Achieving delafossite analog by in situ electrochemical self-reconstruction as an oxygen-evolving catalyst

被引:78
|
作者
Liu, Juzhe [1 ,2 ]
Hu, Qi [3 ]
Wang, Yu [4 ]
Yang, Zhao [1 ]
Fan, Xiaoyu [1 ]
Liu, Li-Min [2 ]
Guo, Lin [1 ]
机构
[1] Beihang Univ, Beijing Adv Innovat Ctr Biomed Engn, Key Lab Bioinspired Smart Interfacial Sci & Techn, Sch Chem, Beijing 100191, Peoples R China
[2] Beihang Univ, Sch Phys, Beijing 100191, Peoples R China
[3] Beijing Computat Sci Res Ctr, Beijing 100193, Peoples R China
[4] Chinese Acad Sci, Shanghai Synchrotron Radiat Facil, Shanghai Inst Appl Phys, Shanghai 201204, Peoples R China
基金
中国博士后科学基金; 中国国家自然科学基金;
关键词
delafossite analog; electrochemical self-reconstruction; oxygen evolution reaction; amorphization; enhanced activity; EVOLUTION; ELECTROCATALYSTS; OXIDE; OXIDATION; COOOH; CO; CONVERSION; ENERGY; PHASE;
D O I
10.1073/pnas.2009180117
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Development of novel and robust oxygen evolution reaction (OER) catalysts with well-modulated atomic and electronic structure remains a challenge. Compared to the well-known metal hydroxides or (oxyhydr)oxides with lamellar structure, delafossites (ABO(2)) are characterized by alternating layers of A cations and edge-sharing BO2 octahedra, but are rarely used in OER due to their poor electron conductivity and intrinsic activity. Here, we propose a delafossite analog by mutation of metal oxyhydroxide and delafossite based on first-principles calculations. Modulation on the electronic structure due to distortion of the original crystal field of the BO2 layers is calculated to enhance electron conductivity and catalytic activity. Inspired by the theoretical design, we have experimentally realized the delafossite analog by electrochemical self-reconstruction (ECSR). Operando X-ray absorption spectroscopy and other experimental techniques reveal the formation of delafossite analog with Ag intercalated into bimetallic cobalt-iron (oxyhydr) oxide layers from a metastable precursor through amorphization. Benefirting from the featured local electronic and geometric structures, the delafossite analog shows superior OER activity, affording a current density of 10 mA.cm(-2) at an overpotential of 187 mV and an excellent stability (300 h) in alkaline conditions.
引用
收藏
页码:21906 / 21913
页数:8
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