Transition Metal Carbonitride MXenes Anchored with Pt Sub-Nanometer Clusters to Achieve High-Performance Hydrogen Evolution Reaction at All pH Range

文献类型： 外文期刊

第一作者： Lei, Zhihao

作者： Lei, Zhihao;Ahmed, Muhammadibrar;Guan, Xinwei;Perumalsamy, Vibin;Fawaz, Mohammed;Yang, Jae-Hun;Bououdina, Mohamed;Vinu, Ajayan;Ali, Sajjad;Qu, Jiangtao;Zheng, Rongkun;Xi, Shibo;Yu, Xiaojiang;Breese, M. B. H.;Liu, Chao;Zhang, Jizhen;Qi, Shuai;Domen, Kazunari;Qiao, Liang;Yi, Jiabao

作者机构：

关键词： MXene; Hydrogen evolution reaction; Single atom; Two-dimensional nanosheets; Density functional theory

期刊名称：NANO-MICRO LETTERS （ 影响因子：36.3； 五年影响因子：30.1 ）

ISSN： 2311-6706

年卷期： 2025 年 17 卷 1 期

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收录情况： SCI

摘要： Transition metal carbides, known as MXenes, particularly Ti3C2Tx, have been extensively explored as promising materials for electrochemical reactions. However, transition metal carbonitride MXenes with high nitrogen content for electrochemical reactions are rarely reported. In this work, transition metal carbonitride MXenes incorporated with Pt-based electrocatalysts, ranging from single atoms to sub-nanometer dimensions, are explored for hydrogen evolution reaction (HER). The fabricated Pt clusters/MXene catalyst exhibits superior HER performance compared to the single-atom-incorporated MXene and commercial Pt/C catalyst in both acidic and alkaline electrolytes. The optimized sample shows low overpotentials of 28, 65, and 154 mV at a current densities of 10, 100, and 500 mA cm-2, a small Tafel slope of 29 mV dec-1, a high mass activity of 1203 mA mgPt-1 and an excellent turnover frequency of 6.1 s-1 in the acidic electrolyte. Density functional theory calculations indicate that this high performance can be attributed to the enhanced active sites, increased surface functional groups, faster charge transfer dynamics, and stronger electronic interaction between Pt and MXene, resulting in optimized hydrogen absorption/desorption toward better HER. This work demonstrates that MXenes with a high content of nitrogen may be promising candidates for various catalytic reactions by incorporating single atoms or clusters.

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