Dynamic chloride ion adsorption on single iridium atom boosts seawater oxidation catalysis

Xinxuan Duan; Qihao Sha; Pengsong Li; Tianshui Li; Guotao Yang; Wei Liu; Ende Yu; Daojin Zhou; Jinjie Fang; Wenxing Chen; Yizhen Chen; Lirong Zheng; Jiangwen Liao; Zeyu Wang; Yaping Li; Hongbin Yang; Guoxin Zhang; Zhongbin Zhuang; Sung-Fu Hung; Changfei Jing; Jun Luo; Lu Bai; Juncai Dong; Hai Xiao; Wen Liu; Yun Kuang; Bin Liu; Xiaoming Sun

doi:10.1038/s41467-024-46140-y

Dynamic chloride ion adsorption on single iridium atom boosts seawater oxidation catalysis

Nat Commun. 2024 Mar 4;15(1):1973. doi: 10.1038/s41467-024-46140-y.

Authors

Xinxuan Duan^#^{1

2}, Qihao Sha^#¹, Pengsong Li³, Tianshui Li¹, Guotao Yang¹, Wei Liu¹, Ende Yu⁴, Daojin Zhou¹, Jinjie Fang⁵, Wenxing Chen⁶, Yizhen Chen⁷, Lirong Zheng⁸, Jiangwen Liao⁸, Zeyu Wang⁹, Yaping Li¹, Hongbin Yang¹⁰, Guoxin Zhang¹¹, Zhongbin Zhuang^{5

12}, Sung-Fu Hung¹³, Changfei Jing¹⁴, Jun Luo¹⁵, Lu Bai¹⁶, Juncai Dong⁸, Hai Xiao⁹, Wen Liu¹, Yun Kuang^{17

18}, Bin Liu^{19

20}, Xiaoming Sun²¹

Affiliations

¹ 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.
² School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, Singapore, 637459, Singapore.
³ Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, PR China.
⁴ Ocean Hydrogen Energy R&D Center, Research Institute of Tsinghua University in Shenzhen, Shenzhen, 518057, PR China.
⁵ State Key Lab of Organic-Inorganic Composites, College of Chemical Engineering, Beijing University of Chemical Technology, 100029, Beijing, PR China.
⁶ Energy & Catalysis Center, School of Materials Science & Engineering, Beijing Institute of Technology, Beijing, 100081, PR China.
⁷ Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, PR China.
⁸ Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, 100049, Beijing, PR China.
⁹ Department of Chemistry, Tsinghua University, 100084, Beijing, PR China.
¹⁰ Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR, 999077, PR China.
¹¹ College of Energy, Shandong University of Science and Technology, Tsingtao, 266590, PR China.
¹² Beijing Key Laboratory of Energy Environmental Catalysis, Beijing University of Chemical Technology, 100029, Beijing, PR China.
¹³ Department of Applied Chemistry and Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu, 300, Taiwan.
¹⁴ School of Materials Science and Engineering, Tianjin Key Lab of Photoelectric Materials & Devices, Tianjin University of Technology, Tianjin, 300384, PR China.
¹⁵ ShenSi Lab, Shenzhen Institute for Advanced Study, University of Electronic Science and Technology of China, Shenzhen, 518110, PR China.
¹⁶ CAS Key Laboratory of Standardization and Measurement for Nanotechnology, National Center for Nanoscience and Technology, 100190, Beijing, PR China.
¹⁷ 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. kuangy@tsinghua-sz.org.
¹⁸ Ocean Hydrogen Energy R&D Center, Research Institute of Tsinghua University in Shenzhen, Shenzhen, 518057, PR China. kuangy@tsinghua-sz.org.
¹⁹ Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR, 999077, PR China. bliu48@cityu.edu.hk.
²⁰ Department of Chemistry & Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Hong Kong SAR, 999077, PR China. bliu48@cityu.edu.hk.
²¹ 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. sunxm@mail.buct.edu.cn.

^# Contributed equally.

Abstract

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 O₂ s^-1) in 6 M NaOH+2.8 M NaCl, superior over Cl^--free 6 M NaOH electrolyte (236 mV overpotential and TOF = 1.05 O₂ s^-1), with 100% catalytic selectivity and stability at high current densities (400-800 mA cm^-2) for more than 1,000 h.

Grants and funding

21935001/National Natural Science Foundation of China (National Science Foundation of China)