Understanding the stability and catalytic behavior of atomically thin metal monolayers is crucial for the rational design of efficient electrocatalysts. This study employs an iterative DFT-AIMD-DFT multiscale simulation strategy to systematically uncover the structural evolution, electronic structures, and their correlations with catalytic performance in grouped transition metal monolayers (Au1L, Ag1L, Cu1L, Pt1L, Rh1L, Ir1L, Pd1L, and Ni1L). The results demonstrate that these monolayer metals exhibit a continuous transition from typical low-index facets to bilayer structures, with their stability strongly dependent on electronic structure and interlayer interactions. Key drivers of structural planarity and stability—spreading energy and interlayer interaction energy—were identified. Low coordination-induced electronic localization reveals the structure-electronic-performance coupling of metal monolayers under the synergistic regulation of work function and d-band center. Further analysis indicates that monolayer metals can maintain good stability over a wide electrochemical window, significantly enhancing their hydrogen oxidation reaction and oxygen reduction reaction catalytic activity, and exhibiting clear advantages over bulk metals. In particular, certain monolayer metals (e.g., Rh1L) achieve a synergistic optimization between stability and catalytic activity, fully demonstrating their tremendous application potential in the field of electrocatalysis.

Photoelectrochemical (PEC) technology offers a promising approach for degrading antibiotic pollutants, yet it remains constrained by low efficiency and incomplete mineralization. Herein, a Co-doped BiVO4/Mo-doped BiVO4 homojunction photoanode and kanamycin strongly complexed PEC system is constructed for efficient pollutant degradation and H2 generation. Mo doping and homojunction formation enhance the electrical conductivity and charge separation of the photoanode, while the strong complexation between the photoanode and kanamycin facilitates interfacial charge transfer. Consequently, the optimized photoanode delivers a current density of 9.61 mA cm-2 at 1.00 V versus reversible hydrogen electrode under simulated sunlight irradiation and maintains excellent stability. Near-unity Faradaic efficiencies for both anodic CO2/N2 generation and cathodic H2 evolution confirm the complete mineralization and chemical energy recovery of kanamycin. To mitigate carbon emissions and valorize the generated CO2 and H2, a photothermal CO2 hydrogenation system is further integrated, demonstrating a superior CO yield of 122.65 mmol g-1 h-1 with nearly 100% selectivity. This synergistic PEC-photothermal platform achieves simultaneous kanamycin remediation and resource valorization, providing a viable strategy to address energy and environmental concerns.

Ulcerative colitis (UC) is an incurable inflammatory bowel disease characterized by chronic mucosal inflammation, with a continuously increasing global prevalence. Although infrared (IR) therapy has demonstrated anti-inflammatory potential, conventional devices which can only emit single-wavelength IR often exhibit limited tissue penetration and suboptimal spectral overlap with mammalian absorption. Herein, we develop a broad-spectrum IR (BSIR) device enabled with an almost defect-free graphene (DFG) based radiator to deliver high output IR aligned with mammalian IR absorption spectra. In a mouse model of UC, BSIR treatment significantly alleviated disease symptoms and promoted mucosal recovery. Crucially, this study shows that BSIR radiation induces the relocation of T lymphocytes to the spleen, leading to reduced immune cell infiltration and inflammation in the colon. Gene expression analysis further reveals enhanced innate immune activity and cell regeneration in colonic tissue. Collectively, these findings demonstrate that BSIR represents a safe, non-invasive therapeutic strategy for UC. More broadly, this study highlights spectrum-matched IR irradiation as a novel modality for immune modulation, with potential translational relevance for other deep-tissue inflammatory diseases.

Developing dielectric films with high energy density and efficiency under extreme conditions is crucial for the stable operation of advanced devices like electric vehicles and energy storage systems. This work designs a rational linear–nonlinear–linear (LNL) sandwich architecture, with MOF-enhanced PEI insulating layers (EZ) as the outer layers and horizontally aligned P(VDF-HFP)/TNTs composite films (PT) as the middle polarization layer. The multi-site bonding network within the EZ layer, constructed by activating the Zn²⁺ sites on ZIF-8 via the thermal field during imidization to coordinate with the PEI monomer (ODA), significantly enhances the breakdown strength (reaching up to 664.50 kV/mm for the EZ1 composite film) and suppresses leakage current. Meanwhile, the horizontal orientation of TNTs in the PT layer, achieved through an electrospinning process combined with hot-pressing, improves polarization performance while maintaining high breakdown strength. The resulting ~20 μm EZ-PT-EZ LNL film achieves a high Ud of 13.68 J/cm³ (η = 85.5%) at 620 kV/mm and 25 °C, and retains a Ud of 8.51 J/cm³ under harsh 120 °C and 520 kV/mm conditions. The excellent performance originates from the synergistic effects of the widened bandgap of the EZ layer, the inhibition of charge carrier transport by the reverse built-in electric field formed at the L/N interface (opposite to the applied field), and the combined hindering effect of the interlayer interface and horizontally oriented fillers on breakdown path propagation. This work provides an effective strategy for designing high-performance polymer dielectrics through synergistic structural design and band structure engineering.

Achieving stable dispersion of graphite flakes (GFs) in aqueous media remains a critical challenge in developing high-performance graphite-flake nanofluids (GNFs) for direct photothermal energy harvesting. This study explored the synergistic effects of anionic and non-ionic surfactants on colloidal stability, optical properties, and photothermal response of GNFs. Among all the engineered formulations, the mixed-surfactant system containing 20 wt.% Tween 80 (T80, non-ionic) and 80 wt.% sodium dodecyl sulfate (SDS, anionic), (GNF@T80₂₀%–SDS₈₀%) exhibited the highest dispersion stability with improved photothermal performance, maintaining uniform suspension for over 40 days. UV–Vis spectroscopy showed a distinct redshift in the π→π* transition, attributed to improved exfoliation and enhanced interfacial polarizability from the dual surfactant system, which stabilized the excited electronic states at lower energies. This optimized formulation achieved photothermal conversion efficiency of 91% under AM 1.5G solar irradiation, outperforming both single-surfactant and base fluid counterparts. Numerical simulations using a morphology-corrected Mie scattering model closely matched the experimental extinction spectra, validating the optical behavior. Radiative transfer analysis further confirmed ~93% total solar absorption before 3 cm depth. This work establishes a synergistic surfactant-assisted design and modeling strategy for producing stable, high-efficiency GNFs, paving the way for their application in next-generation solar thermal energy conversion systems.

The accelerating demand for green hydrogen has intensified the development of efficient and durable photoelectrocatalysts (PECs) for sustainable water splitting. Titanium dioxide (TiO2) is a benchmark semiconductor for PEC because of its chemical stability, low cost, and highly tunable properties. However, its wide bandgap and slow charge transport limit its solar-to-hydrogen energy conversion efficiency. Single atom catalysts (SACs) provide transformative opportunities to overcome these intrinsic limitations. This review provides a comprehensive overview of SACs-modified TiO2-based PECs, including (i) fundamental principles of single-atom catalysis; (ii) rational design strategies through metal selection via noble and non-noble metals, fabrication methods and structural engineering by modification of morphology of TiO2 structures such as nanotubes, nanowires nanofilms and metal organic frameworks and facets engineering; and (iv) advanced characterization techniques—critical to gain insights into mechanisms involved in these platforms. Hydrogen and oxygen evolution reactions driven by SACs-modified TiO2-based PECs are summarized. The limitations of these systems such as low metal loading, single atom aggregation under operating conditions, and insufficient active sites are discussed. We also provide an outlook on future developments combining dual-single atoms and high entropy alloys in TiO2-based PECs, as promising pathways to synergistically integrate activity, stability, and atomic economy. This review provides a valuable framework for designing the next generation TiO2-based PECs for sustainable PEC water splitting.

Exploration of platinum-free-based electrocatalysts for high-performance oxygen reduction reaction (ORR) is tremendous attractive towards the large-scale practical applications, yet great challenging. Herein, it is demonstrate that halogen-doping on carbon nanotube (CNT) could be an effective pathway towards activation of oxygen reduction reaction performance. A novel synergistic molten-salt strategy using a NaCl eutectic mixture to precisely fabricate Cl-doped, defective CNTs, is developed, allowing to creates a high density of topological defects, a large specific surface area, and hierarchical porosity. The as-prepared Cl-CNT catalyst exhibits exceptional ORR activity in alkaline media, with a half-wave potential of 0.84 V (vs. RHE), outperforming most metal-free carbon-based catalysts and rivaling commercial Pt/C. It further demonstrates high selectivity for the direct 4e− pathway (>95%) and excellent methanol tolerance and durability. When deployed in a zinc-air battery, it delivers a peak power density of 156 mW cm−2 and remarkable cycling durability over 120 hours. The experimental results is consistent with the density functional theory (DFT) screening predication that Cl-doping optimally modifies the electronic structure and binding energy of oxygen intermediates, leading to the remarkable reaction kinetics. This work provides both fundamental insight and a scalable synthetic paradigm for harnessing halogen doping in advanced metal-free electrocatalysis.

Two-dimensional staggered heterostructures, featuring by the intrinsically facilitate charge separation, provide promising platforms for efficient photocatalytic water splitting. However, their carrier dynamics generally follow two competing pathways: type-II and Z-scheme, with the distinct governing mechanisms in photocatalysis remain elusive. Here, through stacking or sliding ferroelectric control, we realize three switchable phases within an In2Se3/SnSe heterostructure, and uncover how interlayer polarization governs carrier dynamics for enhanced photocatalytic activities and efficiencies. First-principles results show that transitions between type-II and Z-scheme models can be driven by the reversal of interlayer electric fields (Eint) or donor-acceptor band edge exchanges, which will further modulate their carrier separation, redox potential alignment, interlayer carrier lifetime, carrier dynamics, pontaneous thermodynamic feasibility, and energy conversion efficiency. Compared with the inactive type-II (↑ Se-) phase, strengthened Eint in the type-II (↓ Se-) phase suppresses interlayer e-h recombination to prolonged carrier lifetimes, while the Z-scheme (↓ Sn+) accelerate this recombination, forming new active band edges. Thereby, both yield higher redox potentials for superior photocatalytic activities and efficiencies. Particularly, the Z-scheme (↓ Sn+), identified as the ground state, achieving an optimal solar-to-hydrogen efficiency of 48.3%. These results uncover how stacking-induced polarization defines carrier-dynamics in staggered heterostructures, establishing interlayer engineering as an effective route toward next-generation of switchable and high-efficient 2D photocatalysts.

Developing self-powered photodetectors capable of processing multi-dimensional optical signals is pivotal for next-generation photonic computing and secure communications. However, conventional device architectures are typically limited to single-mode intensity detection, and the complex photophysics within coupled photovoltaic units remain poorly understood. Here, we reveal a unified “Photovoltaic-Capacitance” coupling mechanism within a vertically stacked, self-powered Ga2O3/PEDOT:PSS and ZnO/Graphene architecture. We demonstrate that the system’s wavelength-selective, transient bipolar response is governed by the multifaceted charging and discharging dynamics between the two coupled units. The key to this mechanism is the ZnO/Graphene (3D/2D) interface, which we define as a novel “Photovoltaic Dynamic-Capacitor” (PDC) component, exhibiting a defined four-stage transient (instantaneous polarization, steady-state saturation, reverse discharge, and relaxation). This architecture enables the Ga2O3 unit (photovoltaic source) to dynamically charge the PDC under 270 nm illumination (+0.27 A/W), while 380 nm illumination directly activates the PDC itself, generating a reverse current (–0.009 A/W). This universal (proven with MgZnO) and dynamically-coupled architecture unlocks a new paradigm for self-powered, multi-dimensional optical processing. We leverage this unique behavior to implement a physical-layer secure communication protocol based on a innovative ternary optical logic (“1”, “0”, “-1”), offering enhanced anti-jamming capabilities rooted in a new photonic degree of freedom.

Oxygen evolution reaction (OER), limited by high overpotential and sluggish kinetics, represents a major bottleneck for electrochemical water splitting toward green hydrogen production. Constructing asymmetric A–O–B motifs to modulate the electronic density of states near the Fermi level through orbital coupling is crucial for optimizing the surface chemisorption properties of transition metals, thereby enabling the development of electrocatalysts with high intrinsic activity and stability. Herein, an IrOx nanocluster-coupled Fe/Eu co-doped nickel telluride composite catalyst (IrOx/FeEu-NiTex) with ultralow Eu (0.72 at%) and Ir (0.14 at%) content was synthesized using an in situ hydrothermal method followed by an electrochemical deposition strategy. Benefiting from the design of an asymmetric dual-electron bridge structure with gradient orbital coupling (Ni 3d–O 2p–Eu 4f, Ni 3d–O 2p–Ir 5d), the electronic structure of the catalyst is effectively modulated, thereby enabling the optimization of adsorption behaviors for reaction intermediates. Consequently, the optimized IrOx/FeEu-NiTex electrode exhibits superior OER performance, delivering low overpotentials of 205 mV and 334 mV at current densities of 10 mA cm−2 and 500 mA cm−2, respectively. Furthermore, it maintains long-term stability for over 1000 hours at high current densities of 500 and 1000 mA cm−2. When integrated into an alkaline water electrolyzer, the system achieves a current density of 500 mA cm−2 at a cell voltage of 1.64 V and demonstrates stable operation for over 1000 hours. This study successfully develops a high-performance rare-earth-based OER catalyst by constructing an asymmetric dual-electron bridge structure with gradient orbital coupling, providing new insights into electronic structure engineering strategies.

Modulating the electronic structure of catalysts is widely recognized as an effective strategy to enhance electrocatalytic performance. This study synthesized a nanosheet array composed of Cr-Co2P confined within a P, N co-doped carbon matrix (Cr-Co2P@PNC) through a facile synchronous carbonization-phosphorization method, then anchored it onto a P-doped carbonized wood framework (PCW) to construct a composite catalyst. Benefiting from the synergistic coupling between the Cr-Co2P@PNC nanosheet array architecture and the wood-derived carbon matrix, the Cr-Co2P@PNC/PCW demonstrates remarkable catalytic activity and long-term durability for the oxygen evolution reaction (OER), achieving an overpotential of 283 mV at 50 mA cm-2 with stable operation exceeding 100 hours. Experimental characterization and theoretical calculations confirm that the coupling of wood-derived interconnected hierarchical porous structures with the nanosheet array facilitates extensive contact between active sites and electrolyte, enhancing mass transport during reactions. Cr doping modulates the electronic structure, alleviating strong adsorption at Co sites and reducing the energy barrier of the OER rate-determining step. The P, N co-doped carbon matrix promotes electron transfer and optimizes reaction kinetics. This work demonstrates an optimization strategy for OER composite catalysts while providing new perspectives for exploring renewable wood-derived catalyst designs.

Anion exchange membrane (AEM)-based CO2 electrolyzers powered by renewable energy provide a promising pathway for a sustainable CO2-to-CO conversion. However, they suffer from CO2 crossover via the formation of (bi)carbonates, limiting carbon utilization to 50%, and electrolyte-driven salt precipitation, which shortens device lifetime. A forward-biased bipolar membrane (BPM) addresses these issues by operating with pure-water and regenerating CO2 at the bipolar junction. Nevertheless, instability of the bipolar interface, lower faradaic efficiency, and high cell potential remain open challenges. Here, we present a BPM incorporating a porous anion exchange layer (AEL) to facilitate CO2 release out of the bipolar junction. Two BPM configurations are compared with porous or dense AEL deposited either onto a silverbased gas diffusion electrode (GDE) or onto the CEM. Porous AEL-coated GDEs achieved enhanced stability, lower cell potentials, and partial current densities for CO up to 214 mA cm-2 at 3.25 V. Implementation of this BPM architecture reduces CO2 crossover by at least 80% compared with an AEM-based electrolyzer, although CO2 losses to the anode persist, highlighting the need for further optimization. These findings establish porous AEL-coated GDEs as a promising strategy for advancing BPM CO2 electrolysis.

Pressure sensors are essential for acquiring real-time information that directly influences the performance and safety of modern engine control systems. However, developing pressure sensors that can operate reliably at high temperatures remains a formidable challenge due to the lack of stable sensing materials. Here, we report a novel polymer-derived SiHfBCN ceramic coating exhibiting outstanding pressure-sensing behavior and remarkable thermal stability at elevated temperatures. The SiHfBCN coating was fabricated on sapphire substrates through a preceramic polymer route and subsequently pyrolyzed at various temperatures up to 1500 °C. The amorphous ceramic film features a nanodomain structure composed of amorphous SiHfBCN and crystalline HfC(N) nanoparticles together with in-situ forms carbon ribbons, which provides excellent electrical and mechanical stability. The optimized coating demonstrates a high gauge factor K of up to 42.000, excellent repeatability, and stable signal response under cyclic compression, maintaining its performance up to 1300 °C. These results highlight the potential of SiHfBCN ceramics as next-generation materials for high-temperature pressure-sensing applications.

Recent design strategies for polymeric adsorbents which remove per- and polyfluoroalkyl substances (PFAS) from water have relied on coupling both electrostatic and fluorine-fluorine interactions with PFAS in fluorinated polymer adsorbents. Non-fluorinated polymers are a desirable alternative to reduce cost and reliance on fluorinated precursors. Molecular design of fluorine-free adsorbents requires development of chemically modular synthetic strategies to uncover new, useful structure-property relationships. We utilize a modular synthetic platform using active ester click chemistry to prepare a library of PFAS adsorbents containing a wide range of Lewis base ligands alongside both hydrophilic and hydrophobic co-monomers. Poly(ethylene glycol) diacrylate networks containing both aliphatic groups and strong bases such as piperazine and piperidine exhibit rapid removal of >98% perfluroooctanoic acid (PFOA) from dilute solutions and can be regenerated using light alcohols. PFOA binding capacities are as high as 910 mg/g despite these materials having lower effective fixed charge densities than commercial anion exchange polymers. Sorption behavior is strongly influenced by ligand basicity and equilibrium pH which alter protonation of PFOA and Lewis base ligands. Notably, the highest sorption capacities are achieved when most PFOA was sorbed in neutral form rather than the anionic form, indicating a new potential route for optimizing PFAS adsorbents.

MoS2 is a promising high capacity anode for Li-ion batteries due to its layered structure and theoretical capacity of ~670 mAh/g, but its practical performance is limited by structural degradation under deep lithiation. Here, we employ a combination of global optimization and ab initio molecular dynamics (aiMD) to investigate the phase stability and structural failure mechanisms of Li-intercalated MoS2 over a wide range of Li concentrations. Our results reveal that upon lithiation, MoS2 undergoes a phase transformation from the 2H phase to a distorted 1T’ phase, with 1T’ LixMoS2 emerging as the most stable polymorph for x > 0.4. We further clarify how the initial Li distribution affects phase stability and structural fracture behavior. Through aiMD simulations, we find that pre-lithiated 1T’-LixMoS2 under the deep lithiation condition x > 1.0, exhibits enhanced structural integrity compared to a randomly lithiated (high energy) configuration. During aiMD simulation, our pre-lithiated LixMoS2 preserves the layered S-Mo-S framework up to higher Li concentrations (x ≈ 1.5), showing almost no S dislodgement while opening out-of-plane Li-ion diffusion channels via localized Mo-S bond cleavage. In contrast, dynamically-lithiated structures suffer from Mo-S bond breaking, early S dislodgement, and LixSy cluster formation at the interfaces (notably around x ≈ 1.25). These findings suggest that controlling the initial Li intercalation geometry can significantly mitigate mechanical degradation in MoS2 anodes, offering design guidelines for next-generation high-performance anodes with improved cycling stability and rate capability.

The deliberate assembly of heterostructures has emerged as a powerful strategy for electrochemical energy storage, where integration of complementary components enables synergistic performance gains. Moving beyond serial production of individual components and their subsequent liquid phase assembly, we report a one-step, continuous gas-phase synthesis of high-purity silicon/few-layer graphene (Si–FLG) heterostructures by coupling microwave-plasma and hot-wall reactors. This in-flight assembly yields exceptionally pure amorphous Si uniformly integrated within conductive FLG, eliminating liquid-phase processing. Electrochemical performance exhibits a non-monotonic dependence of performance on FLG content: capacity and cycle life maximize at an intermediate 15 wt.% FLG, attributed to a percolated, strain-buffering FLG network that preserves electrical contact while minimizing inactive mass. The optimized heterostructure delivers specific capacities of ~ 2800 mAh g-1Si + FLG (0.05 C) and ~ 1400 mAh g-1Si + FLG after 100 cycles at 1 C, outperforming other Si/graphene systems reported in the literature under similar conditions. These results highlight gas-phase self-assembly as a scalable route to integrate 0D/2D nanostructures into high-capacity, long-life Li-ion anodes and establish a new performance benchmark for low-carbon-fraction Si/graphene composites.

not-yet-known not-yet-known not-yet-known unknown Cobalt phosphide (Co2P) is a promising non-noble electrocatalyst material for hydrogen evolution reaction (HER) due to its affordability and stability in alkaline medium. Nevertheless, its HER activity still requires further improvement for practical applications in alkaline water electrolysis. In this study, we have incorporated nickel (Ni) into Co2P to form the junction of Ni-Co2P, using co-sputtering technique. This heterojunction, a key factor for HER activity, was quantitatively analyzed based on the ratio of Ni-P bonds, showing that a high heterojunction fraction results in enhanced HER activity. DFT results demonstrate that water dissociation is significantly promoted at the Ni-Co2P junction, while hydrogen evolution is facilitated at Ni sites, synergistically enhancing HER activity. An improper Ni concentration reduces the heterojunction fraction due to either insufficient Ni incorporation or Ni agglomeration. In contrast, the fraction is maximized at the optimal Ni concentration while maintaining high electrochemical surface area, P content, and crystallinity. Our optimized Ni-Co2P exhibits remarkable HER performance, achieving a low overpotential of ~76 mV at 10 mA/cm2 and a Tafel slope of ~47 mV/dec. Furthermore, its current density remains stable during the on/off stability test, which simulates renewable energy-integrated operation, indicating excellent durability under dynamic conditions.

Fish scales, as products of long-term natural evolution, are biomaterials featuring a intricate integration of inorganic and organic components, exhibiting species-specific multi-layered micro-nano structures. Owing to its characteristic gradient mineralization, the scale is hard on the outside but gets progressively softer inside, making for a smooth shift from rigid to flexible from the outer layer inward. This gradient structure, extending from the surface to the interior, provides important inspiration for the development of novel flexible biomimetic protective materials. Beyond structural design inspiration, the primary components of fish scales (e.g., hydroxyapatite (HAp), and collagen) possess excellent biocompatibility and multifunctionality, endowing them with broad prospects across diverse fields including biomedicine, environmental remediation, energy storage, cosmetics, food, and agriculture. However, transforming this potential into practical use is challenged by the lack of standardized processing methods and a limited understanding of how their structure affects their properties. This review comprehensively summarizes recent advances in fish scales research, with a focus on their role as biomimetic models and functional applications, and critically discusses the challenges and future opportunities toward industrialization.