Intrinsic Electrocatalytic Activity for Oxygen Evolution of Crystalline 3d‐Transition Metal Layered Double Hydroxides

Angewandte Chemie - Tập 133 Số 26 - Trang 14567-14578 - 2021
Fabio Dionigi1,2, Jing Zhu3,2, Zhenhua Zeng4, Thomas Merzdorf1, Hannes Sarodnik1, Manuel Gliech1, Lujin Pan1, Wei‐Xue Li3, Jeffrey Greeley4, Peter Strasser1
1The Electrochemical Energy, Catalysis, and Materials Science Laboratory, Department of Chemistry, Chemical Engineering Division, Technical University Berlin, Strasse des 17. Juni 124, 10623 Berlin, Germany
2these authors contributed equally to this work
3School of Chemistry and Materials Science, CAS Excellence Center for Nanoscience, Hefei National Laboratory for Physical Sciences at Microscale, University of Science and Technology of China, Hefei, 230026 Anhui, China
4Davidson School of Chemical Engineering, Purdue University, West Lafayette, IN, 47907 USA

Tóm tắt

AbstractLayered double hydroxides (LDHs) are among the most active and studied catalysts for the oxygen evolution reaction (OER) in alkaline electrolytes. However, previous studies have generally either focused on a small number of LDHs, applied synthetic routes with limited structural control, or used non‐intrinsic activity metrics, thus hampering the construction of consistent structure–activity‐relations. Herein, by employing new individually developed synthesis strategies with atomic structural control, we obtained a broad series of crystalline α‐MA(II)MB(III) LDH and β‐MA(OH)2 electrocatalysts (MA=Ni, Co, and MB=Co, Fe, Mn). We further derived their intrinsic activity through electrochemical active surface area normalization, yielding the trend NiFe LDH > CoFe LDH > Fe‐free Co‐containing catalysts > Fe‐Co‐free Ni‐based catalysts. Our theoretical reactivity analysis revealed that these intrinsic activity trends originate from the dual‐metal‐site nature of the reaction centers, which lead to composition‐dependent synergies and diverse scaling relationships that may be used to design catalysts with improved performance.

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Angewandte Chemie

Tập 133 Số 26

14567-14578

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