MXene-Based Hierarchical Electron Coupling Engineering of F-Doped NiFe LDH/MOF-74 Electrocatalysts for Efficient Overall Water Splitting

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-01-28 DOI:10.1021/acscatal.4c07798

Jibo Jiang, Chang Xi, Yun Zhao, Yu Zhu, Kairan Hu, Yucheng Wang, Shilong Wang, Ziyun Zhang, Sheng Han

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引用次数: 0

Abstract

Enhancing the intrinsic activity and exposing the real active sites in transition metal-based electrocatalysts are still a formidable challenge. In this work, we introduce an efficient partial in situ transformation strategy (PTS) that converts the NiFe MOF-74 precursor into NiFe LDH@MOF composite structure, and subsequently the incoming F coordinates accelerate the structural reconstruction of F-doped NiFe LDH@MOF on MXene (F_d-PTS-NLM) during overall water splitting. The electrocatalytic mechanism exploration reveal that the rate of electron transfer in a material can be modulated by manipulating the electron diffusion process, thereby reducing the energy barrier associated with catalytic reactions. F-doping and PTS strategies effectively modify the d-band center and significantly improve the bifunctional activity of the catalyst. The results of in situ Raman characterization of F_d-PTS-NLM proved that metal hydroxyl oxides are the real active species in the OER reaction. In alignment with anticipated outcomes, the catalysts exhibited impressive electrochemical performance, with overpotentials of 150 mV and 171 mV for HER and OER at current densities of 10 mA cm^–2. Furthermore, a mere cell overpotential of 1.50 V was sufficient to generate a 10 mA cm^–2 current density in a two-electrode setup, F_d-PTS-NLM exhibited Faraday efficiencies (FEs) approaching 100%. The endurance of this material highlights its potential to minimize expenses in widespread industrial uses.

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用于高效整体水分离的掺杂 F 的 NiFe LDH/MOF-74 电催化剂的基于 MXene 的分层电子耦合工程

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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.