The electronic transport characteristics of two-dimensional (2D) systems have widespread application prospects in the fabrication of multifunctional nanodevices. However, the current research for basic transport phenomena, such as anomalous valley Hall effect (AVHE) and piezoelectric response, is limited to discrete discussion. Here, we theoretically propose a valley-piezoelectricity coupling strategy beyond the existing paradigm to realize AVHE and layer Hall effect (LHE) in ferrovalley (FV) systems, and its essential principle can be extended to general valleytronic materials. Through first-principles calculations, we demonstrate that the large polarized electric field of 2.8×10 6 (1.67×10 7 ) V/m can be induced by 0.1% uniaxial strain in FV 2 H -LaHF (1 T -LaHF) monolayers. In addition, the microscopic mechanism of interlayer antiferromagnetic (AFM) state of 2 H -LaHF bilayer is uncovered by the spin Hamiltonian and super-superexchange (SSE) interaction. Our findings pave the way for new explorations of valley Hall-related effect involving piezoelectricity.

Polarons play a crucial role in determining the (photo)electrocatalytic activity of semiconductors. Traditionally, polarons are introduced ex situ and irreversibly during catalyst synthesis, but herein we present a fundamentally different approach of introducing polarons in situ in a reversible manner using the external electrode potential. We study the potential-dependent polaron formation and its impact on electrocatalysis on a prototypical TiO2 semiconductor electrode for the acidic hydrogen evolution reaction. By combining grand canonical ensemble density functional theory calculations with (in situ spectro) electrochemical experiments, we demonstrate notable changes in TiO2´s electronic structure driven by the reduction of Ti4+ to Ti3+ surface polarons at reducing potentials. Our results show that potential-dependent polaron formation creates highly active sites for the hydrogen evolution reaction, breaks down the linear relationship between adsorption energy and electrode potential, and leads to complex electrochemical reaction kinetics. We discuss how the in situ polaron generation can be leveraged in improving semiconductor (photo)electrodes. Overall, our findings provide compelling evidence and an atomistic understanding of potential-dependent polaron formation in semiconductor (photo)electrocatalysis. Polarons play a crucial role in determining the (photo)electrocatalytic activity of semiconductors. Here, the authors report a reversible, potential-driven method to generate Ti³⁺ polarons on TiO₂, creating dynamic active sites that break the adsorption-potential linearity and boost hydrogen evolution.

The interplay between displacement defects governs the evolution of irradiation damage in materials and is of great fundamental interests with important practical implications, from microelectronics industry to advanced nuclear system. Hydrogen, a ubiquitous impurity, is known to segregate to vacancies, but its role in altering vacancy-interstitial recombination-the key process underlying defect annihilation-has not been established. Here, using tungsten as a model system, we show that hydrogen adsorption on the inner surfaces of vacancy clusters significantly suppresses recombination with self-interstitial atoms, thereby inhibiting defect annihilation. We identify a stress-mediated mechanism in which hydrogen adsorption transforms the local stress field of vacancy clusters, weakening their long-range attraction to self-interstitial atoms. Based on this mechanism, we develop a predictive model that quantitatively relates the relative reduction of recombination radius to the hydrogen inner surface density, independent of cluster size. By integrating atomistic parametrization with multiscale simulations, we investigate the co-evolution of hydrogen and displacement defects, which show quantitative agreement with recent experiments, including the hydrogen isotope retention, distribution and desorption. Our results establish a direct link between impurity-defect interactions and defect-defect recombination, providing a physically grounded framework for understanding and controlling irradiation damage in structural materials.

ZUSAMMENFASSUNG Die Methanolzersetzung ist eine Modellreaktion zum Verständnis oberflächenvermittelter Redoxchemie und photokatalytischer Prozesse an Oxidmaterialien. Während ihr Mechanismus auf TiO 2 unter Ultrahochvakuum‐Bedingungen (UHV) umfassend untersucht wurde, ist der Reaktionsweg unter Umgebungsbedingungen in der Flüssigphase noch weitgehend unerforscht. Hier untersuchen wir die photokatalytische Zersetzung von Methanol auf Rutil‐TiO 2 (110) nach direkter Adsorption aus flüssiger Lösung, indem wir oberflächenempfindliche Summenfrequenzspektroskopie (SFG) mit Rechnungen auf Grundlage der Dichtefunktionaltheorie (DFT) kombinieren. SFG‐Messungen identifizieren Methoxy als die dominierende Oberflächenspezies unter diesen Bedingungen. DFT‐Rechnungen zeigen, dass kooperative Wasserstoffbrückenwechselwirkungen sowohl den Übergangszustand als auch die dissoziierte Konfiguration stabilisieren, was zu einer systematischen Verringerung der Aktivierungsbarrieren führt. Gleichzeitig erleichtert eine lokalisierte Überschussladung durch ihre dynamische Umverteilung entlang der Reaktionskoordinate den Protonentransfer, wodurch die Barriere für die O─H‐Bindungsspaltung gesenkt wird und Reaktionszwischenprodukte stabilisiert werden. Unter resonanter Bandlückenanregung reorientiert sich Methoxy zunächst und wird anschließend oxidiert unter Bildung einer stabilen Hydroxymethylspezies an der Oberfläche. DFT‐Rechnungen zeigen darüber hinaus, dass Grenzflächenwasser und Hydroxylgruppen lokalisierte Ladungsträger stabilisieren, Aktivierungsbarrieren verringern und den protonengekoppelten Elektronentransfer fördern. Diese Ergebnisse illustrieren auf molekularer Ebene, wie die Grenzflächenhydratisierung photokatalytische Reaktionswege an Oxid–Flüssigkeits‐Grenzflächen steuert.

Protecting sensitive equipment from electromagnetic radiation damage requires the development of high-performance electromagnetic interference shielding films. As the film thickness is reduced to micro/nano scales, electromagnetic interference shielding capability generally decreases rapidly due to the weaker reflection. As a result, enhanced electromagnetic interference shielding performance in sub-μm thin films remains as an unsolved challenge. Inspired by the naturally wrinkling of fruit skin, we propose a homogeneous strain strategy to achieve self-wrinkling-induced lattice-structured MXene by uniform polymer shrinkage due to dehydration. Uniform wrinkle amplitude can be tuned from 0.8 to 6 μm, which results in additional surface scattering of electromagnetic-waves and electrical conduction paths. The obtained lattice-structured films demonstrate an excellent electromagnetic interference shielding of up to 81.5 dB for a thickness of 17 μm, maintaining high electromagnetic interference shielding performance and stability after enduring various harsh testing conditions. These results demonstrate the potential of wrinkling-induced, surface regular patterns for improving the electromagnetic interference shielding performance of ultra-thin films based on conventional materials. This study reports self-wrinkling MXene films with lattice structures achieving exceptional electromagnetic interference shielding (81.5 dB at 17 μm), offering ultra-thin protection for sensitive electronics.

The catalytic properties of Fe-doped bilayer NiOOH were studied. Bilayer NiOOH exhibits a lower OER overpotential than its monolayer. Besides, Fe-doped bilayer NiOOH can further reduce the OER overpotential to 0.24 V. The upward shift in Ni-3d spin-up orbitals reduces the adsorption energy of intermediates and enhances the OER catalytic activity.

Molecular regulation of the gas-liquid-solid interface is challenging but essential for steering CO2 electroreduction on Cu toward multi-carbon products (C2+). In particular, C-C coupling pathways require a delicate balance among CO2 delivery, interfacial water activity, proton availability, and *CO coverage. Despite advances in catalyst and electrode engineering, how interfacial water affects CO2 access and *CO retention on Cu, thereby steering C-C coupling and hydrogenation over hydrogen evolution, remains insufficiently understood. Here, we report a physically retained perfluorohexane-modified Cu catalyst that constructs a fluorocarbon-rich hydrophobic microenvironment for selective CO2 electroreduction to C2+. Molecular dynamics simulations reveal that the C6F14-rich interface suppresses near-surface water density and weakens the interfacial hydrogen-bond network, while increasing local CO2 accessibility within the electric double layer. Density functional theory calculations show that the fluorocarbon modifier does not substantially shift the Cu d-band center, form obvious Cu-F bonding, or directly activate CO2, excluding an intrinsic electronic-structure modulation mechanism. Structural and surface analyses confirm that C6F14 is enriched as organic fluorocarbon species without inducing Cu phase transformation. The optimized Cu-C6F14 interface (Cu-F-20) increases the C2+ Faradaic efficiency to about 73.9% and maintains stable operation over 10.5h. Operando Raman spectroscopy reveals intensified Cu-CO vibrations, enhanced LFB-*CO signals, and stronger *CH2CHO features, linking the fluorocarbon microenvironment to increased *CO signal intensity and promoted C-C coupling. This work provides a microenvironment-oriented approach for understanding and regulating multiphase electrochemical reactions, offering insights into interfacial engineering beyond conventional catalyst electronic-structure modulation.

Conventional ionic ferroelectrics enable exciton control through switchable polarization but face challenges like high switching barriers and fatigue. Sliding ferroelectricity in van der Waals structures is capable of addressing these limitations with low energy consumption and excellent endurance, presenting a promising platform for excitonic applications. In this work, we construct a Janus bilayer MoSeTe and investigate its exciton-related optoelectronic properties using the GW-Bethe-Salpeter equation method. Along the AB-BA sliding path, the system exhibits low energy barriers (3.56 meV/atom) and high polarization (1.147 pC/m), accompanied by an exchange between layers in their contributions to the valence band maximum and conduction band minimum. This leads to a transition of the first bright excitonic state from the sliding layer to the fixed layer. Notably, because of band degeneracy and hybridization, the nonpolar state that emerge during the sliding process exhibits enhanced and localized excitonic absorption as well as interlayer exciton components, which are absent in both AB and BA stackings. This work highlights the considerable potential of sliding ferroelectricity in modulating exciton dynamics and provides a theoretical basis for the design of low-power, high-performance optoelectronic devices.

The precise regulation of Cu surface electronic structure governs C-C coupling pathways and intermediate adsorption to enhance ethylene selectivity. However, how heteroatom dopants modulate the flux of oxygen-bound intermediates remains unclear. Herein, we establish a predictive framework based on six dopant elements' electron orbital characteristics, demonstrating that p-orbital metal doping enables favorable orbital-center proximity for hybridization with Cu active centers. Al-incorporated Cu balances adsorption affinities for *CO, *H, and *O, thereby reducing the *OCCO formation barrier. Controlled Al doping in CuAl single-atom alloy (CuAlSA) induces lattice expansion and d-band center downshifting (ΔεCu = -2.94 eV), achieving favorable d-p orbital proximity (δd, p = -1.00 eV) and a low C-C coupling energy barrier (ΔE = 0.30 eV). In situ Raman spectroscopy confirms that the optimized d-p proximity promotes C-C bond formation and *OCCO hydrogenation to *CH2CHO, redirecting intermediate flux from methane toward ethylene. CuAlSA consequently exhibits 78.8% ethylene Faraday efficiency under pure CO2 and retains 70.2% under 15% CO2. This work establishes a strategy for directing oxygen-bound intermediates in CO2-to-C2H4 electrosynthesis.

Methanol decomposition is a benchmark reaction for understanding surface-mediated redox chemistry and photocatalytic processes on oxide materials. While its mechanism on TiO2 has been extensively studied under ultra-high-vacuum (UHV) conditions, the reaction pathway under ambient, liquid-phase environments remains largely unexplored. Here, we investigate the photocatalytic decomposition of methanol on rutile TiO2(110) following direct adsorption from liquid solution by combining surface-sensitive sum frequency generation (SFG) spectroscopy with density functional theory (DFT) calculations. SFG measurements identify methoxy as the dominant surface species under these conditions. DFT calculations reveal that cooperative hydrogen-bonding interactions stabilize both the transition state and the dissociated configuration, leading to a systematic reduction in activation barriers. Concurrently, localized excess charge facilitates proton transfer through dynamic redistribution along the reaction coordinate, thereby lowering the barrier for O─H bond cleavage and stabilizing reaction intermediates. Under resonant bandgap excitation, methoxy undergoes structural reorientation followed by oxidation to form a stable surface hydroxymethyl species. DFT calculations further demonstrate that interfacial water and hydroxyl groups stabilize localized charge carriers, reduce activation barriers, and promote proton-coupled electron transfer. These findings provide molecular-level insight into the role of interfacial hydration in governing photocatalytic reaction pathways at oxide-liquid interfaces.

Bisphenol A (BPA) poses significant risks to human health and ecosystems due to its severe adverse effects. Consequently, effective BPA removal from water sources is imperative. While naturally occurring laccase (Lac) can degrade BPA, its widespread use is limited by high costs and instability. Nanozymes, with their superior catalytic activity and robust properties, offer a viable alternative. Herein, we synthesized a novel layered nanozyme by incorporating rare-earth metals (La, Gd, Dy, Er) with copper. The La-based material demonstrated the highest laccase-like activity. Comparative analyses revealed that La-based material with optimized composition exhibits significantly enhanced and more stable enzymatic activity toward BPA than natural laccase under varying conditions. Under optimized degradation parameters, the La-based material achieved nearly 90% BPA degradation within 20 min. This study provides an efficient and scalable strategy for BPA removal, demonstrating strong potential for practical environmental remediation.

Nickel-iron (Ni-Fe) hydroxides are considered efficient electrocatalysts for the oxygen evolution reaction (OER) under alkaline conditions. However, studies have focused extensively on the catalytic sites, with fewer investigations into the oxidation state of the metal ion and its impact on the OER, which is related to the hydrogen sites. Herein, the distribution of hydrogen over the metal ions is thoroughly explored to reveal the intrinsic relationship between the electronic structure and reactivity by virtue of first-principles calculations. The results demonstrate that the hydrogen arrangement induces valence states for Ni, and the change in the defined hydrogen arrangement energy correlates with the Gibbs free energy change in the intermediate. Simultaneously, an inverse linear scaling relationship between the hydrogen arrangement energy and the d-band center of the metal atoms in intermediates for nickel and iron was discovered. This shows the different modulating effects of hydrogen on the d-band centers of nickel and iron atoms. These findings explain the different reactive properties of nickel and iron and are also relevant for optimizing the catalyst by regulating the d-band center for the OER.

Electric fields are powerful tools for boosting the intrinsic polarization intensity of materials by precisely regulating their charge distribution. However, conventional strategies predominantly rely on the macroscopic design of heterostructures or composite systems to construct built-in electric fields, aiming to optimize polarization response. Although such approaches yield additional interfacial polarization, they obscure the intrinsic regulatory mechanism of external electric fields on material properties. Therefore, the core challenge is to develop a new electric field regulation paradigm that directly targets the intrinsic polarization. Herein, we propose a curvature-induced polarization amplification strategy. By utilizing hollow carbon spheres with tunable curvatures, Polarization is triggered under electromagnetic (EM) field excitation, forming localized surface electric fields that disrupt the symmetric electron cloud distribution of single-atom sites as ideal polarization units. This strategy establishes a curvature-driven control paradigm for high-efficiency EM wave absorbers. Geometrically induced surface electric fields remarkably enhance the inherent dipole moments of single atoms, thereby boosting their EM polarization loss capability. The optimized material demonstrates exceptional broadband EM wave absorption, with a loss efficiency exceeding 99.9%. This approach provides unprecedented design freedom for EM response materials, showing broad application prospects in fields such as EM compatibility and terahertz communication.

Rechargeable Li-CO 2 batteries offer great potential for greenhouse gas utilize and high-energy-density storage. However, their practical application is hindered by the formation of thermodynamically stable Li 2 CO 3 product that is hard to decompose during charging. Highly crystalline and conductive reticular material iron-polyphthalocyanine (pFe ‖ Pc) as solid-phase redox mediator into Li-CO 2 batteries tailors the cathode reaction pathway, enabling stable Li 2 C 2 O 4 generation and an extraordinary discharge plateau of 3.2 V beyond the theoretical limit. Beyond delivering an ultrahigh discharge capacity of 28790 mAh g -1 and reversible cyclability over 1400 hours (1000 mAh g -1 cut-off capacity) at 100 mA g -1 , the Li-CO 2 batteries exhibit excellent temperature adaptability (-40 to 80°C). The Li-CO 2 pouch cells employing pFe‖Pc as solid-phase redox mediator achieve a high energy density of 678 Wh kg -1 based on total device mass and maintain reversible cycling for 251 hours. Our work pioneers a promising pathway toward practical high-efficiency Li-CO 2 batteries.

ABSTRACT Spent graphite (SG) from end‐of‐life lithium‐ion batteries suffers from persistent structural disorder, yet the defect chemistry governing its regeneration remains poorly understood. Here, we identify carbon vacancies and quasi‐sp 3 topological defects as the dominant degradation motifs and leverage this insight to devise a defect‐targeted regeneration strategy. Under electrothermal coupling enabled by flash Joule heating in a CoCl 2 molten‐salt medium, cobalt species are selectively directed to defect sites, where strong Co‐defect interactions reduce the energy barrier for topological reconstruction. The resulting Co‐induced charge redistribution activates quasi‐sp 3 ‐carbon via population of π * antibonding states, while thermally assisted and field‐directed carbon migration promotes its conversion into a more ordered sp 2 ‐rich lattice. Concurrently, residual interphases and impurities are eliminated, lattice stress is relieved, and the cobalt catalyst is efficiently recovered. The regenerated graphite (RG) delivers a capacity of 257 mAh g −1 after 1000 cycles at 1 A g −1 , corresponding to 83% retention relative to the post‐activation capacity, and outperforms commercial graphite under identical conditions. This work establishes a chemically informed route for the rapid upcycling of SG through defect‐selective topological repair.

Although electrochemical nitrogen fixation emerges as a sustainable pathway to revolutionize the nitrogen cycle using renewable electricity, the overwhelming dominance of the hydrogen evolution reaction over N 2 activation in aqueous systems imposes fundamental limitations on simultaneously achieving high production rates and Faradaic efficiency. Inspired by Le Chatelier's principle, in this work, an appropriate pressure field was innovatively coupled with electrochemical reduction into the N 2 ‐CO 2 co‐fed urea synthesis system, achieving concurrently suppression of gaseous byproducts of CO/H 2 and enhancement of C–N coupling. Atomically dispersed amorphous Bi x Ni 1‐ x O y clusters were engineered as tandem catalyst, the pressure‐driven in situ electronic modulation of the liquid‐immersed catalyst—originating from increased surface coverage—is for the first time confirmed: Bi sites exhibit a progressive increase in oxidation state, while Ni centers undergo gradual reduction. The rational atomic‐scale integration of multimetallic active centers and system engineering principles for interfacial microenvironment modulation via moderate pressurization achieved breakthrough performance with a high urea production rate of 8.71 mmol h −1 g −1 cat , coupled with remarkable 50% nitrogen fixation efficiency, pointing to one of the best catalysts in aqueous systems among those reported so far. By integrating pressure engineering with atomic‐scale catalyst design, this work provides a guiding paradigm for gas‐involved electrochemical reactions.

Ferroelectrics hold significant promise for a wide range of applications owing to their spontaneous polarization characteristics. Despite exhibiting multiple polarization mechanisms that demonstrate significant potential for electromagnetic functional materials, the practical deployment of ferroelectric polymers has been inhibited by the lack of precise control over polymer chains at the atomic scale and the relatively low stability of the polar phase. Here, a procedure of fortifying the ferroelectric polyvinylidene fluoride phase is proposed by the facet modulation, achieving stable ferroelectric polymer through engineering the interaction between the inorganic rigid crystal facets and organic flexible molecular chains at the atomic scale. The constructed polar ferroelectric polymers composite systems exhibit a broad distribution of relaxation times along with multi-polarization characteristics from megahertz to terahertz frequencies. The composite system mitigates the apparent loss-bandwidth trade-off, thereby achieving broadband polarization properties across multiple frequency bands while maintaining a dissipation efficiency above 99.9%. The demonstrated approach presents a breakthrough in achieving the stable ferroelectric polymers through facet-induced stabilization, providing deep insights for the development of high-performance electromagnetic functional materials.

Ferrovalley (FV) materials have attracted much attention due to their unique spin-valley coupled properties. In this work, we predict FV single-layer TiClAsH, which has 77 meV of intrinsic valley polarization. The electronic correlation effect can drive the topological phase transition from the FV state to the quantum anomalous Hall state, and its critical half-valley metallic phase can achieve complete spin polarization. By breaking the mirror symmetry of bilayer TiClAsH, the layer-locked Berry curvature distribution is achieved, and furthermore, the layer-polarized anomalous Hall effect (LPAHE) is induced. Meanwhile, reversible LPAHE switching can be achieved through sliding control of ferroelectricity. Our findings offer a good material platform to manipulate the spin splitting, valley polarization, ferroelectricity, and topological states for multi-functional device applications.

Although electrochemical nitrogen fixation emerges as a sustainable pathway to revolutionize the nitrogen cycle using renewable electricity, the overwhelming dominance of the hydrogen evolution reaction over N2 activation in aqueous systems imposes fundamental limitations on simultaneously achieving high production rates and Faradaic efficiency. Inspired by Le Chatelier's principle, in this work, an appropriate pressure field was innovatively coupled with electrochemical reduction into the N2-CO2 co-fed urea synthesis system, achieving concurrently suppression of gaseous byproducts of CO/H2 and enhancement of C-N coupling. Atomically dispersed amorphous BixNi1- xOy clusters were engineered as tandem catalyst, the pressure-driven in situ electronic modulation of the liquid-immersed catalyst-originating from increased surface coverage-is for the first time confirmed: Bi sites exhibit a progressive increase in oxidation state, while Ni centers undergo gradual reduction. The rational atomic-scale integration of multimetallic active centers and system engineering principles for interfacial microenvironment modulation via moderate pressurization achieved breakthrough performance with a high urea production rate of 8.71 mmol h-1 g-1 cat, coupled with remarkable 50% nitrogen fixation efficiency, pointing to one of the best catalysts in aqueous systems among those reported so far. By integrating pressure engineering with atomic-scale catalyst design, this work provides a guiding paradigm for gas-involved electrochemical reactions.