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Research on high‐efficiency and cost‐efficient catalysts for oxygen reduction reaction (ORR) is still a vital but challenging issue for commercializing metal–air batteries. Herein, a single‐molecule/atom hybrid catalyst is developed to boost the ORR, in which iron phthalocyanine molecules containing molecular Fe─N4 moieties couple with atomic Co─N4 sites on the surface of polyhedral carbon. Density functional theory calculations reveal that face‐to‐face laminated construction of Fe─N4 and Co─N4 in the hybrid catalyst can effectively modulate the electronic structure of active iron atoms and reduce the energy barrier of the rate‐determining step for ORR. As a result, this hybrid catalyst demonstrates excellent ORR performance, featuring a half‐wave potential of 0.904 V, a peak power density of 238.3 mW cm−2 for zinc–air battery, and outstanding electrocatalytic stability. This work offers a distinctive and robust molecular/atomic engineering approach to creating efficient electrocatalysts, advancing the fields of metal–air batteries. [ABSTRACT FROM AUTHOR]

Biological systems are composed of hierarchical structures made of a large number of proteins. These structures are highly sophisticated and challenging to replicate using artificial synthesis methods. To exploit these structures in materials science, biotemplating is used to achieve biocomposites that accurately mimic biological structures and impart functionality of inorganic materials, including electrical conductivity. However, the biological scaffolds used in previous studies are limited to stereotypical and simple morphologies with little synthetic diversity because of a lack of control over their morphologies. This study proposes that the specific protein assemblies within the cell‐derived extracellular matrix (ECM), whose morphological features are widely tailorable, can be employed as versatile biotemplates. In a typical procedure, a fibrillar assembly of fibronectin—a constituent protein of the ECM—is metalized through an antibody‐guided biotemplating approach. Specifically, the antibody‐bearing nanogold is attached to the fibronectin through antibody–antigen interactions, and then metals are grown on the nanogold acting as a seed. The biomimetic structure can be adapted for hydrogen production and sensing after improving its electrical conductivity through thermal sintering or additional metal growth. This study demonstrates that cell‐derived ECM can be an attractive option for addressing the diversity limitation of a conventional biotemplate. [ABSTRACT FROM AUTHOR]

To address the problem of the serious capacity fading in lithium–sulfur batteries, a multi‐functional PEO(polyethylene oxide)/LiFSI (lithium bis(fluorosulfonyl)imide)/PVDF (polyvinylidene fluoride) (PLP) gel polymer electrolyte is exploited by coating PLP on a carbon nanotubes (CNTs) based sulfur cathode (PLP‐S/CNTs) with a controlled thermal annealing process. The annealing process leads to the conformal infusion of PLP through the matrix of S/CNTs with retaining the amorphous phase of the PLP, which enhance the rate performance compared to the bare S/CNTs. The PLP coating drives the transformation of more elemental sulfur to Li2S2/Li2S without forming intermediary product by restraining soluble‐polysulfides formation. Furthermore, the PLP coating successfully inhibits the dissolution of Li2Sx (x > 4) in PEO and prevents the loss of active material in the cathode, which is confirmed by density functional theory calculations. Comprehensively, the PLP coating applied to the surface of the S/CNTs cathode exhibit significantly suppressed shuttle effect and greatly improve long‐term cycle stability of the lithium–sulfur battery. The synthesized PLP‐coated S/CNTs composite cathode demonstrates a high specific capacity of 573.6 mAh g−1 at a current density of 0.5 C after 1 000 cycles, even achieving 318.1 mAh g−1 at an extremely high C‐rate (6 C). which is unprecedented performance among the reported studies on coating technology. [ABSTRACT FROM AUTHOR]

Covalent organic frameworks (COFs), featuring ordered nanopores with numerous accessible redox sites, have drawn much attention as promising electrode materials for rechargeable batteries. Thus far, however, COF‐based battery electrodes have exhibited limited capacity and unsatisfactory cycling stability due to the unwanted side reactions over their large surface area. Herein, a fluorine‐rich covalent organic framework (F‐COF) as an electrode material with improved stability and performance for potassium‐ion batteries is developed. The fluorinated COF not only stabilizes intercalation kinetics of K+ ions but also reinforces its electron affinity and conductivity, improving the reversibility of bond transitions during discharge–charge cycles. As a result, F‐COF affords a high specific capacity (95 mAh g−1 at fast rates up to 5 C) and excellent cycling stability (5000 cycles with ≈99.7% capacity retention), outperforming the pristine COF‐based electrodes devoid of F atoms. Notably, the experimental capacity of F‐COF approaches its theoretical value, confirming that a large proportion of electroactive sites are being actively utilized. Altogether, this work addresses the significant role of F atoms in improving the K+‐ion storage capability of COFs and provides the rational design principles for the continued development of stable and high‐performance organic electrode materials for energy storage devices. [ABSTRACT FROM AUTHOR]

The lithium metal anode is notoriously unstable and reactive to electrolytes, forming brittle solid‐electrolyte interphase (SEI) layers with uneven distribution, exacerbating Li dendrites that ultimately limit the battery life. Here, this work passivates Li metal with electrolyte‐swellable polymer nanolayers deposited monolithically by the initiated chemical vapor deposition (iCVD) to reinforce the native SEI layers and stabilize their interface. The 100 nm iCVD poly(dimethylaminomethyl styrene) (pDMAMS) layer is swelled by 264% under a carbonate electrolyte, establishing the electrolyte‐filled soft scaffold for Li‐ion transport. Notably, the solvogel accommodates homogeneous Li2O‐free and Li2CO3‐rich native SEI layers, providing a record‐high Li‐ion transference number of 0.95 and ionic conductivity of 6.54 mS cm−1. The developed pDMAMS‐Li anodes extend the cycle life by 550% in Li–Li symmetric cells and 600% in LiNi0.6Mn0.2Co0.2O2 full cells compared to pristine Li metal. The mechanistic details of the swollen‐soft‐scaffold strategy are elucidated by depth profile analysis of the pDMAMS homopolymer compared to pDMAMS/electrolyte‐phobic copolymers, providing new insights to manage the interface of liquid‐state electrolyte and solid‐state Li metal by using a novel class of bifunctional solvogel. [ABSTRACT FROM AUTHOR]

Activation of metal oxides by light is a robust yet facile approach to manipulating their surface chemistry for favorable reactions with target molecules in heterogeneous catalysis and gas sensors. However, a limited understanding of interface chemistry and the involved mechanism impedes the development of a rational design of oxide interfaces for light‐activated gas sensing. Herein, the TiOx‐assisted photosensitization of In2O3 toward NO2 sensing is investigated as a case study to elucidate the detailed mechanism of light‐activated surface chemistry at the metal/gas interface. The resultant heterogeneous oxides exhibit outstanding NO2 sensing performance under light irradiation thanks to abundant photoexcited electrons and holes that serve as adsorption and desorption sites, respectively, to accelerate both surface reactions. Furthermore, the facile transfer of electrons and holes across the TiOx‐In2O3 interface contributes to improving the reversibility of sensing kinetics. Through this study, the mechanistic understanding is established of how the surface chemistry of metal oxide surfaces can be tuned by light activation providing an effective route to the design fabrication of high‐performance gas sensors. [ABSTRACT FROM AUTHOR]

To realize the development of high‐performance electrodes materials, real‐time observation tool that can visualize dynamical changes of electrode materials upon lithiation and sodiation is highly critical. Recently, in situ transmission electron microscopy (TEM) has gained much attraction as it provides rich information on both phase and morphological transitions of electrode materials upon lithiation and sodiation in an atomic scale. Nevertheless, two significant limitations are present for current in situ TEM study: i) most of the in situ TEM experiments use a specially designed TEM holder, which is costly and suitable for use in only selective types of TEM; and ii) recently developed in situ TEM techniques with no applied bias have inherent limitations in the size of the sample (difficult for a size above 50 nm). Overcoming these two aforementioned issues, bias‐free graphene solid cells (GSCs) are now introduced, which can conduct real‐time observation of electrode materials in any size dimensions and morphologies without using bias. In this work, dynamical changes of hollow SnO2 nanotubes (NTs) are visualized upon lithiation and sodiation in real time using GSCs, where rich information is obtained on the morphology‐dependent, ion‐dependent characteristics of dynamical changes. [ABSTRACT FROM AUTHOR]

Due to the unique properties which are considerably different from macro‐scale or bulk materials, 1D) nanostructures have received great interests. In particular, they have greatly contributed to building next‐generation batteries by providing beneficial features such as short ion/electron pathways, structural versatility (i.e., formation of 3D current collectors, free‐standing electrodes, and separators), and excellent stress relaxation. Owing to these definite advantages, 1D nanostructure is often followed by discovery of new electrode materials. This review provides a systematic overview of the state‐of‐the‐art research progresses on 1D nanostructures, which are extensively used for rechargeable batteries. Specifically, a brief introduction of some important 1D nanostructuring methods is started and then, in situ structural characterizations using 1D nanostructures are summarized, which allow a great step forward in atomic‐scale monitoring of reaction kinetics and observing dynamic structural evolution of electrode materials. 1D nanstructuring in solid‐state electrolytes and stabilization of metal anodes are also highlighted which are not only substantially important in current research trends for future batteries but also rarely discussed in previous reviews. At the end, critical perspective and future research direction of 1D nanoengineering for future batteries are suggested. [ABSTRACT FROM AUTHOR]

Transition metal dichalcogenides (TMDs) have attracted significant interest as gas‐sensing materials due to their unique crystal structure and surface. However, there are still issues when it comes to expanding the types of sensing gases for the TMD gas sensors. To extend gas‐sensing selectivity for the TMD gas sensors in this study, a monolayer (ML) 2D metal–organic framework (MOF) is introduced on top of the PtSe2 gas sensor, thereby tuning the major sensing analyte of PtSe2 from NO2 to H2S. Density functional theory calculations elucidate that the metal species of ML MOFs are attributed to the tuned selectivity of the analytes, based on the difference in binding energies. It is also demonstrated that ML MOF maintained the high responsivity of the pristine PtSe2 even at a low concentration of gas (200 ppb). This is further confirmed through the molecular dynamics simulations, which reveal that the ML feature of the ML MOF is highly essential to preserve the intrinsic ultra‐low limit detection properties of pristine PtSe2. [ABSTRACT FROM AUTHOR]

Thermochromic sensors provide an intuitive and real‐time solution for monitoring the local temperature with naked eyes. Conventional thermochromic sensors often utilize either solution‐type or dense film‐type platforms, which are suboptimal morphologies for exposing a large number of dye molecules to the surface, leading to low sensitivity and sluggish responding speeds. Herein, this article introduces rational synthetic routes to fabricate highly sensitive nanofiber (NF) sensor membranes loaded with thermochromic dyes (C3H6N6·CH2O)x‐loaded nanofibers (NFs) sensor membranes by alignment‐controllable electrospinning techniques (x–y perpendicular and rotary). The NF‐based porous sensor membranes exhibit two‐ to fivefold improved thermochromic sensitivity (ΔRGB) compared to those of dense film‐type sensors at 31.6–42.7 °C. This is attributed to the uniform distribution of dyes throughout the porous NF structure (≈95.7%), which exhibits excellent light transmittance that is 10–30‐fold higher than that of film‐type sensors. Based on the available shape‐conforming synthetic strategies, this article further demonstrates wearable thermochromic sensors in the forms of mask‐, patch‐, and bracelet‐type devices, which can accurately monitor body temperature in real time. [ABSTRACT FROM AUTHOR]

Flexible and mechanically robust gas sensors are the key technologies for wearable and implantable electronics. Herein, the authors demonstrate the high-performance, flexible nitrogen dioxide (NO2) chemiresistors using a series of n-type conjugated polymers (CPs: PNDIT2/IM-x) and a polymer dopant (poly(ethyleneimine), PEI). Imine double bonds (C = N) are incorporated into the backbones of the CPs with different imine contents (x) to facilitate strong and selective interactions with NO2. The PEI provides doping stability, enhanced electrical conductivity, and flexibility. As a result, the NO2 sensors with PNDIT2/IM-0.1 and PEI (1:1 by weight ratio) exhibit outstanding sensing performances, such as excellent sensitivity (𝚫R/Rb = 240%@1 ppm), ultralow detection limit (0.1 ppm), high selectivity (𝚫R/Rb < 8%@1 ppm of interfering analytes), and high stability, thereby outperforming other state-of-the-art CP-based chemiresistors. Furthermore, the thin film of PNDIT2/IM-0.1 and PEI blend is stretchable and mechanically robust, providing excellent flexibility to the NO2 sensors. Our study contributes to the rational design of high-performance flexible gas sensors. [ABSTRACT FROM AUTHOR]

Single‐atom catalysts (SACs) supported on inorganic materials have attracted much attention in numerous research fields for their high catalytic performance. However, such SACs have been limited by the low metal loading, especially on different types of inorganic supports. Herein, a general approach is presented for preparing SACs on metallic, metal oxide, and perovskite nanosheet (NS) supports to reach a high metal loading of up to 3.94 wt%, by utilizing N‐doped graphene as a sacrificial template that spatially confines the single atoms (SAs). Specifically, the target support material precursors are adsorbed onto the SAs‐stabilized sacrificial template, followed by subsequent heat treatment to transfer the SAs to the support material and to remove the graphene layer. Pt SAs on oxide support exhibits little to no aggregation throughout >10 000 min of annealing at 275 °C, demonstrating high thermal stability, as also supported by ex situ post‐anneal electron microscopy and X‐ray absorption fine structure studies. As a proof‐of‐concept, Pt SACs on SnO2 NSs exhibit high catalytic activity toward chemiresistive sensing of acetone gas (response = 95.4 at 10 ppm, 7.6‐fold enhancement compared with pristine SnO2 NSs) and unprecedented stability under highly humid conditions (27.4% response deterioration at 95% relative humidity). [ABSTRACT FROM AUTHOR]

Designing energy storage devices from thick carbon electrodes with high areal/volumetric energy density via a simple and green way is very attractive but still challenging. Cellulose, as an excellent precursor for thick carbon electrodes with abundant sources and low cost, is usually activated by a chemical activator and pyrolysis route to achieve high electrochemical performance. However, there are still some problems to be addressed, such as the harsh activation conditions, easy collapse of porous structures, and the high cost. Herein, a 3D self‐supporting thick carbon electrode derived from wood‐based cellulose is proposed for high areal and volumetric energy density of supercapacitor from a mild, simple, and green enzymolysis treatment. Benefiting from the high specific surface area (1418 m2 g−1) and abundant active sites on the surface of wood‐derived hierarchically porous structures and enzymolysis‐induced micropores and mesopores, the assembled symmetry supercapacitor from the thick carbon electrode can realize the high areal/volumetric energy density of 0.21 mWh cm−2/0.99 mWh cm−3 with excellent stability of 86.58% after 15 000 long‐term cycles at 20 mA cm−2. Significantly, the simple and universal strategy to design material with high specific surface area, provides a new research idea for realizing multi‐functional application. [ABSTRACT FROM AUTHOR]