In-situ Pt reduction induced topological transformation of NiFe-MOF for industrial seawater splitting

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis Pub Date : 2025-05-01 DOI:10.1016/S1872-2067(24)60271-8

Guohao Na , Hongshun Zheng , Mingpeng Chen , Huachuan Sun , Yuewen Wu , Dequan Li , Yun Chen , Boran Zhao , Bo Zhao , Tong Zhou , Tianwei He , Yuxiao Zhang , Jianhong Zhao , Yumin Zhang , Jin Zhang , Feng Liu , Hao Cui , Qingju Liu

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引用次数: 0

Abstract

Metal-support interaction (MSI) is regarded as an indispensable manner to stabilize active metals and modulate catalytic activity, which shows great potentials in developing of efficient hydrogen evolution reaction (HER) electrode with high activity and strong robustness. Herein, this work presents a novel heterostructure with ultrafine platinum quantum dots (Pt QDs) on defective catalytic supports derived from metal-organic frameworks (MOFs). It is indicated substantial oxygen vacancies can be generated and Pt–Pt bonds can be optimized through topological transformation. The resulting Pt/T-NiFe-BDC (BDC: C₈H₆O₄) exhibits competitive HER activity in alkaline seawater, attaining ultralow overpotentials of 158 and 266 mV at 500 and 1000 mA cm^–2 with fast kinetics and outstanding stability. An asymmetric water electrolyzer using Pt/T-NiFe-BDC as a cathode only requires a voltage of 1.89 V to generate an industrial density of 1000 mA cm^–2 and shows no attenuation in 500-h continuous test at 500 mA cm^–2. Theoretical calculations and in-situ spectroscopic analysis reveal the reversible hydrogen spillover mechanism, in which oxygen vacancies facilitate the sluggish water dissociation and Pt QDs promote the H* combination. This study provides a new paradigm to engineer metal-supported catalysts for efficient and robust seawater splitting.

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原位还原Pt诱导NiFe-MOF在工业海水裂解中的拓扑转变

金属-载体相互作用（MSI）被认为是稳定活性金属和调节催化活性的重要手段，在开发高活性、强鲁棒性的高效析氢反应（HER）电极方面具有很大的潜力。本文提出了一种新型异质结构，其超细铂量子点（Pt QDs）位于金属有机框架（MOFs）的缺陷催化载体上。结果表明，通过拓扑转化可以产生大量的氧空位，并优化Pt-Pt键。得到的Pt/ t - nfe -BDC （BDC: C8H6O4）在碱性海水中表现出竞争性的HER活性，在500和1000 mA cm-2下可达到158和266 mV的超低过电位，动力学快，稳定性好。使用Pt/ t - nfe - bdc作为阴极的不对称水电解槽只需要1.89 V的电压就能产生1000 mA cm-2的工业密度，并且在500 mA cm-2下连续测试500小时没有衰减。理论计算和原位光谱分析揭示了可逆的氢溢出机制，其中氧空位促进了缓慢的水解离，Pt量子点促进了H*结合。该研究为设计金属负载催化剂以实现高效、稳健的海水裂解提供了新的范例。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Chinese Journal of Catalysis 工程技术-工程：化工

CiteScore

25.80

自引率

10.30%

发文量

235

审稿时长

1.2 months

期刊介绍： The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.