Structural Reconstruction of a Cobalt- and Ferrocene-Based Metal–Organic Framework during the Electrochemical Oxygen Evolution Reaction,ACS Applied Materials & Interfaces

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Structural Reconstruction of a Cobalt- and Ferrocene-Based Metal–Organic Framework during the Electrochemical Oxygen Evolution Reaction
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2024-07-23 , DOI: 10.1021/acsami.4c03262
Thomas Doughty ₁ , Andrea Zingl ₂ , Maximilian Wünschek ₂ , Christian M Pichler _{2,

3} , Matthew B Watkins ₄ , Souvik Roy ₁

Affiliation

Metal–organic frameworks (MOFs) are increasingly being investigated as electrocatalysts for the oxygen evolution reaction (OER) due to their unique modular structures that present a hybrid between molecular and heterogeneous catalysts, featuring well-defined active sites. However, many fundamental questions remain open regarding the electrochemical stability of MOFs, structural reconstruction of coordination sites, and the role of in situ-formed species. Here, we report the structural transformation of a surface-grown MOF containing cobalt nodes and 1,1′-ferrocenedicarboxylic acid linkers (denoted as CoFc-MOF) during the OER in alkaline electrolyte. Ex situ and in situ investigations of CoFc-MOF film suggest that the MOF acts as a precatalyst and undergoes a two-step restructuring process under operating conditions to generate a metal oxyhydroxide phase. The MOF-derived metal oxyhydroxide catalyst, supported on nickel foam electrodes, displays high activity toward the OER with an overpotential of 190 mV at a current density of 10 mA cm^–2. While this study demonstrates the necessity of investigating structural evolution of MOFs during electrocatalysis, it also shows the potential of using MOFs as precursors in catalyst design.

中文翻译：

电化学析氧反应过程中钴基和二茂铁基金属有机框架的结构重建

金属有机框架（MOF）作为析氧反应（OER）的电催化剂越来越多地被研究，因为它们具有独特的模块化结构，呈现出分子催化剂和非均相催化剂之间的混合体，并具有明确的活性位点。然而，关于 MOF 的电化学稳定性、配位位点的结构重建以及原位形成物质的作用，许多基本问题仍然悬而未决。在这里，我们报告了含有钴节点和 1,1'-二茂铁二甲酸连接体（表示为 CoFc-MOF）的表面生长 MOF 在碱性电解质中 OER 过程中的结构转变。 CoFc-MOF 薄膜的异位和原位研究表明，MOF 作为预催化剂，在操作条件下经历两步重组过程，生成金属羟基氧化物相。 MOF 衍生的金属羟基氧化物催化剂负载在泡沫镍电极上，对 OER 显示出高活性，在 10 mA cm ^–2的电流密度下具有 190 mV 的过电势。虽然这项研究证明了研究电催化过程中 MOF 结构演化的必要性，但它也表明了在催化剂设计中使用 MOF 作为前体的潜力。

更新日期：2024-07-23

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