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

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‐...

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Published in:Angewandte Chemie International Edition 2021-06, Vol.60 (26), p.14446-14457
Main Authors: Dionigi, Fabio, Zhu, Jing, Zeng, Zhenhua, Merzdorf, Thomas, Sarodnik, Hannes, Gliech, Manuel, Pan, Lujin, Li, Wei‐Xue, Greeley, Jeffrey, Strasser, Peter
Format: Article
Language:English
Subjects:
Catalysts
Cobalt
Crystal structure
Crystallinity
Electrocatalysts
electrochemical surface area
Electrochemistry
Electrolytes
hydrothermal synthesis
Hydroxides
Iron
Iron compounds
layered double hydroxides
Manganese
Nickel compounds
Oxygen
oxygen evolution reaction
Oxygen evolution reactions
Reaction centers
Transition metals
water splitting
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Summary: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‐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. Catalytic activities for oxygen evolution on crystalline 3d transition metal layered double hydroxides are derived using electrochemical surface area based normalization. Density functional calculations reveal a dual‐metal‐site feature of the reaction centers that provides opportunities to design new catalysts with improved performance.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202100631