Spinel-Anchored Iridium Single Atoms Enable Efficient Acidic Water Oxidation via Intermediate Stabilization Effect

被引:61
作者
Liu, Yang [1 ]
Chen, Yawei [1 ]
Mu, Xulin [2 ]
Wu, Zhongyi [1 ]
Jin, Xu [3 ]
Li, Jianming [3 ]
Xu, Yanzhi [4 ]
Yang, Li [5 ]
Xi, Xiaoke [1 ]
Jang, Haeseong [6 ]
Lei, Zhanwu [1 ]
Liu, Qinghua [4 ]
Jiao, Shuhong [1 ]
Yan, Pengfei [2 ]
Li, Xiyu [7 ,8 ]
Cao, Ruiguo [1 ]
机构
[1] Univ Sci & Technol China, Dept Mat Sci & Engn, Hefei Natl Lab Phys Sci Microscale, CAS Key Lab Mat Energy Convers, Hefei 230026, Anhui, Peoples R China
[2] Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
[3] Res Inst Petro Explorat & Dev RIPED, Res Ctr New Energy, Beijing 100083, Peoples R China
[4] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
[5] Anhui Univ, Inst Phys Sci & Informat Technol, Hefei 230601, Peoples R China
[6] Chung Ang Univ, Dept Adv Mat Engn, Anseong 17546, South Korea
[7] Univ Sci & Technol China, Hefei 230026, Peoples R China
[8] Songshan Lake Mat Lab, Dongguan 523808, Peoples R China
来源
ACS CATALYSIS | 2023年 / 13卷 / 06期
基金
中国国家自然科学基金; 中国博士后科学基金;
关键词
single-atom catalysts; intermediate stabilization; spinel; acidic oxygen evolution reaction; electrochemical water splitting; OXYGEN EVOLUTION ELECTROCATALYSIS; TOTAL-ENERGY CALCULATIONS; STABILITY CHALLENGES; CATALYST; SITES;
D O I
10.1021/acscatal.2c05940
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Iridium oxide is considered the only practical catalyst for oxygen evolution reaction (OER) in commercial proton exchange membrane (PEM) electrolyzers. However, its low activity and high cost greatly hinder the large-scale development of PEM electrolyzers for hydrogen production. Herein, we report atomically dispersed Ir atoms incorporated into a spinel Co3O4lattice as an acidic OER catalyst, which exhibits excellent activity and stability for water oxidation. The catalyst significantly lowers the over-potential down to 226 mV at 10 mA cm-2 with an ultrahigh turnover frequency value of 3.15 s-1 (eta = 300 mV), 3 orders of magnitude higher than that of commercial IrO2. Meanwhile, the catalyst shows superior corrosion resistance in an acidic OER condition, reaching a lifespan of up to 500 h at 10 mA cm-2. First-principles calculations reveal that the key *OOH intermediate can be stabilized by the lattice oxygen coordinated to the Ir active site via hydrogen bond formation, which substantially regulates the rate-limiting step and lowers the activation free energy of the OER process. This work demonstrates a strategy for improving the OER activity of Ir-based catalysts and provides insights into the regulation of the reaction mechanism.
引用
收藏
页码:3757 / 3767
页数:11
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