期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 117, 期 36, 页码 21906-21913出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.2009180117
关键词
delafossite analog; electrochemical self-reconstruction; oxygen evolution reaction; amorphization; enhanced activity
资金
- National Natural Science Foundation of China [51532001, 51861130360, 11974037, U1930402]
- China Postdoctoral Science Foundation [2019TQ0013]
- Newton Advanced Fellowship [NAFR1180242]
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.
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