Zheao Huang, Zhouzhou Wang, Qiancheng Zhou, Hannah Rabl, Dr. Shaghayegh Naghdi, Dr. Ze Yang, Prof. Dominik Eder
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引用次数: 0
Abstract
Currently, lack of ways to engineer specific and well-defined active sites in zeolitic imidazolate frameworks (ZIFs) limits our fundamental knowledge with respect to the mechanistic details for (photo)electrocatalytic hydrogen evolution reaction (HER). Here, we introduce the open metal sites into ZIFs through the selective ligand removal (SeLiRe) strategy, comprehensively characterize the altered structural and electronic features, and evaluate their role in HER. In situ electrochemical analysis and X-ray absorption spectroscopy reveal the formation of high-valence HO−Zn−N2 sites through the binding of Zn−N2 with electrolyte hydroxide. The optimal OMS-ZIF exhibits a low overpotential of 0.41 V to achieve an ampere-level 1.0 A cm−2 with 120-hour stability. Theoretical simulations indicate that these active sites accelerate the water molecules activation kinetics, consequently enhancing the efficiency of the Volmer step. This work demonstrates a versatile strategy to introduce highly active catalytic sites in ZIFs, providing new insights into the electrocatalytic mechanism in alkaline media.
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.