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

doi:10.1016/j.actphy.2026.100372

物理化学学报 >> 2026, Vol. 42 >> Issue (11): 100372.doi: 10.1016/j.actphy.2026.100372

论文上一篇

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

收稿日期:2026-07-04 修回日期:2026-07-19 录用日期:2026-07-23 发布日期:2026-09-29
通讯作者: 钟威, 张金锋, 代凯 E-mail:zhongwei@sztu.edu.cn;jfzhang@chnu.edu.cn;daikai940@chnu.edu.cn
基金资助:
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。

Heterointerface engineering of Mo₂C MXene to modulate H* adsorption affinity for efficient photocatalytic H₂ evolution

Xiaochun Ke¹, Wei Zhong², Zhongliao Wang³, Jinfeng Zhang³, Kai Dai³

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

Received:2026-07-04 Revised:2026-07-19 Accepted:2026-07-23 Published:2026-09-29
Contact: Wei Zhong, Jinfeng Zhang, Kai Dai E-mail:zhongwei@sztu.edu.cn;jfzhang@chnu.edu.cn;daikai940@chnu.edu.cn

1. 2026.100372-ACTPHY-D-26-00487-20p-SI-2#.pdf(1641KB)

摘要/Abstract

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: 光催化产氢, 助剂, Mo₂CT_x-MoSe_2-yS_y异质结, Mo₂C MXene, 反键轨道占据态

Abstract: Mo₂C MXene (Mo₂CT_x) has been recognized as one of the most effective cocatalysts for photocatalytic H₂production, but its intrinsic cocatalytic performance are usually impeded by the strong H intermediates (H*) adsorption on catalytic Mo atoms. In this case, an ingenious strategy to modulate H* adsorption affinity of active Mo atoms in Mo₂CT_x is developed to effectively weaken Mo-H_ads bond by fabricating Mo₂CT_x-MoSe_2-yS_y heterojunction cocatalyst, achieving efficient photocatalytic H₂ production. Herein, the Mo₂CT_x-MoSe_2-yS_y heterojunction is skillfully synthesized via a facile NaBH₄-assisted solvothermal approach, followed by coupling with TiO₂ through a ultrasonication-assisted method to prepare TiO₂/Mo₂CT_x-MoSe_2-yS_y composite photocatalyst. As expected, the resultant TiO₂/Mo₂CT_x-MoSe_1.5S_0.5 sample demonstrates a superior photocatalytic H₂-production rate of 1142.76 μmol g^-1 h^-1, surpassing TiO₂/Mo₂CT_x and TiO₂/Mo₂CT_x_δ-MoSe₂ by 4.76 and 1.95 times. Characterization results and density functional theory (DFT) calculation reveal a directional free-electron transfer from MoSe_1.5S_0.5to Mo₂CT_x, thus essentially charging electrons to d orbitals of Mo atoms on Mo₂CT_x to generate electron-rich Mo^δ^- sites. The electron-rich Mo^δ^- sites can increase the antibonding-orbital occupancy of Mo-H_ads, ultimately weakening the Mo-H_ads bond for acquiring the near-balanced H* adsorption/desorption dynamics on Mo₂CT_xto boost H₂ production performance. This study opens new avenues for the rational design of Mo₂CT_x-based cocatalysts for optimizing the efficiency of active sites.

Key words: Photocatalytic H₂ production, Cocatalysts, Mo₂CT_x-MoSe_2-yS_y heterojunction, Mo₂C MXene, Antibonding-orbital occupancy

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

Xiaochun Ke, Wei Zhong, Zhongliao Wang, Jinfeng Zhang, Kai Dai. Heterointerface engineering of Mo₂C MXene to modulate H* adsorption affinity for efficient photocatalytic H₂ evolution[J]. Acta Phys. -Chim. Sin. 2026, 42(11), 100372. doi: 10.1016/j.actphy.2026.100372

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2026.100372

https://www.whxb.pku.edu.cn/CN/Y2026/V42/I11/100372

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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

Heterointerface engineering of Mo₂C MXene to modulate H* adsorption affinity for efficient photocatalytic H₂ evolution

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