Ligand engineering enhances (photo) electrocatalytic activity and stability of zeolitic imidazolate frameworks via in-situ surface reconstruction

Zheao Huang, Zhouzhou Wang, Hannah Rabl, Shaghayegh Naghdi, Qiancheng Zhou, Sabine Schwarz, Dogukan Hazar Apaydin, Ying Yu () and Dominik Eder ()
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Zheao Huang: Technische Universität Wien
Zhouzhou Wang: College of Physical Science and Technology, Central China Normal University
Hannah Rabl: Technische Universität Wien
Shaghayegh Naghdi: Technische Universität Wien
Qiancheng Zhou: College of Physical Science and Technology, Central China Normal University
Sabine Schwarz: Technische Universität Wien
Dogukan Hazar Apaydin: Technische Universität Wien
Ying Yu: College of Physical Science and Technology, Central China Normal University
Dominik Eder: Technische Universität Wien

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract The current limitations in utilizing metal-organic frameworks for (photo)electrochemical applications stem from their diminished electrochemical stability. In our study, we illustrate a method to bolster the activity and stability of (photo)electrocatalytically active metal-organic frameworks through ligand engineering. We synthesize four distinct mixed-ligand versions of zeolitic imidazolate framework-67, and conduct a comprehensive investigation into the structural evolution and self-reconstruction during electrocatalytic oxygen evolution reactions. In contrast to the conventional single-ligand ZIF, where the framework undergoes a complete transformation into CoOOH via a stepwise oxidation, the ligand-engineered zeolitic imidazolate frameworks manage to preserve the fundamental framework structure by in-situ forming a protective cobalt (oxy)hydroxide layer on the surface. This surface reconstruction facilitates both conductivity and catalytic activity by one order of magnitude and considerably enhances the (photo)electrochemical stability. This work highlights the vital role of ligand engineering for designing advanced and stable metal-organic frameworks for photo- and electrocatalysis.

Date: 2024
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DOI: 10.1038/s41467-024-53385-0

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