Journal of Materials Chemistry A最新文献

{"title":"A DFT Investigation of Photocatalytic Water Splitting Properties of the InS/GaTe Heterostructure: Direct Z-Scheme vs Traditional Type-II","authors":"Redi Kristian Pingak, Oliver Conquest, Catherine Stampfl","doi":"10.1039/d5ta04464b","DOIUrl":"https://doi.org/10.1039/d5ta04464b","url":null,"abstract":"Density Functional Theory is used to predict the structural, electronic, and optical properties, as well as the reaction energetics, of the InS/GaTe heterostructure. The system is stable and found to have an ideal band gap of 1.34 eV, significantly lower than its monolayer counterparts. This makes it more effective in absorbing light in the visible region, as confirmed by our analysis of its optical properties. The oxygen evolution reaction (OER) was investigated for both the direct Z-scheme and the type-II mechanisms. The photogenerated hole potential for the Z-scheme ranges from 2.37 eV for pH=0 to 4.02 eV for pH=14, while that for the type-II mechanism is from 1.44 eV (pH=0) to 3.09 eV (pH=14). Based on the analysis of the electronic properties of the InS/GaTe heterostructure, and its Gibbs free energy reaction pathway for OER when the light is turned on, the transfer mechanism of the photogenerated electrons and holes in InS/GaTe is predicted to follow the direct Z-scheme mechanism. Notably, the OER reaction is predicted to be spontaneous for a wide pH range: 2 ≤ pH ≤ 14 (Z-scheme) and 3 ≤ pH ≤ 14 (type-II). This makes the InS/GaTe heterostructure more promising for OER compared to many other catalysts. While the type-II mechanism cannot facilitate HER, the Z-scheme mode of InS/GaTe is predicted to have good performance for HER, with an ideal Gibbs free energy of -0.02 eV at pH = 7. The solar-to-hydrogen efficiency is predicted to be 44.8%, which is higher than that of many other photocatalysts, and is far higher than the 10% threshold for commercial applications. These results strongly indicate that the InS/GaTe heterostructure, in its Z-scheme mode, holds high potential as a photocatalyst to facilitate both OER and HER for water splitting applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"54 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203540","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Recent progress on ZnIn2S4 -based composite photocatalyst for photocatalytic hydrogen production coupling organic synthesis","authors":"Jung Wang, Yu Wei, Bo-Hao Zhang, Weiya Huang, Kai yang, Kang-Qiang Lu","doi":"10.1039/d5ta06861d","DOIUrl":"https://doi.org/10.1039/d5ta06861d","url":null,"abstract":"Compared with sacrificial-agent-dependent half-reactions in photocatalytic water-splitting hydrogen production, coupling photocatalytic organic synthesis with hydrogen production markedly boosts electron-hole utilization efficiency and cuts reaction costs. In recent years, hexagonal ZnIn2S4 has been widely applied in the field of photocatalytic hydrogen production coupled with organic synthesis due to its advantages such as narrow band gap, high hydrogen evolution efficiency, good chemical stability, non-toxicity, and low cost. Herein, we present a comprehensive review of the latest progress in ZnIn2S4-based photocatalysts. We first summarize the preparation methods of ZnIn2S4 and the strategies to improve its performance, including metal doping, morphological engineering, heterostructure construction and defect engineering. Subsequently, we focus on the research progress of ZnIn2S4-based photocatalysts in hydrogen production coupling organic synthesis, including the selective conversion of alcohols, oxidative coupling of amines, thiol dehydrogenation, and biomass oxidation. Finally, the challenges and opportunities that ZnIn2S4 face in the practical application are discussed. It is expected that this review will offer insightful guidance for the rational design of semiconductor-based dual-functional photoredox reaction systems, thereby injecting impetus into the research on harvesting environmentally solar fuel production as well as the high-value-added fine chemicals.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"99 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203597","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synergy of metal halide doping and a polymeric interface enables improved electrochemical performance of all solid-state Li batteries","authors":"Madan Bahadur Saud, M. Bilal Faheem, Hansheng Li, Haining Zhang, Bilawal Khan, Samprash Risal, Abiral Baniya, Xinlu Wang, Yuchen Zhang, Ruosi Qiao, Poojan Kaswekar, Ian Dean Hosein, Yeqing Wang, Jr-Hau He, Zheng Fan, Quinn Qiao","doi":"10.1039/d5ta06438d","DOIUrl":"https://doi.org/10.1039/d5ta06438d","url":null,"abstract":"Sulfide solid-state electrolytes are promising candidates for all-solid-state lithium metal batteries (ASSLBs) having higher energy density and practical safety due to their high ionic conductivity and favorable mechanical properties. However, their practical integration is hindered by low critical current density (CCD), a narrow electrochemical stability window, and high impedance with electrodes. Herein, we demonstrate that doping lithium phosphorus sulfide (Li<small>₇</small>P<small>₃</small>S<small>₁₁</small>) solid electrolyte with zirconium chloride (ZrCl<small>₄</small>) significantly enhances its electrochemical performance. Unlike previously reported doping strategies, ZrCl<small>₄</small> doping uniquely introduces dual dopants (Zr<small>⁴⁺</small> and Cl<small>⁻</small>) into the Li<small>₇</small>P<small>₃</small>S<small>₁₁</small> matrix. Density functional theory (DFT) and <em>ab initio</em> molecular dynamics (AIMD) simulations reveal that the Zr<small>⁴⁺</small> ions increase dynamic structural flexibility, while Cl<small>⁻</small> ions create additional Li<small>⁺</small> vacancies, collectively enhancing structural stability and ionic conductivity beyond the capacity of single-element doping strategies. Optimized doping content of ZrCl<small>₄</small> improved the CCD of Li<small>₇</small>P<small>₃</small>S<small>₁₁</small> from 0.55 mA cm<small>⁻²</small> to 1.7 mA cm<small>⁻²</small>, while the ionic conductivity improved from 1.8 × 10<small>⁻³</small> S cm<small>⁻¹</small> to 3.0 × 10<small>⁻³</small> S cm<small>⁻¹</small>. Li/Li symmetrical cells with doped electrolyte exhibited improved cycling stability at 0.1 mA cm<small>⁻²</small> compared to the control counterparts. Furthermore, a thin solid polymer electrolyte (SPE) was used at the interface between the cathode and solid electrolyte to enable the stack pressure free operation of full cells. Li/LiFePO<small>₄</small> (LFP) full cells using doped solid electrolyte (SE) in combination with SPE catholyte demonstrated stable performance compared to undoped SE based cells. The enhanced Li-dendrite suppression and improved electrochemical properties due to doped Li<small>₇</small>P<small>₃</small>S<small>₁₁</small> and the stack free operation due to the addition of SPE as catholyte will add significant potential for advancing ASSLB technology.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"101 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203538","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Effect of Ni-W-S electrocatalysts on the stability and electrochemical properties of photocathode","authors":"Zhengwu Liu, Hongwei Liu, Xiaoliang Ren, Pusen Lu, Jianjun Ye, Kang Wang, Feng Jiang","doi":"10.1039/d5ta06369h","DOIUrl":"https://doi.org/10.1039/d5ta06369h","url":null,"abstract":"Silicon-based photocathodes are attractive for photoelectrochemical (PEC) water splitting, yet their deployment is constrained by reliance on precious metal catalysts like platinum (Pt). Here, we introduce a cost-efficient, tungsten-doped nickel sulfide (NiWS) catalyst, photoelectrodeposited onto a TiO 2 -passivated silicon substrate. X-ray photoelectron spectroscopy reveals that W incorporation tailors the local electronic environment of Ni and S, facilitating charge redistribution and accelerating interfacial charge transfer kinetics. The engineered NiWS/TiO 2 /Si photocathode delivers a high photocurrent density of -30.8 mA cm -2 at 0 V RHE , with an onset potential of 0.58 V RHE , an applied bias photon-to-current efficiency (ABPE) of 4.47%, and a Faradaic efficiency of ~90% for hydrogen evolution in neutral phosphate buffer (pH 6.5). It also demonstrates exceptional durability, retaining stable operation over 1014 hours under continuous illumination. When integrated with a silicon photovoltaic cell in a tandem architecture, the system enables unbiased solar-driven water splitting, delivering a solar-to-hydrogen (STH) efficiency of 4.01% and sustaining performance for 115 hours under AM 1.5G conditions. This work positions NiWS as a scalable, earth-abundant alternative to noble metals for long-term PEC hydrogen production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"6 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203549","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Graphene accelerates electron transfer over copper-cobalt nanoparticles for efficient electroreduction of nitrate to ammonia","authors":"Yi Li, Junbo Zeng, Jiahao Mo, Fuping Zhou, Tao Duan, Youkui Zhang","doi":"10.1039/d5ta06585b","DOIUrl":"https://doi.org/10.1039/d5ta06585b","url":null,"abstract":"Nitrate sewage will give rise to the hazarding of aquatic ecosystems and human life. Electrochemical reduction of nitrate to ammonia (NO 3 -RR) was reckoned as the prospective pathway for ecological remediation and nitrogen cycle but faced with challenges. In this work, through decorating graphene on copper-cobalt (CuCo) nanoparticles, the electron transferring between Co and Cu is intensified, which is conducive to NO 3 -RR. The optimized catalyst (CuCo-Gr0.1) performs eminent ammonia yield of 0.29 mmol h -1 cm -2 with Faradic efficiency (FE) of 97.2 % at -0.16 V versus reversible hydrogen electrode (vs RHE) and increasing to 0.91 mmol h -1 cm -2 at -0.56 V vs RHE in acid electrolyte. Besides, CuCo-Gr0.1 also exhibits high performance for the reduction of nitrate to ammonia in neutral condition, which can combine with uranyl ions to produce ammonium uranium oxide hydrate. The density functional theory calculations reveal that the decorated graphene on CuCo can promote electron transfer and NO 3 -adsorption, thus accelerating the catalytic kinetics of NO 3 - RR. This work provides new insights into the design of efficient NO 3 -RR electrocatalyst for nitrogen and uranium cycling in nuclear industry wastewater treatment.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"10 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203537","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Phase diagrams and chemical expansion upon hydration of proton conductors BaZrxCe0.8-xY0.1Yb0.1O2.9(H2O)n (0 ≤ x ≤ 0.8; 0 ≤ n ≤ 0.1)","authors":"Lozane Hamze, Olivier Joubert, Eric Quarez","doi":"10.1039/d5ta07218b","DOIUrl":"https://doi.org/10.1039/d5ta07218b","url":null,"abstract":"Proton-conducting ceramics are promising candidates for applications in sustainable energy technologies, with BaZrxCe0.8-xY0.1Yb0.1O2.9 (BZCYYb) perovskites standing out as excellent proton conductors. However, comprehensive structural studies of these materials, particularly concerning their hydrated and dehydrated states, as well as the effects of composition (x) and temperature, are still limited. This study explores the crystal structures of BaZrxCe0.8-xY0.1Yb0.1O2.9(H2O)n and BaZrxCe0.8-xY0.1Yb0.1O2.9 (0 ≤ x ≤ 0.8) using neutron and X-ray diffraction techniques. The chemical expansion due to water incorporation is quantified by measuring unit cell volumes via X-ray diffraction, showing strong agreement with mass loss data from thermogravimetric analysis (TGA). Phase diagrams for both hydrated and dehydrated phases are developed, revealing a decrease in symmetry and a reduction in phase transition temperatures as x increases. Hydration notably affects octahedral tilting, as evidenced by comparisons of hydrated and dehydrated structures at room temperature (RT). Furthermore, a bond valence sum (BVS)-based approach is proposed, offering improved predictions of octahedral tilting and structural stability compared to the traditional Goldschmidt tolerance factor. These structural insights, particularly the influence of hydration, are essential for advancing our understanding of these materials and providing a solid foundation for linking their structure to their properties.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"23 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203539","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Stress and Airflow-Sensitive 3D-Printed Hydrogel Sensor Based on Cu2+-Alanine Coordination and Graphene Sheet Networks","authors":"Jiamin Wu, Xiangke Wang, Bo Liu, Jingzhi Tang, Xinyuan Wan, Gengsheng Weng","doi":"10.1039/d5ta06290j","DOIUrl":"https://doi.org/10.1039/d5ta06290j","url":null,"abstract":"Flexible sensors with applications in real-time monitoring of human health conditions, e.g., breath, are of vital importance. Herein, we report a 3D-printed hybrid network (HN) hydrogel sensor showing stress and airflow monitoring performance based on the sensitive Cu2+-alanine (Ala) coordination cross-linked poly(N,N-dimethylacrylamide-co-3-alanine-2-hydroxypropylmethacrylate) (PDA) network and the graphene (GR) filler network. The highly stress and airflow-sensitive HN hydrogel sensor is prepared by sequential 3D printing of the polyacrylic acid hydrogel layer and the patterned PDA/Cu/GR hydrogel layer cross-linked by the Cu2+-Ala coordination. The graphene sheets in the PDA/Cu/GR hydrogel form lamellar structures, which generate a rough and porous network structure. The stress sensitivity of the HN hydrogel sensor stems from the dynamic Cu2+-Ala coordination within the PDA network and the rough, porous network structure of the graphene filler, while its airflow sensitivity is attributed to the reversible and rapid water loss and reabsorption behavior. The sensor’s stress sensitivity enables the detection of the motion speed of the object, hand gestures, and facial expressions. The fist punching out/pulling back test and human breath detection demonstrate the application for airflow detection. Our work provides a new opportunity for fabricating multimodal hydrogel sensors with potential applications for human healthcare and activity monitoring.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"22 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203536","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Flexocatalytic driven Water Splitting: Unprecedented Hydrogen Production by Symmetry invariant ZnIn2S4 Nanosheets","authors":"Jatin Mahajan, Shivali Dhingra, Anand Babu, Ajay Partap Singh Rana, Arpna Jaryal, Chandan Bera, Dipankar Mandal, Kamalakannan Kailasam","doi":"10.1039/d5ta05386b","DOIUrl":"https://doi.org/10.1039/d5ta05386b","url":null,"abstract":"Flexocatalytic water splitting offers an intriguing avenue for “sustainable hydrogen” generation and has potential to overcome several inherent limitations of photocatalytic, electrocatalytic, and even piezocatalytic methods. In particular, flexocatalysis does not necessitate a non-centrosymmetric crystal structure, unlike piezocatalysis which allows to choose from a large materials database. In this context, centrosymmetric 2D zinc indium sulfide (ZnIn2S4) nanosheets were utilized as an active material for flexoelectric-driven water-splitting. Notably, utilizing methanol as a sacrificial agent under an ultrasonic frequency of 40 kHz, an unprecedented H2 evolution rate of 60 mmol g-1 h-1 (0.120 mmol h-1) was achieved without using a co-catalyst, demonstrating the practical viability of the ZnIn2S4 (ZIS) nanosheets. FEA (finite element analysis) simulation reveals that induced flexoelectric polarization developed over the ZIS nanosheets due to inhomogeneous stress distribution that facilitates the progressive water-splitting reaction. A series of control experiments with electrochemical impedance spectroscopy, and surface potential studies were conducted to bestow mechanistic insights into the flexocatalytic-driven water splitting over ZIS nanosheets. The density functional theory corroborates the experimental findings, revealing that applying stress on the catalyst lowers the Gibbs free energy, promoting H2 production over ZIS nanosheets. Thus, the present study presents the symmetry invariant pathway for transforming mechanical energy into H2 production, thereby paving the potential way for sustainable and economically feasible H2 production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"9 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203600","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Revisiting the Original 2003 Garnet-like Li-ion Conducting Solid Electrolytes Li5La3M2O12 (M = Nb, Ta, Nb/Ta): A Look into Phase Formation and the Identification of Carbonate and Alumina Contamination","authors":"Heather A Ritchie, Ioanna Maria Pateli, Oxana V. Magdysyuk, Aaron Naden, Heitor Secco Seleghini, Federico Grillo, Gavin Peters, Sharon Elizabeth Ashbrook, John Irvine, Venkataraman Thangadurai","doi":"10.1039/d5ta06905j","DOIUrl":"https://doi.org/10.1039/d5ta06905j","url":null,"abstract":"Garnet-type electrolytes are a promising class of solid-state oxide materials for next-generation lithium batteries. In this study, parent-phase garnets, Li5La3M2O12 (M = Nb, Ta, Nb/Ta), were synthesised via solid-state reaction at 900 °C and 1100 °C, enabling comprehensive structural and chemical stability characterisation. Powder X-ray diffraction (PXRD) and Raman spectroscopy confirmed single-phase garnets with Ia¯3 d symmetry, while scanning electron microscopy (SEM) imaging revealed improved densification at 1100 °C. Electrochemical impedance spectroscopy showed the high ionic conductivities of 4.8 × 10⁻⁵ S cm⁻¹ at 55 °C for Nb and Ta co-substituted Li5La3NbTaO12 prepared at 1100 °C. X-ray photoelectron spectroscopy and thermogravimetric analysis identified a surface lithium carbonate layer formed under ambient conditions, which was not discussed in the original garnet reported in 2003. Solid-state nuclear magnetic resonance spectroscopy provided an insight into the lithium environment in the surface and bulk of the samples and confirmed aluminium contamination in samples sintered at the base of alumina crucibles at 1100 °C, with LaAlO3 identified as the dominant secondary phase, corroborated by PXRD, SEM, and energy dispersive X-ray spectroscopy analysis. Nb-doped garnet showed the most severe reaction with the alumina crucible. The use of a sacrificial mother powder of targeted garnet oxides, an approach commonly used for the preparation of Li-garnets, or sintering at 900 °C effectively reduced Al contamination. This work delivers a detailed evaluation of the parent-phase garnet, offering renewed insights into phase and structure two decades on from its initial development in 2003.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"9 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203541","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Bifunctional Electrocatalyst Engineered via Polyanionic Synergy and Heterointerface Modulation for Robust Seawater Electrolysis","authors":"Fang Zheng, Zhenhua Fang, Mayur Anandrao Gaikwad, Suyoung Jang, Seyeon Cho, Jongsung Park, Jin Hyeok Kim","doi":"10.1039/d5ta05443e","DOIUrl":"https://doi.org/10.1039/d5ta05443e","url":null,"abstract":"The sustainable production of hydrogen (H2) through water electrolysis is a promising solution for renewable energy storage, yet its scalability is restricted by the scarcity of freshwater resources. Seawater electrolysis offers an alternative, but chloride-induced corrosion and chlorine evolution reactions hinder practical use. Here, we report an Fe-Ni layered double hydroxide/Co-doped nickel sulfide (LDH/Co-Ni3S2) hybrid electrocatalyst, engineered with a multi-anion synergistic interface. The electrocatalyst utilizes an interlayer carbonate (CO32⁻) in the LDH and in-situ generated sulfate (SO42⁻) from Co-Ni3S2 to form a double electric layer shielding effect, preventing Cl- penetration. In-situ Raman spectroscopy shows that FeNi-LDH partially converts to iron-nickel oxyhydroxide (FeNiOOH) during operation, which, with strong Lewis acidity, reduces hydroxide adsorption energy. The hybrid structure provides abundant active sites and efficient mass transport, achieving an OER overpotential of 451 mV at 500 mA cm⁻2 in alkaline seawater. The electrocatalyst demonstrated remarkable stability for 500 h at 500 mA cm⁻2 in 1 M KOH seawater, while also exhibiting 120 h of durability in the 6 M KOH seawater at the same current density. As a bifunctional electrocatalyst, it enables methanol-assisted seawater splitting at 1.68 V for 100 mA cm⁻2 with near-unity Faradaic efficiency, effectively suppressing chloride oxidation. This dual engineering strategy offers new insights for robust seawater-based H2 production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"82 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145195490","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}