Chloride-resistant NiFe oxyhydroxides via dual-atom doping for industrial-grade alkaline seawater electrolysis

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL

AIChE Journal Pub Date : 2025-06-09 DOI:10.1002/aic.18929

Lin Wang, Xiaohe Zheng, Zhengfei Chen, Jiadong Wu, Qiang Zhou, Zhongjian Li, Bin Yang, Cheng Lian, Jianguo Lu, Yuanyuan Li, Lecheng Lei, Yang Hou

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Abstract

Developing efficient and stable electrocatalysts for seawater splitting remains a huge challenge because of low catalytic selectivity and poor resistance to chlorine-induced corrosion. Here, we developed a nickel-iron layered double hydroxide nanosheets doped with chromium and sulfur dual atoms (Cr,S-NiFe LDH). Cr,S-NiFe LDH exhibited low overpotentials of 321 and 406 mV at industrial current densities of 500 and 1000 mA cm⁻², respectively. An anion exchange membrane electrolyzer based on Cr,S-NiFe LDH anode can maintain 2000 mA cm⁻²@1.764 V for 100 h. Electronic structure analysis revealed that the sulfur doping facilitates electron transfer from nickel to sulfur sites, while chromium incorporation strengthens the electronic interactions between iron and chromium sites. This modification induced the formation of high-valence nickel and chromium species, which favor seawater electrolysis. Mechanistic studies revealed that dual heteroatom doping modifies the local electronic environment of nickel/iron sites, repelling chlorine ions and optimizing the adsorption of oxygenated intermediates.

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通过双原子掺杂制备工业级碱性海水电解用耐氯NiFe氧化氢氧化物

由于催化选择性低、抗氯腐蚀能力差，开发高效、稳定的海水分解电催化剂仍然是一个巨大的挑战。在这里，我们开发了一种掺杂铬和硫双原子（Cr,S-NiFe LDH）的镍铁层状双氢氧化物纳米片。在工业电流密度为500和1000 mA cm−2时，Cr，S-NiFe LDH的过电位分别为321和406 mV。基于Cr，S-NiFe LDH阳极的阴离子交换膜电解槽可维持2000 mA cm−2@1.764 V 100 h。电子结构分析表明，硫的掺杂促进了电子从镍位向硫位的转移，而铬的掺入则增强了铁位与铬位之间的电子相互作用。这种改性导致了高价镍和铬的形成，有利于海水电解。机理研究表明，双杂原子掺杂改变了镍/铁位点的局部电子环境，排斥氯离子，优化了含氧中间体的吸附。

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.