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

Overview

Journal Angew Chem Int Ed Engl

Specialty Chemistry

Date 2021 Apr 12

PMID 33844879

Citations 16

Authors

Fabio Dionigi

Jing Zhu

Zhenhua Zeng

Thomas Merzdorf

Hannes Sarodnik

Manuel Gliech

Lujin Pan

Wei-Xue Li

Jeffrey Greeley

Peter Strasser

Affiliations

Soon will be listed here.

Abstract

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 (II)M (III) LDH and β-M (OH) electrocatalysts (M =Ni, Co, and M =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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