Developing high-performance photocatalytic systems for nitrogen fixation is a crucial yet challenging for sustainable ammonia synthesis. Herein, an amorphous Fe2CoOx cocatalyst is successfully loaded onto Bi2MoO6 (BMO) to construct a highly efficient photocatalytic nitrogen reduction reaction (NRR) system. Visible-light-driven ammonia production over the optimized 1.0Fe2CoOx/BMO composite reaches 860.7 μmol g-1 h-1, about 15.4 times that of pristine BMO, outperforming most reported photocatalysts. The results of comprehensive characterizations and density functional theory calculations demonstrate that the amorphous Fe2CoOx cocatalyst not only rapidly captures photogenerated electrons and suppresses charge recombination, but also provides abundant Fe sites as dominant active centers that boost N2 adsorption and activation. More importantly, the introduction of Fe2CoOx unlocks the previously kinetically blocked distal pathway in addition to the intrinsic alternating pathway, thereby broadening the reaction pathways and significantly accelerating the overall NRR kinetics. In addition, the universal performance enhancement capability of this amorphous cocatalyst is verified on multiple representative photocatalysts, including ZnIn2S4, Bi2WO6, TiO2 and g-C3N4. This work demonstrates that engineering amorphous bimetallic oxide cocatalysts is an effective strategy for developing highly efficient photocatalytic NRR systems.

The development of efficient and low-cost photocathodes is critical for the commercial advancement of solar photoelectrochemical (PEC) cells for water-splitting hydrogen evolution applications. Herein, Ag/Cu3BiS3/graphitic-C3N4 (g-C3N4) composite photocathode was fabricated using the two-step in-situ growth approach, serving as an alternative to conventional noble metal counter electrodes. Within this configuration, Cu3BiS3 nanomaterial (CBS) acts as the principal light-harvester responsible for the generation of photo-induced excitons, while CBS/g-C3N4 heterojunction facilitates efficient charge separation. Simultaneously, Ag forms Schottky junctions with CBS to promote directional electron extraction and transport, and especially, its surface plasmon resonance (SPR) effect further enhances exciton separation efficiency. Consequently, this multiphase synergistic system optimizes charge generation, separation and transfer processes. PEC measurements reveal the half-cell solar-to‑hydrogen conversion efficiency (STH) reaching 4.37%, representing the highest reported value to date for hydrogen evolution in solar bias-free PEC cells. Furthermore, when integrated with MnS/CdSe/TiO2 photoanode, the assembled tandem PEC device demonstrates markedly superior performance, achieving the hydrogen evolution yield of 350.92 μmol/cm2 over 4 h period relative to Pt sheet counter electrode-based cell (252.52 μmol/cm2). The stability assessments conducted over 32 h indicated that H2 yield decreased approximate 9.6%. This work presents viable strategy for substituting noble-metal electrodes in stable PEC hydrogen evolution systems.

The cycloaddition of CO2 with epoxides to produce cyclic carbonates typically requires harsh conditions, motivating the development of efficient heterogeneous catalysts for mild operation. In this work, four triazine-based organic polymers (CTP-TPT, CTP-TPB, CTP-TIT, and CTP-TIB) were synthesized via one-step quaternization polycondensation of cyanuric chloride with four nitrogen-containing ligands. Their structures were characterized by FT-IR, solid-state 13C NMR, XPS, SEM, and BET, and their catalytic performances in CO2-epoxide cycloaddition were evaluated. CTP-TIT exhibited the best activity, achieving 95.6% epichlorohydrin yield at 80 °C, 0.5 MPa CO2, and 6 h, along with good substrate generality and 90.6% yield retention after five cycles. Electrostatic potential calculations revealed the largest potential gradient (+34.8/-28.15 kcal/Mol) in CTP-TIT, arising from the synergy between the electron-withdrawing triazine framework and the positive potential of imidazole C2H. NPA charge analysis confirmed the coexistence of positive charge at imidazole C2H (+0.284 e) and negative charge at imidazole N (-0.395 e) within the same ring, forming a spatially separated push-pull polarization. DFT calculations showed that CTP-TIT exhibits the lowest ring-opening energy barrier (12.14 kcal/Mol) and the largest potential difference in the transition state, establishing a direct link between the push-pull effect and barrier reduction. In situ FTIR combined with DFT supported a synergistic pathway involving epoxide activation by imidazole C2H, CO2 activation by triazine N, and nucleophilic ring-opening by Cl-. This work provides a systematic theoretical basis for designing metal-free triazine-based polymers for efficient CO2 yield under mild conditions.

Multiphase interface engineering provides an effective strategy for regulating interfacial charge transfer and improving light-driven catalytic energy conversion. Here, Te-incorporated Bi4O4SeCl2 hybrid ceramics containing retained BiOCl and β-Bi2O3 phases together with Te-induced conductive Bi2Te3 nanophases are constructed to generate abundant coherent and semi-coherent interfaces. These multiphase interfaces effectively reconstruct the electronic structure and microstructure of the Bi4O4SeCl2 matrix, leading to optimized carrier transport pathways, broadened visible-NIR absorption, and improved interfacial charge separation. The optimized composite exhibits enhanced electrical transport while maintaining low thermal conductivity due to intensified phonon scattering at heterogeneous interfaces. Density functional theory calculations reveal pronounced work-function-driven electron transfer at the Bi4O4SeCl2/BiOCl interface, whereas the Bi4O4SeCl2/Bi2Te3 junction forms a quasi-ohmic contact that facilitates rapid electron exchange. Electrochemical impedance spectroscopy and electron paramagnetic resonance measurements further demonstrate reduced charge-transfer resistance and regulated oxygen-vacancy-associated defect states at the optimized composition. Under illumination, the engineered interfaces promote efficient separation and migration of photogenerated carriers. Consequently, the optimized hybrid catalyst achieves a hydrogen evolution rate of 85.74 μmol g-1 h-1, representing a 287% enhancement compared with pristine BiOSeCl-0Te. These results establish multiphase interface engineering as an effective route for regulating interfacial charge-transfer pathways and light-driven hydrogen evolution in layered bismuth-based materials.

In this work, a bilayer hydrogel with dual responsiveness to temperature and near-infrared (NIR) light, together with strain-sensing capability, was prepared via stepwise in situ free-radical polymerization. Upon heating or NIR irradiation, the poly(N-isopropylacrylamide-co-acrylamide) (PNAM)/Ti₃C₂Tₓ MXene active layer contracts, while the poly(acrylamide) (PAAm)/poly(vinyl alcohol) (PVA) passive layer provides flexible mechanical support and undergoes relatively limited deformation, resulting in directional bending of the bilayer hydrogel. Meanwhile, MXene serves as both the photothermal component for NIR actuation and the conductive component for real-time strain sensing. The hydrogel consists of a PNAM/MXene active layer and a PAAm/PVA passive layer, wherein MXene nanosheets provide excellent photothermal conversion capability and electrical conductivity, while the PAAm/PVA network offers favorable flexibility and mechanical support. Owing to its bilayer structure, the hydrogel exhibits favorable flexibility and stretchability, with a tensile strength of 12.5 kPa and an elongation at break of 397%. Under thermoresponsive actuation, it achieves a maximum bending rate of 12° s-1. Under NIR irradiation, the surface temperature of the optimized hydrogel reaches 68.7 °C within 60 s. The hydrogel can also be fabricated into various shapes to realize biomimetic behaviors. In addition, it exhibits high sensitivity (GF = 3.28) and excellent cyclic stability. Therefore, the PNAM/MXene//PAAm/PVA hydrogel developed in this study represents a multifunctional soft material with potential applications in intelligent soft actuators, wearable sensors, and human-machine interfaces.

Helium (He), widely used in cryogenic and superconductivity technologies, occurs naturally in subsurface reservoirs, where its migration, trapping, and retention are governed by wettability. Although clean quartz is initially strongly water-wet and He is inert and non-polar, and has negligible adsorption tendency, contact angle can still vary with pressure, temperature, and brine salinity through changes in the gas-brine-solid interfacial energy balance. Yet systematic wettability data for He-rock systems remain scarce, limiting reliable assessment of its subsurface behaviour. To address this gap, we present the first comprehensive experimental dataset of He-quartz-brine contact angles, as well as He-brine interfacial tension values, measured using tilted plate method under reservoir-relevant conditions, including pressures of 0.1-20.0 MPa, temperatures of 303-333 K, and brine salinities of 0.0-0.3 m (0-17,430 ppm) NaCl. Next, using 36 experimental data points, empirical correlations were developed to relate advancing and receding contact angles to pressure, temperature and salinity, while a complementary density-based relationship forecasted contact angle with higher accuracy. Lastly, the trends and governing mechanisms were compared with published wettability data for more reactive gases including CO2 and H2. The results demonstrated that He remains strongly brine-wet across all conditions, with advancing and receding angles of 12-44° and 8-38°, respectively. Additionally, contact angles increase systematically with pressure, temperature, and salinity, with salinity exerting the dominant control (increase of 16-25° as the brine salinity increased from 0.0 to 0.3 m NaCl) through electrical double layer thickness reduction. Importantly, despite these systematic variations, the Helium-quartz-brine system remained consistently brine-wet across all tested conditions. These findings established a quantitative framework for evaluating He contact angle in quartz-rich reservoirs, with potential implications for subsurface gas storage systems involving CO2 and H2.

Photocatalytic CO2 reduction coupled with water oxidation provides a sustainable route for solar fuel production, but its efficiency is limited by insufficient near-infrared light utilization, rapid carrier recombination and weak CO2 activation. Herein, biomass-derived nickel phytate (PA-Ni) was immobilized on lead-free double perovskite Cs2AgBiBr6 (CABB) to construct a full-spectrum-responsive photocatalyst for gas-solid CO2 photoreduction without sacrificial reagents. PA-Ni extends the optical absorption of CABB into the near-infrared region and introduces surface Ni sites for CO2 adsorption and activation. The optimized PA-Ni@CABB(1:1) composite achieved a CO evolution of 54.9 μmol g-1, approximately 2.5- and 6-fold higher than pristine CABB and PA-Ni. More importantly, PA-Ni@CABB(1:1) exhibited distinct near-infrared-driven CO2 reduction activity with a CO yield of 16.3 μmol g-1 under λ ≥ 800 nm irradiation, while both individual components were almost inactive. Systematic experiments and density functional theory calculations reveal that interfacial electron transfer accelerates charge separation, favors CO2 adsorption and *COOH generation, thereby accounting for the enhanced CO2 photoreduction activity. This work provides a biomass-based interfacial modification strategy for designing lead-free perovskite photocatalysts with broadened solar utilization.

The co-precipitation synthesis of yttrium oxide (Y2O3) nanoparticles involves coupled precursor, acidity, dispersant, and thermal variables. We developed a machine-learning workflow to model average particle size from 30 MaxMin-sampled experiments in a six-dimensional process space. Nine regression algorithms were compared using leave-one-out prediction vectors with Bayesian hyperparameter optimization. The selected support vector regression model gave R2 = 0.83, RMSE = 20.82 nm, MAE = 16.63 nm, and MedAE = 15.38 nm. SHAP and LIME identified model-level associations among synthesis variables, while follow-up DLS, zeta-potential, conductivity, FTIR, and TG measurements were consistent with a tentative SDBS/PEG6000 precursor-state regulation hypothesis. Physically constrained virtual screening generated six experimentally tested G2 routes. Their measured particle sizes ranged from 35.4 to 63.2 nm, and one G2-S05 batch yielded phase-pure, quasi-spherical Y2O3 nanoparticles with a TEM-derived particle-level size distribution of 35.4 ± 8.3 nm and a BET surface area of 32.79 m2·g-1. These results establish a proof-of-concept workflow for hypothesis generation and process selection in data-limited oxide synthesis.

Polyhedral packing provides a fundamental framework for understanding how anisotropic nanoscale building blocks organize into ordered superstructures. However, controlling the assembly pathways of tetrahedral nanoparticles remains challenging due to their intrinsic geometric frustration and complex free-energy landscapes. Herein, we develop an adaptive solution-phase assembly strategy for gold tetrahedral nanoparticles by regulating their frustrated packing pathways. Thiol-terminated polyethylene glycol (PEG) ligands grafted onto tetrahedra provide dynamic interparticle interactions through Hofmeister-effect-mediated conformational adaptation. Concurrently, strongly hydrated carbonate ions (CO32-) regulate the hydration environment of PEG chains, inducing controllable hydrophilic-hydrophobic transitions and tuning effective interactions between tetrahedral nanoparticles. This ion-mediated solvation switching enables adaptive regulation of the frustrated packing landscape and promotes ordered assembly of tetrahedral building blocks in solution. The interplay between geometric frustration of tetrahedra and adaptive flexibility of PEG ligands generates diverse hierarchical packing states, including textile-like ordered assemblies, pentagonal bipyramidal motifs, and trigonal crystalline arrays.

The construction of defect sites and tandem catalytic systems is an important strategy for the high-value conversion of CO2. In this study, Cu-In2O3 with asymmetric oxygen vacancies (Cu-In2O3-AOv) was prepared through local structural regulation. It was then combined with UiO-66 to form a tandem catalytic system that enables the cascade process of CO2 activation, conversion of oxygenated intermediates, and aromatization. Low-temperature controlled reduction and local Cu coordination modulation constructed non-equivalent InO coordination environments on the In2O3 surface, which generated oxygen vacancies with structural and electronic heterogeneity. Aberration-corrected High-Angle Annular Dark-Field Scanning Transmission Electron Microscopy (HAADF-STEM) results show that Cu substitutes for a portion of the In sites and forms a local asymmetric coordination environment. Synchrotron X-ray Absorption Near-Edge Structure (XANES) and Extended X-ray Absorption Fine Structure (EXAFS) further shows local structural distortion and the presence of multiple coordination environments in the catalyst. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results indicate that Cu-In2O3-AOv promotes the conversion of CO2, the formation of key oxygenated intermediates (i.e., HCOO* and CH2O*), and accelerates the formation of aromatic precursors. Density functional theory (DFT) calculations demonstrate that asymmetric oxygen vacancies are capable of tuning the local electron distribution, enhancing CO2 adsorption and activation, and reducing the energy barriers of key reaction steps. Under the reaction conditions of 320 °C, 3.0 MPa, a H2/CO2 molar ratio of 3:1, and a W(1%Cu-In2O3-AOV)/W(UiO-66) ratio of 1:2, the tandem catalyst shows the best catalytic performance with the CO2 conversion of 28.6% and the aromatics selectivity of 72.3%. This study reveals the structural effect and reaction mechanism of asymmetric oxygen vacancies in CO2 hydrogenation. It also provides experimental and theoretical support for the rational design of defective metal oxide/MOFs tandem catalytic systems for high-value CO2 conversion.

Surface wettability is commonly characterized using single or average contact angle measurements. However, for chemically and physically heterogeneous solid-liquid interfaces, particularly under sub-monolayer adlayer conditions, average contact angles may not adequately represent spatial variations in adsorption-induced hydrophobicity. We hypothesize that measuring, mapping, and analyzing the variation of contact angles across a representative surface, reported as a distribution of contact angles, provides a more meaningful descriptor of adsorption-induced wettability heterogeneity, capturing its mesoscale manifestation even on high-purity mineral and metal surfaces.

The practical deployment of aqueous zinc-ion batteries (AZIBs) is severely hindered by disordered zinc deposition and water-induced parasitic reactions, which degrade the long-term cycling stability of Zn anodes. Herein, a poly(1,3-dioxolane) (PDOL) protective layer is rationally constructed on the zinc surface via a facile one-step pre-polymerization strategy. The abundant ether oxygen sites of PDOL can strongly coordinate with Zn2+ to reorganize the solvation sheath, effectively weakening water competition and suppressing the hydrogen evolution reaction (HER). Meanwhile, the PDOL interlayer homogenizes interfacial Zn2+ flux and alleviates localized current concentration, inducing preferential growth of the Zn (002) crystal plane and restraining dendrite proliferation caused by the tip effect. Furthermore, a robust organic-inorganic hybrid SEI film enriched with Zn-O/Zn-F inorganic phases is in-situ generated during cycling, which further accelerates interfacial ion kinetics and passivates the reactive zinc surface. Benefiting from the synergistic effects of solvation modulation, water confinement, and interfacial reconstruction, the PDOL@Zn symmetric cell achieves an ultra-long lifespan of over 2000 h at 10 mA cm-2 (1 mAh cm-2). Both coin and pouch full cells deliver prominently enhanced cycling durability. This work provides a facile and reliable interfacial engineering strategy toward high-stability aqueous zinc-ion batteries.

The membrane-disrupting peptide Mastoparan-1 (MP-1), derived from the wasp Polybia paulista is known to possess antimicrobial properties, and exhibits enhanced activity against a number of cancer cell lines relative to healthy cells. Due to the mechanism of action of MP-1 it is likely that differences in plasma membrane lipid composition arising from cancer associated mutations, such as localisation of phosphatidylserine (PS) lipids to the outer leaflet of the plasma membrane, are involved in driving that enhanced activity. Rapid screening of MP-1 mutants in a combined approach using model membrane and cell-based biological assays, has led to the identification of a number of derivative peptides with enhanced selectivity for cancer-like membrane models and breast cancer cell lines and provided insights into the mechanism of membrane disruption and cell death. Notably, the morphology of the membrane perturbations observed by Atomic Force Microscopy (AFM) and activity in cell model systems can change considerably in response to single-point mutations in the MP-1 sequence, indicating a complex structure-activity relationship.

Designing highly dispersed and tightly bound heterojunction to achieve rapid ion transport and electron transfer is a promising strategy for improving electrochemical performance of energy storage system. However, weak interfacial interactions derived from two phase-heterostructure usually enhance charge transfer resistance, which makes poor system efficiency. In this work, an ion exchange strategy was employed to derive iron cobalt layered double hydroxide (FeCo-LDH) from zeolitic imidazolate framework (ZIF-67) on nickel cobalt oxide (NiCo2O4) substrate. The resulting nanoflower-nanosheet FeCo-LDH/NiCo2O4 heterojunction was grown on Ni foam and denoted as FC0.5-LDH/NC-NF. Benefiting from interfacial charge redistribution and enhanced electron transfer, the FeCo-LDH/NiCo2O4 heterointerface lowers the deprotonation energy barrier and thereby improves the charge-storage kinetics. Significantly, the heterostructured electrode materials display large specific surface area, abundant mesoporous structures, outstanding rate capability and superior specific capacitance of 1935 F g-1 at 0.5 A g-1. Moreover, an asymmetric supercapacitor was assembled using FC0.5-LDH/NC-NF as the positive electrode and activated carbon as the negative electrode (FC0.5-LDH/NC-NF//AC). The device exhibits a wide operating window of 1.5 V, an energy density of 76.6 Wh kg-1 at a power density of 375 W kg-1, and excellent cycling stability, retaining 83.6% of its capacitance with a Coulombic efficiency of 99.6% after 20,000 cycles (620 h). This interfacial engineering strategy not only offers a promising approach for the construction of heterojunction to improve electrochemical performance, but also provides broad prospects for the practical application of SCs in high-efficiency storage systems.

Multi-enzyme systems often face rate-limiting mismatches between catalytic steps, as well as the inherent limitations of enzymes under harsh conditions in practical applications. Herein, we report a co-immobilization cascade system of a chiral nanozyme and glucose oxidase (GOD) for the enantioselective catalysis of chiral 3,4-dihydroxyphenylalanine (DOPA). In the design of hybrid catalysts, a bio-bimetallic-organic framework (Fe-Zn-Glu(Bzim)) serves as the chiral recognition center and the peroxidase (POD)-like nanozyme, enabling integrated enantioselective and oxidative functions. GOD is covalently immobilized onto the surface of the chiral Fe-Zn-Glu(Bzim) nanozyme to construct a bionic cascade catalyst of GOD@Fe-Zn-Glu(Bzim). In addition, nanozyme exhibits excellent temperature and solvent resistance. Experimental results demonstrate that the covalent immobilization of GOD onto the nanozyme surface can generate H2O2 in situ in aqueous solution, efficiently driving the cascade reaction to achieve enantioselective catalysis of chiral DOPA. Notably, GOD@Fe-Zn-Glu(Bzim) shows 2.15-fold higher activity than free GOD at identical protein loading. The hybrid catalyst provides a promising strategy for effectively integrating the enzymatic and nanozyme catalysis, with potential implications for interface-enabled cascade biocatalysis.