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Intrinsic Electrocatalytic Activity for Oxygen Evolution of Crystalline 3d‐Transition Metal Layered Double Hydroxides
Author(s) -
Dionigi Fabio,
Zhu Jing,
Zeng Zhenhua,
Merzdorf Thomas,
Sarodnik Hannes,
Gliech Manuel,
Pan Lujin,
Li WeiXue,
Greeley Jeffrey,
Strasser Peter
Publication year - 2021
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202100631
Subject(s) - oxygen evolution , layered double hydroxides , catalysis , transition metal , electrochemistry , electrolyte , materials science , inorganic chemistry , active site , chemistry , chemical engineering , electrode , organic chemistry , engineering
Layered 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‐M A (II)M B (III) LDH and β‐M A (OH) 2 electrocatalysts (M A =Ni, Co, and M B =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.