Journal
ADVANCED MATERIALS
Volume 31, Issue 8, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201805127
Keywords
coordinatively unsaturated structure; density functional theory calculation; heterogeneous catalyst; oxygen evolution reaction; X-ray absorption spectroscopy
Categories
Funding
- National Key R&D Program of China [2017YFA0303500]
- National Natural Science Foundation of China [U1532112, 11574280, 21706248]
- Innovative Research Groups of National Natural Science Foundation of China (NSFC) [11621063]
- NSFC-Ministero degli Affari Esteri e della Cooperazione Internazionale (MAECI) [51861135202]
- CAS Interdisciplinary Innovation Team
- CAS Key Research Program of Frontier Sciences [QYZDB-SSW-SLH018]
- Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology [2016FXCX003]
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Unravelling the intrinsic mechanism of electrocatalytic oxygen evolution reaction (OER) by use of heterogeneous catalysts is highly desirable to develop related energy conversion technologies. Albeit dynamic self-reconstruction of the catalysts during OER is extensively observed, it is still highly challenging to operando probe the reconstruction and precisely identify the true catalytically active components. Here, a new class of OER precatalyst, cobalt oxychloride (Co-2(OH)(3)Cl) with unique features that allow a gradual phase reconstruction during OER due to the etching of lattice anion is demonstrated. The reconstruction continuously boosts OER activities. The reconstruction-derived component delivers remarkable performance in both alkaline and neutral electrolytes. Operando synchrotron radiation-based X-ray spectroscopic characterization together with density functional theory calculations discloses that the etching of lattice Cl- serves as the key to trigger the reconstruction and the boosted catalytic performance roots in the atomic-level coordinatively unsaturated sites (CUS). This work establishes fundamental understanding on the OER mechanism associated with self-reconstruction of heterogeneous catalysts.
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