功函数工程调控Mo<sub>2</sub>C MXene的Mo 4<i>d</i>电子结构以提升光催化产氢效率

引用本文: 刘瑞云, 王苹, 王雪飞, 陈峰, 余火根. 功函数工程调控Mo₂C MXene的Mo 4d电子结构以提升光催化产氢效率[J]. 物理化学学报, 2025, 41(11): 100137. doi: 10.1016/j.actphy.2025.100137 shu

Citation: Ruiyun Liu, Ping Wang, Xuefei Wang, Feng Chen, Huogen Yu. Work-function-engineered Mo 4d electronic structure modulation in Mo₂C MXene cocatalyst for efficient photocatalytic H₂ evolution[J]. Acta Physico-Chimica Sinica, 2025, 41(11): 100137. doi: 10.1016/j.actphy.2025.100137 shu

功函数工程调控Mo₂C MXene的Mo 4d电子结构以提升光催化产氢效率

刘瑞云 ^1, ,
王苹 ^{1,
,} ,
王雪飞 ^1, ,
陈峰 ^1, ,
余火根 ^{2,
,}

1.
武汉理工大学化学化工与生命科学学院, 湖北武汉 430070
2.
中国地质大学(武汉)材料与化学学院太阳能燃料实验室, 湖北武汉 430074

通讯作者: 王苹, wangping0904@whut.edu.cn; 余火根, yuhuogen@cug.edu.cn

基金项目:
国家自然科学基金 22472127

国家自然科学基金 22178275

国家自然科学基金 U22A20147

湖北省自然科学基金 2022CFA001

摘要: Mo₂C MXene(Mo₂CT_x)由于其表面Mo活性位点具有类Pt的电子结构在光催化中展现出优异的析氢潜力。然而，Mo₂CT_x中的Mo位点在析氢反应(HER)过程中通常表现出过强的H吸附能力，显著限制了Mo₂CT_x的本征催化活性。为了削弱Mo活性位点的H吸附能力，本论文通过功函数诱导效应原位构建MoC-Mo₂C MXene异质结，实现了d轨道电子的调控。利用Co诱导的熔盐法将Mo₂C MXene原位转化为MoC，随后通过简单的超声辅助方法与TiO₂耦合，制备了MoC-Mo₂CT_x/TiO₂光催化剂。光催化产氢测试表明，最优的MoC-Mo₂CT_x/TiO₂样品实现了1886 μmol∙h⁻¹∙g⁻¹的产氢速率，分别是TiO₂和Mo₂CF_x/TiO₂(Mo₂CF_x通过常规蚀刻剂NH₄F+HCl制备)的117.9倍和3.9倍。实验和理论计算证实，MoC与Mo₂C MXene之间的功函数梯度诱导电子从MoC向Mo₂C MXene转移，从而削弱了Mo₂CT_x助催化剂中Mo活性位点的H吸附能力，进而提升了其HER活性。该研究为原位构建基于Mo₂C MXene的异质结以调控Mo活性位点的H吸附能力提供了一种新策略。

关键词:

English

Work-function-engineered Mo 4d electronic structure modulation in Mo₂C MXene cocatalyst for efficient photocatalytic H₂ evolution

Ruiyun Liu ^1, ,
Ping Wang ^{1,
,} ,
Xuefei Wang ^1, ,
Feng Chen ^1, ,
Huogen Yu ^{2,
,}

1.
School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, Hubei Province, China
2.
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, Hubei Province, China

Corresponding author: Email: wangping0904@whut.edu.cn (P. Wang); Email: yuhuogen@cug.edu.cn (H. Yu)

Received Date: 29 June 2025
Accepted Date: 24 July 2025
Revised Date: 22 July 2025
Available Online: 15 November 2025
Fund Project:
the National Natural Science Foundation of China

the National Natural Science Foundation of China

the National Natural Science Foundation of China

the Natural Science Foundation of Hubei Province of China

Abstract: Mo₂C MXene (Mo₂CT_x) exhibits exceptional hydrogen-evolution potential in photocatalysis due to the Pt-like electronic structure of surface Mo active sites. However, the Mo sites in Mo₂CT_x usually show excessively strong H-adsorption during HER, significantly limiting the intrinsic catalytic activity of Mo₂CT_x. To weaken the H-adsorption capacity of Mo active sites, a strategy of modulating d-orbital electron is implemented via in-situ constructing MoC-Mo₂C MXene heterojunction by a work-function-induced effect. The MoC-Mo₂CT_x heterojunction was synthesized by in situ conversion of Mo₂C MXene into MoC via a Co-induced molten salt method, followed by coupling with TiO₂ through a simple ultrasonication-assisted method to prepare the MoC-Mo₂CT_x/TiO₂ photocatalyst. Photocatalytic tests showed that the optimal MoC-Mo₂CT_x/TiO₂ sample achieves an excellent hydrogen production rate of 1886 μmol∙h⁻¹∙g⁻¹, representing 117.9 and 3.9 fold enhancements over TiO₂ and Mo₂CF_X/TiO₂ (Mo₂CF₂ prepared by a conventional etchant NH₄F+HCl), respectively. Experimental and theoretical calculations substantiate that the work-function gradient between MoC and Mo₂C MXene induces electron transfer from MoC to Mo₂C MXene to weaken the H-adsorption of Mo active sites in Mo₂CT_x cocatalyst, thereby enhancing its HER activity. This research provides a new strategy of in situ constructing Mo₂C MXene-based heterojunction for adjusting the H-adsorption capacity of Mo active sites.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

功函数工程调控Mo₂C MXene的Mo 4d电子结构以提升光催化产氢效率

通讯作者: 王苹, wangping0904@whut.edu.cn; 余火根, yuhuogen@cug.edu.cn

English

Work-function-engineered Mo 4d electronic structure modulation in Mo₂C MXene cocatalyst for efficient photocatalytic H₂ evolution

Corresponding author: Email: wangping0904@whut.edu.cn (P. Wang); Email: yuhuogen@cug.edu.cn (H. Yu)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

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CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

功函数工程调控Mo2C MXene的Mo 4d电子结构以提升光催化产氢效率

通讯作者: 王苹, wangping0904@whut.edu.cn; 余火根, yuhuogen@cug.edu.cn

English

Work-function-engineered Mo 4d electronic structure modulation in Mo2C MXene cocatalyst for efficient photocatalytic H2 evolution

Corresponding author: Email: wangping0904@whut.edu.cn (P. Wang); Email: yuhuogen@cug.edu.cn (H. Yu)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

功函数工程调控Mo₂C MXene的Mo 4d电子结构以提升光催化产氢效率

Work-function-engineered Mo 4d electronic structure modulation in Mo₂C MXene cocatalyst for efficient photocatalytic H₂ evolution

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs