异质结工程调控Mo<sub>2</sub>C MXene助剂上H*的吸附亲和力以实现高效光催化产氢

引用本文: 柯晓春, 钟威, 王中辽, 张金锋, 代凯. 异质结工程调控Mo₂C MXene助剂上H*的吸附亲和力以实现高效光催化产氢[J]. 物理化学学报, 2026, 42(11): 100372. doi: 10.1016/j.actphy.2026.100372 shu

Citation: Xiaochun Ke, Wei Zhong, Zhongliao Wang, Jinfeng Zhang, Kai Dai. 异质结工程调控Mo₂C MXene助剂上H*的吸附亲和力以实现高效光催化产氢[J]. Acta Physico-Chimica Sinica, 2026, 42(11): 100372. doi: 10.1016/j.actphy.2026.100372 shu

异质结工程调控Mo₂C MXene助剂上H*的吸附亲和力以实现高效光催化产氢

柯晓春 ^1, ,
钟威 ^{2,
,} ,
王中辽 ^3, ,
张金锋 ^{3,
,} ,
代凯 ^{3,
,}

1.
安庆师范大学化学化工学院, 安徽省先进催化与能源材料重点实验室, 光电磁功能配合物和纳米配合物安徽省重点实验室, 安徽安庆 261433;
2.
深圳技术大学新材料与新能源学院, 广东深圳 518118;
3.
淮北师范大学化学与化工学院, 绿色和精准合成化学及应用教育部重点实验室, 淮北市小分子资源低碳转化重点实验室, 安徽淮北 235000

通讯作者: 钟威,E-mail:zhongwei@sztu.edu.cn; 张金锋,E-mail:jfzhang@chnu.edu.cn; 代凯,E-mail:daikai940@chnu.edu.cn

基金项目:
本研究得到了国家自然科学基金(22402126、52402116、22278169和22578154)；污染物分析与资源化技术湖北省重点实验室(湖北师范大学) (PA250202)；安庆师范大学科研启动基金(257035)、深圳技术大学高层次人才自然科学基金(GDRC202535)；广东省基础与应用基础研究基金(2023A1515110535)；深圳市科技计划(RCBS20231211090522041)以及安徽省学科(专业)专业带头人培养项目(DTR2024015)的资助。

摘要: Mo₂C MXene (Mo₂CT_x)被认为是光催化产氢领域最高效的助剂之一，但其固有的助催化性能常受限于催化活性Mo原子对氢中间体(H*)过强的吸附作用。为此，本研究提出了一种巧妙的策略：通过构建Mo₂CT_x-MoSe_2-yS_y异质结助剂，调节Mo₂CT_x中活性Mo原子的H*吸附亲和力，从而有效削弱Mo-H_ads键，以实现高效的光催化产氢。具体而言，利用简便的NaBH₄辅助溶剂热法合成Mo₂CT_x-MoSe_2-yS_y异质结，随后通过超声辅助法将其与TiO₂复合，制备出了TiO₂/Mo₂CT_x-MoSe_2-yS_y复合光催化剂。结果表明，TiO₂/Mo₂CT_x-MoSe_1.5S_0.5样品表现出了优异的光催化产氢速率(1142.76 μmol g^-1 h^-1)，分别比TiO₂/Mo₂CT_x和TiO₂/Mo₂CT_x-MoSe₂高出4.76倍和1.95倍。实验表征与密度泛函理论(DFT)计算结果表明，自由电子从MoSe_1.5S_0.5定向转移至Mo₂CT_x，能向Mo₂CT_x上Mo原子的d轨道注入电子，从而形成富电子的Mo^δ^-位点。富电子的Mo^δ^-位点能够增加Mo-H_ads反键轨道的占据态，进而削弱Mo-H_ads键，使Mo₂CT_x的表面实现近乎平衡的H*吸附/脱附动力学，从而显著提升产氢性能。本研究为合理设计Mo₂CT_x基助剂以优化其活性位点效率开辟了新途径。

关键词:

English

异质结工程调控Mo₂C MXene助剂上H*的吸附亲和力以实现高效光催化产氢

Xiaochun Ke ^1, ,
Wei Zhong ^{2,
,} ,
Zhongliao Wang ^3, ,
Jinfeng Zhang ^{3,
,} ,
Kai Dai ^{3,
,}

1.
Anhui Provincial Key Laboratory of Advanced Catalysis and Energy Materials, Anhui Key Laboratory of Optoelectronic Magnetic Functional Complex and Nano Complex, School of Chemistry and Chemical Engineering, Anqing Normal University, Anqing 261433, Anhui Province, China;
2.
College of New Materials and New Energies, Shenzhen Technology University, Shenzhen 518118, Guangdong Province, China;
3.
Key Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, Huaibei Key Laboratory for Low-Carbon Conversion of Small-Molecule Resources, School of Chemistry and Chemical Engineering, Huaibei Normal University, Huaibei 235000, Anhui Province, China

Corresponding author: Wei Zhong, ; Jinfeng Zhang, ; Kai Dai,

Received Date: 04 July 2026
Accepted Date: 23 July 2026
Revised Date: 19 July 2026

Abstract: Mo₂C MXene (Mo₂CT_x)被认为是光催化产氢领域最高效的助剂之一，但其固有的助催化性能常受限于催化活性Mo原子对氢中间体(H*)过强的吸附作用。为此，本研究提出了一种巧妙的策略：通过构建Mo₂CT_x-MoSe_2-yS_y异质结助剂，调节Mo₂CT_x中活性Mo原子的H*吸附亲和力，从而有效削弱Mo-H_ads键，以实现高效的光催化产氢。具体而言，利用简便的NaBH₄辅助溶剂热法合成Mo₂CT_x-MoSe_2-yS_y异质结，随后通过超声辅助法将其与TiO₂复合，制备出了TiO₂/Mo₂CT_x-MoSe_2-yS_y复合光催化剂。结果表明，TiO₂/Mo₂CT_x-MoSe_1.5S_0.5样品表现出了优异的光催化产氢速率(1142.76 μmol g^-1 h^-1)，分别比TiO₂/Mo₂CT_x和TiO₂/Mo₂CT_x-MoSe₂高出4.76倍和1.95倍。实验表征与密度泛函理论(DFT)计算结果表明，自由电子从MoSe_1.5S_0.5定向转移至Mo₂CT_x，能向Mo₂CT_x上Mo原子的d轨道注入电子，从而形成富电子的Mo^δ^-位点。富电子的Mo^δ^-位点能够增加Mo-H_ads反键轨道的占据态，进而削弱Mo-H_ads键，使Mo₂CT_x的表面实现近乎平衡的H*吸附/脱附动力学，从而显著提升产氢性能。本研究为合理设计Mo₂CT_x基助剂以优化其活性位点效率开辟了新途径。

Key words:

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异质结工程调控Mo₂C MXene助剂上H*的吸附亲和力以实现高效光催化产氢

通讯作者: 钟威,E-mail:zhongwei@sztu.edu.cn; 张金锋,E-mail:jfzhang@chnu.edu.cn; 代凯,E-mail:daikai940@chnu.edu.cn

English

异质结工程调控Mo₂C MXene助剂上H*的吸附亲和力以实现高效光催化产氢

Corresponding author: Wei Zhong, ; Jinfeng Zhang, ; Kai Dai,

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？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

异质结工程调控Mo2C MXene助剂上H*的吸附亲和力以实现高效光催化产氢

通讯作者: 钟威,E-mail:zhongwei@sztu.edu.cn; 张金锋,E-mail:jfzhang@chnu.edu.cn; 代凯,E-mail:daikai940@chnu.edu.cn

English

异质结工程调控Mo2C MXene助剂上H*的吸附亲和力以实现高效光催化产氢

Corresponding author: Wei Zhong, ; Jinfeng Zhang, ; Kai Dai,

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

异质结工程调控Mo₂C MXene助剂上H*的吸附亲和力以实现高效光催化产氢

异质结工程调控Mo₂C MXene助剂上H*的吸附亲和力以实现高效光催化产氢

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs