In-Situ Generated High-Valent Iron Single-Atom Catalyst for Efficient Oxygen Evolution

被引：61

作者：

Zhang, Zhirong ^{[1
]}

Feng, Chen ^{[1
]}

Li, Xiangyang ^{[1
]}

Liu, Chunxiao ^{[1
]}

Wang, Dongdi ^{[1
]}

Si, Rui ^{[2
]}

Yang, Jinlong ^{[1
]}

Zhou, Shiming ^{[1
]}

Zeng, Jie ^{[1
]}

机构：

[1] Chinese Acad Sci, Univ Sci & Technol China,Dept Chem Phys, Hefei Natl Lab Phys Sci Microscale,Key Lab Surfac, Natl Synchrotron Radiat Lab,Key Lab Strongly Coup, Hefei 230026, Anhui, Peoples R China

[2] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China

来源：

NANO LETTERS | 2021年 / 21卷 / 11期

基金：

中国博士后科学基金;

关键词：

single atom catalysts; high-valent iron; oxygen evolution; SYNERGISTIC CATALYST; PEROVSKITE COBALTITE; WATER OXIDATION; OXIDE; ELECTROCATALYSTS; REDUCTION; GRAPHENE; STATE; CHALLENGES;

D O I：

10.1021/acs.nanolett.1c01335

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Oxygen evolution reaction (OER) plays an important role in renewable energy supplies as the anodic reaction for electrochemical transformation of various chemicals. Iron-based OER catalysts are potential candidates due to their abundance but suffer from poor activity. Here we demonstrate that a single-atom iron catalyst with in-situ generated Fe4+ centers is highly active toward OER. Only an overpotential of 320 mV was needed to reach 10 mA cm(-2). The catalyst exhibited an ultrahigh turnover frequency of 0.62 s(-1) at an overpotential of 0.35 V, which is comparable to currently reported transitional-metal based OER catalysts. Experimental and theoretical studies revealed that the valence state of the metal center transferred from Fe3+ to highly active Fe4+ prior to the OER process. This transformation was originated from the strong interaction between atomic Fe and carbon support via C-O-Fe bonding, leading to a lower energy barrier of the rate-limiting *OOH formation.

引用

页码：4795 / 4801

页数：7