单铱原子上的动态氯离子吸附促进海水氧化催化
Dynamic chloride ion adsorption on single iridium atom boosts seawater oxidation catalysis.
作者信息
Duan Xinxuan, Sha Qihao, Li Pengsong, Li Tianshui, Yang Guotao, Liu Wei, Yu Ende, Zhou Daojin, Fang Jinjie, Chen Wenxing, Chen Yizhen, Zheng Lirong, Liao Jiangwen, Wang Zeyu, Li Yaping, Yang Hongbin, Zhang Guoxin, Zhuang Zhongbin, Hung Sung-Fu, Jing Changfei, Luo Jun, Bai Lu, Dong Juncai, Xiao Hai, Liu Wen, Kuang Yun, Liu Bin, Sun Xiaoming
机构信息
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing, 100029, PR China.
School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, Singapore, 637459, Singapore.
出版信息
Nat Commun. 2024 Mar 4;15(1):1973. doi: 10.1038/s41467-024-46140-y.
Seawater electrolysis offers a renewable, scalable, and economic means for green hydrogen production. However, anode corrosion by Cl pose great challenges for its commercialization. Herein, different from conventional catalysts designed to repel Cl adsorption, we develop an atomic Ir catalyst on cobalt iron layered double hydroxide (Ir/CoFe-LDH) to tailor Cl adsorption and modulate the electronic structure of the Ir active center, thereby establishing a unique Ir-OH/Cl coordination for alkaline seawater electrolysis. Operando characterizations and theoretical calculations unveil the pivotal role of this coordination state to lower OER activation energy by a factor of 1.93. The Ir/CoFe-LDH exhibits a remarkable oxygen evolution reaction activity (202 mV overpotential and TOF = 7.46 O s) in 6 M NaOH+2.8 M NaCl, superior over Cl-free 6 M NaOH electrolyte (236 mV overpotential and TOF = 1.05 O s), with 100% catalytic selectivity and stability at high current densities (400-800 mA cm) for more than 1,000 h.
海水电解为绿色制氢提供了一种可再生、可扩展且经济的方法。然而，氯离子对阳极的腐蚀给其商业化带来了巨大挑战。在此，不同于旨在排斥氯吸附的传统催化剂，我们在钴铁层状双氢氧化物（Ir/CoFe-LDH）上开发了一种原子铱催化剂，以调整氯吸附并调节铱活性中心的电子结构，从而为碱性海水电解建立独特的Ir-OH/Cl配位。原位表征和理论计算揭示了这种配位状态在将析氧反应（OER）活化能降低1.93倍方面的关键作用。Ir/CoFe-LDH在6 M NaOH + 2.8 M NaCl中表现出显著的析氧反应活性（过电位为202 mV，周转频率TOF = 7.46 O s），优于无氯的6 M NaOH电解液（过电位为236 mV，TOF = 1.05 O s），在高电流密度（400 - 800 mA cm）下具有100%的催化选择性和超过1000小时的稳定性。
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