Layered double hydroxide (LDH) is a common electrocatalyst for oxygen evolution reaction (OER). However, LDH materials usually undergo a relatively slower reconstruction process, which hinders the efficiency of electrochemical water splitting. Herein we modify pristine NiFe-LDH with Se species-containing FeSe2 to fabricate NiFe-LDH/FeSe2 heterojunction catalyst. At the same time, heterojunction constructing also triggers vacancy formation, which is further proved by electron paramagnetic resonance (EPR) and X-ray absorption spectroscopy (XAS) measurements. In situ Raman spectra and a series of electrochemical experiments have proved the synergistic effect of Se species introduction and vacancy to accelerate the surface reconstruction process of the catalyst, thus greatly enhance OER performance, with a low overpotential of 256 mV under the current density of 10 mA cm-2. This work shed light on ways to design catalysts wither rapid surface reconstruction process and develop catalysts with high efficiency toward electrochemical water splitting.

The accelerating demand for efficient and high-performance energy storage solutions has positioned lithium-ion and sodium-ion batteries at the forefront of technological innovation. While the rapid structural evolution of high-capacity anode materials has historically outpaced electrolyte development, it is increasingly evident that their practical deployment is fundamentally constrained by electrode-electrolyte coupling. This review provides a progressive perspective on the synergistic codesign of advanced anodes and compatible electrolytes. We systematically trace the evolution of anode materials, from carbon-based frameworks to alloy and conversion-based electrodes, highlighting how their distinct physicochemical limitations necessitate tailored electrolyte solutions. Building upon this foundation, lithium and sodium metal anodes are positioned as the central focus to comprehensively showcase advanced electrolyte engineering. Detailed discussions elucidate how tailored liquid and solid-state electrolyte formulations, through solvation regulation and the construction of robust solid electrolyte interphases (SEI), effectively resolve the extreme interfacial bottlenecks of metal anodes. Ultimately, current technological hurdles are outlined, emphasizing that the rational codesign of electrodes and compatible electrolytes remains the definitive pathway for actualizing next-generation high-energy battery systems.

Incorporating light non-metallic elements into compositionally complex alloy (CCA) electrocatalysts can potentially overcome the activity-stability trade-off challenge. However, practical realization of this potential is limited by the lack of a generic method to incorporate multiple types of non-metal into single-phase CCAs. Here we present a facile solvothermal strategy enabling the incorporation of fluorine, boron and nitrogen into the interstitial sites of Pt-based CCAs. Mechanistic investigations unravel three decisive factors for the synthesis: prior formation of Pt clusters catalysing 3d-transition-metal reduction, coordination and activation of non-metal precursors by 3d-transition-metal ions, and rational selection of non-metal-containing functional groups. This methodology yields a library of non-metal-hybridized interstitial CCAs with tuneable compositions. Notably, selected Pt-based CCAs demonstrate exceptional performance as oxygen reduction electrocatalysts for fuel cells, with outstanding activity and durability surpassing state-of-the-art benchmarks. These non-metal-hybridized interstitial CCAs offer a promising platform for tackling demanding electrocatalytic processes involving complex tandem reaction steps.

This study presents a phase-regulation strategy for enhancing the thermoelectric performance of BiSbSe3-based materials through the controlled formation of a semiconductor-semimetal heterostructure. By incorporating sulfur and aluminum dopants, a hexagonal phase is induced within an orthorhombic BiSbSe3 matrix, thereby establishing a bidirectionally adjustable phase composition through compositional regulation. The hexagonal phase exhibits semimetallic behavior, with a Fermi level positioned higher than that of the semiconductor matrix. This electronic structure difference is consistent with low-barrier interfacial charge transfer and a modulation-doping-like redistribution of electrons across the phase boundaries, contributing to enhanced carrier concentration without severely sacrificing carrier mobility. Moreover, the inherently low thermal conductivity of both phases, combined with enhanced phonon scattering at the interfaces and simultaneous control over grain refinement during phase regulation, effectively suppresses the lattice thermal conductivity. The resulting biphasic structure enables coupled regulation of electronic and thermal transport, synergistically improving thermoelectric performance, achieving a peak thermoelectric figure of merit (zT) of 1.50 at 773 K in Bi0.98Sb0.98Al0.04Se2.8S0.2 under the fixed 2 wt % CuI donor-additive condition. This improvement relative to BiSbSe3 materials demonstrates the effectiveness of phase engineering in decoupling electrical and thermal transport properties. These results highlight interface-engineered semiconductor-semimetal heterostructures as an effective design route for high-performance thermoelectric materials.

Morphological control is essential in achieving high performance in polypropylene production, which can be attributed to the morphology replication effect of MgCl2-supported Ziegler-Natta catalysts (ZNCs). Although well-established models, such as the "sea urchin" crystallization theory developed by Chang et al., have successfully elucidated the internal crystallographic orientation, the mechanism of morphological formation of the hierarchical secondary particles still remains unclear. In our study, we use in situ imaging technology to observe the formation of ZNC particles in real-time in a synthesis environment. The following thermally driven crystallization mechanism was revealed in the experiment: liquid-liquid phase separation, initial nucleation and aggregation, crystals growth and solidification. From the SEM analysis, the morphology of the particle is unique botryoidal, or grape-like, and consists of 5 to 30 tightly fused primary units (3-8 µm) that assemble into secondary particles (15-25 µm). The control experiment shows that the invasive in situ probe neither interferes with the formation of the catalyst nor affects the types and distribution of the active sites, which enables us to observe the actual formation process of the catalyst particles. Finally, the propylene polymerization experiment produced polymer particles that perfectly replicated the botryoidal structure of the catalysts, achieving a particle size of 3 mm. The activity and stereoregularity control capabilities of the prepared catalysts are comparable to the commercial catalysts.

Imine-linked two-dimensional covalent organic frameworks (2D COFs) are commonly considered structurally simple materials, yet precise structure determination by X-ray diffraction remains challenging due to the difficulty of obtaining large single crystals. Here, we show that a single-atom change in the aldehyde substituent is sufficient to switch both pore architecture and lattice symmetry in a prototypical 2D COF system. Comparing the widely studied TAPB-DMPDA (COF-OMe) with its -SMe analogue (COF-SMe), we establish a bimodal mesoporous framework for COF-OMe and a unimodal one for COF-SMe through a combination of advanced imaging and diffraction techniques alongside finely sampled gas/vapor physisorption, which resolves two-step capillary processes exclusively in COF-OMe. Electron ptychography reveals previously unrecognized structural features in COF-OMe and enables refinement of its model to propeller-like 1,3,5-tris(4-aminophenyl)benzene nodes with unusually large dihedral angles. Simulated electrostatic potential and X-ray diffraction pattern based on the refined model reproduce the experimental data with high fidelity. COF-SMe undergoes a symmetry reduction from hexagonal to triclinic during kinetic-to-thermodynamic phase evolution, driven by subtle interlayer slippage and intralayer distortion while retaining a single pore type. Together, these results uncover unexpected structural diversity and substituent-governed flexibility in 2D COFs, underscoring the need for state-of-the-art characterization to reassess long-accepted structural models.

Rechargeable zinc-air batteries (RZABs) hold great promise for next-generation energy storage owing to their high energy density and intrinsic safety. However, their large-scale commercialization remains constrained by sluggish oxygen electrocatalysis at the air cathode, where efficient and durable bifunctional oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) catalysts are urgently needed. Here, Co0.85Se nanoparticles and Co single-atom sites are synergistically engineered to overcome the OER/ORR trade-off by dynamically modulating oxygen intermediate adsorption during cycling while simultaneously addressing the efficiency-stability dilemma through mutual optimization between heterogeneous sites. The RZAB assembled with this catalyst achieves energy densities of 914.6 and 807.1 Wh center dot kgZn-1 at discharge rates of 25 and 50 mA center dot cm-2 and a lifetime exceeding 5,500 h at 10 mA center dot cm-2, setting a new benchmark for RZAB performance at high charge/discharge rates. This work pioneers the design of bifunctional electrocatalysts through cross-tuning heterogeneous sites, addressing efficiency and stability challenges in RZABs.

Hydrogen peroxide (H2O2) is an environment-friendly and effective oxidant and has been widely applied. However, medical demand is calling for more effective and convenient H2O2 preparation method. Photocatalysis can effectively produce H2O2 with simple process and easy access catalyst. This article presents a synergistic strategy which combines the advantages of defect engineering and heterojunction to achieve optimal performance. Acetic acid is applied as modulator to introduce linker defect and UiO-67 in-situ grows on surface to build type-II heterojunction. The defect level was quantified with H-1 NMR (nuclear magnetic resonance) and transmission electron microscope convince successful combination. Synergistic effect of defect engineering and heterojunction significantly improves photocatalytic performance and achieves 3.92-fold higher photocatalytic H2O2 evolution rates. Photoelectrochemical characterization indicates defect engineering and type-II heterojunction bring about high photo-absorption, carrier separation, and photoelectron response. This article provides a perspective that synergistic effect of defect engineering and heterojunction can increase photocatalytic performance from overall process.

Modulating charge transfer dynamics across heterojunction interfaces and constructing stable interfacial architectures is key to efficient spatial separation of photogenerated carriers. However, it remains a critical challenge in developing integrated systems for simultaneous pollutant degradation and photocatalytic hydrogen (H2) production. Here, we proposes an interface band structure engineering strategy for constructing a strongly coupled S-scheme heterojunction between polyoxometalate (POM) and ZnIn2S4 (ZIS) with continuous S-O covalent bonds via a one-step hydrothermal synthesis technique. In this process, using the three-dimensional (3D) soluble helical [K(H2O)]6 & sdot;[H2SiW12O40]3 & sdot;nH2O (KSiW) as precursors, a series of x% KSiW/ZIS composites were successfully prepared. The resulting architecture exhibits a hydrangea-like morphology, which effectively combines the respective advantages of POM and ZIS and significantly promotes the separation and transfer of photogenerated charges. The 30% KSiW/ZIS exhibits highly efficient couples photocatalytic degradation of tetracycline hydrochloride (TCH) and H2 production, which demonstrates an integrated synergistic mechanism. Under full-spectrum illumination, it achieves 15.3 mmol g-1 h-1 H2 production and 95.6% TCH degradation, furthermore, in the co-reaction system it maintains 132 mu mol g-1 h-1 H2 generation alongside 89.5% degradation efficiency. The in situ X-ray photoelectron spectroscopy (XPS), irradiated Kelvin probe force microscopy (KPFM) and density functional theory (DFT) calculations confirm the "S-scheme" electron transfer theory in KSiW/ZIS photocatalysts, and high activity reflects the formation of a space charge region and band bending between KSiW and ZIS with consecutive sulfur-oxygen covalent bond, resulting in matched kinetics for hydrogen evolution and oxidation degradation. Such a material demonstrates exceptional cycling stability, reusability and versatility, positioning it as a promising candidate for applications in pollutant degradation and photocatalytic water splitting for hydrogen production.

ABSTRACT Organic electrode materials (OEMs) offer tunable molecular structures and sustainability. To meet the requirements for applications, a high mass‐loading electrode is essential. However, as the mass loading of an electrode increases and the electrode thickens, the electrochemical kinetics significantly deteriorate. Here, we propose an intramolecular hydrogen‐bond strategy that disrupts this seesaw effect, enabling high areal capacity even at high mass‐loadings. Poly(2,3,7,8‐tetraaminophenazine‐1,4,6,9‐tetraone) (PTAPT) was synthesized as a representative material. During discharge, protons as charge carriers diffuse into the material. We use these protons to combine with active sites (C═O/C═N) of PTAPT. This interaction generates secondary intramolecular hydrogen bonds within PTAPT and concurrently forms consecutive proton transport channels. The proton diffusion energy barrier is substantially reduced, facilitating rapid proton conduction along these pathways via the Grotthuss mechanism. Consequently, a proton‐dominated charge transport mechanism occurs in PTAPT, significantly enhancing ion‐transport kinetics in thick electrodes. Furthermore, the extended proton conduction channels increase the degree of structural conjugation, endowing PTAPT with excellent electronic conductivity. A single‐layer pouch cell delivers a maximum discharge capacity of 249 mAh and a significant areal capacity of 5 mAh cm −2 . This work provides a novel strategy to improve the area capacity of OEMs, representing a key step toward their practical application.

Achieving single-atom catalyst with zero-order approximation or homogeneity necessitates precise control over anchoring sites, which imposes a great challenge as abundance and diversity associated coordination environments. A sound strategy towards such a challenge is to anchor a single atom at a specific localization site on the surface of a twin crystal. Therefore, this article aims to anchor single bismuth (Bi) atom at a specific surface of Zn0.5Cd0.5S twins to maximize charge transfer and achieve redox bifunctional reactions. Such a synergistic mechanism was experimentally and theoretically validated through preparation of Zn0.5Cd0.5S compound as model catalyst with twin phase junction (tetragonal and hexagonal) and Bi atoms doped exclusively in tetragonal form. Bi-anchored (1 mol%) Zn0.5Cd0.5S twins exhibit a peak photocatalytic hydrogen productivity of 5680 mu mol g- 1h- 1 and an oxidative dehydrogenation rate of 4420 mu mol g- 1h- 1 for benzyl alcohol. The presence of biphasic junctions within the sample generates a built-in electric field that accelerates the separation and migration of photogenerated charges from tetragonal to hexagonal. Moreover, following the doping of Bi atoms into the tetragonal phase, 5d electrons of Bi couple with electrons of Zn and Cd, magnifying potential differences between the two conduction bands, which enhanced the transfer rate of photogenerated carriers. Density functional theory (DFT) modelling reveals that Bi atoms served as active center for the oxidation reaction, lowering the reaction potential barrier for intermediates. Consequently, we employ an atomic-level selective doping strategy to optimize photocatalytic activity and establish the relevant structure-activity relationships.

Establishing robust atomic-level interfaces, particularly through the selective modulation of surface active sites within heterojunctions to achieve superior solar energy conversion, remains largely unexplored. Herein, sulfur vacancy sites (VS) in ZnIn2S4 (ZIS) are selected, driven by the interaction between unsaturated zinc sites and the nitrogen-rich sites of g-C3N4, forming a step-scheme (S-scheme) heterojunction. The defect-induced interfacial Zn-N-C bonds not only provide rapid channels at the atomic level, thereby lowering the energy barrier for charge transfer, but also selectively tune the highly active pyrrolic N site to enhance H2 evolution. Furthermore, molecular dynamics simulations (MD) combined with density functional theory (DFT) calculations reveal that VS regulates the pyrrolic N sites within the heterojunction, leading to a reduction in the Gibbs free energy for hydrogen production. Kinetic analysis by carrier transport activation energy (CTAE) indicates that the charge transfer energy barrier is accelerated, decreasing from 211.20 eV for ZIS/CN-360 % to 155.71 eV for VS-ZIS/CN-360 %. Consequently, the designed catalyst significantly enhances the H2 yield (27.94 mmol g-1 h-1) in the absence of platinum. This work emphasizes the importance of generating defect-induced interfacial atomic channels, as well as changes in the surface microenvironment, which underscore the significance of defect heterostructures in promoting the photocatalytic process.

The electrocatalytic oxygen evolution reaction(OER),serving as a crucial half-reaction in clean energy technologies such as water splitting and metal-air batteries,plays a significant role in addressing energy crises and solving environmental pollution problems.However,the intricate electron/proton transfer mechanisms and sluggish reaction kinetics of OER result in high overpotentials that significantly limit energy conversion efficiency.The development of highly efficient and stable OER electrocatalysts is therefore urgently required.Metal-organic frame-works(MOFs)have emerged as promising electrocatalysts due to their abundant metal centers,large specific surface areas,and tunable structural configurations.This review systematically summarizes the design strategies for high-performance MOF-based electrocatalysts,while also discussing current challenges and future research directions in this field.

Nickel-cobalt double hydroxide is gaining significant interest due to its high theoretical specific capacitance. However, its tendency to agglomerate and low electrical conductivity present major challenges for its application. This study employed a one-step hydrothermal method to integrate exfoliated few-layer MXene materials with NiCo-LDH, facilitating the uniform vertical growth of NiCo-LDH nanosheets on the surface of the MXene, effectively minimizing agglomeration. Additionally, the interfacial synergy between MXene and NiCo-LDH enhances the transfer of electrons from NiCo-LDH to MXene, resulting in an electron-rich MXene and an oxygen vacancy-rich NiCo-LDH. Together, these characteristics significantly improve the electrochemical performance of the material at high current densities, achieving 7776 W kg-1 and 66.96 W h kg-1 at 15 A g-1. After cycling 40 000 times, it retains an impressive capacity retention rate of 89.5%. These findings demonstrate that MXene materials effectively tackle the main challenges associated with NiCo-LDH, opening new possibilities for their application in electrode materials.

Diabetic wounds present significant treatment challenges due to their complex microenvironment, marked by persistent inflammation from bacterial infections, hypoxia caused by diabetic microangiopathy, and biofilm colonization. Sonodynamic therapy (SDT) offers potential for treating such wounds by targeting deep tissues with antibacterial effects, but its efficacy is limited by hypoxic conditions and biofilm barriers. To overcome these obstacles, we developed a novel approach using oxygen-carrying microbubbles loaded with Mn2+-doped carbon dots (MnCDs@O2MBs) to enhance SDT and disrupt biofilms. Through precursor screening and design, MnCDs are engineered to exhibit tailored properties of sonodynamic activity and enzyme-like catalytic capabilities. This system provides a dual oxygen supply for amplifying the SDT effects: MnCDs, serving as a sonosensitizer, also chemically convert excess H2O2 at infection sites into oxygen, while the O2MBs physically release oxygen through ultrasound-induced cavitation. The cavitation effect also disrupts biofilms, improving the delivery of sonosensitizers and boosting SDT efficacy. In a diabetic wound model, this strategy downregulated TLR, NF-κB, and TNF inflammatory pathways, reduced pro-inflammatory factor secretion, promoted angiogenesis, and accelerated wound healing, thereby acting as a promising treatment approach for diabetic wound healing.

The complex coupling between thermoelectric parameters makes it extremely challenging to improve the performance of materials. Typically, the reduction of thermal conductivity by incorporating porous structures often leads to a compromise in electrical conductivity. Herein, we present high-ion-conductive zeolite X (including Na-, Ca-, and Li-low silica type-X (LSX)) as the subnanoporous additive in the Bi0.4Sb1.6Te3 (BST) matrix. Owing to the high pore charge density of zeolite X, the decrease in conductivity is effectively suppressed while maintaining a low thermal conductivity. Positively charged metal cation (M+) and valence electron of oxygen atom in aluminum-oxide tetrahedron of zeolite X achieve charge balance. Cationic with different electronegativity regulated electrons of oxygen atom transferred from the oxygen atoms to the BST matrix. The lower electronegativity of Na+ leads to a higher electron density surrounding oxygen atoms in Na-LSX. Thus, more electrons are transferred to the BST matrix from the oxygen atoms in Na-LSX and form Teu2013O bonds. Ultimately, the figure-of-merit (ZT) peak of BST/0.8 wt.% Na-LSX nanocomposites reached 1.47 at 373 K, with a huge cooling temperature difference of 69.4 K and an excellent thermoelectric conversion efficiency of 6.95%. This work exploits the stable and unique three-dimensional pore structure of X-type molecular sieves, broadening their potential application in the thermoelectric medium temperature range.

Electrochemical CO2 reduction reaction (eCO(2)RR) offers a sustainable route to convert greenhouse gases into value-added chemicals. Bismuth (Bi) has emerged as a promising electrocatalyst for CO2-to-HCOOH conversion due to its low cost, nontoxicity, and favorable adsorption properties for the key *OCHO intermediate. However, its relatively contracted 5d and expanded 6p orbitals lead to inevitable thermodynamically driven structural reconstruction during eCO(2)RR, resulting in a persistent trade-off between activity and stability. Here, by tuning the balance between the electrochemical and thermodynamic steady states of layered Bi species leveraging interlayer interactions and spatial confinement provided by a two-dimensional covalent organic framework (COF), we achieve the selective exposure and stable maintenance of the highly active, metastable Bi (101) facet during eCO(2)RR for the first time. The resulting catalyst achieves top-tier performance with 98.7 +/- 0.1% HCOOH selectivity, exceptional stability over 230 h, and a flow cell HCOOH partial current density exceeding 350 mA cm(-2) at -1.0 V versus RHE, ranking it among the most efficient and stable electrocatalysts reported to date.

Resistance to SO2 poisoning is a major technical challenge faced by catalysts in VOC oxidation. In this study, we prepared a series of nanotubular perovskite-based catalysts using electrostatic spinning technique. The catalytic activity of the prepared LaCoO3 (LCO) catalyst could be significantly enhanced by doping with a small amount of Ce. Furthermore, acid treatment significantly enhanced the adsorption of VOC molecules on the catalyst surface, thus leading to the exposure of more Co3+ on the catalyst surface. Owing to the protective effects of CeO2 and Co3O4, the acid etched Ce-doped LaCoO3 catalyst exhibited outstanding catalytic performance towards toluene, even in the presence of water vapor and SO2. The reason was that Ce addition increased the content of Co3+ and active oxygen species, and the acid treatment led to a further increase in the exposed Co3+ species on the catalyst surface. Meanwhile, Ce acted as a sacrificial site to protect Co3+ from being poisoned by SO2. The synergistic effect of Ce doping and acid etching significantly improved the catalyst's resistance to SO2. In situ FTIR confirmed that toluene primarily underwent a synergistic interaction of MvK and L-H mechanisms over the LCCO-2 catalyst. The possible reaction pathway is as follows: gaseous toluene -> adsorbed toluene -> benzyl alcohol -> benzaldehyde -> benzoate -> anhydride -> CO2 and H2O. Thus, this work provides innovative ideas for designing VOC catalytic combustion catalysts with excellent SO2 resistance in the future.

Understanding the atomic and electronic structures of monocomponent materials with local defects is crucial for uncovering the origins of 'self-activated' redox dual-sites and ultimately establishing structure-property relationships. Therefore, a series of inert monocomponent materials, including ZnIn2S4, TiO2, and Zn0.5Cd0.5S are employed as proof-of-concept models, with a particular focus on ZnIn2S4. Zinc vacancies (V-Zn) in mono-component ZnIn2S4 disrupt the symmetry of the atomic arrangement and influence the local electronic structure of the surface. Theoretical calculations and experiments suggest that VZnacts as an oxidation reaction center rich in photoexcited holes, while sulfur (S) atoms serve as reduction reaction centers abundant in photogenerated electrons. The introduction of VZn transforms the formation of the key intermediate center dot CH(OH)Ph from endothermic to spontaneous exothermic while creating spatially separated redox sites. This dual effect enhances photogenerated charge separation and reduces energy barriers for both O2activation and center dot CH(OH)Ph formation, leading to exceptional production rates of 7440 mu mol g(-1) h(-1) (H2O2) and 6480 mu mol g(-1) h(-1) (benzaldehyde) with excellent stability. This work successfully demonstrates defect-induced self-activated redox dual-sites in a monocomponent photocatalyst, providing new insights for designing multifunctional photocatalysts.