Electro-Bendable Metal–Organic Framework Nanosheets Enable Durable Electrocatalytic Water Oxidation at 1 A/cm2

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-05-16 DOI:10.1021/acscatal.5c02167

Yuanwu Liu, Lirong Wang, Congcong Liu, Johannes Kresse, Marielle Deconinck, René Hübner, Daria Mikhailova, Yana Vaynzof, Xiaoming Zhang, Alexander Eychmüller

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Abstract

The oxygen evolution reaction (OER) is a pivotal process in electrochemical systems, including metal-air batteries and water-splitting technologies. Despite the promise of metal–organic frameworks (MOFs) as OER electrocatalysts, their stability at elevated current densities (>500 mA cm^–2) remains a key challenge for industrial applications. Herein, we developed a bimetallic MOF electrocatalyst, Fe_8.47Ni_91.53-2-amino-1,4-benzendedicarboxylate (Fe_8.47Ni_91.53-BDC-NH₂), exhibiting good stability at 1 A cm^–2 for 100 h, with overpotentials of only 210 mV at 10 mA cm^–2 and 273 mV at 100 mA cm^–2. The enhanced activity of the catalyst originates from the bending of freestanding FeNi-BDC-NH₂ nanosheets toward the nickel foam substrate during the OER, facilitating the formation of enlarged Mott–Schottky regions and accelerating electron transfer. Additionally, the reversible structural transformation of Ni-2-amino-1,4-benzendedicarboxylate (Ni-BDC-NH₂) during the OER, coupled with the introduction of Fe ions, effectively prevents the overoxidation of the active β-NiOOH intermediate to γ-NiOOH, further boosting the OER performance. This work provides insights into structural and electronic modifications that enable MOFs to achieve both high performance and stability at industrial current densities.

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电可弯曲金属-有机框架纳米片在1 A/cm2下实现持久的电催化水氧化

析氧反应（OER）是电化学系统的关键过程，包括金属-空气电池和水分解技术。尽管金属有机框架（mof）有望成为OER电催化剂，但其在高电流密度（>500 mA cm-2）下的稳定性仍然是工业应用的关键挑战。在此，我们开发了一种双金属MOF电催化剂fe8.47 ni91.53 -2-氨基-1,4-苯三羧酸盐（Fe8.47Ni91.53-BDC-NH2），在1 a cm-2下具有良好的稳定性100 h，在10 mA cm-2下过电位仅为210 mV，在100 mA cm-2下过电位仅为273 mV。催化剂活性的增强是由于在OER过程中，独立的FeNi-BDC-NH2纳米片向泡沫镍基底弯曲，促进了Mott-Schottky区域的形成，加速了电子转移。此外，在OER过程中，ni -2-氨基-1,4-苯三羧酸盐（Ni-BDC-NH2）的可逆结构转变，加上Fe离子的引入，有效地阻止了活性β-NiOOH中间体过度氧化为γ-NiOOH，进一步提高了OER性能。这项工作提供了结构和电子修改的见解，使mof能够在工业电流密度下实现高性能和稳定性。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.