open access publication

Article, 2024

In Situ Tracking of Water Oxidation Generated Nanoscale Dynamics in Layered Double Hydroxides Nanosheets

Journal of the American Chemical Society, ISSN 0002-7863, 1520-5126, Volume 146, 25, Pages 17032-17040, 10.1021/jacs.4c01035

Contributors

Wang, Yuqing 0000-0002-5853-932X [1] Chen, Chao [2] Xiong, Xuya 0000-0001-9554-1974 [1] Skaanvik, Sebastian Amland [1] Zhang, Yuge [1] Bøjesen, Espen Drath 0000-0002-9352-9514 [1] Wang, Ze-Gao 0000-0002-0033-6538 (Corresponding author) [1] [3] Liu, Wei (Corresponding author) [2] Dong, Ming-Dong 0000-0002-2025-2171 (Corresponding author) [1]

Affiliations

  1. [1] Aarhus University
    2. [NORA names: AU Aarhus University; University; Denmark; Europe, EU; Nordic; OECD];
  2. [2] Changchun Institute of Applied Chemistry
    3. [NORA names: China; Asia, East];
  3. [3] Sichuan University
    4. [NORA names: China; Asia, East]

Abstract

Layered double hydroxides (LDHs) are potential catalysts for water oxidation, and it is recognized that they undergo dynamic evolution during the operation. However, little is known about the interfacial behaviors at the nanoscale under working conditions nor the underlying effects on electrocatalytic performance. Herein, using electrochemical atomic force microscopy, we in situ visualize the heterogeneous evolution of LDH nanosheets during oxygen evolution reaction (OER). By further combining density functional theory calculations, we elucidate the origin of the heterogeneous dynamics and their impact on the OER efficiency. Our findings demonstrate that NiCo LDHs transform to the catalytically active NiCoOx(OH)2-x phase during OER, and the redox transition between is accompanied by compressive and tensile strain, leading to in-plane contraction and reversible expansion of the nanosheets. Nonisotropic strain and out-of-plane strain relaxation due to defects and interparticle interactions result in cracking and wrinkling in the nanostructure, which is responsible for the partial activation and long-term deterioration of LDH electrocatalysts toward the OER. With this knowledge, we suggest and validate that engineering defects can precisely tune these dynamic behaviors, improving the OER activity and stability among LDH-based electrocatalysts.

Keywords

LDH nanosheets, NiCo, activity, atomic force microscopy, behavior, calculations, catalyst, catalytically, conditions, contraction, crack, defects, density, density functional theory calculations, double hydroxides, dynamic behavior, dynamic evolution, dynamics, efficiency, electrocatalysts, electrocatalytic performance, electrochemical atomic force microscopy, engineered defects, engineering, evolution, evolution reaction, expansion, findings, force microscopy, functional theory calculations, heterogeneous dynamics, heterogeneous evolution, hydroxide, hydroxide nanosheets, impact, in situ tracking, in-plane contraction, interaction, interfacial behavior, interparticle, interparticle interactions, knowledge, layered double hydroxide nanosheets, layered double hydroxides, long-term deterioration, microscopy, nanoscale, nanoscale dynamics, nanosheets, nanostructures, operation, origin, oxidation, oxygen, oxygen evolution reaction, oxygen evolution reaction activity, oxygen evolution reaction efficiency, partial activation, performance, phase, potential catalyst, reaction, redox, redox transitions, relaxation, reversible expansion, stability, strain, strain relaxation, tensile, tensile strain, theory calculations, transformation, transition, water, water oxidation, work, working conditions, wrinkles

Funders

  • Danish Agency for Science and Higher Education
  • European Commission
  • The Velux Foundations

Data Provider: Digital Science

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