the inner layer hydrogel (Gel 2) first responds to bacterial hyaluronidase (Hyal) to deliver aggregation-induced emission photosensitizer functionalized adipose-derived stem cell nanovesicles, which generate ROS upon light irradiation to eliminate bacteria; then the outer layer hydrogel (Gel 1) continuously starts a long-lasting consumption of excess ROS at the wound site to accelerate tissue regeneration. Simultaneously, the stem cell nanovesicles trapped in the burns wound also provide nutrients and mobilize neighboring tissues to thoroughly assist in inflammation regulation, cell…

Abstract Crafting semiconducting heterojunctions represents an effective route to enhance photocatalysis by improving interfacial charge separation and transport. However, lattice mismatch ( δ ) between different semiconductors can significantly hinder charge dynamics. Here, meticulous lattice tailoring is reported to create a covalent heterointerface with a built‐in electric field (BIEF), imparting markedly improved hydrogen peroxide (H 2 O 2 ) photosynthesis. Specifically, an In 2 S 3 /CdS heterojunction with a coherent heterointerface, characterized by covalent In─S─Cd bridge and exceptionally low lattice mismatch of 0.27%, and a BIEF from In 2 S 3 to CdS, is rationally designed. This heterojunction entails rapid charge separation and transfer, achieving an outstanding H 2 O 2 production rate of 2.09 mmol g −1 h −1 without the need for scavengers and oxygen bubbling, and a high apparent quantum efficiency of 17.73% at 400 nm. Density functional theory (DFT) calculations further reveal that this Z‐scheme heterojunction facilitates the adsorption of * O 2 and the generation of *…

The development of high-performance electrocatalysts for energy conversion reactions is crucial for advancing global energy sustainability. The design of catalysts based on their electronic properties (e.g., work function) has gained significant attention recently. Although numerous reviews on electrocatalysis have been provided, no such reports on work function-guided electrocatalyst design are available. Herein, a comprehensive summary of the latest advancements in work function-guided electrocatalyst design for diverse electrochemical energy applications is provided. This includes the development of work function-based catalytic activity descriptors, and the design of both monolithic and heterostructural catalysts. The measurement of work function is first discussed and the applications of work function-based catalytic activity descriptors for various reactions are fully analyzed. Subsequently, the work function-regulated material-electrolyte interfacial electron transfer (IET) is employed for monolithic catalyst design, and methods for regulating the work function and optimizing…

Abstract Achieving radar‐infrared compatible camouflage with dynamic adaptability has been a long‐sought goal, but faces significant challenges owing to the limited dispersion relations of conventional material systems operating in different wavelength ranges. Here, this work proposes the concept of pneumatic multiscale shape morphing and design a periodically arranged pneumatic unit consisting of MXene‐based morphable conductors and intake platforms. During gas actuation, the morphable conductor transforms centimeter‐scale 2D flat sheets into 3D balloon shapes to enhance microwave absorption behavior, and also reconfigures micrometer‐scale MXene wrinkles into smooth planes in combination with cavity‐induced low heat transfer to minimize infrared (IR) signatures. Through theory‐guided reverse engineering, the final pneumatic matrix shows remarkable frequency tunability (2.64–18.0 GHz), moderate IR emissivity regulation (0.14 at 7–16.5 µm), rapid responsiveness (≈30 ms), wide‐angle operation (>45°), and excellent environmental tolerance. Additionally, the multiplexed pneumatic matrix…

Bioelectricity provides electrostimulation to regulate cell/tissue behaviors and functions. In the human body, bioelectricity can be generated in electromechanically responsive tissues and organs, as well as biomolecular building blocks that exhibit piezoelectricity, with a phenomenon known as the piezoelectric effect. Inspired by natural bio-piezoelectric phenomenon, efforts have been devoted to exploiting high-performance synthetic piezoelectric biomaterials, including molecular materials, polymeric materials, ceramic materials, and composite materials. Notably, piezoelectric biomaterials polarize under mechanical strain and generate electrical potentials, which can be used to fabricate electronic devices. Herein, a review article is proposed to summarize the design and research progress of piezoelectric biomaterials and devices toward bionanotechnology. First, the functions of bioelectricity in regulating human electrophysiological activity from cellular to tissue level are introduced. Next, recent advances as well as structure-property relationship of various natural and…

Abstract Solid polymer electrolytes (SPEs) for lithium metal batteries have garnered considerable interests owing to their low cost, flexibility, lightweight, and favorable interfacial compatibility with battery electrodes. Their soft mechanical nature compared to solid inorganic electrolytes give them a large advantage to be used in low pressure solid‐state lithium metal batteries, which can avoid the cost and weight of the pressure cages. However, the application of SPEs is hindered by their relatively low ionic conductivity. In addressing this limitation, enormous efforts are devoted to the experimental investigation and theoretical calculations/simulation of new polymer classes. Recently, metal–organic frameworks (MOFs) have been shown to be effective in enhancing ion transport in SPEs. However, the mechanisms in enhancing Li + conductivity have rarely been systematically and comprehensively analyzed. Therefore, this review provides an in‐depth summary of the mechanisms of MOF‐enhanced Li + transport in MOF‐based solid polymer electrolytes (MSPEs) in terms of polymer, MOF,…

Abstract Thanks to the extensive efforts toward optimizing perovskite crystallization properties, high‐quality perovskite films with near‐unity photoluminescence quantum yield are successfully achieved. However, the light outcoupling efficiency of perovskite light‐emitting diodes (PeLEDs) is impeded by insufficient light extraction, which poses a challenge to the further advancement of PeLEDs. Here, an anisotropic multifunctional electron transporting material, 9,10‐bis(4‐(2‐phenyl‐1H‐benzo[d]imidazole‐1‐yl)phenyl) anthracene (BPBiPA), with a low extraordinary refractive index (ne) and high electron mobility is developed for fabricating high‐efficiency PeLEDs. The anisotropic molecular orientations of BPBiPA can result in a low ne of 1.59 along the z‐axis direction. Optical simulations show that the low ne of BPBiPA can effectively mitigate the surface plasmon polariton loss and enhance the photon extraction efficiency in waveguide mode, thereby improving the light outcoupling efficiency of PeLEDs. In addition, the high electron mobility of BPBiPA can facilitate balanced carrier…

Abstract Renewable electricity‐powered nitrate/carbon dioxide co‐reduction reaction toward urea production paves an attractive alternative to industrial urea processes and offers a clean on‐site approach to closing the global nitrogen cycle. However, its large‐scale implantation is severely impeded by challenging C–N coupling and requires electrocatalysts with high activity/selectivity. Here, cobalt‐nanoparticles anchored on carbon nanosheet (Co NPs@C) are proposed as a catalyst electrode to boost yield and Faradaic efficiency (FE) toward urea electrosynthesis with enhanced C–N coupling. Such Co NPs@C renders superb urea‐producing activity with a high FE reaching 54.3% and a urea yield of 2217.5 µg h −1 mg cat. −1 , much superior to the Co NPs and C nanosheet counterparts, and meanwhile shows strong stability. The Co NPs@C affords rich catalytically active sites, fast reactant diffusion, and sufficient catalytic surfaces‐electrolyte contacts with favored charge and ion transfer efficiencies. The theoretical calculations reveal that the high‐rate formation of *CO and *NH 2…

Direct Laser Writing (DLW) has been increasingly selected as a microfabrication route for efficient, cost-effective, high-resolution material synthesis and conversion. Concurrently, lasers participate in the patterning and assembly of functional geometries in several fields of application, of which electronics stand out. In this review, recent advances and strategies based on DLW for electronics microfabrication are surveyed and outlined, based on laser material growth strategies. First, the main DLW parameters influencing material synthesis and transformation mechanisms are summarized, aimed at selective, tailored writing of conductive and semiconducting materials. Additive and transformative DLW processing mechanisms are discussed, to open space to explore several categories of materials directly synthesized or transformed for electronics microfabrication. These include metallic conductors, metal oxides, transition metal chalcogenides and carbides, laser-induced graphene, and their mixtures. By accessing a wide range of material types, DLW-based electronic applications are…

Abstract Layered transition‐metal (TM) oxide cathodes have attracted growing attention in sodium‐ion batteries (SIBs). However, their practical implementation is plagued by Jahn–Teller distortion and irreversible cation migration, leading to severe voltage decay and structure instability. Herein, O3‐Na 0.898 K 0.058 Ni 0.396 Fe 0.098 Mn 0.396 Ti 0.092 O 2 (KT‐NFM) is reported as an ultrastable cathode material via multisite substitution with rigid KO 6 pillars and flexible TiO 6 octahedra. The K pillars induce contracted TMO 2 slabs and their strong Coulombic repulsion to inhibit Ni/Fe migration; and Ti incorporation reinforces the hybridization of Ni(3deg*)‐O(2p) to mitigate the undesired O3–O'3 phase transition. These enable the reversible redox of Ni 2 +↔Ni 3 . 20 + and Fe 3 +↔Fe 3.69 + for 138.6 mAh g −1 and ultrastable cycles with >90% capacity retention after 2000 cycles in a pouch cell of KT‐NFM||hard carbon. This will provide insights into the design of ultrastable layered cathode materials of sodium‐ion batteries and beyond.

Abstract Efficient and stable red perovskite light‐emitting diodes (PeLEDs) demonstrate promising potential in high‐definition displays and biomedical applications. Although significant progress has been made in device performance, meeting commercial demands remains a challenge in the aspects of long‐term stability and high external quantum efficiency (EQE). Here, an in situ crystallization regulation strategy is developed for optimizing red perovskite films through ingenious vapor design. Mixed vapor containing dimethyl sulfoxide and carbon disulfide (CS 2 ) is incorporated to conventional annealing, which contributes to thermodynamics dominated perovskite crystallization for well‐aligned cascade phase arrangement. Additionally, the perovskite surface defect density is minimized by the CS 2 molecule adsorption. Consequently, the target perovskite films exhibit smooth exciton energy transfer, reduced defect density, and blocked ion migration pathways. Leveraging these advantages, spectrally stable red PeLEDs are obtained featuring emission at 668, 656, and 648 nm, which yield record…

Abstract The advancement of aqueous zinc‐ion batteries (AZIBs) is often hampered by the dendritic zinc growth and the parasitic side reactions between the zinc anode and the aqueous electrolyte, especially under extreme temperature conditions. This study unveils the performance decay mechanism of zinc anodes in harsh environments, characterized by “dead zinc” at low temperatures and aggravated hydrogen evolution and adverse by‐products at elevated temperatures. To address these issues, a temperature self‐adaptive electrolyte (TSAE), founded on the competitive coordination principle of co‐solvent and anions, is introduced. This electrolyte exhibits a dynamic solvation capability, engendering an inorganic‐rich solid electrolyte interface (SEI) at low temperatures while an organic alkyl ether‐ and alkyl carbonate‐containing SEI at elevated temperatures. The self‐adaptability of the electrolyte significantly enhances the performance of the zinc anode across a broad temperature range. A Zn//Zn symmetrical cell, based on the TSAE, showcases reversible plating/stripping exceeding 16 800 h…

Abstract Reconstruction of catalysts is now well recognized as a common phenomenon in electrocatalysis. As the reconstructed structure may promote or hamper the electrochemical performance, how to achieve the designed active surface for highly enhanced catalytic activity through the reconstruction needs to be carefully investigated. In this review, the genesis and electrochemical effects of reconstruction in various electrochemical catalytic processes, such as hydrogen evolution reaction (HER), oxygen evolution reaction (OER), carbon dioxide reduction reaction (CO 2 RR), and nitrate reduction reaction (NO 3 RR) are first described. Then, the strategies for optimizing the reconstruction, such as valence states control, active phase retention, phase evolution engineering, and surface poisoning prevention are comprehensively discussed. Finally, the general rules of reconstruction optimization are summarized and give perspectives for future study. It is believed that the review shall provide deep insights into electrocatalytic mechanisms and guide the design of pre‐catalysts with highly…

Abstract Atomically dispersed active sites in a photocatalyst offer unique advantages such as locally tuned electronic structures, quantum size effects, and maximum utilization of atomic species. Among these, asymmetric atomic dual‐sites are of particular interest because their asymmetric charge distribution generates a local built‐in electric potential to enhance charge separation and transfer. Moreover, the dual sites provide flexibility for tuning complex multielectron and multireaction pathways, such as CO 2 reduction reactions. The coordination of dual sites opens new possibilities for engineering the structure–activity–selectivity relationship. This comprehensive overview discusses efficient and sustainable photocatalysis processes in photocatalytic CO 2 reduction, focusing on strategic active‐site design and future challenges. It serves as a timely reference for the design and development of photocatalytic conversion processes, specifically exploring the utilization of asymmetric atomic dual‐sites for complex photocatalytic conversion pathways, here exemplified by the…

Single-atom nanozymes (SAzymes) showcase not only uniformly dispersed active sites but also meticulously engineered coordination structures. These intricate architectures bestow upon them an exceptional catalytic prowess, thereby captivating numerous minds and heralding a new era of possibilities in the biomedical landscape. Tuning the microstructure of SAzymes on the atomic scale is a key factor in designing targeted SAzymes with desirable functions. This review first discusses and summarizes three strategies for designing SAzymes and their impact on reactivity in biocatalysis. The effects of choices of carrier, different synthesis methods, coordination modulation of first/second shell, and the type and number of metal active centers on the enzyme-like catalytic activity are unraveled. Next, a first attempt is made to summarize the biological applications of SAzymes in tumor therapy, biosensing, antimicrobial, anti-inflammatory, and other biological applications from different mechanisms. Finally, how SAzymes are designed and regulated for further realization of diverse biological…

Abstract To obtain high‐performance electromagnetic microwave (EM) absorption materials with broad effective absorption bandwidth (EAB) and reduced thickness, designing structures has proved to be a promising way. Herein, ultra‐broadband multilayer bidirectional MXene/polyimide EM absorption aerogels containing multi‐structures on scales ranging from the micro‐ to the macroscale are produced with the aid of electric and temperature fields. On the microscale, under the action of electric force and temperature gradient, the ordered structures made of aligned Ti3C2Tx MXene nanosheets and the microscale layered aerogel walls enable the bidirectional aerogel to achieve a wide EAB of 8.58 GHz at a thickness of 2.1 mm. This is ascribed to the numerous aligned nanosheets and layered aerogel walls perpendicular to the incident EMs, facilitating the conversion of electromagnetic energy into electrical energy. Furthermore, on the macroscale, the multilayer bidirectional aerogel with non‐gradient structures effectively resolves the conflict between impedance matching and energy loss, resulting…

Abstract Demetalation caused by the electrochemical dissolution of metallic Fe atoms is a major challenge for the practical application of Fe─N─C catalysts. Herein, an efficient single metallic Mn active site is constructed to improve the strength of the Fe─N bond, inhibiting the demetalation effect of Fe─N─C. Mn acts as an electron donor inducing more delocalized electrons to reduce the oxidation state of Fe by increasing the electron density, thereby enhancing the Fe─N bond and inhibiting the electrochemical dissolution of Fe. The oxygen reduction reaction pathway for the dissociation of Fe─Mn dual sites can overcome the high energy barriers to direct O─O bond dissociation and modulate the electronic states of Fe─N 4 sites. The resulting FeMn─N─C exhibits excellent ORR activity with a high half‐wave potential of 0.92 V in alkaline electrolytes. FeMn─N─C as a cathode catalyst for Zn‐air batteries has a cycle stability of 700 h at 25 °C and a long cycle stability of more than 210 h under extremely cold conditions at −40 °C. These findings contribute to the development of efficient…

This study underscores the significance of precisely manipulating the morphology of the active layer in organic solar cells (OSCs). By blending polymer donors of D18 with varying molecular weights, a multiscale interpenetrating fiber network structure within the active layer is successfully created. The introduction of 10% low molecular weight D18 (LW-D18) into high molecular weight D18 (HW-D18) produces MIX-D18, which exhibits an extended exciton diffusion distance and orderly molecular stacking. Devices utilizing MIX-D18 demonstrate superior electron and hole transport, improves exciton dissociation, enhances charge collection efficiency, and reduces trap-assisted recombination compared to the other two materials. Through the use of the nonfullerene acceptor L8-BO, a remarkable power conversion efficiency (PCE) of 20.0% is achieved. This methodology, which integrates the favorable attributes of high and low molecular weight polymers, opens a new avenue for enhancing the performance of OSCs.

The challenges associated with heat dissipation in high-power electronic devices used in communication, new energy, and aerospace equipment have spurred an urgent need for high-performance thermal interface materials (TIMs) to establish efficient heat transfer pathways from the heater (chip) to heat sinks. Recently, emerging 2D materials, such as graphene and boron nitride, renowned for their ultrahigh basal-plane thermal conductivity and the capacity to facilitate cross-scale, multi-morphic structural design, have found widespread use as thermal fillers in the production of high-performance TIMs. To deepen the understanding of 2D material-based TIMs, this review focuses primarily on graphene and boron nitride-based TIMs, exploring their structures, properties, and applications. Building on this foundation, the developmental history of these TIMs is emphasized and a detailed analysis of critical challenges and potential solutions is provided. Additionally, the preparation and application of some other novel 2D materials-based TIMs are briefly introduced, aiming to offer constructive…

The rapid growth of electric vehicle use is expected to cause a significant environmental problem in the next few years due to the large number of spent lithium-ion batteries (LIBs). Recycling spent LIBs will not only alleviate the environmental problems but also address the challenge of limited natural resources shortages. While several hydro- and pyrometallurgical processes are developed for recycling different components of spent batteries, direct regeneration presents clear environmental, and economic advantages. The principle of the direct regeneration approach is restoring the electrochemical performance by healing the defective structure of the spent materials. Thus, the development of direct regeneration technology largely depends on the formation mechanism of defects in spent LIBs. This review systematically details the degradation mechanisms and types of defects found in diverse cathode materials, graphite anodes, and current collectors during the battery's lifecycle. Building on this understanding, principles and methodologies for directly rejuvenating materials within…

Solar-driven interfacial evaporation (SDIE) has played a pivotal role in optimizing water-energy utilization, reducing conventional power costs, and mitigating environmental impacts. The increasing emphasis on the synergistic cogeneration of water and green electricity through SDIE is particularly noteworthy. However, there is a gap of existing reviews that have focused on the mechanistic understanding of green power from water-electricity cogeneration (WEC) systems, the structure-activity relationship between efficiency of green energy utilization in WEC and material design in SDIE. Particularly, it lacks a comprehensive discussion to address the challenges faced in these areas along with potential solutions. Therefore, this review aims to comprehensively assess the progress and future perspective of green electricity from WEC systems by investigating the potential expansion of SDIE. First, it provides a comprehensive overview about material rational design, thermal management, and water transportation tunnels in SDIE. Then, it summarizes diverse energy sources utilized in the SDIE…

Multi-dimensional multiplexed metasurface holography extends holographic information capacity and promises revolutionary advancements for vivid imaging, information storage, and encryption. However, achieving multifunctional metasurface holography by forward design method is still difficult because it relies heavily on Jones matrix engineering, which places high demands on physical knowledge and processing technology. To break these limitations and simplify the design process, here, an end-to-end inverse design framework is proposed. By directly linking the metasurface to the reconstructed images and employing a loss function to guide the update of metasurface, the calculation of hologram can be omitted; thus, greatly simplifying the design process. In addition, the requirements on the completeness of meta-library can also be significantly reduced, allowing multi-channel hologram to be achieved using meta-atoms with only two degrees of freedom, which is very friendly to processing. By exploiting the proposed method, metasurface hologram containing up to 12 channels of…

State-of-the-art Fenton-like reactions are crucial in advanced oxidation processes (AOPs) for water purification. This review explores the latest advancements in heterogeneous metal-based catalysts within AOPs, covering nanoparticles (NPs), single-atom catalysts (SACs), and ultra-small atom clusters. A distinct connection between the physical properties of these catalysts, such as size, degree of unsaturation, electronic structure, and oxidation state, and their impacts on catalytic behavior and efficacy in Fenton-like reactions. In-depth comparative analysis of metal NPs and SACs is conducted focusing on how particle size variations and metal-support interactions affect oxidation species and pathways. The review highlights the cutting-edge characterization techniques and theoretical calculations, indispensable for deciphering the complex electronic and structural characteristics of active sites in downsized metal particles. Additionally, the review underscores innovative strategies for immobilizing these catalysts onto membrane surfaces, offering a solution to the inherent…

Abstract Cost‐effectiveness plays a decisive role in sustainable operating of rechargeable batteries. As such, the low cost‐consumption of sodium‐ion batteries (SIBs) and potassium‐ion batteries (PIBs) provides a promising direction for “how do SIBs/PIBs replace Li‐ion batteries (LIBs) counterparts” based on their resource abundance and advanced electrochemical performance. To rationalize the SIBs/PIBs technologies as alternatives to LIBs from the unit energy cost perspective, this review gives the specific criteria for their energy density at possible electrode‐price grades and various battery‐longevity levels. The cost ($ kWh −1 cycle −1 ) advantage of SIBs/PIBs is ascertained by the cheap raw‐material compensation for the cycle performance deficiency and the energy density gap with LIBs. Furthermore, the cost comparison between SIBs and PIBs, especially on cost per kWh and per cycle, is also involved. This review explicitly manifests the practicability and cost‐effectiveness toward SIBs are superior to PIBs whose commercialization has so far been hindered by low energy density.…

Abstract Interfacial instability within aqueous zinc batteries (AZBs) spurs technical obstacles including parasitic side reactions and dendrite failure to reach the practical application standards. Here, an interfacial engineering is showcased by employing a bio‐ derived zincophilic macromolecule as the electrolyte additive (0.037 wt%), which features a long‐chain configuration with laterally distributed hydroxyl and sulfate anion groups, and has the propensity to remodel the electric double layer of Zn anodes. Tailored Zn2+‐rich compact layer is the result of their adaptive adsorption that effectively homogenizes the interfacial concentration field, while enabling a hybrid nucleation and growth mode characterized as nuclei‐rich and space‐confined dense plating. Further resonated with curbed corrosion and by‐products, a dendrite‐free deposition morphology is achieved. Consequently, the macromolecule‐modified zinc anode delivers over 1250 times of reversible plating/stripping at a practical area capacity of 5 mAh cm−2, as well as a high zinc utilization rate of 85%. The Zn//NH4V4O10…

Abstract Recently, hydrogel‐based soft materials have demonstrated huge potential in soft robotics, flexible electronics as well as artificial skins. Although various methods are developed to prepare tough and strong hydrogels, it is still challenging to simultaneously enhance the strength and toughness of hydrogels, especially for protein‐based hydrogels. Herein, a biomimetic “salting out—alignment—locking” tactic (SALT) is introduced for enhancing mechanical properties through the synergy of alignment and the salting out effect. As a typical example, tensile strength and modulus of initially brittle gelatin hydrogels increase 940 folds to 10.12 ± 0.50 MPa and 2830 folds to 34.26 ± 3.94 MPa, respectively, and the toughness increases up to 1785 folds to 14.28 ± 3.13 MJ m −3 . The obtained strength and toughness hold records for the previously reported gelatin‐based hydrogel and are close to the tendons. It is further elucidated that the salting out effect engenders hydrophobic domains, while prestretching facilitates chain alignment, both synergistically contributing to the…

Although nanozymes have drawn great attention over the past decade, the activities of peroxidase-like, oxidase-like, and catalase-like nanozymes are often pH dependent with elusive mechanism, which largely restricts their application. Therefore, a systematical discussion on the pH-related catalytic mechanisms of nanozymes together with the methods to overcome this limitation is in need. In this review, various nanozymes exhibiting pH-dependent catalytic activities are collected and the root causes for their pH dependence are comprehensively analyzed. Subsequently, regulatory concepts including catalytic environment reconstruction and direct catalytic activity improvement to break this pH restriction are summarized. Moreover, applications of pH-independent nanozymes in sensing, disease therapy, and pollutant degradation are overviewed. Finally, current challenges and future opportunities on the development of pH-independent nanozymes are suggested. It is anticipated that this review will promote the further design of pH-independent nanozymes and broaden their application range with…

4D printing has attracted tremendous worldwide attention during the past decade. This technology enables the shape, property, or functionality of printed structures to change with time in response to diverse external stimuli, making the original static structures alive. The revolutionary 4D-printing technology offers remarkable benefits in controlling geometric and functional reconfiguration, thereby showcasing immense potential across diverse fields, including biomedical engineering, electronics, robotics, and photonics. Here, a comprehensive review of the latest achievements in 4D printing using various types of materials and different additive manufacturing techniques is presented. The state-of-the-art strategies implemented in harnessing various 4D-printed structures are highlighted, which involve materials design, stimuli, functionalities, and applications. The machine learning approach explored for 4D printing is also discussed. Finally, the perspectives on the current challenges and future trends toward further development in 4D printing are summarized.

Abstract Maintaining a match between input solar energy and required energy by water supply management is key to achieving efficient interfacial solar‐driven evaporation (ISDE). In practice, the solar radiation flux is constantly changing throughout the day, so keeping a dynamic water‐energy‐balance of ISDE is a big challenge. Herein, a photothermal water diode (WD) evaporator concept is proposed by an integrated hydrophilic/hydrophobic Janus absorber to overcome the issue. Due to the unique unidirectional water transport properties induced by asymmetric wettability, a self‐adaptive balance between photothermal energy input and water uptake is established, thus realizing the energy matching and utilization maximization. The experimental and simulation results exhibit that with the increase of sunlight intensity, the water supply speed is significantly accelerated due to the dynamic management and self‐regulation on water replenishment. Therefore, an excellent evaporation rate of up to 2.14 kg m –2 h –1 with a high efficiency of 93.7% under 1 sun illumination is achieved. This water…

Addressing large bone defects remains a significant challenge owing to the inherent limitations in self-healing capabilities, resulting in prolonged recovery and suboptimal regeneration. Although current clinical solutions are available, they have notable shortcomings, necessitating more efficacious approaches to bone regeneration. Organoids derived from stem cells show great potential in this field; however, the development of bone organoids has been hindered by specific demands, including the need for robust mechanical support provided by scaffolds and hybrid extracellular matrices (ECM). In this context, bioprinting technologies have emerged as powerful means of replicating the complex architecture of bone tissue. The research focused on the fabrication of a highly intricate bone ECM analog using a novel bioink composed of gelatin methacrylate/alginate methacrylate/hydroxyapatite (GelMA/AlgMA/HAP). Bioprinted scaffolds facilitate the long-term cultivation and progressive maturation of extensive bioprinted bone organoids, foster multicellular differentiation, and offer valuable…

Long-lived and highly efficient room temperature phosphorescence (RTP) materials are in high demand for practical applications in lighting and display, security signboards, and anti-counterfeiting. Achieving RTP in aqueous solutions, near-infrared (NIR) phosphorescence emission, and NIR-excited RTP are crucial for applications in bio-imaging, but these goals pose significant challenges. Supramolecular self-assembly provides an effective strategy to address the above problems. This review focuses on the recent advances in the enhancement of RTP via supramolecular self-assembly, covering four key aspects: small molecular self-assembly, cocrystals, the self-assembly of macrocyclic hosts and guests, and multi-stage supramolecular self-assembly. This review not only highlights progress in these areas but also underscores the prominent challenges associated with developing supramolecular RTP materials. The resulting strategies for the development of high-performance supramolecular RTP materials are discussed, aiming to satisfy the practical applications of RTP materials in biomedical…

Interfacial solar evaporation-based seawater desalination is regarded as one of the most promising strategies to alleviate freshwater scarcity. However, the solar evaporation rate of real seawater is significantly constricted by the ubiquitous salts present in seawater. In addition to the common issue of salt accumulation on the evaporation surface during solar evaporation, strong hydration between salt ions and water molecules leads to a lower evaporation rate for real seawater compared to pure water. Here a facile and general strategy is developed to reverse this occurrence, that is, making real seawater evaporation faster than pure water. By simply introducing specific mineral materials into the floating photothermal evaporator, ion exchange at air-water interfaces directly results in a decrease in seawater evaporation enthalpy, and consequently achieves much higher seawater evaporation rates compared to pure water. This process is spontaneously realized during seawater solar evaporation. Considering the current enormous clean water production from evaporation-based desalination…

Abstract Oxygen reduction and evolution reactions are two key processes in electrochemical energy conversion technologies. Synthesis of nonprecious metal, carbon‐based electrocatalysts with high oxygen bifunctional activity and stability is a crucial, yet challenging step to achieving electrochemical energy conversion. Here, an approach to address this issue: synthesis of an atomically dispersed Fe electrocatalyst (Fe 1 /NCP) over a porous, defect‐containing nitrogen‐doped carbon support, is described. Through incorporation of a phosphorus atom into the second coordination sphere of iron, the activity and durability boundaries of this catalyst are pushed to an unprecedented level in alkaline environments, such as those found in a zinc‐air battery. The rationale is to delicately incorporate P heteroatoms and defects close to the central metal sites (FeN 4 P 1 ‐OH) in order to break the local symmetry of the electronic distribution. This enables suitable binding strength with oxygenated intermediates. In situ characterizations and theoretical studies demonstrate that these synergetic…

Electrocatalytic water splitting driven by sustainable energy is a clean and promising water-chemical fuel conversion technology for the production of high-purity green hydrogen. However, the sluggish kinetics of anodic oxygen evolution reaction (OER) pose challenges for large-scale hydrogen production, limiting its efficiency and safety. Recently, the anodic OER has been replaced by a nucleophilic oxidation reaction (NOR) with biomass as the substrate and coupled with a hydrogen evolution reaction (HER), which has attracted great interest. Anode NOR offers faster kinetics, generates high-value products, and reduces energy consumption. By coupling NOR with hydrogen evolution reaction, hydrogen production efficiency can be enhanced while yielding high-value oxidation products or degrading pollutants. Therefore, NOR-coupled HER hydrogen production is another new green electrolytic hydrogen production strategy after electrolytic water hydrogen production, which is of great significance for realizing sustainable energy development and global decarbonization. This review explores the…

Abstract Integration of photocatalytic hydrogen (H2) evolution with oxidative organic synthesis presents a highly attractive strategy for the simultaneous production of clean H2 fuel and high‐value chemicals. However, the sluggish dynamics of photogenerated charge carriers across the photocatalysts result in low photoconversion efficiency, hindering the wide applications of such a technology. Herein, this work overcomes this limitation by inducing the full‐space electric field via charge polarization engineering on a Mo cluster‐decorated Zn2In2S5 (Mo‐Zn2In2S5) photocatalyst. Specifically, this full‐space electric field arises from a cascade of the bulk electric field (BEF) and local surface electric field (LSEF), triggering the oriented migration of photogenerated electrons from [Zn–S] regions to [In–S] regions and eventually to Mo cluster sites, ensuring efficient separation of bulk and surface charge carriers. Moreover, the surface Mo clusters induce a tip enhancement effect to optimize charge transfer behavior by augmenting electrons and proton concentration around the active…

Abstract Tunnel‐type vanadium oxides are promising cathodes for aqueous zinc ion batteries. However, unlike layer‐type cathodes with adjustable layer distances, enhancing ion‐transport kinetics in tunnels characterized by fixed sizes poses a considerable challenge. This study highlights that the macroscopic arrangement of the electrode crucially determines tunnel orientation, thereby influencing ion transport. By changing the material morphology, the tunnel orientation can be optimized to facilitate rapid ion diffusion. In a proof‐of‐concept demonstration, it is revealed that (00 l ) facets‐dominated VO 2 (B) nanobelts with dispersive morphology (VO 2 ‐D) tend to adopt a stacking pattern with directional ion transport along the c ‐axis on the electrode and guarantee fast ion diffusion. Compared with the aggregated sample (VO 2 ‐A) that tends to random arrangement on the electrode with isotropic and slow ion transfer behavior, the electrode featuring dispersive (00 l ) facets‐dominated VO 2 (B) nanobelts displays directional and fast ion diffusion behavior, thus exhibits an…

Abstract The immunosuppressive tumor microenvironment (TME) is a huge hurdle in immunotherapy. Sono‐immunotherapy is a new treatment modality that can reverse immunosuppressive TME, but the sonodynamic effects are compromised by overexpressed glutathione (GSH) and hypoxia in the TME. Herein, this work reports a new sono‐immunotherapy strategy using Pd δ+ single atom catalysts to enhance positive sonodynamic responses to the immunosuppressive and sono‐suppressive TME. To demonstrate this technique, this work employs rich and reductive Ti vacancies in Ti 3‐x C 2 T y nanosheets to construct the atomically dispersed Pd‐C 3 single atom catalysts (SAC) with Pd content up to 2.5 wt% (Pd SA /Ti 3‐x C 2 T y ). Compared with Pd nanoparticle loaded Ti 3‐x C 2 T y , Pd SA /Ti 3‐x C 2 T y single‐atom enzyme showed augmented sonodynamic effects that are ascribed to SAC facilitated electron–hole separation, rapid depletion of overexpressed GSH by ultrasound (US) excited holes, and catalytic decomposition of endogenous H 2 O 2 for relieving hypoxia. Importantly, the sono‐immunotherapy strategy can…

Catalytic materials play crucial roles in various energy-related processes, ranging from large-scale chemical production to advancements in renewable energy technologies. Despite a century of dedicated research, major enduring challenges associated with enhancing catalyst efficiency and durability, particularly in green energy-related electrochemical reactions, remain. Focusing only on either the crystal structure or electronic structure of a catalyst is deemed insufficient to break the linear scaling relationship (LSR), which is the golden rule for the design of advanced catalysts. The discourse in this review intricately outlines the essence of heterogeneous catalysis reactions by highlighting the vital roles played by electron properties. The physical and electrochemical properties of electron charge and spin that govern catalysis efficiencies are analyzed. Emphasis is placed on the pronounced influence of external fields in perturbing the LSR, underscoring the vital role that electron spin plays in advancing high-performance catalyst design. The review culminates by proffering…

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is a promising approach to realize ammonia generation and wastewater treatment. However, the transformation from NO 3 − to NH 3 involves multiple proton‐coupled electron transfer processes and by‐products (NO 2 − , H 2 , etc.), making high ammonia selectivity a challenge. Herein, a two‐phase nanoflower P‐Cu/Co(OH) 2 electrocatalyst consisting of P‐Cu clusters and P‐Co(OH) 2 nanosheets is designed to match the two‐step tandem process (NO 3 − to NO 2 − and NO 2 − to NH 3 ) more compatible, avoiding excessive NO 2 − accumulation and optimizing the whole tandem reaction. Focusing on the initial 2e − process, the inhibited * NO 2 desorption on Cu sites in P‐Cu gives rise to the more appropriate NO 2 − released in electrolyte. Subsequently, P‐Co(OH) 2 exhibits a superior capacity for trapping and transforming the desorbed NO 2 − during the latter 6e − process due to the thermodynamic advantage and contributions of active hydrogen. In 1 m KOH + 0.1 m NO 3 − , P‐Cu/Co(OH) 2 leads to superior NH 3 yield rate of 42.63 mg h − 1 cm −…

Abstract In the pursuit of high‐performance energy storage systems, four‐electron zinc–iodine aqueous batteries (4eZIBs) with successive I−/I2/I+ redox couples are appealing for their potential to deliver high energy density and resource abundance. However, susceptibility of positive valence I+ to hydrolysis and instability of Zn plating/stripping in conventional aqueous electrolyte pose significant challenges. In response, polyethylene glycol (PEG 200) is introduced as co‐solvent in 2 m ZnCl2 aqueous solution to design a wide temperature electrolyte. Through a comprehensive investigation combining spectroscopic characterizations and theoretical simulations, it is elucidated that PEG disrupts the intrinsic strong H‐bonds of water by global weak PEG–H2O interaction, which strengthens the O─H covalent bond of water and intensifies the coordination with Zn2+. This synergistic effect substantially reduces water activity to restrain the I+ hydrolysis, facilitating I−/I2/I+ redox kinetics, mitigating I3− formation and smoothening Zn deposition. The 4eZIBs in the optimized hybrid…

Sodium-ion batteries (SIBs), recognized for balanced energy density and cost-effectiveness, are positioned as a promising complement to lithium-ion batteries (LIBs) and a substitute for lead-acid batteries, particularly in low-speed electric vehicles and large-scale energy storage. Despite their extensive potential, concerns about range anxiety due to lower energy density underscore the importance of fast-charging technologies, which drives the exploration of high-rate electrode materials. Polyanionic cathode materials are emerging as promising candidates in this regard. However, their intrinsic limitation in electronic conductivity poses challenges for synchronized electron and ion transport, hindering their suitability for fast-charging applications. This review provides a comprehensive analysis of sodium ion migration during charging/discharging, highlighting it as a critical rate-limiting step for fast charging. By delving into intrinsic dynamics, key factors that constrain fast-charging characteristics are identified and summarized. Innovative modification routes are then…

Abstract Biological tissues, such as tendons or cartilage, possess high strength and toughness with very low plastic deformations. In contrast, current strategies to prepare tough hydrogels commonly utilize energy dissipation mechanisms based on physical bonds that lead to irreversible large plastic deformations, thus limiting their load‐bearing applications. This article reports a strategy to toughen hydrogels using fibrillar connected double networks (fc‐DN), which consist of two distinct but chemically interconnected polymer networks, that is, a polyacrylamide network and an acrylated agarose fibril network. The fc‐DN design allows efficient stress transfer between the two networks and high fibril alignment during deformation, both contributing to high strength and toughness, while the chemical crosslinking ensures low plastic deformations after undergoing high strains. The mechanical properties of the fc‐DN network can be readily tuned to reach an ultimate tensile strength of 8 MPa and a toughness of above 55 MJ m −3 , which is 3 and 3.5 times more than that of fibrillar double…

Abstract The contemporary production of carbon materials heavily relies on fossil fuels, contributing significantly to the greenhouse effect. Biomass is a carbon‐neutral resource whose organic carbon is formed from atmospheric CO 2 . Employing biomass as a precursor for synthetic carbon materials can fix atmospheric CO 2 into solid materials, achieving negative carbon emissions. Hydrothermal carbonization (HTC) presents an attractive method for converting biomass into carbon materials, by which biomass can be transformed into materials with favorable properties in a distinct hydrothermal environment, and these carbon materials have made extensive progress in many fields. However, the HTC of biomass is a complex and interdisciplinary problem, involving simultaneously the physical properties of the underlying biomass and sub/supercritical water, the chemical mechanisms of hydrothermal synthesis, diverse applications of resulting carbon materials, and the sustainability of the entire technological routes. This review starts with the analysis of biomass composition and distinctive…

The ambition of human beings to create a comfortable environment for work and life in a sustainable way has triggered a great need for advanced thermal insulation materials in past decades. Aerogels and foams present great prospects as thermal insulators owing to their low density, good thermal insulation, mechanical robustness, and even high fire resistance. These merits make them suitable for many real-world applications, such as energy-saving building materials, thermally protective materials in aircrafts and battery, and warming fabrics. Despite great advances, to date there remains a lack of a comprehensive yet critical review on the thermal insulation materials. Herein, recent progresses in fire-safe thermal-insulating aerogels and foams are summarized, and pros/cons of three major categories of aerogels/foams (inorganic, organic and their hybrids) are discussed. Finally, key challenges associated with existing aerogels are discussed and some future opportunities are proposed. This review is expected to expedite the development of advanced aerogels and foams as fire-safe…

Abstract Hydrogel‐based electronic devices in aquatic environments have sparked widespread research interest. Nevertheless, the challenge of developing hydrogel electronics underwater has not been profoundly surmounted because of the fragility and swelling of hydrogels in aquatic environments. In this work, a zwitterionic double network hydrogel comprised of polyvinyl alcohol (PVA), poly(sulfobetaine methacrylate) (PSBMA), and sulfuric acid (H 2 SO 4 ) demonstrates super‐tough and non‐swelling performance. The Hofmeister effect of H 2 SO 4 and PSBMA induces the PVA chains to form numerous nanocrystalline domains, which serve as the primary physical crosslinking points and provide effective energy dissipation. H 2 SO 4 induces a strong salting‐out effect to facilitate PVA crystallization and the formation of a dense and stable network structure that inhibits swelling. The resulting hydrogel exhibits an ultra‐high toughness of 4.61 MJ m −3 , non‐swelling, and long‐term stability for up to a month in pure water and seawater. Based on this, a hydrogel‐based seawater strain sensor has…

Ionic liquids and their various analogues are without doubt the scientific sensation of the last few decades, paving the way to a more sustainable society. Their versatile suite of properties, originating from an almost inconceivably large number of possible cation and anion combinations, allows tuning of the structure to serve a desired purpose. Ionic liquids hence offer a myriad of useful applications from solvents to catalysts, through to lubricants, gas absorbers, and azeotrope breakers. The purpose of this review is to explore the more unexpected of these applications, particularly in the energy space. It guides the reader through the application of ionic liquids and their analogues as i) phase change materials for thermal energy storage, ii) organic ionic plastic crystals, which have been studied as battery electrolytes and in gas separation, iii) key components in the nitrogen reduction reaction for sustainable ammonia generation, iv) as electrolytes in aluminum-ion batteries, and v) in other emerging technologies. It is concluded that there is tremendous scope for further…

Nerve guidance conduits (NGCs) are considered as promising treatment strategy and frontier trend for peripheral nerve regeneration, while their therapeutic outcomes are limited by the lack of controllable drug delivery and available physicochemical cues. Herein, novel aligned piezoelectric nanofibers derived hydrogel NGCs with ultrasound (US)-triggered electrical stimulation (ES) and controllable drug release for repairing peripheral nerve injury are proposed. The inner layer of the NGCs is the barium titanate piezoelectric nanoparticles (BTNPs)-doped polyvinylidene fluoride-trifluoroethylene [BTNPs/P(VDF-TrFE)] electrospinning nanofibers with improved piezoelectricity and aligned orientation. The outer side of the NGCs is the thermoresponsive poly(N-isopropylacrylamide) hybrid hydrogel with bioactive drug encapsulation. Such NGCs can not only induce neuronal-oriented extension and promote neurite outgrowth with US-triggered wireless ES, but also realize the controllable nerve growth factor release with the hydrogel shrinkage under US-triggered heating. Thus, the NGC can positively…

Abstract 2D layered metallic graphite composites are promising electromagnetic wave absorption materials (EWAMs) for their combined properties of abundant interlayer free spaces, rich metallic polarized sites, and high conductivity, but the controllable synthesis remains rather challenging. Herein, a dual‐step redox engineering strategy is developed by employing cobalt boron imidazolate framework (Co‐BIF) to construct 2D CoNi‐alloy embedded B, N‐doped carbon layers (2D‐CNC) as a promising EWAM. In the first step, a chemical etching oxidation process on Co‐BIF is used to obtain an optimized 2D‐CoNi‐layered double hydroxide (2D‐CoNi‐LDH) intermediate and in the second, high‐temperature calcination reduction is implemented to modify graphitization of the degree of the 2D‐CNC. The obtained sample delivers superior reflection loss (RLmin) of −60.1 dB and wide effective absorption bandwidth (EAB) of 6.24 GHz. The synergy mechanisms of interfacial/dipole polarization and magnetic coupling are in‐depth evidenced by the hologram and Lorentz electron microscopy, revealing its significant…

Abstract High mechanical load‐carrying capability and thermal insulating performance are crucial to thermal‐insulation materials under extreme conditions. However, these features are often difficult to achieve simultaneously in conventional porous ceramics. Here, for the first time, it is reported a multiscale structure design and fast fabrication of 9‐cation porous high‐entropy diboride ceramics via an ultrafast high‐temperature synthesis technique that can lead to exceptional mechanical load‐bearing capability and high thermal insulation performance. With the construction of multiscale structures involving ultrafine pores at the microscale, high‐quality interfaces between building blocks at the nanoscale, and severe lattice distortion at the atomic scale, the materials with an ≈50% porosity exhibit an ultrahigh compressive strength of up to ≈337 MPa at room temperature and a thermal conductivity as low as ≈0.76 W m −1 K −1 . More importantly, they demonstrate exceptional thermal stability, with merely ≈2.4% volume shrinkage after 2000 °C annealing. They also show an ultrahigh…

In the fabrication of inverted perovskite solar cells (PSCs), the wettability, adsorbability, and compactness of self-assembled monolayers (SAMs) on conductive substrates have critical impacts on the quality of the perovskite films and the defects at the buried perovskite-substrate interface, which control the efficiency and stability of the devices. Herein, three bisphosphonate-anchored indolocarbazole (IDCz)-derived SAMs, IDCz-1, IDCz-2, and IDCz-3, are designed and synthesized by modulating the position of the two nitrogen atoms of the IDCz unit to improve the molecular dipole moments and strengthen the π-π interactions. Regulating the work functions (WF) of FTO electrodes through molecular dipole moments and energy levels, the perovskite band bends upwards with a small offset for ITO/IDCz-3/perovskite, thereby promoting hole extraction and blocking electrons. As a result, the inverted PSC employing IDCz-3 as hole-collecting layer exhibits a champion PCE of 25.15%, which is a record efficiency for the multipodal SAMs-based PSCs. Moreover, the unencapsulated device with IDCz-3 can…