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In the past decade, the surface plasmon resonance of Ag and Au nanoparticles has been investigated to improve the efficiency of photocatalytic processes. The photocatalytic production of fuels is particularly interesting for its ability to store the sun's energy in chemical bonds that can be released later without producing harmful byproducts. This Feature Article reviews recent work demonstrating plasmon-enhanced photocatalytic water splitting, reduction of CO2 with H2O to form hydrocarbon fuels, and degradation of organic molecules. Focus is placed on several possible mechanisms that have been previously discussed in the literature. A particular emphasis is given to several aspects of these mechanisms that are not fully understood and will require further investigation. [ABSTRACT FROM AUTHOR]

A covalently tethered polyoxometalate (POM)-pyrene hybrid (Py-SiW11) is utilized for the noncovalent functionalization of single-walled carbon nanotubes (SWNTs). The resulting SWNTs/Py-SiW11 nanocomposite shows that both SiW11 and pyrene moieties could interact with SWNTs without causing any chemical decomposition. When used as anode material in lithium-ion batteries, the SWNTs/Py-SiW11 nanocomposite exhibits higher discharge capacities, and better rate capacity and cycling stability than the individual components. When the current density is 0.5 mA cm−2, the nanocomposite exhibits the initial discharge capacity of 1569.8 mAh g−1, and a high discharge capacity of 580 mAh g−1 for up to 100 cycles. [ABSTRACT FROM AUTHOR]

Artificial photoreceptors offer a promising solution for developing biomimetic vision systems that incorporate in‐sensor processing, which can greatly reduce power consumption and operation latency compared to traditional machine vision systems. This work presents a tetrachromatic optical synaptic device based on a 2D tungsten diselenide optoelectronic p‐type transistor with a unique UV light‐activated surface electron doping layer. Fully light‐controlled bidirectional synaptic excitation and inhibition are demonstrated with visible and UV light stimuli, respectively, with a reasonable power density of <10 mW cm−2 that matches the imaging condition of a biological vision. The weight updates of up to 64 states, high dynamic range, and low nonlinearity are demonstrated for long‐term potentiation and depression behaviors. This artificial tetrachromatic photoreceptor can mimic the alert and foraging behaviors of a reindeer with low power consumption and enhanced signal contrast. Furthermore, it can be employed as an intelligent collision detection solution with in‐sensor processing capabilities. This bioinspired tetrachromatic photoreceptor offers a low‐cost, energy‐efficient, and low‐latency solution for future artificial machines. [ABSTRACT FROM AUTHOR]

Layered crystal materials have blazed a promising trail in the design and optimization of electrodes for magnesium ion batteries (MIBs). The layered crystal materials effectively improve the migration kinetics of the Mg2+ storage process to deliver a high energy and power density. To meet the future demand for high‐performance MIBs, significant work has been applied to layered crystal materials, including crystal modification, mechanism investigation, and micro/nanostructure design. Herein, this review presents a comprehensive overview of layered crystal materials applied to MIBs, from development history to current applications. It focuses on the relationship between the layered crystal structure and the energy storage mechanism. Meanwhile, recent achievements in the design principles of layered crystal materials and their application to electrodes are summarized. Finally, future perspectives on the application of layered materials in MIBs are presented. The overview of the development process and structural characteristics contributes to a thorough understanding of these materials, while a discussion of design strategies and practical applications can inspire further research. Therefore, this review provides guidance and assistance for constructing high‐performance MIBs. [ABSTRACT FROM AUTHOR]

The booming development of artificial intelligence (AI) requires faster physical processing units as well as more efficient algorithms. Recently, reservoir computing (RC) has emerged as an alternative brain‐inspired framework for fast learning with low training cost, since only the weights associated with the output layers should be trained. Physical RC becomes one of the leading paradigms for computation using high‐dimensional, nonlinear, dynamic substrates. Among them, memristor appears to be a simple, adaptable, and efficient framework for constructing physical RC since they exhibit nonlinear features and memory behavior, while memristor‐implemented artificial neural networks display increasing popularity towards neuromorphic computing. In this review, the memristor‐implemented RC systems from the following aspects: architectures, materials, and applications are summarized. It starts with an introduction to the RC structures that can be simulated with memristor blocks. Specific interest then focuses on the dynamic memory behaviors of memristors based on various material systems, optimizing the understanding of the relationship between the relaxation behaviors and materials, which provides guidance and references for building RC systems coped with on‐demand application scenarios. Furthermore, recent advances in the application of memristor‐based physical RC systems are surveyed. In the end, the further prospects of memristor‐implemented RC system in a material view are envisaged. [ABSTRACT FROM AUTHOR]

The hypoxic tumor microenvironment (TME) significantly affects cancer treatment. Conventional chemotherapeutic agents cannot effectively target hypoxic tumor tissue, which decreases efficacy and results in severe toxic side effects. To alleviate this problem, a self‐driving biomotor is developed by functionalizing MCDP nanoparticles containing calcium peroxide and doxorubicin (DOX) loaded onto polydopamine‐coated metal–organic frameworks（MOF）, with the anaerobic Bifidobacterium infantis (Bif) for synergistic chemotherapy and chemodynamic therapy (CDT) against breast cancer. The materials of institute Lavoisier (MIL) frameworks + CaO2 + DOX + polydopamine (MCDP)@Bif biohybrid actively targets hypoxic regions of solid tumors via the inherent targeting ability of Bif. Once it has accumulated in the tumor tissue, MCDP generates hydroxyl radicals through the enhanced Fenton‐type reactions between Fe2+ and self‐generated hydrogen peroxide in the acidic TME. The disruption of Ca2+ homeostasis and resulting mitochondrial Ca2+ overload triggers apoptosis and enhances oxidative stress, promoting tumor cell death. The results found that the DOX concentration in MCDP@Bif‐treated tumors is 3.8 times higher than that in free‐DOX‐treated tumors, which significantly prolongs the median survival of the tumor‐bearing mice to 69 days and reduces the toxic side effects of DOX. Therefore, the novel bacteria‐driven drug delivery system is highly effective in achieving synergistic chemotherapy and CDT against solid tumors. [ABSTRACT FROM AUTHOR]

Plasmonic metasurfaces can significantly enhance the interaction between light and 2D materials. Hybrid structures of plasmonic lattices and 2D materials show great promise for both fundamental and practical studies because of their unprecedented ability for precise manipulation of light at the nanoscale. This review starts with an overview of the basic concepts of plasmonic lattices and optical properties of 2D materials, as well as fabrication strategies for hybrid metasurfaces. Then, the enhanced photoluminescence, quantum emission, optoelectronic detection, nonlinear process, and valleytronics in hybrid metasurfaces are summarized, and their development for nanophotonic functional devices are reviewed. Further, several compelling topics are also outlined that provide outlooks for future directions of hybrid metasurfaces such as novel structural design and high‐quality fabrication, all‐dielectric metasurfaces, dynamic metasurfaces, and plasmonic mediation of chemical reactions and physical processes. It is believed that hybrid metasurfaces of plasmonic lattices and 2D materials can open prospects for versatile platforms for light‐matter interactions and contribute to the revolutions on nanophotonic devices. [ABSTRACT FROM AUTHOR]

Optoelectronic technologies are based on families of semiconductor alloys. It is rare that a new semiconductor alloy family is developed to the point where epitaxial growth is possible; since the 1950s, this has happened approximately once per decade. Herein, this work demonstrates epitaxial thin film growth of semiconducting chalcogenide perovskite alloys in the Ba‐Zr‐S‐Se system by gas‐source molecular beam epitaxy (MBE). This work stabilizes the full range y = 0 − 3 of compositions BaZrS(3‐y)Sey in the perovskite structure. The resulting films are environmentally stable and the direct band gap (Eg) varies strongly with Se content, as predicted by theory, with Eg = 1.9 − 1.5 eV for y = 0 − 3. This creates possibilities for visible and near‐infrared (VIS–NIR) optoelectronics, solid‐state lighting, and solar cells using chalcogenide perovskites. [ABSTRACT FROM AUTHOR]

Solid‐state energy storage devices (SSESDs) are believed to significantly improve safety, long‐term electrochemical/thermal stability, and energy/power density as well as reduce packaging demands, showing the huge application potential in large‐scale energy storage. Nevertheless, some key issues like low ionic conductivities, poor interface contact, and dendrites growth limit the practical application of SSESDs. In recent years, MXenes for SSESDs have received reassuring advances on account of unique parameters. Nevertheless, overall reviews about the subject are seldom. In this review, current advances of MXenes and their derivatives in solid‐state Li–metal, Li‐ion, Li–I/S, Na‐ion, Zn–air, Zn–metal batteries, and supercapacitors in cathode/anode optimization, interface medication, and electrolyte fillers, etc., are comprehensively reviewed. First of all, essential principles of MXenes are shown, such as precursors, etching/delamination strategies, as well as superior properties for energy storage systems. Meanwhile, the classification and evaluation parameters of solid‐state electrolytes are summarized. Subsequently, the application, modification mechanism, and design strategy of MXenes for boosting electrochemical behaviors of SSESDs are systematically reviewed and discussed. At last, perspectives and challenges about the future construction strategies of MXenes for SSESDs are recommended. This review shall assist scientists design and build advanced SSESDs with superior energy density along with safety. [ABSTRACT FROM AUTHOR]

Solid‐state nanopores are implemented in new and promising platforms that are capable of sensing fundamental biomolecular constituents at the single‐molecule level. However, several limitations and drawbacks remain. For example, the current strategies based on both electrical and optical sensing suffer from low analyte capture rates and challenging nanofabrication procedures. In addition, their limited discrimination power hinders their application in the detection of complex molecular constructs. In contrast, Raman spectroscopy has recently demonstrated the ability to discriminate both nucleotides and amino acids. Herein, a plasmonic nanoassembly is proposed supporting nanopores at high density, in the order of 100 pores per µm2. These findings demonstrate that the device has a high capture rate in the range of a few fm. The pore size is ≈10 nm in diameter and provides an amplification of the electromagnetic field exceeding 103 in intensity at 785 nm. Owing to these features, single‐molecule detection is achieved by means of surface‐enhanced Raman scattering from a solution containing 50 fm DNA molecules (≈4.4 kilobase pairs). Notably, the reported spectra show an average number of 2.5 Raman counts per nucleotide. From this perspective, this number is not far from what is necessary to discriminate the DNA sequence. [ABSTRACT FROM AUTHOR]

The elucidation of lithium ion transport pathways through a solid electrolyte separator is a vital step toward development of reliable, functional all‐solid‐state batteries. Here, advantage has been taken of the significantly higher neutron attenuation coefficient of one of the most abundant stable isotopes of lithium, 6Li, with respect to that of naturally occurring lithium isotope mixture, to perform neutron imaging on a purpose built all‐solid‐state lithium–sulfur battery. Increasing the 6Li content in the anode while using natural lithium in the solid electrolyte separator and the cathode enhances the contrast such that it is possible to differentiate, during the initial discharge, between the mobile lithium ions diffusing through the cell from the anode and those that are initially located in the solid electrolyte. The sensitivity of neutrons to the different lithium isotopes means that operando neutron radiography allows demonstration of the lithium ion diffusion through the cell while in situ neutron tomography has permitted presentation, in three dimensions, of the distribution of the trapped lithium ions inside the cell in charged and discharged states. [ABSTRACT FROM AUTHOR]

Thermodynamically favorable electrooxidation of organics coupled with hydrogen production as an alternative to overall water splitting is rapidly developing due to low energy consumption and high value. But understanding the relationship between catalyst reconstruction and performance in depth remains a challenge. Herein, DFT calculations are used as a theoretical guide to adjust the local coordination environment and electronic structure of Ni3S2 by Fe doping, which promotes the self‐reconstruction of catalyst and nitrile evolution reaction performance. The overall reaction of benzylamine electrooxidation coupled with hydrogen production achieves a 14.5‐fold improvement in hydrogen production compared to water electrolysis at the same potential, almost completely converting benzylamine to high‐value benzonitrile (99% product yield). In situ spectroscopy and X‐ray absorption fine structure spectroscopy demonstrate that the excellent electrocatalytic performance due to Fe doping induces surface self‐reconstruction of Ni3S2 to NiOOH at low potential, and significantly reduces the rate‐determining step energy barriers for CN bonds to CN bonds. This work provides theoretical guidance in designing and preparing efficient catalysts for the electrosynthesis of nitrile compounds coupled with hydrogen production. [ABSTRACT FROM AUTHOR]

Precise design and construction of catalysts with satisfied performance for ambient electrolytic nitrogen reduction reaction (e‐NRR) is extremely challenging. By in situ integrating an electron‐rich polyoxometalates (POMs) into stable metal organic frameworks (MOFs), five POMs‐based MOFs formulated as [FexCoy(Pbpy)9(ox)6(H2O)6][P2W18O62]·3H2O (abbreviated as FexCoyMOF‐P2W18) are created and directly used as catalysts for e‐NRR. Their electrocatalytic performances are remarkably improved thanks to complementary advantages and promising possibilities of MOFs and POMs. In particular, NH3 yield rates of 47.04 µg h−1 mgcat.−1 and Faradaic efficiency of 31.56% by FeCoMOF‐P2W18 for e‐NRR are significantly enhanced by a factor of 4 and 3, respectively, compared to the [Fe0.5Co0.5(Pbpy)(ox)]2·(Pbpy)0.5. The cyclic voltammetry curves, density functional theory calculations and in situ Fourier‐transform infrared spectroscopy confirm that there is a directional electron channel from P2W18 to the MOFs unit to accelerate the transfer of electrons. And the introduction of bimetals Fe and Co in the P2W18‐based MOFs can reduce the energy of the *N2 to *N2H step, thereby increasing the production of NH3. More importantly, this POM in situ embedding strategy can be extended to create other e‐NRR catalysts with enhanced performances, which opens a new avenue for future NH3 production for breakthrough in the bottleneck of e‐NRR. [ABSTRACT FROM AUTHOR]

Silicon‐based anodes are considered ideal candidate materials for next‐generation lithium‐ion batteries due to their high capacity. However, the low conductivity and large volume variations during cycling inevitably result in inferior cyclic stability. Herein, a dry method without binders is designed to fabricate Si‐based electrodes with single‐walled carbon nanotubes (SWCNTs) network and to explore the different mechanisms between SWCNT and multiwalled carbon nanotubes (MWCNTs) as a conductive network. As expected, higher initial discharge capacity (1785 mAh g−1), higher initial Coulombic efficiency (ICE, 81.52%) and outstanding cyclic stability are obtained from the SiOx@C|SWCNT anodes. Furthermore, its lithium‐ion diffusion coefficient (DLi+) is 3–4 orders of magnitude higher than that of SiOx@C|MWCNT. The underlying mechanism is clarified by in situ Raman spectroscopy and theoretical analysis. It is found that the SWCNTs can maintain good contact with SiOx@C even under tensile stresses up to 6.2 GPa, while the MWCNTs lose electrical contact due to alternating compressive stress up to 8.9 GPa and tensile stress up to 2.5 GPa during long‐term cycling. Under such very large stresses, the more flexible SWCNTs and their stronger van der Waals forces ensure that SiOx@C still has good contact with SWCNTs. [ABSTRACT FROM AUTHOR]

Glycerol electrooxidation (GOR), as a typical nucleophile oxidation reaction, is deemed as a promising alternative anodic route to assist cathodic hydrogen evolution reaction. However, the investigations of high‐performance catalysts and industrial‐scale application of GOR remain a grand challenge. Herein, biphasic Ni3N/Co3N heterostructure nanowires (denoted as Ni3N/Co3N‐NWs) are proposed as an efficient bifunctional catalyst, which realizes a high Faradaic efficiency of 94.6% toward formate production. Importantly, the flow electrolyzer achieves an industry‐level current density of 1 A cm−2 at 2.01 V with impressive stability for steady running over 200 h, realizing lower electricity expense of 4.82 kWh m−3H2 and energy saving efficiency of 9.7%, as well as outstanding co‐production rates of 11 and 21.4 mmol cm−2 h−1 toward formate and H2, respectively. Theoretical calculations reveal that the efficient electron transfer on Ni3N/Co3N heterointerfaces simultaneously optimizes nucleophile reaction tendency and glycerol dehydrogenation kinetics, thus contributing to excellent GOR performance. [ABSTRACT FROM AUTHOR]

Hydrogen is a promising alternative to fossil fuels that can reduce greenhouse gas emissions. Decoupled water electrolysis system using a reversible proton storage redox mediator, where the oxygen evolution reaction and hydrogen evolution reaction are separated in time and space, is an effective approach to producing hydrogen gas with high purity, high flexibility, and low cost. To realize fast hydrogen production in such a system, a redox mediator capable of releasing protons rapidly is required. Herein, α‐MoO3, with an ultrafast proton transfer property that can be explained by a dense hydrogen bond network in the lattice oxygen arrays of HxMoO3, is examined as a high‐rate redox mediator for fast hydrogen production in acidic electrolytes. The α‐MoO3 redox mediator shows both a large capacity of 204 mAh g−1 and fast hydrogen production at a current rate of 10 A cm−2(≈153 A g−1), outperforming most of the previously reported solid‐state redox mediators. [ABSTRACT FROM AUTHOR]

Overactive inflammatory response and excessive oxidative stress are the main pathophysiological culprits for cerebral ischemia/reperfusion injury (IRI) that arouse neuronal damage. The neurotransmitter acetylcholine (ACh) exerts anti‐inflammatory roles by stimulating α7 nicotinic acetylcholine receptor (α7nAChR) on microglia to activate the cholinergic anti‐inflammatory pathway. Simultaneously, as a circadian rhythm‐dependent hormone , melatonin (MT) possesses promising neuroprotective effects that eliminate reactive oxygen species (ROS) in the ischemic region. Relying on these, a biocompatible fluorescein isothiocyanate (FITC)‐labeled SiO2@PAA‐MT/ACh nanospheres are constructed to effectively alleviate oxidative stress and polarize microglial phenotype to suppress inflammatory response in cerebral IRI. Despite of biosafety and curative effects of ACh and MT, the poor aggregation in ischemic penumbra hinders their neuroprotection. To address that, complement component 5a (C5a) is used as a molecular target for delivery of ACh and MT. C5a conspicuously exists at local inflammatory sites of cerebral IRI, recruits immune cells, and mediates further release of inflammatory cytokines. Upon binding of anti‐C5a (aC5a) aptamers onto FITC‐labeled SiO2@PAA‐MT/ACh nanospheres, they can effectively target the ischemic penumbra and promote neurological recovery. Taken together, the current study suggests that the FITC‐labeled SiO2@PAA‐MT/ACh‐aC5a nanospheres after intravenous (i.v.) administration can act as an effective targeted nanotherapy to salvage neurons in cerebral IRI. [ABSTRACT FROM AUTHOR]

Van der Waals (vdW) materials of transition metal dichalcogenides (TMD) family with semiconducting properties are currently at the forefront of research in the field of optoelectronics. The ability to couple them with one another at atomic interface precision in a synergistic way opens up unprecedented opportunities to design photodetectors of broad spectral range with excellent figures of merits not accessible to discrete materials. Recent years have seen a surge of interest in group VII TMD materials (ReS2 and ReSe2) due to their strong optical response from bulk to monolayer and good ambient stability. Their band gap energies spanning over visible and near‐infrared ranges and the strong linear polarization sensitivity stemming from the distorted octahedral symmetry, are ideally suited for polarization‐sensitive photodetectors. This review aims at providing a comprehensive understanding of the fundamental properties, optical identification of various structural features, long‐debated question of band gap nature and interlayer coupling, and recent advances in the development of photodetectors based on ReS2, ReSe2, and their vdW heterostructures with other layered materials of practical importance. We critically review various conceptual device designs implemented based on band engineering, emphasize on the merits of these photodetectors and their potential applications, and provide an outlook for future prospects. [ABSTRACT FROM AUTHOR]

Methanol steam reforming (MSR) is viewed as an important technology in the growth of a future hydrogen economy, with methanol serving as an easily transportable and storable liquid hydrogen carrier. However, the thermocatalytic MSR reaction is energy intensive as it requires high temperatures. Herein, a novel L‐Cu catalyst is successfully fabricated for photo‐driven MSR through reduction of CuAl layered double hydroxide (CuAl‐LDH) nanosheets. L‐Cu offers outstanding activity for the photothermal conversion of methanol and water to hydrogen (160.5 µmol gcat−1 s−1) under ultraviolet‐visible irradiation, with this rate being much higher than that achieved for L‐Cu at the same temperature in the dark. Characterization studies using X‐ray diffraction, X‐ray photoelectron spectroscopy, X‐ray absorption spectroscopy, and high‐resolution transmission electron microscopy determine that L‐Cu catalyst comprise Cu nanoparticles on an amorphous alumina support. Computational calculations reveale that Cu localized surface plasmon resonance effects promote the activation of H2O, thereby underpinning the remarkable hydrogen production rates achieved during photo‐driven MSR. This study introduces a novel photothermal strategy for hydrogen generation from methanol, demonstrating the enormous potential of photothermal catalysis in the chemical and energy sectors. [ABSTRACT FROM AUTHOR]

The sensitive detection of light polarization besides the intensity and wavelength, can provide a new degree of freedom for more and clearer information of imaging targets in night, fog, and smoke environment. However, the conventional filter‐integrated polarimetric photodetectors suffer from the complicated fabrication process and limited spectral range. Herein, broadband and polarization‐sensitive photodetectors are achieved with reconfigurable operation mode, utilizing the linear dichroism and narrow band gap of 2D As0.4P0.6 with in‐plane anisotropic structure. In As0.4P0.6‐MoTe2 heterojunction device, both photo‐gating and photovoltaic modes are operated and switchable, contributing to high responsivity (1590 A W−1 at 405 nm and 14.7 A W−1 at 1550 nm) and ultrafast speed (25 µs) in the wide spectral band (405–1550 nm). Interestingly, an optical reversal is observed on both linear dichroism and polarimetric photocurrent due to the wavelength‐dependent polarization reverse nature of the As0.4P0.6 flakes. The dichroism ratio of photocurrent can be modulated from unity to ≈10 by varying the gate voltage, enabling the reconfigurable detection mode from polarization‐independence to polarization‐susceptibility. This study demonstrates a new prototype device comprising low symmetric van der Waals heterostructure, possessing the gate‐tunability on both photo‐gain and dichroism ratio, toward high performance, reconfigurable, broadband, and polarization‐resolved photodetection and imaging applications. [ABSTRACT FROM AUTHOR]

Simulating biological synaptic functionalities through artificial synaptic devices opens up an innovative way to overcome the von Neumann bottleneck at the device level. Artificial optoelectronic synapses provide a non‐contact method to operate the devices and overcome the shortcomings of electrical synaptic devices. With the advantages of high photoelectric conversion efficiency, adjustable light absorption coefficient, and broad spectral range, nanowires (NWs)‐based optoelectronic synapses have attracted wide attention. Herein, to better promote the applications of nanowires‐based optoelectronic synapses for future neuromorphic systems, the functionalities of optoelectronic synaptic devices and the current progress of NWs optoelectronic synaptic devices in UV–vis–IR spectral range are introduced. Furthermore, a bridge between NWs‐based optoelectronic synaptic device and the neuromorphic system is established. Challenges for the forthcoming development of NWs optoelectronic synapses are also discussed. This review may offer a vision into the design and neuromorphic applications of NWs‐based optoelectronic synaptic devices. [ABSTRACT FROM AUTHOR]

Molecular metal oxides or polyoxometalates (POMs) offer unrivaled properties in areas ranging from catalysis and energy conversion through to molecular electronics, biomimetics, and theranostics. While POMs are ubiquitous metal oxide model systems studied in most areas of chemistry and materials science, their technological deployment is often hampered by their molecular nature, as this leads to increased degradation, leaching, and loss of reactivity, particularly when harsh applications, such as water electrolysis, thermal catalysis or highly basic/acidic reaction solutions are targeted. Therefore, immobilization of POMs on heterogeneous substrates has recently become a central theme in POM research. While early studies focused mainly on metal oxide and semiconductor supports, more recently, POM integration in soft matter matrices including polymers, conductive polymers, hydrogels, and stimuli‐responsive matrices leads to breakthroughs in multifunctional composite design. This Review summarizes pioneering experimental and theoretical progress in this emerging field over the last decade, highlighting current challenges that need to be overcome to allow a more widespread technological deployment and providing the authors' view of some of the most promising future directions of the research field. In addition, the current understanding of correlations between structure (on the molecular, nano‐ and microscale) and reactivity in POM polymer composites is summarized, so that rational materials design can be further developed. [ABSTRACT FROM AUTHOR]

Polarization‐sensitive photodetectors are gaining numerous attention since polarization detection is important in geological remote sensing, atmospheric monitoring, military recon, and medical examination. Among various reported photoactive materials for photodetectors, metal halide perovskites have outstanding advantages such as tunable band gaps, excellent optoelectronic properties, and easy fabrication. Moreover, the characteristics of crystal structure anisotropy and controllable growth orientation of perovskite crystals endow the perovskite photodetector with the ability to identify light polarization states. This review outlines the recent research progress of perovskite photodetectors on polarization‐sensitive detection. Firstly, key device parameters of polarization‐sensitive detection are introduced. Then, the recent progress of polarization‐sensitive perovskite detectors in the field of linear and circular polarization is reviewed according to the different principles of polarization response. Finally, the challenges of polarization‐sensitive perovskite photodetector are discussed. [ABSTRACT FROM AUTHOR]

Engineered nanozymes have been developed to catalyze the production of reactive oxygen species (ROS) for cancer therapy, but currently, the ROS generation efficiency is still far from optimistic. In this study, a human self‐driven electrical stimulation enhanced catalytic system based on wearable triboelectric nanogenerator (TENG) and fully π‐conjugated covalent organic framework nanocages (hCOF) for improving cancer therapy is created. The fully π‐conjugated hCOF nanocage with high electron mobility under the self‐generated electric field can not only rearrange the local electric field for optimizing energy utilization, but also facilitates the access of electrolytes to optimize the utilization of the electric field. With the self‐powered wearable TENG, the peroxidase‐like activity of hCOF increased by 2.44‐fold and has electricity‐responsive doxorubicin delivery capacity for enhancing the therapeutic outcomes. The high‐efficient self‐driven electrical stimulation enhanced nanocatalytic system provides a new optimized model for the catalytic energy supply of nanozymes. [ABSTRACT FROM AUTHOR]

Memristor‐based reservoir computing systems represent an attractive approach in processing the time‐series information with a low training cost, in a range of fields from finance to engineering. Previous investigations have identified the charming potential of organic devices for next‐generation memory devices. However, the structural inhomogeneity and wide energy bandgap of most organic polymers usually lead to low‐yield and high operation power microelectronic devices, that permit their further application in neuromorphic computing. Herein, an organic‐inorganic hybrid memristor that can be conveniently processed into crossbar devices with tolerable yield via spin‐coating is shown. The doped inorganic polyoxometalate (POM) clusters via supramolecular assembly strategy not only act as the charge trapping modules but also assist the formation of conductive filaments due to their delocalized electrostatic adsorption property. With the dynamic short‐term memory property, the designed memristor devices can be used as a reservoir framework to process temporal information directly. A smaller reservoir with 100 memristors can be used for the recognition of emotion patterns efficiently. This strategy demonstrates the unique role of POM in developing low‐power and repeated memristors, which provides a new material platform to design advanced function memristors for neuromorphic computing. [ABSTRACT FROM AUTHOR]

Integrating electronics with clothing and the human body to support people's lifestyle is quickly becoming a reality. Some of these electronics, including health sensors, communication devices, and personal electronics, contain the potential to revolutionize life in the future. One of the most demanding aspects of such electronic designs is their power supply systems, which necessitate not only a continuous power supply, but also wearable characteristics and durability, which many conventional power‐supply methods have failed to fulfill. The triboelectric nanogenerator (TENG), which depends on static charging between materials, can convert mechanical vibrations into electricity. TENGs are foreseen as a leading candidate to power wearable electronics due to their advantages such as high instantaneous power outputs and efficiency, low cost, ease of fabrication, lightweight, and wearability. This paper is a comprehensive review on the most prominent wearable TENG categories; textiles‐based TENGs for clothing applications, footwear‐incorporated TENG designs, and other TENG accessories. Herein, the most important developments in these categories, with a focus on their materials, fabrication, features, advantages, and drawbacks, are examined. Finally, a detailed analysis is provided on the main challenges impeding the progress of wearable TENGs with the insights into potential improvement techniques, targeting the widespread commercialization of this technology. [ABSTRACT FROM AUTHOR]

Metal cations are potent environmental pollutants that negatively impact human health and the environment. Despite advancements in sensor design, the simultaneous detection and discrimination of multiple heavy metals at sub‐nanomolar concentrations in complex analytical matrices remain a major technological challenge. Here, the design, synthesis, and analytical performance of three highly emissive conjugated polyelectrolytes (CPEs) functionalized with strong iminodiacetate and iminodipropionate metal chelates that operate in challenging environmental samples such as seawater are demonstrated. When coupled with array‐based sensing methods, these polymeric sensors discriminate among nine divalent metal cations (CuII, CoII, NiII, MnII, FeII, ZnII, CdII, HgII, and PbII). The unusually high and robust luminescence of these CPEs enables unprecedented sensitivity at picomolar concentrations in water. Unlike previous array‐based sensors for heavy metals using CPEs, the incorporation of distinct π‐spacer units within the polymer backbone affords more pronounced differences in each polymer's spectroscopic behavior upon interaction with each metal, ultimately producing better analytical information and improved differentiation. To demonstrate the environmental and biological utility, a simple two‐component sensing array is showcased that can differentiate nine metal cation species down to 500 × 10−12 m in aqueous media and to 100 × 10−9 m in seawater samples collected from the Gulf of Mexico. [ABSTRACT FROM AUTHOR]

Improving charge transfer efficiency via vibronic coupling is vital to the performance of semiconducting surface‐enhanced Raman spectroscopy (SERS). Previous attempts have focused on defects‐based metastable‐state assisted band structure matching strategy to enhance vibronic coupling. However, defect‐related charge transfer transitions can be easily deteriorated due to enhanced phonon‐assisted relaxation upon continuous laser irradiation. Herein, perovskite‐based steady‐state assisted band structure matching strategy is proposed to enhance vibronic coupling within perovskite‐molecule charge transfer complex, leading to remarkable Raman enhancement up to 5.9 × 106. Particularly, vibronic coupling can be modulated by tuning valence band position and introducing ultrathin Au coating, which allows selective enhancement of molecules with different band structures, including narrow‐bandgap molecules and wide‐bandgap molecules. Importantly, based on intrinsically stable conduction band and valence band states, this system achieves ultrahigh photostability, preserving 91.3% of the original intensity after 50 000 s of irradiation. This system also provides an outstanding tool for trace molecular detection, allowing sensitive and selective identification of 9 types of gastric cancer related aldehydes, which enables distinguishing the breath of gastric cancer patients from healthy controls with a discriminatory accuracy of 81.09%. This study is anticipated to shed new light into the future strategy design of efficient and stable semiconducting SERS. [ABSTRACT FROM AUTHOR]

Sparked by natural photosynthesis, solar photocatalysis using metal‐free graphitic carbon nitride (g‐C3N4) with appealing electronic structure has turned up as the most captivating technique to the quest for sustainable energy generation and pollution‐free environment. Nonetheless, low‐dimensional g‐C3N4 is thwarted from sluggish kinetics and rapid recombination of photogenerated carriers upon light irradiation. Among multifarious modification strategies, engineering 2D cocatalysts is anticipated to accelerate redox kinetics, augment active sites and ameliorate electron–hole separation of 2D g‐C3N4 for boosted activity thanks to its face‐to‐face contact surface. It is of timely and technological significance to review the 2D/2D interfaces with state‐of‐the‐art 2D cocatalysts, spanning from carbon‐containing to phosphorus‐containing, metal dichalcogenide, and other cocatalysts. Fundamental principles for each photocatalytic application will be introduced. Thereafter, the recent advances of 2D/2D cocatalyst‐mediated g‐C3N4 systems will be critically evaluated based on their interfacial engineering, emerging roles, and impacts toward stability and catalytic efficiency. Importantly, mechanistic insights into the charge dynamics and structure–performance relationship will be deciphered. Last, noteworthy research directions are prospected to deliver insightful ideas for future development of g‐C3N4. Overall, this review is anticipated to serve as a scaffold and cornerstone in designing dimensionality‐dependent 2D cocatalyst‐assisted g‐C3N4 toward renewable energy and ecologically green environment. [ABSTRACT FROM AUTHOR]

Lead halide perovskites have emerged as promising photovoltaic (PV) materials owing to their superior optoelectronic properties. However, they suffer from poor stability and potential toxicity. Here, computational screening with experimental synthesis is combined to explore stable, lead‐free, and defect‐tolerant PV materials. Heavy cations with lone‐pair electrons and mixed anions of chalcogens and halogens as a descriptor for simultaneous realization of defect tolerance and high stability are adopted. Together with the criteria of possessing direct band gap and optimal gap value, the inorganic material database is screened and CuBiSCl2 in the post‐perovskite structure is identified with an ideal band gap of 1.37 eV. The electronic structure and defect calculations suggest its defect‐tolerant characteristics. By optical absorption measurement, its band gap is confirmed to be ≈1.44 eV, with strong absorption near the band edge. The material is stable against thermal decomposition up to 300 °C and can survive from 25 days of storage at ambient conditions with 60% relative humidity. Prototype solar cells are fabricated and demonstrate an open circuit voltage of 1.09 V and a power conversion efficiency of 1.00%. With the excellent properties above, CuBiSCl2 is proposed to be a promising candidate for PV application. [ABSTRACT FROM AUTHOR]

Artificial optoelectronic synapses with both electrical and light‐induced synaptic behaviors have recently been studied for applications in neuromorphic computing and artificial vision systems. However, the combination of visual perception and high‐performance information processing capabilities still faces challenges. In this work, the authors demonstrate a memristor based on 2D bismuth oxyiodide (BiOI) nanosheets that can exhibit bipolar resistive switching (RS) performance as well as electrical and light‐induced synaptic plasticity eminently suitable for low‐power optoelectronic synapses. The fabricated memristor exhibits high‐performance RS behaviors with a high ON/OFF ratio up to 105, an ultralow SET voltage of ≈0.05 V which is one order of magnitude lower than that of most reported memristors based on 2D materials, and low power consumption. Furthermore, the memristor demonstrates not only electrical voltage‐driven long‐term potentiation, depression plasticity, and paired‐pulse facilitation, but also light‐induced short‐ and long‐term plasticity. Moreover, the photonic synapse can be used to simulate the "learning experience" behaviors of human brain. Consequently, not only the memristor based on BiOI nanosheets shows ultra‐low SET voltage and low‐power consumption, but also the optoelectronic synapse provides new material and strategy to construct low‐power retina‐like vision sensors with functions of perceiving and processing information. [ABSTRACT FROM AUTHOR]

Single‐atom catalysts (SACs) have attracted great attention in the field of electrocatalysis due to their exceptional activity, selectivity, 100% atom utilization, and tailorability of active sites at atomic level. The metal–support interactions and interatomic synergies, however, are severely limited due to the isolation of active sites in SACs which hinder their applications in some complex reactions. To this end, supported sub‐nanometer cluster catalysts (SNCCs, <2 nm) with nearly fully exposed active atoms may outperform the SACs in some specific catalytic reactions. The presence of abundant chemical bonds in the clusters can flexibly regulate the support–cluster interaction and build ensemble effect in the sub‐nanometer clusters for different electrocatalysis applications. In this review, recent advances of supported SNCCs in electrocatalysis applications are summarized and discussed for the first time. In particular, the importance of the support–cluster interactions and ensemble effect of the clusters in determining the catalytic performance of SNCCs are highlighted. Lastly, challenges and opportunities in SNCCs electrocatalysis are prospected. [ABSTRACT FROM AUTHOR]

2D materials, such as graphene, transition metal dichalcogenides, black phosphorus, and tellurium, have been demonstrated to be promising building blocks for the fabrication of next‐generation high‐performance infrared (IR) photodetectors with diverse device architectures and impressive device performance. Integrating IR photodetectors with nanophotonic structures, such as surface plasmon structures, optical waveguides, and optical cavities, has proven to be a promising strategy to maximize the light absorption of 2D absorbers, thus enhancing the detector performance. In this review, the state‐of‐the‐art progress of IR photodetectors is comprehensively summarized based on 2D materials and nanophotonic structures. First, the advantages of using 2D materials for IR photodetectors are discussed. Following that, 2D material‐based IR detectors are classified based on their composition, and their detection mechanisms, key figures‐of‐merit, and the principle of absorption enhancement are discussed using nanophotonic approaches. Then, recent advances in 2D material‐based IR photodetectors are reviewed, categorized by device architecture, i.e., photoconductors, van der Waals heterojunctions, and hybrid systems consisting of 2D materials and nanophotonic structures. The review is concluded by providing perspectives on the challenges and future directions of this field. [ABSTRACT FROM AUTHOR]

Reprogramming tumor‐associated macrophages (TAMs) from tumor‐supportive M2 phenotype to anti‐tumor M1 phenotype holds great promise in tumor immunotherapy. However, there are few reports on the remodeling of TAMs by inorganic nanoparticles due to their unclear intrinsic polarization mechanism. In this article, a novel signaling pathway of repolarizing TAMs into M1‐like macrophages is reported to boost anti‐tumor immunity using ultra‐small Cu2−xSe nanoparticles (CS NPs). The mechanism is totally different from the conventional ROS‐mediated polarization mechanism. It is revealed that CS NPs can effectively generate ROS in the macrophages to trigger auto‐ubiquitination of tumor necrosis factor receptor‐associated factor 6 (TRAF6), which activates the interferon regulatory factor 5 (IRF5) to facilitate the expression of its downstream gene interleukin‐23 (IL‐23), and eventually remodels the TAMs into M1‐like macrophages. It is shown that CS NPs can significantly inhibit the growth of melanoma tumor (B16F10) by repolarizing TAMs into M1‐like macrophages, and enhance the adaptive anti‐tumor immunity by inducing the infiltration of CD8+ T cells. Moreover, it is found that CS NPs can also effectively inhibit the recurrence of distal tumor. The study shows the novel macrophage polarization mechanism for TAMs‐targeted cancer immunotherapy, and demonstrates the great potential of ultra‐small Cu2−xSe nanoparticles in cancer immunotherapy. [ABSTRACT FROM AUTHOR]

Availability of computing will be strongly limited by global energy production in 1–2 decades. Computing consumes 4–5% of global electricity supply and continues to increase. This is underpinned by memory and switching devices encountering leakage as they are downscaled. Two‑dimensional (2D) materials offer a potential solution to the fundamental problem owing to carrier confinement which significantly reduces scattering events. Herein, a mixed ionic‑electronic transport is used in layered black phosphorus (BP) based vertically stacked resistance change memories. The memory device relies on a unique interplay between the oxygen and silver ion diffusion through the stack which is generated using a combination of bottom (electrochemically active silver) and top (indium tin oxide) electrodes. The use of a transparent top‐electrode enabled for the first time to conduct spectroscopic characterization of the device and experimentally reveal fundamental mechanisms. Endurance of the devices are observed to be >104 switching cycles, with ON/OFF current ratio of >107 and standby power consumption of <5 fW, which effectively suppresses leakage current and sneak paths in a memory array. By undertaking detailed microscopic and spectroscopic investigations, supported by theoretical calculations, this work opens opportunities to enhance resistive switching performances of 2D materials for next‑generation information storage and brain‑inspired computation. [ABSTRACT FROM AUTHOR]

Additive manufacturing, also called 3D printing, is a rapidly evolving technique that allows for the fabrication of functional materials with complex architectures, controlled microstructures, and material combinations. This capability has influenced the field of biomedical sensing devices by enabling the trends of device miniaturization, customization, and elasticity (i.e., having mechanical properties that match with the biological tissue). In this paper, the current state‐of‐the‐art knowledge of biomedical sensors with the unique and unusual properties enabled by 3D printing is reviewed. The review encompasses clinically important areas involving the quantification of biomarkers (neurotransmitters, metabolites, and proteins), soft and implantable sensors, microfluidic biosensors, and wearable haptic sensors. In addition, the rapid sensing of pathogens and pathogen biomarkers enabled by 3D printing, an area of significant interest considering the recent worldwide pandemic caused by the novel coronavirus, is also discussed. It is also described how 3D printing enables critical sensor advantages including lower limit‐of‐detection, sensitivity, greater sensing range, and the ability for point‐of‐care diagnostics. Further, manufacturing itself benefits from 3D printing via rapid prototyping, improved resolution, and lower cost. This review provides researchers in academia and industry a comprehensive summary of the novel possibilities opened by the progress in 3D printing technology for a variety of biomedical applications. [ABSTRACT FROM AUTHOR]

Precise detection of early melanomas is essential as the stage of disease guides treatment options. One growing field that may facilitate the advancement of early melanoma detection, is achieved through profiling serum extracellular vesicles (EVs) using sensitive nanotechnology. As a proof of principle, using a detection platform that combines a microfluidic device and surface‐enhanced Raman spectroscopy (SERS), the expression profiles of 4 protein biomarkers in serum EVs (termed as "EV SERS signatures") derived from 20 early stage melanoma patients (including in situ melanoma) and 21 healthy participants are multiplexed. Significantly higher signal intensities of selected protein biomarkers are observed in serum EVs from melanoma patients compared with healthy participants, with mean fold‐changes ranging from 3.7 to 4.2. It is demonstrated that the EV SERS signatures can accurately separate melanoma patients and healthy individuals, with an area under the curve of 0.95. Thus, with further development, this ultra‐sensitive detection platform, combined with the panel of melanoma‐associated biomarkers, has the ability to differentiate early stage melanoma patients from healthy participants. [ABSTRACT FROM AUTHOR]

Resistive random access memory (RRAM) based on ultrathin 2D materials is considered to be a very feasible solution for future data storage and neuromorphic computing technologies. However, controllability and stability are the problems that need to be solved for practical applications. Here, by introducing a damage‐less ion implantation technology using ultralow‐energy plasma, the transport mechanisms of space charge limited current and Schottky emission are successfully realized and controlled in RRAM based on 2D Bi2Se3 nanosheets. The memristors exhibit stable resistive switching behavior with a high resistive switching ratio (>104), excellent cycling endurances (300 cycles), and great retention performance (>104 s). The reliability and controllability of Bi2Se3 memory endowed by oxygen plasma injection demonstrate the great potential of this ultralow‐energy ion implantation technology in the application of 2D RRAM. [ABSTRACT FROM AUTHOR]

Machine learning (ML) is a versatile technique to rapidly and efficiently generate insights from multidimensional data. It offers a much‐needed avenue to accelerate the exploration and investigation of new materials to address time‐sensitive global challenges such as climate change. The availability of large datasets in recent years has enabled the development of ML algorithms for various applications including experimental/device optimization and material discovery. This perspective provides a summary of the recent applications of ML in material discovery in a range of fields, from optoelectronics to batteries and electrocatalysis, as well as an overview of the methods behind these advances. The paper also attempts to summarize some key challenges and trends in current research methodologies. [ABSTRACT FROM AUTHOR]

The extraordinary optical properties of surface plasmons in metal nanostructures provide the possibilities to enhance and accelerate the spontaneous emission, and manipulate the decay and emission processes of quantum emitters. The extremely small mode volume of plasmonic nanocavities also benefits the realization of plasmon–exciton strong coupling. Here, the progress on the study of plasmon modified spontaneous emission and plasmon–exciton strong coupling are reviewed. The fundamentals of surface plasmons and quantum emitters, and the methods for assembling coupling systems of plasmonic nanostructures and quantum emitters are first introduced. Then the major aspects of plasmon modified spontaneous emission, including emission intensity, lifetime, spectral profile, direction, polarization, and energy transfer are reviewed. The coupling of quantum emitters and plasmonic waveguides is then discussed. Next, the developments of strong coupling between plasmonic structures and various quantum emitters are reviewed. Finally a few applications are highlighted followed by conclusions and outlook. [ABSTRACT FROM AUTHOR]

Photoresponsive biomaterials are experiencing a transition from in vitro models to in vivo demonstrations that point toward clinical translation. Dynamic hydrogels for cell encapsulation, light‐responsive carriers for controlled drug delivery, and nanomaterials containing photosensitizers for photodynamic therapy are relevant examples. Nonetheless, the step to the clinic largely depends on their combination with technologies to bring light into the body. This review highlights the challenge of photoactivation in vivo, and presents strategies for light management that can be adopted for this purpose. The authors' focus is on technologies that are materials‐driven, particularly upconversion nanoparticles that assist in "direct path" light delivery through tissue, and optical waveguides that "clear the path" between external light source and in vivo target. The authors' intention is to assist the photoresponsive biomaterials community transition toward medical technologies by presenting light delivery concepts that can be integrated with the photoresponsive targets. The authors also aim to stimulate further innovation in materials‐based light delivery platforms by highlighting needs and opportunities for in vivo photoactivation of biomaterials. [ABSTRACT FROM AUTHOR]

The advancement of a naturally rich and effective bifunctional substance for hydrogen and oxygen evolution reaction is crucial to enhance hydrogen fuel production efficiency via the electrolysis process. Herein, facile and scalable hydrothermal synthesis of bifunctional electrocatalyst of polyoxometalate anchored zinc cobalt sulfide nanowire on Ni‐foam (NF) for overall water splitting is reported for the first time. The electrochemical analysis of POM@ZnCoS/NF displays significantly low HER and OER overpotentials of 170/337 and 200/300 mV to attain a current density of 10/40 and 20/50 mA cm−2, respectively, demonstrating the notable performance of POM@ZnCoS/NF toward H2 and O2 evolution reaction in alkaline medium. Additionally, the electrolyzer consisting of the POM@ZnCoS/NF anode and cathode shows an appealing potential of 1.56 V to deliver 10 mA cm−2 current density for overall water splitting. The high electrocatalytic activity of the POM@ZnCoS/NF is attributed to modulation of the electronic and chemical properties, increment of the electroactive sites and electrochemically active surface area of the zinc cobalt sulfide nanowires due to the anchorage of polyoxometalate nanoparticles. These results demonstrate the advantage of the polyoxometalate incorporation strategy for the design of cost‐effective and highly competent bifunctional catalysts for complete water splitting. [ABSTRACT FROM AUTHOR]

The making of BaZrS3 thin films by molecular beam epitaxy (MBE) is demonstrated. BaZrS3 forms in the orthorhombic distorted‐perovskite structure with corner‐sharing ZrS6 octahedra. The single‐step MBE process results in films smooth on the atomic scale, with near‐perfect BaZrS3 stoichiometry and an atomically sharp interface with the LaAlO3 substrate. The films grow epitaxially via two competing growth modes: buffered epitaxy, with a self‐assembled interface layer that relieves the epitaxial strain, and direct epitaxy, with rotated‐cube‐on‐cube growth that accommodates the large lattice constant mismatch between the oxide and the sulfide perovskites. This work sets the stage for developing chalcogenide perovskites as a family of semiconductor alloys with properties that can be tuned with strain and composition in high‐quality epitaxial thin films, as has been long‐established for other systems including Si‐Ge, III‐Vs, and II‐VIs. The methods demonstrated here also represent a revival of gas‐source chalcogenide MBE. [ABSTRACT FROM AUTHOR]

Polyoxometalate (POM) clusters containing lanthanide ion (LnPOM) possess excellent luminescence features, but the envisaged applications are hindered by the challenges in integration into functional architectures. Herein, a novel cross‐linked cyclodextrin (CL‐CD) and LnPOM composite is developed and applied for discriminative detection of inorganic and organic phosphate phases. For inorganic phosphates, a ratiometric fluorescence response is demonstrated with excellent selectivity, and anti‐interference ability in complex analyte mixtures. The outstanding performance is attributed to the high affinity of POM and distinct interactions between La3+ and Eu3+ with the phosphate. For organophosphates, a "signal‐off" fluorescence response for p‐nitrophenyl‐substituted organophosphates is discovered due to the encapsulation of nitrophenyl group into the hydrophobic cavity of CD that enhances the interactions between POM and p‐nitrophenyl phosphate. The discriminative responses of CL‐CD–LnPOM to inorganic phosphates and organophosphates bring new insights into POM‐based fluorescence probes for the detection of inorganic and organic phases based on the intrinsic structural difference between the phosphate analogs. [ABSTRACT FROM AUTHOR]

Dissolvable microneedle patches (MNPs) enable simplified delivery of therapeutics via the skin. However, most dissolvable MNPs do not deliver their full drug loading to the skin because only some of the drug is localized in the microneedles (MNs), and the rest remains adhered to the patch backing after removal from the skin. In this work, biphasic dissolvable MNPs are developed by mounting water‐soluble MNs on a water‐insoluble backing layer. These MNPs enable the drug to be contained in the MNs without migrating into the patch backing due to the inability of the drugs to partition into the hydrophobic backing materials during MNP fabrication. In addition, the insoluble backing is poorly wetted upon MN dissolution in the skin, which significantly reduces drug residue on the MNP backing surface after application. These effects enable a drug delivery efficiency of >90% from the MNPs into the skin 5 min after application. This study shows that the biphasic dissolvable MNPs can facilitate efficient drug delivery to the skin, which can improve the accuracy of drug dosing and reduce drug wastage. [ABSTRACT FROM AUTHOR]

A general and versatile technology to engineer light‐responsive protein‐based biomaterials can enable the manipulation and interrogation of proteins, pathways, and cells, and it will assist the design of "smart" light‐responsive biomaterials. This study reports the evolution of chromosomal aminoacyl‐tRNA synthetases (aaRSs) for azobenzene‐bearing unnatural amino acids (uAAs) with up to ≈40‐fold increased protein production and improved fidelity, as compared with a previously described aaRS. The evolved translation systems enable efficient and accurate incorporation of up to 10 instances of the various light‐responsive uAAs in elastin‐like polypeptides (ELPs). Azobenzene‐containing ELPs are capable of isothermal, reversible, light‐mediated soluble‐to‐insoluble phase transition, with up to a 12 °C difference in the ELP transition temperature upon cis‐to‐trans azobenzene isomerization. Furthermore, the incorporation of azobenzene‐uAAs in ELP diblock‐copolymers enables the creation of light‐responsive self‐assembled nanostructures. Finally, light‐responsive resilin‐inspired polymers are also generated by multi‐site azobenzene‐incorporation. The translation machinery evolved in this study can be used for the multi‐site incorporation of azobenzene moieties at the polypeptide level and constitute a universal methodology for the design of light‐responsive proteins and additional families of protein‐based biomaterials with customized and tunable light‐responsive behavior. [ABSTRACT FROM AUTHOR]

Radicals are closely related to human life and health and have been widely used in biology, chemistry, functional materials, etc. However, the high reactivity, disorder, and short half-lives limit their wide applications. Therefore, it remains a great challenge to prepare stable and ordered radicals. Herein, radicals are prepared with protective umbrellas (diethylmethyleneamine, DEMA) that are integrated on the surface of 2D layered materials to isolate water and oxygen and enhance the stability of radicals. Taking 2D black phosphorus (BP) as an example: triethylamine reacts with dichloromethane to form quaternary ammonium salts with further Hoffmann elimination to produce DEMA radicals that could react with one electron of a lone pair electrons in P on the surface of BP to produce P radicals, which shows a prolonged half-life of 21 days at room temperature. First-principle calculations and electron paramagnetic resonance fitting confirm that the steric hindrance constructed by dense DEMA passivation layer acts as a protective umbrella and the 2D coupling of P radicals and other P atoms in 2D BP plane to enhance the stability and strong superexchange interaction ofP radicals. Furthermore, it is a general strategy to produce stable radicals integrated on the 2D plane. [ABSTRACT FROM AUTHOR]

Self‐assembling peptide nanofibrils (PNF) have gained increasing attention as versatile molecules in material science and biomedicine. One important application of PNF is to enhance retroviral gene transfer, a technology that has been central for gene therapy approaches. The best‐investigated and commercially available PNF is derived from a 12‐mer peptide termed EF‐C. The mechanism of transduction enhancement depends on the polycationic surface of EF‐C PNF, which bind to the negatively charged membranes of viruses and cells, thereby overcoming electrostatic repulsions and increasing virion attachment and fusion. To better understand how EF‐C PNF interact with the cell surface, scanning electron and time‐lapse confocal microscopy were performed. The fibrils are found to be actively engaged by cellular protrusions such as filopodia. Consequently, chemical suppression of protrusion formation abrogates fibril binding and virion delivery to the cell surface of immortalized and primary T cells. Vice versa, induction of plasma membrane blebs result in increased fibril binding. Thus, the mechanism of PNF‐mediated viral transduction enhancement involves an active engagement of virus‐loaded fibrils by cellular protrusions, which may explain its superior performance over soluble transduction enhancers. [ABSTRACT FROM AUTHOR]

Hydrazine oxidation assisted water electrolysis offers a unique rationale for energy‐saving hydrogen production, yet the lack of effective non‐noble‐metal bifunctional catalysts is still a grand challenge at the current stage. Here, the Mo doped Ni3N and Ni heterostructure porous nanosheets grow on Ni foam (denoted as MoNi3N/Ni/NF) are successfully constructed, featuring simultaneous interface engineering and chemical substitution, which endow the outstanding bifunctional electrocatalytic performances toward both hydrazine oxidation reaction (HzOR) and hydrogen evolution reaction (HER), demanding a working potential of −0.3 mV to reach 10 mA cm−2 for HzOR and −45 mV for that of HER. Impressively, the overall hydrazine splitting (OHzS) system requires an ultralow cell voltage of 55 mV to deliver 10 mA cm−2 with remarkable long‐term durability. Moreover, as a proof‐of‐concept, economical H2 production systems utilizing OHzS unit powered by a waste AAA battery, a commercial solar cell, and a homemade direct hydrazine fuel cell (DHzFC) are investigated to inspire future practical applications. The density functional theory calculations demonstrate that the synergy of Mo substitution and abundant Ni3N/Ni interface owns a more thermoneutral value for H* absorption ability toward HER and optimized dehydrogenation process for HzOR. [ABSTRACT FROM AUTHOR]

Thermodynamically favorable electrooxidation reactions of biomass derivatives integrated with hydrogen evolution reaction (HER) can simultaneously provide value‐added chemicals and hydrogen, and eventually meeting the need for clean and sustainable energy development. Herein, the integration of a six‐electron involved anodic half‐reaction‐selective electrooxidation of 5‐hydroxymethylfurfural into 2,5‐furandicarboxylic acid (FDCA) on a hierarchically layered double hydroxide (CoFe@NiFe) with a cathodic HER in a two‐chamber system is reported. The overall reaction reaches 38 mA cm−2 at 1.40 V and exhibits 100% selectivity to yield FDCA and a nearly 100% Faraday efficiency with hydrogen production of 901 µmol cm−2. Several operando techniques confirm that the trivalent nickel species in the CoFe@NiFe catalyst are mainly responsible for this 100%‐selective oxidation reaction. This integrated overall reaction is thus a new strategy to utilize cheap catalysts and biomass derivatives to simultaneously produce value‐added chemicals and sustainable energy materials, and eventually to solve current challenges of energy depletion and environmental pollution. [ABSTRACT FROM AUTHOR]