Low-temperature protonic ceramic fuel cells (LT-PCFCs) are promising for the hydrogen economy but are fundamentally limited by sluggish ion transport in reducible oxides, arising from defect-induced localized electronic states that act as electrostatic scattering centers. Herein, we propose and demonstrate an electronic state passivation (ESP) strategy, validated by uniformly rare-earth (RE)-passivated ceria-based oxides synthesized via the sol-gel method, compared with defective CeO2−δ. Combined density functional theory (DFT) calculations and electron paramagnetic resonance (EPR) spectroscopy results find that defect-associated electrons localized at Ce3+ sites generate gap states, acting as electrostatic scattering centers that impede ion transport. The substitution of RE3+ passivates these defect states via charge compensation, which is verified by X-ray photoelectron spectroscopy (XPS) and theoretical calculations, effectively removing gap states as directly observed by EPR spectroscopy and DFT calculations, thus revealing an obvious passivation effect. RE3+ passivation allows calculated ion migration energy barriers to reduce from 1.3 to ∼0.5 eV. Electrochemically, the peak power density of the fuel cell increases from 510 mW cm−2 (CeO2−δ) to 1100 mW cm−2 (La0.1Ce0.9O2−δ), with ionic conductivity enhanced to 0.49 S cm−1 at 520 °C, consistent with the theoretical results. This work establishes ESP as a general design principle for regulating defect-induced electronic states in reducible oxide electrolytes.

Abstract Efficient and broadband circularly polarized light (CPL) detection remains challenging for integrated InGaAs photodetectors, which typically rely on external polarization components. In addition, most reported chiral metasurfaces suffer from limited bandwidth and weak chiroptical response. Here, we propose a two-dimensional all-dielectric chiral metasurface with a lightning-shaped geometry, designed for monolithic integration with an InGaAs absorption layer to enable intrinsic CPL discrimination. The underlying mechanism is attributed to the hybridization of symmetry-broken electric dipole modes and Fabry–Pérot cavity resonances supported by the air gaps between adjacent silicon trapezoids, leading to enhanced spin-selective light–matter interaction. Numerical results demonstrate an average circular dichroism of 0.8 (maximum 0.93) and a high transmittance of 97% over the wavelength range of 1.76–1.99 μ m, corresponding to a bandwidth of 230 nm. Compared with previously reported designs, the proposed structure achieves simultaneous improvements in bandwidth, transmission efficiency, and chiroptical contrast without increasing structural complexity. These results provide a viable route for compact, high-performance CPL-sensitive photodetectors.

During the oxygen evolution reaction (OER), reconstruction of transition metal sulfides (TMSs) is inevitable. However, the lack of a clear theoretical understanding of this process has impeded the development of effective reconstruction regulation strategies. In this study, we first explored the reconstruction mechanism of CoS2 during OER from the perspective of electronic structure and identified two possible pathways: the OH-assisted mechanism and the O-assisted mechanism. Further verification showed that these mechanisms are universally applicable to other TMSs (e.g., FeS2). Based on the reconstruction mechanism, we investigated the basic reasons for the influence of various regulation strategies, such as vacancy modification and facet engineering, on the reconstruction ability. This verified that the method of analyzing the change in the reconstruction ability of catalysts based on the reconstruction mechanism has a high degree of applicability. Importantly, we proposed a core regulation strategy: the coordination symmetry regulation strategy. Specifically, by breaking the symmetry of the surface coordination environment of TMSs (such as introducing heteroatom doping or strain), the reconstruction process will be facilitated. Our findings provide a comprehensive mechanistic explanation for the reconstruction of TMS catalysts and offer a new idea for the rational design of OER catalysts with controllable reconstruction capacity.

Malodorous sulfur-containing volatile organic compounds (SVOCs) pose severe environmental and health risks, while existing physical or chemical abatement technologies suffer from low efficiency and poor economic viability. Herein, a low concentration ozone-assisted swelling-fixation of SVOCs (OSS) strategy is proposed using YMn2O5 mullite as a sulfur-fixing material, with CH3SH as a model pollutant. A sulfur fixation capacity of 1344.2 wt % (13.4× the YMO mass) is achieved and validated in a prototype device. Combined experimental characterizations and theoretical simulations reveal that ozone-derived reactive oxygen species synergize with Mn-Mn dimers, enable the thermodynamically and kinetically favorable conversion of CH3SH into liquid CH3SO2SCH3 and solid Mn(CH3SO3)2/SO42- products. The accumulation of these products builds a swollen surface layer on YMn2O5 that remains reactive toward CH3SH/O3 and allows continued sulfur fixation. Life-cycle assessment reveals a favorable trend in reducing carbon emissions, pollutant emissions, and eco-costs compared with conventional adsorption and oxidation routes. This room-temperature strategy enables scalable and sustainable SVOCs abatement, odor control, and sulfur resource fixation.

Metal-nitrogen-carbon single-atom catalysts (M-N-C SACs) exhibit promising activity for ozone (O-3) decomposition under ambient conditions. However, theoretical studies often predict high barriers, revealing a gap between experimental and computational results. To address this, a dual-side synergistic mechanism (DSM) is proposed and investigated on metal atom embedded in N-4-doped carbon (M- N4C) SACs (M = Cr, Mn, Fe, Co, Ni, Cu, Zn) using density functional theory calculations. O-3 decomposition via the conventional single-side Eley-Rideal (E-R) mechanism exhibits high reaction barriers (>0.77 eV). Instead, the DSM, in which axially adsorbed intermediates on one side to facilitate O-3 decomposition on the other, shows a much lower energy barrier (<0.26 eV). Axially adsorbed intermediates modulate the orbital interaction between O-2 and the metal center by reducing the z-component density of states of metal d orbitals near the Fermi level, thereby weakening O-2 binding. This modulation is crucial for efficient O-3 decomposition at room temperature. Among the candidates, Cr-N4C exhibits the lowest reaction barrier (0.14 eV) and superior water resistance due to stronger O-3 adsorption over H2O. These findings provide mechanistic insight into ambient-temperature O-3 decomposition and offer design principles for developing efficient and moisture-tolerant SAC catalysts for environmental remediation.

Ground-level ozone (O3), a ubiquitous tropospheric pollutant, requiring its efficient removal via zero-energy-consumption methods. However, catalytic decomposition of ozone at room temperature under high humidity remains a great challenge due to water poisoning of active sites. Herein, cobalt-based hexagonal perovskites Sr6Co5O15, with and without Mn doping, are proposed as hydrophobic n-type semiconductors for O3 decomposition. Sr6Co5O15 undergoes an in-situ phase transformation under humid O3 exposure, forming an active hexagonal SrCoO3 phase, enhancing O3 conversion from 31.8 % to 54.6 % at relative humidity RH = 90 %. Further Mn doping forms a SrMnO3/Mn-Sr6Co5O15 heterojunction, achieving 100 % O3 decomposition at RH = 90 %, with stability exceeding 60 h, surpassing previously reported catalysts. Combined theoretical simulations and experiments reveal that this superior performance stems from the interfacial charge transfer. At the interface, a built-in field is created to trigger charge transfer from SrMnO3 to Sr6Co5O15, accumulating negative charges on the surface of Sr6Co5O15. This enhances water resistance by repelling water's oxygen end, thereby weakening their adsorption on active sites during O3 decomposition. This study offers insights into designing water-resistant catalysts through heterojunction engineering to boost the O3 decomposition in high humid air.

Circular dichroism (CD) inversion in chiral photonic structures provides a sensitive probe of chiral-selective light-matter interactions, yet its physical origin remains insufficiently explored in the mid-infrared region. Here, we report a pronounced narrowband CD inversion in a bilayer all-dielectric chiral metasurface integrated on an InSb-based platform. The structure consists of vertically stacked Si/SiO2 deformed V-shaped resonators, where geometric asymmetry enables chiral-selective coupling under circularly polarized illumination. Numerical simulations reveal that within an ultranarrow spectral interval around 3.1 & micro;m, the CD spectrum exhibits a sharp transition from a negative dip to a positive peak, with a maximum CD value of 0.87. By analyzing the electric-field distributions and resonance evolution, we attribute this behavior to mode hybridization between two spectrally adjacent resonances, consistent with a Fano-like interference mechanism exhibiting opposite phase responses for left-handed and right-handed circularly polarized (LCP and RCP) light. Outside the resonant window, the absence of effective mode coupling leads to a vanishing CD response. These results provide a clear physical picture of CD inversion in low-loss dielectric metasurfaces and offer a viable route toward polarization-sensitive mid-infrared photodetection and chiral sensing.

Dynamic control of Airy beam focusing is important for applications in optical manipulation, imaging, and laser processing. However, most metasurface-based Airy beam generators are statically designed, and tunability typically relies on mechanical translation, which limits system compactness and integration. Here, we propose a tunable Airy zoom metasurface based on the moir & eacute; effect. The device consists of two rotationally symmetric dielectric metasurfaces composed of titanium dioxide nanopillars. By encoding the Airy autofocusing phase and exploiting the rotational moir & eacute; modulation between the two layers, the output phase distribution can be continuously tuned through relative rotation, enabling dynamic control of the Airy beam focal position. Numerical simulations demonstrate that at a wavelength of 610 nm the focal length can be continuously tuned from 8 mu m to 32 mu m. Compared with conventional quadratic-phase moir & eacute; zoom metasurfaces, the proposed design preserves the nondiffracting characteristics of Airy beams while providing improved focusing efficiency and enhanced lateral resolution. This work offers a compact and mechanically simple approach for dynamically controllable metasurface optics and may facilitate the development of integrated and programmable photonic systems.

Transition-metal oxides are promising catalysts for the oxygen reduction reaction (ORR) in metal-air batteries, yet their rational design remains challenging because lattice periodicity and connectivity-induced distortions can substantially perturb the local electronic structure of active entities. Herein, we propose an interpretable and graph-theory-based “From Active Unit to Catalyst” (FAUC) inverse design strategy that constructs bulk catalysts by first optimizing an intrinsically active [MnO5] entity and then systematically assembling it through single and mixed sharing modes. Across 0D, 1D, and 2D architectures, we establish a clear connectivity-electronics-activity principle: increasing the sharing degree shifts the Mn dz2 states away from the Fermi level with enhanced filling, leading to degraded ORR activity, whereas corner-sharing best preserves semi-occupied dz2 states crossing EF and delivers low overpotential. Guided by FAUC, graph-neural-network-assisted structural search and first-principles validation identify corner-sharing Ca3Mn2O6 as a dynamically stable oxide catalyst, previously unreported in the specific I4/mmm structure, with a low ORR overpotential of 0.26 V. FAUC provides a transferable blueprint for designing oxide air–cathode catalysts from optimal coordination entities.

The practical use of MnO2 catalysts for hydrogen peroxide (H2O2) decomposition is often hindered by limited chemical and thermal stability. In this study, we propose a rare-earth incorporation strategy that improves structural robustness while maintaining high catalytic activity. We introduce the concept of "atomic glue" and demonstrate it by incorporating yttrium (Y) into MnOx via a one-step hydrothermal synthesis. Y incorporation induces local lattice strain that suppresses crystallization growth and promotes an amorphous, high-surface-area framework. As a result, Y-MnOx achieves complete H2O2 decomposition within 3 min at room temperature, outperforming delta-MnO2 (4 min) and undoped MnOx (12 min) under identical conditions. This performance is enabled by the abundant accessible surface redox-active sites provided by the amorphous, high-surface-area architecture. More importantly, Y-MnOx exhibits markedly enhanced durability, maintaining essentially unchanged activity over four consecutive cycling tests, whereas undoped MnOx and delta-MnO2 deactivate rapidly. Thermal annealing further confirms the superior robustness of Y-MnOx, which retains its structural features up to 500 degrees C. This work establishes "atomic glue" as a practical design principle and provides a simple route to durable, high-performance MnOx-based catalysts for H2O2 decomposition.

Humidity-induced deactivation severely limits room-temperature catalytic ozone decomposition by blocking active sites and retarding oxygen-intermediate turnover. Herein, an Ag/YMO (Ag/YMn2O5) heterointerface catalyst is constructed for robust ozone decomposition under humid conditions, achieving near-complete O3 conversion at 25 °C and 90% relative humidity (RH) under a weight hourly space velocity (WHSV) of 1,200,000 mL g−1 h−1 with stable operation. A confined-space filter test further verifies the device-level applicability of Ag/YMO for rapid ozone removal. Structural analyses confirm Ag particles anchored on YMO with partially oxidized Ag species at the particle surface. X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS) and ultraviolet photoelectron spectroscopy (UPS) reveal electron transfer from Ag-containing domains to adjacent Mn sites, producing an electron-rich Mn interface and a polarized surface. This interfacial polarization and the resulting local electric field repel highly polar H2O molecules through Coulombic interactions, thereby suppressing their adsorption on Mn-related interfacial active sites. Helium temperature-programmed desorption-mass spectrometry (He-TPD-MS), water contact-angle measurements, and in situ diffuse reflectance infrared Fourier-transform spectroscopy (in situ DRIFTS) show that this interface weakens H2O retention on Mn-related sites and accelerates peroxide-intermediate conversion. This work highlights electron-rich metal–oxide heterointerfaces as an effective route to humidity-tolerant ozone decomposition catalysts.

Humidity severely inhibits catalytic residual ozone decomposition at room temperature due to competitive adsorption between H2O and O3, thereby hindering the wide application of ozone as an oxidant. Here, we propose a synergistic strategy to fundamentally overcome catalytic water poisoning by modulating interfacial electric dipoles and active site spin states, and demonstrate its validation with a specifically designed PdO/YMn2O5 heterojunction catalyst, which enables 100% ozone removal under the harsh condition of 90% relative humidity (RH) and a weight gas hourly space velocity (WHSV) of 2,400,000 mL·g-1·h-1 with superior durability at room temperature. Moreover, it also enables efficient ozone decomposition from -45 to 45 °C under humid condition. XPS, EXAFS, and DFT calculations reveal that electron transfer from PdO to YMn2O5 establishes a strong interfacial dipole, creates electron-rich Mn sites that electrostatically repel polar water molecules while enhancing ozone adsorption. Critically, this electronic restructuring concurrently modulates the Mn spin state, drastically lowering the energy barrier for the rate-limiting desorption of triplet oxygen. This work elucidates the fundamental mechanism of dipole-spin synergy, establishing a new paradigm for designing humidity-resistant catalysts for efficient environmental remediation under extreme operating conditions.

The low thermal and chemical stability of manganese dioxide (MnO2) in aqueous solutions poses a significant challenge for practical applications. Herein, we stabilize MnO2 through interfacing with mullite oxide YMn2O5 for the efficient catalytic degradation of H2O2. Compared to the pure-phase MnO2, the composite material (MnO2/YMO) exhibits the enhanced thermal and chemical stability, which completely degrades H2O2 (0.5 M) within one minute at 25 degrees C, surpassing the reported catalysts. Experimental and theoretical results demonstrated that active surface of MnO2 preferentially exposes on YMn2O5. Such an interfacial bonding is crucial for stabilizing the MnO2 phase, as it suppresses phase transition during thermal treatment or chemical reactions. Theoretical calculations revealed that charge transfer between the interfaces optimize the adsorption energy of reaction intermediates, further improving catalytic activity. This work solves the issue of MnO2 instability through interface engineering while remaining its high catalytic performance, providing insight into the development of the next generation of catalysts.

The development of high‐performance ORR catalysts is challenged by the understanding how the delocalized electrons in s ‐ and p ‐orbitals influence oxygen intermediate adsorption and overall catalytic performance. To address these challenges, the from active unit to bulk catalyst (FAUC) design strategy is employed to investigate the roles of s‐ and p‐ orbitals in ORR activity. Specifically, six M‐N 4 ‐OH (M = V, Cr, Mn, Fe, Co, and Ni) catalyst systems are constructed and analyzed using density functional theory (DFT), this study reveals that, compared to d ‐orbitals, the delocalized electrons in the s‐ and p‐ orbitals (N s,p ) exhibit a significant volcano relationship with ORR activity. This superior predictive capability arises from the weaker dependence of s‐ and p‐ orbitals on the local coordination environment. Additionally, a structure‐activity relationship is established where shortening M─O and M─N bond lengths significantly increases N s,p . Through modification strategies such as doping and loading, the Co─N bond lengths are regulated in Co‐N 4 ‐OH‐C, resulting in shorter bonds and increased N s,p , which shifted ORR catalytic activity closer to the volcano peak. These findings validate the N s,p descriptor's rationality and universality across various 3 d transition metals, providing new insights for the design of high‐performance ORR catalysts.

The Mn-Mn dimer has been found to be catalytically active in various manganese oxides for NO oxidation. However, to date, it remains unclear how the dimer determines catalytic performance. Herein, we employed a combination of DFT theoretical calculations and an experimental approach to investigate the O2 dissociation capability and NO oxidation activity of single Mn sites and Mn-Mn dimer sites with varying bond lengths. Our results indicate that Mn-Mn dimer sites outperform single Mn active sites in both O2 activation and NO oxidation. This enhancement is primarily attributed to the short-range ordered geometry of the Mn-Mn dimers, which suppresses the formation of NO3* intermediates and promotes NO2* desorption. Among the three types of Mn-Mn dimers examined, the Mn-Mn dimer in BaMnO3, with the shortest Mn-Mn bond length, aligns most favorably with O-O, supporting the most efficient O2 activation. Conversely, MnO2, characterized by the longest Mn-Mn bond length, exhibits greater charge transfer and synergistic effects at the local active site, achieving the highest NO catalytic activity. Furthermore, we found that dual-site exposure of Mn-Mn dimers is more effective for catalytic reactions than single-site exposure. This study provides important insights into the structure–activity relationship between the geometric structure of catalytic active sites and the adsorption of intermediates.

Circularly polarized light (CPL) detection sensors have significant potential for applications in quantum communication and biosensing. In this work, we propose a three-layer complementary chiral metasurface (TCCM) for on-chip integration in the mid-infrared range (2–6 μm). The TCCM consists of an Al nanorod layer, a SiO2 dielectric layer, and an Al nanoslit layer, with strong circular dichroism (CD) achieved through the symmetry breaking of the inclined rectangular rods. Finite-difference time-domain (FDTD) simulation results demonstrate that the electric fields excited by left circularly polarized (LCP) light and right circularly polarized (RCP) light exhibit different bonding and antibonding modes, which explains the CD mechanism. The CD response and spectral tunability are influenced by the angle and length of the inclined rectangular rods. Through simulation optimization of structural parameters, a maximum CD value of 0.72 is achieved. Compared to traditional multilayer chiral metasurfaces, the TCCM simplifies the fabrication process. These findings provide valuable insights and practical strategies for the development of compact infrared devices, particularly in optical communication, chiral sensing, and full-Stokes polarization detection.

Polarimetric imaging technology captures both traditional intensity information and multidimensional polarization data, significantly enhancing target–background contrast and boosting detection system recognition. However, monolithic integration of grating polarizers into large-area focal plane arrays faces challenges, including complex fabrication, low extinction ratios, and high rates of blind elements. In this article, we present a simulation model for the fabrication of high-performance polarized gratings using electron-beam cured HSQ (Hydrogen Silsesquioxane Polymer) materials technology. By optimizing structural design, a high transmittance of 88–97% and an extinction ratio of ≥55 dB over a wide spectral range of 3–5 µm was achieved. This result offers a new approach to advancing high-performance infrared polarization imaging technology.

The electrochemical synthesis of hydrogen peroxide (H2O2) suffers from low selectivity toward the 2e- oxygen reduction reaction (ORR) pathway over the competing 4e- pathway. The key to this selectivity lies in precisely controlling the adsorption strength of the critical intermediate *OOH. In this work, we address this challenge through a local micro-environment engineering approach that modulates the surface coverage of active oxygen species (*O) to optimize *OOH adsorption behavior through cobalt-doped zinc oxide catalyst post-treated by ozone (Co-ZnO-O3). The incorporation of Co improves the ratio of oxygen vacancies and enhances the concentration of *O from 28.1 % in pristine ZnO to 39.4 %, and then ozone treatment further increases the surface *O concentration to 52.6 %. The regulatory mechanism via ozone activation on the *O concentration of ZnO and CoZnO and further demonstrate that high *O concentration is more favorable for the 2e- ORR. As a result, Co-ZnOO3 achieves a remarkable H2O2 selectivity of up to 96 % due to the moderate *OOH adsorption determined optimized by Co-doping and ozone activation. A flow-cell electrolyzer equipped with Co-ZnO-O3 can deliver an industrial-scale current density of over 300 mA cm-2 at 0.2 V and a record-high H2O2 yield rate of 58.56 mol g- 1 h- 1, maintaining a Faradaic efficiency of over 90 % for 50 h. Furthermore, its practical applicability is demonstrated in the degradation of organic pollutants, such as methylene blue and rhodamine B, highlighting its potential application in various fields.

Reconstruction during the oxygen evolution reaction（OER） significantly transforms the geometric structure of transition metal compounds,leading to enhanced catalytic performance.However,the resulting structural disorder complicates the development of accurate theoretical models.In this study,CoS 2 is used as a model system to establish a framework for rationally modeling reconstructed OER catalysts based on density functional theory（DFT）.In the reconstruction process,sulfur atoms are likely to be substituted by oxygen atoms,leading to the formation of the CoOOH phase.Based on the difference in reconstruction degree,we constructed three types of models:doping,heterostructure,and fully reconstructed,representing the reconstruction degree from minimal to full phase transition,respectively.Fully reconstructed models,which account for strain and vacancy effects,effectively simulate the unique coordination environments of reconstructed catalysts.Model e-CoOOH achieves a theoretical overpotential of0.38 V,outperforming pristine CoOOH（0.56 V）,demonstrating that the unique structural features resulting from reconstruction improve OER performance.The doping model and the heterostructure model are helpful to explain the electronic structure and performa nce transformation of the reconstruction process.This work provides a rational theoretical modeling approach,which is conducive to improving the reliability of the theoretical OER performance of the reconstructed catalyst.