This study demonstrates a strategic paradigm in photocatalytic nitrogen fixation by engineering semiconductor hole oxidation dynamics to circumvent ammonium degradation. Diverging from conventional approaches focused on light absorption and carrier mobility enhancement, we develop a sacrificial agent-free system leveraging attenuated hole oxidation capacity to fundamentally suppress oxidative depletion of NH4+. Bi2O2Se (BOS) serves as an archetypal catalyst, revealing mechanistic correlations between weak hole oxidizing environments and nitrogen reduction efficiency. Experimental analyses confirm BOS's superior performance over traditional photocatalysts, attributed to its intrinsic capacity to prevent NH4+ oxidation while enabling effective product enrichment. Remarkably, the catalyst maintains equivalent nitrogen fixation efficiency in ambient air and inert atmospheres, demonstrating exceptional oxygen compatibility. Furthermore, BOS exhibits panchromatic photon utilization extending into near-infrared regions (AQE = 0.12 % at 700 nm). The unmodified bulkphase characteristics of BOS highlight its inherent catalytic superiority, challenging conventional modificationdependent catalyst design frameworks. This work establishes oxidation potential modulation as a critical determinant in photocatalytic nitrogen fixation while providing a material platform and conceptual blueprint for sustainable ammonia synthesis technologies.

Geminal-site catalysts (GSCs) are prospective candidates for fulfilling the goal of aqueous electrochemical reductive cross-coupling reactions (ERCR) at near-stoichiometric yields. Nevertheless, a problem lies in the lack of a synthetic route for GSCs with few single sites. Here we report a defect-accompanying strategy for synthesizing GSCs containing metal-defect catalytic pairs (M-D GSCs), meaning that Fe-D GSCs can realize the electrochemical synthesis of cyclohexanone oximes (CHOs) from high concentrations (0.5 M) of nitrites (NO2 -) and cyclohexanone (CYC) at near-stoichiometric yields (the Faradic efficiency or yieldC/N: 91.3%). Multiple in-/ex-situ characterizations demonstrated that metal-citrate complexes were converted to metal-defect catalytic pairs via the liberation of gaseous carbon/nitrogen species during pyrolysis. Furthermore, we developed an innovative cathodic oxime-alkali process, where high concentration NaNO2 and CYC can be electrochemically converted to high-purity products including NaOH and CHO. This work showcases the enormous potential of M-D GSCs in achieving near-stoichiometric conversion for ERCR reactions.

Understanding the detailed structures of active sites and the dynamic nucleation evolution during zeolite precursor formation offers effective guidance on rational design and construction of titanosilicate with optimized performance. Herein, we tracked the evolution of titanosilicate precursors (TSPs) during TS-1 nucleation, revealing the coexistence of dual Ti species, namely highly dispersed amorphous TiO2 and tetrahedral Ti species incorporated within the silicalite framework. During nucleation, Ti atoms are initially incorporated into silicalite framework and then partially reconstruction into TiO2 species, displaying a volcano-shaped dependence of tetrahedral Ti proportion on nucleation time. Significantly, the coexisting dual Ti species in TSPs activate highly reactive peroxyl radicals, which selectively promote olefin oxidative cleavage other than epoxidation, differing from the behavior of TS-1 and anatase TiO2. Our research clarified the dynamic evolution of TSPs and the structure-activity relationship between their dual Ti species and oxidation pathways, thereby guiding the targeted development of titanosilicate catalysts.

Electrocatalytic C-N coupling of organic carbon and nitrogen sources has emerged as a promising route to high-value chemicals in heterogeneous catalysis over the past decade. Most research has focused on optimizing catalyst active sites to accelerate C-N coupling at the catalyst/electrolyte interface, but the electrolyte's role remains poorly understood. Here, we introduce Li+, Na+, and K+ into the electrolyte and use slow-growth molecular dynamics with explicit solvation models to examine their impact on C-N coupling at the Cu/electrolyte interface. We show that K+ enables a one-step mechanism in which C-N bond formation and hydrogenation occur simultaneously, yielding the *OC-NOH intermediate with a barrier of 0.68 eV. Differential electrochemical mass spectrometry (DEMS) demonstrates that the m/z = 59, assigned to the *OC-NOH intermediate, is detected over the Cu catalyst in 0.1 M KHCO3. Without K+, the reaction follows a two-step pathway with a higher overall barrier of 1.0 eV (0.71 eV for C-N formation, 0.29 eV for hydrogenation), and the *OC-NOH intermediate is not detected by DEMS. Interfacial analysis reveals that K+ enriches hydrogen near the interface and enhances charge transfer to activate *NO, enabling concurrent coupling and hydrogenation. This results in a Faradaic efficiency of 67.25 ± 3.27% and a urea production rate of 21.02 ± 0.83 mmol g-1 h-1 on pure Cu in 0.1 M KHCO3 at -0.5 V vs RHE─surpassing all previous Cu-based systems. Our work identifies a more efficient one-step C-N coupling mechanism through simple electrolyte modulation.

Sulfide solid electrolytes (SSEs) are promising for all-solid-state lithium batteries (ASSLBs) due to their high ionic conductivity, mechanical deformability, and interfacial compatibility. However, SSE interfaces with anodes, cathodes, conductive additives, and current collectors are unstable, triggering safety failures like capacity degradation, internal resistance build-up, thermal runaway, and short circuits. This review summarizes recent progress on interface-induced safety failure mechanisms in sulfide-based ASSLBs, focusing on interface types, failure mechanisms, and thermal/mechanical degradation under multi-field coupling. We survey interface modification strategies and highlight advanced characterization techniques for probing interfacial phenomena. Key challenges and future research directions are discussed. Integrating recent findings, we identify interfacial instability as the primary bottleneck governing safety failures, providing a theoretical and technical framework for rational interface design, performance optimization, and safety enhancement. Throughout this review, we use SSE as the standard abbreviation for sulfide solid electrolytes.

The design strategies and structural advantages of high-entropy-cooperated single-atom catalysts were comprehensively reviewed, which bridged the configurational complexity and atomic precision for critical catalytic systems.

ABSTRACT The practical implementation of Li 2 S cathodes in all‐solid‐state lithium‐sulfur batteries is severely hindered by sluggish ionic/electronic transport and a high activation barrier, particularly under high‐mass‐loading conditions. Herein, lithium thiostannate (Li 4 SnS 4 ) is introduced as a molecular mediator to activate Li 2 S redox chemistry. In situ growth of Li 4 SnS 4 on Li 2 S constructs a continuous Li + ‐transport network, increasing the ionic conductivity from 2.25 × 10 −5 to 3.99 × 10 −5 S cm −1 . More importantly, the hybridization between unsaturated Sn p orbitals and interfacial sulfur atoms induces the formation of Sn─S bonds, leading to local electron‐density redistribution around sulfur. This interfacial electronic reconstruction weakens Li + confinement within the sulfur lattice, softens the Li─S bond, and lowers the oxidation barrier, thereby reducing the initial charge potential from 2.94 to 2.41 V. Consequently, the Li 2 S@Li 4 SnS 4 cathode delivers stable cycling over 100 cycles under demanding conditions of 50 wt.% Li 2 S and areal loading of 5 mg cm −2 . Moreover, a prototype pouch cell retains sufficient capacity to power a light‐emitting diode panel after 100 cycles. This work demonstrates that interfacial electronic‐structure engineering offers an effective strategy for activating Li 2 S cathodes toward high‐energy all‐solid‐state Li‐S batteries.

Accounting for over one-third of global energy use, buildings face a rapidly rising cooling demand driven by expanding floor areas and extensive air-conditioning, making them a major source of global energy consumption and carbon emissions. Radiative cooling (RC) materials offer a promising route to address the conflict between global decarbonization goals and energy-intensive cooling demands through zero-energy, eco-friendly building temperature regulation. However, their practical adoption is still hindered by the unique functional demands of different building components. To address these site-specific requirements, natural organisms guide the rapid development of bioinspired RC materials. Herein, we review recent advances in bioinspired RC materials for building energy savings spanning from material design to practical applications. First, we discuss the design of static and dynamic RC materials from the perspective of bioinspired structural design and material selection. Then, we introduce the specific requirements of RC materials in practical building applications, such as mechanical durability and self-cleaning capability for roofs, angle-selective design and thermal insulation for walls, and transparency and adaptability for windows. Next, we summarize the performance assessment of RC materials, covering both basic optical metrics and building-specific evaluations. Later, we present the discovery and structural design of RC materials driven by machine learning. Finally, we outline the path forward for RC materials, such as intelligent integration with other cooling methods, addressing the key challenges and prospects for their real-world building applications.

Membrane fouling restricts the application of dynamic membrane (DM) technology, and conventional cleaning strategies pose secondary pollution risks. Herein, a piezoelectric-coupled DM driven by low-intensity ultrasound was developed using polypropylene (PP) fibers. 25 kHz was identified as the optimal frequency for piezoelectric ROS generation, yielding a maximum open-circuit voltage of ~90 mV and reactive oxygen species (e.g., ·OH and H2O2) for active antifouling. The system achieved 99.9% inactivation of E. coli (106 CFU/mL) and synchronous removal of methyl orange, nitrate, and ammonia nitrogen. However, continuous ultrasound operation caused adverse effects: high-frequency (120 kHz) accelerated fouling via EPS leakage, while continuous operation at 25 kHz compromised effluent quality by physically disrupting the fouling layer. To address this, an optimized intermittent strategy (10 s/3 min) was implemented, extending stable operation by 41.6% without impairing sludge activity. This strategy was further validated in retired membrane recycling scenarios, prolonging the lifespan of retired membranes by 119% with effluent turbidity below 6 NTU. This work provides a low-carbon, chemical-free pathway for DM fouling mitigation and waste resource utilization.

ABSTRACT The pursuit of high‐energy‐density solid‐state batteries using Li metal anodes and high‐voltage Ni‐rich cathodes is hindered by severe interfacial degradation. Conventional polymer electrolytes with electronegative groups strongly adsorb high‐valent nickel, accelerating cathode decomposition and oxygen release. Here, we develop a deep‐eutectic polymer electrolyte (p‐DEPE) via in situ copolymerization of cyanoacrylate and butyl acrylate within a LiTFSI/LiDFOB dual‐salt network to reshape the interfacial chemistry. This design creates an intermolecular hydrogen‐bonding matrix that establishes a competitive coordination environment at the cathode interface, effectively weakening Ni 4+ adsorption on electronegative sites. The suppression of high‐value Ni inhibits the growth of a high‐resistance cathode–electrolyte interphase and retards the detrimental phase transition from a layered to a rock‐salt structure. Furthermore, the locally confined interaction between the cyano‐group and the cathode surface at high states of charge minimizes parasitic chemical reactions with lattice oxygen, thereby substantially reducing oxygen release. Consequently, Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 cells with p‐DEPE deliver outstanding high‐rate performance, cycling over 200 cycles at 2 C at room temperature and at 3 C at 70°C. Moreover, a 4.5 V high‐loading Li||NCM811 pouch cell retains 97.3% of its initial capacity after 100 cycles. This work demonstrates a scalable polymer electrolyte strategy for high‐energy‐density lithium metal batteries.

Activating benzylic C(sp3)–H bonds is essential in organic synthesis. However, electrocatalytic oxidation of methyl arenes to aromatic aldehydes remains challenging, particularly under aqueous electrolysis conditions. In this work, we have confirmed CoO2 as the active phase for the electrochemical methyl arene oxidation reaction on Co-based catalysts through theoretical calculations, and propose oxygen-vacancy-rich Co3O4 for efficient electrochemical methyl arene oxidation reaction performances. The generation of CoO2−x species is extremely difficult for Co3O4, so that it is almost inactive for the electrochemical methyl arene oxidation reaction on Co3O4. Through a combination of in/ex situ characterizations, we proved that oxygen vacancy could induce the electrochemical reconstruction of Vo-Co3O4 to CoO2−x species on the catalyst surface for achieving excellent electrochemical methyl arene oxidation reaction performance, and the aromatic aldehyde yield and the Faraday efficiency are 90

Solid polymer electrolytes are promising for lithium metal batteries, yet achieving both high ionic conductivity and interfacial stability remains a major challenge. Here, we report a molecular rotor strategy that addresses this trade-off by incorporating 3-(1-Pyridinio)-1-propanesulfonate zwitterions (PP-Z) into a polyvinylidene difluoride electrolyte. This design establishes a dipole-rotation-assisted ion transport mechanism distinct from conventional polymer relaxation-dependent conduction. Molecular dynamics simulations and experiments reveal that the anchored cationic group of PP-Z serves as a pivot, while the mobile anionic end creates a dynamic coulombic field. This configuration facilitates rapid Li+ migration through coordinated intrachain transport and interchain hopping, significantly enhancing ionic conductivity (5.1 × 10-4 S cm-1 at 25°C and 1.5 × 10-4 S cm-1 at 0°C) and the Li+ transference number (0.52). The anionic terminals further participate in Li+ solvation and promote formation of a LiF-rich solid electrolyte interphase, enabling stable cycling for 1200 h in Li||Li cells at 0.3 mA cm-2 and >  500 cycles in Li||LiFePO4 cells at 1C (25°C). Even at 0°C, the Li||LiNi0.8Co0.1Mn0.1O2 (1.8 mAh cm-2) pouch cell retains 85.1% capacity over 50 cycles while delivering 78.3% of its room-temperature capacity initially.

Lithium metal batteries are widely regarded as one of the most promising candidates for achieving energy densities beyond 500 Wh kg−1. However, their practical commercialization is severely hindered by the high reactivity of lithium metal, which leads to pronounced interfacial instability. Constructing an artificial solid electrolyte interphase (SEI) via surface pretreatment has been demonstrated to be an effective strategy for suppressing dendrite growth and mitigating parasitic side reactions. Herein, we take advantage of the rapid reaction between lipoic acid (LA) and lithium metal to pre-form a uniform artificial SEI on the anode surface. This interphase is composed of organic COO-Li species and sulfur-containing compounds. Electrochemically, the LA-modified lithium anode exhibits remarkable stability, sustaining more than 1500 h of cycling in symmetric cells at 5 mA cm−2 and 5 mAh cm−2. Furthermore, full-cell configurations, including lithium-sulfur and lithium-LiFePO4 pouch cells, deliver significantly improved cycling performance compared with those employing bare lithium anodes. These results establish a practical and scalable route for fabricating stable artificial SEI layers on lithium metal, thereby providing a feasible pathway toward the realization of high-energy-density lithium metal batteries.

Anode-free lithium metal batteries (LMBs) have emerged as a promising next-generation secondary battery technology due to the ultrahigh energy density. However, the practical application is severely limited by irreversible Li plating/stripping behavior and an unstable solid electrolyte interphase (SEI) on the anode. Porous carbon coatings, which combine excellent electronic conductivity with tailorable pore structures, offer a viable approach to regulate Li deposition morphology and interfacial chemistry. Still, the systematic correlation between the structural parameters of carbon materials and cathode electrochemical behavior remains inadequately understood. In this study, porous conductive carbon coatings are constructed on Cu current collectors to systematically investigate the correlations among carbon structural parameters, SEI composition, and electrochemical performance. ECP600, EC300, and Super P with distinct specific surface areas and structural ordering were selected as model materials, and XRD, Raman, BET, and XPS were combined to elucidate how interlayer spacing, graphitization degree, and pore architecture regulate Li deposition modes and the inorganic/organic component ratio of the SEI. The results reveal that Super P, featuring a moderate specific surface area and a high graphitization degree, induces the formation of a thin SEI enriched in LiF/Li2O/Li2CO3, uniform in-pore confined deposition, and stable interfacial impedance, whereas the excessively high specific surface areas of ECP600 and EC300 lead to overly thick or compositionally unstable SEI layers, thereby amplifying polarization. This work proposes a carbon structure-centered interfacial engineering strategy, providing design guidelines for precise SEI regulation in anode-free LMBs.

Lubricant infused surface (LIS) always displays efficient anti-fouling performance. However, the inherent liquid properties of infused lubricants often lead to their rapid depletion in harsh conditions such as water flushing, thereby reducing the antifouling capability of LIS. Herein, we reported a thermal-responsive lubricant infused surface (TLIS) based on composite phase change materials (CPCMs), exhibiting durable and efficient anti-scaling performance. During multicycle scalingdescaling test, the anti-scaling efficiencies of TLIS based on paraffin and vaseline can be increased to 91.4% +/- 0.5% for first cycle and 85.3% +/- 3.3% for sixth cycle. The paraffin acts as solid scaffolds for structural stability while the vaseline acts as liquid lubricants for anti-scaling enhancement. The universality of this surface can be revealed by suppressing various scales (e.g., CaCO3, CaSO4, CaC2O4, and MgCO3) and varying CPCMs types (e.g., n-alkanes, ionic liquids, and fatty acids). Therefore, this study presents a promising strategy that enhances the durability of anti-scaling capability and potentially applys in heat exchange systems.

ABSTRACT Sulfide‐based all‐solid‐state batteries (ASSBs) are regarded as next‐generation energy storage systems due to their high safety and energy density. However, the mechanical stress arising from electrode volume changes during cycling, especially at the anode–electrolyte interface, imposes more severe constraints on cycle life and commercial prospects than cathode‐related volume variations. This review summarizes the recent progress in low‐strain anode materials for sulfide‐based ASSBs. We firstly categorize the design strategies and performance characteristics of several low‐strain systems, including metal–organic frameworks (MOFs), alloy‐based anodes, silicon‐based anodes, and composite anodes, with particular emphasis on interfacial optimization and structural stabilization mechanisms. And then, we address the key challenges in translating material innovations into scalable manufacturing processes. By identifying current research bottlenecks and outlining future directions, this review aims to provide theoretical insight and practical guidance for both fundamental studies and industrial applications of low‐strain anodes in sulfide‐based ASSBs.

The oxygen evolution reaction (OER) in conventional zinc-air batteries (ZABs) involves a complex multielectron transfer process, leading to slow reaction kinetics, high charging voltage, and low energy efficiency. To address these limitations, a zinc-ethanol/air battery (ZEAB) system that strategically replaces the OER with the ethanol oxidation reaction (EOR) possessing a lower thermodynamic potential has been proposed. Herein, a bimetallic catalyst CuCo-embedded nitrogen-doped carbon (CuCo-20%-1), derived from a Cu/Co/Cd co-coordinated metal-organic precursor, is synthesized and exhibits an excellent performance for both EOR and ORR. A series of characterizations and in situ Raman spectroscopy analyses confirmed the formation of high-density M-Nx sites and Cu-doped CoOOH through an in situ electrochemical process from bimetallic CuCo species as the catalytic active sites for the oxygen reduction reaction (ORR) and EOR, respectively. Combined density functional theory calculations elucidated the catalytic reaction pathway and enhancement mechanism of Cu doping in CoOOH for EOR. The ZEAB system exhibits remarkable operational metrics, achieving an energy efficiency of 63.4%, representing a 32.7% energy consumption reduction compared to conventional ZABs. This strategic alternative model from the OER to EOR not only circumvents the fundamental kinetic limitations but also establishes a possible framework for promoting the practical application of next-generation metal-air battery technology.

Five-fold twinned (FFT) noble metal nanocrystals have attracted considerable interest in nanoscience due to their unique structures. This review gives a comprehensive analysis on four common types of FFT noble metal NCs (Au, Ag, Pd, and Pt) synthesized in solution, covering both monometallic structures (e.g., nanodecahedra, nanorods, nanowires, nanobipyramids, and their derivatives) and multimetallic heterostructures, with a brief discussion on FFT Cu nanowires and Rh nanodecahedra. We start with a clear overview of their structural properties, thermodynamic and kinetic stability, and twinning behavior, which is followed by a detailed discussion of key synthetic methods and growth mechanisms driving their development. Next, we provide a summary of their applications. Finally, the review also includes personal insights and identifies future challenges, suggesting potential research directions in this field.

Sulfurized polyacrylonitrile (SPAN) cathodes represent a highly promising category of sulfur-based materials, distinguished by their superior electronic conductivity. Nevertheless, their implementation in all-solid-state lithium-sulfur batteries (ASSLSBs) is hindered by inferior electrochemical performance, primarily arising from the severe exacerbation of inherent electron/ion transport kinetic limitations in conventional micron-sized granular SPAN (GSPAN) microstructures. To circumvent these limitations, a nanofibrous SPAN cathode (FSPAN) is fabricated via electrospinning coupled with programmed pyrolysis. The fabricated 3D-interwoven nanofiber architecture establishes a continuous conductive network, enabling unobstructed transport pathways for efficient charge-carrier migration. This structural design significantly suppresses the interfacial resistance, thereby enhancing the electrode redox kinetics through optimized ion/electron transport dynamics. As a result, the all-solid-state FSPAN cathode demonstrates exceptional electrochemical performance, manifesting a high reversible specific capacity of 1467.2 mAh g-1 at 0.2 C. Notably, the FSPAN cathode delivers a stable discharge capacity of ≈500 mAh g-1 at 2 C, marking a fivefold enhancement over conventional GSPAN cathodes. These findings validate a rational materials design paradigm that significantly enhances the performance metrics of all-solid-state SPAN cathodes via spatially synergistic optimization of charge transport pathways.

Lithium‐sulfur (Li‐S) batteries represent a promising high‐energy‐density secondary battery technology, with a theoretical energy density of 2600 Wh kg −1 . However, its performance is still hindered by the polysulfide (LiPS) shuttle effect, leading to the active material loss and anode electrode interface failure. Herein, a dynamic polysulfide reconstruction strategy is reported employing 5‐fluoroisatonic anhydride (FAIn) in the electrolyte as a reversible regulator that chemically reacts with the dissolved polysulfides, reconstituting them into elemental sulfur and thereby suppressing the polysulfide shuttle effect. During charging, the reaction products (Li‐FAIn) are electrochemically oxidized to regenerate the FAIn regulator, preserving the FAIn additive's dynamic equilibrium in the electrolyte. As a result, our design enables Li‐S pouch cells to retain 726 mAh g −1 after 199 cycles at 0.5 C (80% retention), with Ah‐level cells achieving 100 cycles at this rate. This study presents an efficient dynamic polysulfide reconstruction strategy through FAIn incorporation, providing a novel approach to suppress shuttle effects and enhance battery performance.