Polyoxometalated metal-organic framework superstructure for stable water oxidation

• 成果类型: Article
• 署名作者: Yue, Kaihang; Lu, Ruihu; Gao, Mingbin; Song, Fei; Dai, Yao; Xia, Chenfeng; Mei, Bingbao; Dong, Hongliang; Qi, Ruijuan; Zhang, Daliang; Zhang, Jiangwei; Wang, Ziyun; Huang, Fuqiang; Xia, Bao Yu; Yan, Ya
• 署名单位: Chinese Academy of Sciences; Shanghai Institute of Ceramics, CAS; Huazhong University of Science & Technology; Chinese Academy of Sciences; University of Chinese Academy of Sciences, CAS; University of Auckland; Chinese Academy of Sciences; Dalian Institute of Chemical Physics, CAS; Chinese Academy of Sciences; Shanghai Advanced Research Institute, CAS; East China Normal University; Chongqing University; Chongqing University; Inner Mongolia University; Shanghai Jiao Tong University; Sungkyunkwan University (SKKU)
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-11560
• DOI: 10.1126/science.ads1466
• 发表日期: 2025-04-25
• 页码: 430-436
• 关键词: oxygen evolution reaction; initio molecular-dynamics; activity trends; electrocatalysts; efficient; nickel; cobalt; STABILITY; reduction; (oxy)hydroxide

摘要

Stable, nonprecious catalysts are vital for large-scale alkaline water electrolysis. Here, we report a grafted superstructure, MOF@POM, formed by self-assembling a metal-organic framework (MOF) with polyoxometalate (POM). In situ electrochemical transformation converts MOF into active metal (oxy)hydroxides to produce a catalyst with a low overpotential of 178 millivolts at 10 milliamperes per square centimeter in alkaline electrolyte. An anion exchange membrane water electrolyzer incorporating this catalyst achieves 3 amperes per square centimeter at 1.78 volts at 80 degrees C and stable operation at 2 amperes per square centimeter for 5140 hours at room temperature. In situ electrochemical spectroscopy and theoretical studies reveal that the synergistic interactions between metal atoms create a fast electron-transfer channel from catalytic iron and cobalt sites, nickel, and tungsten in the polyoxometalate to the electrode, stabilizing the metal sites and preventing dissolution.