电荷-光热-催化协同提升ZnCdS/Co2SnO4光催化产氢与苯甲醇氧化性能

doi:10.1016/S1872-2067(26)65183-2

催化学报 ›› 2026, Vol. 90: 184-196.DOI: 10.1016/S1872-2067(26)65183-2

电荷-光热-催化协同提升ZnCdS/Co₂SnO₄光催化产氢与苯甲醇氧化性能

张晓^a^,^b^,¹, 王雨欣^b^,¹, 孙书涵^b, 熊贤强^b^,^c^,^*(), 李覃^a, 吕康乐^a^,^*()

^a 中南民族大学资源与环境学院, 湖北武汉 430074
^b 台州学院医药化工学院, 浙江台州 318000
^c 台州市生物医化产业研究院有限公司, 浙江台州 318000

收稿日期:2026-01-27 接受日期:2026-04-01 出版日期:2026-11-18 发布日期:2026-09-09
通讯作者: *电子信箱: 11337061@zju.edu.cn (熊贤强),
lvkangle@mail.scuec.edu.cn (吕康乐).
作者简介:¹共同第一作者.
基金资助:
国家自然科学基金(22272115);国家自然科学基金(51672312);浙江省自然科学基金(LMS26E020023);台州市科技计划项目(25gyb87);2025年度“尖兵领雁+X”科技计划(2025C02218);中南民族大学中央高校基本科研业务费专项资金(CZZ25013);中南民族大学学术创新团队经费项目(XTZ24019);中南民族大学实验室研究项目(SYYJ2025020);中南民族大学实验室研究项目(SYYJ2025022)

Charge-photothermal-catalysis synergy in ZnCdS/Co₂SnO₄ for enhanced photocatalytic hydrogen evolution and benzyl alcohol oxidation

Xiao Zhang^a^,^b^,¹, Yuxin Wang^b^,¹, Shuhan Sun^b, Xianqiang Xiong^b^,^c^,^*(), Qin Li^a, Kangle Lv^a^,^*()

^a College of Resources and Environment, South-Central Minzu University, Wuhan 430074, Hubei, China
^b School of Pharmaceutical and Chemical Engineering, Taizhou University, Taizhou 318000, Zhejiang, China
^c Taizhou Biomedical and Chemistry Industry Institute, Taizhou 318000, Zhejiang, China

Received:2026-01-27 Accepted:2026-04-01 Online:2026-11-18 Published:2026-09-09
Contact: *E-mail:11337061@zju.edu.cn(X. Xiong),lvkangle@mail.scuec.edu.cn(K. Lv).
About author:¹Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(22272115);National Natural Science Foundation of China(51672312);Zhejiang Provincial Natural Science Foundation of China(LMS26E020023);Taizhou City Science and Technology Plan Project(25gyb87);“Lingyan” R&D Plan Project of Zhejiang Province(2025C02218);Fundamental Research Funds for the Central Universities of South-Central Minzu University(CZZ25013);Fund for Academic Innovation Teams of South-Central Minzu University of China(XTZ24019);Laboratory Research Project of South-Central Minzu University(SYYJ2025020);Laboratory Research Project of South-Central Minzu University(SYYJ2025022)

摘要/Abstract

摘要：

开发能够同时高效驱动析氢与有机氧化的双功能光催化剂是光催化领域的研究前沿与难点, 其核心挑战在于如何协同优化电荷分离、光谱吸收与表面反应动力学这三个相互制约的关键环节. 该工作通过构筑ZnCdS/Co₂SnO₄ (ZCS/CSO)梯型(S型)异质结, 成功克服了这一挑战. 其中, 尖晶石型CSO被创新性地设计为一个三功能协同模块, 实现了光、电荷、热能的协同管理.

首先, CSO作为S型异质结的理想还原组分, 与ZCS形成的内建电场驱动了定向的界面电荷转移, 在实现光生电子与空穴高效空间分离的同时, 最大限度地保留了载流子的高氧化还原电位. 其次, CSO的窄带隙特性使其成为高效的光热转换单元, 能够将通常被浪费的近红外光转化为局域热能, 使催化剂表面温度有效提升. 实验与动力学分析表明, 该光热效应将析氢反应的表观活化能从13.17 kJ mol^-1降至11.96 kJ mol^-1, 从热力学上加速了反应进程. 再者, CSO自身富含的Co活性位点展现出接近理想的氢吸附自由能(ΔG_H* ≈ 0.30 eV), 其尖晶石表面可作为优异的本征催化位点, 显著提升了质子还原的动力学速率. 这种“电荷分离-光热转换-表面催化”的三元协同机制产生了显著的性能增益. 优化后的ZCS/CSO-7%异质结在可见-近红外全光谱照射下, 实现了H₂与苯甲醛的高效联产, 其产率分别达到31.7和28.8 mmol g^-1 h^-1, 分别是纯ZCS的4.93倍和5.8倍, 并展现出优异的循环稳定性. 通过系统的原位表征、光电化学测试及理论计算, 完整阐明了上述多机制协同作用的本质.

综上, 该工作为ZCS基光催化剂的设计提供了全新的多功能集成策略, 也为构建面向实际应用的全光谱响应、高效人工光合系统提供了新的设计范式, 即通过对光能、电荷与热能进行协同管理, 从而突破传统光催化体系的性能瓶颈.

关键词: ZnCdS/Co₂SnO₄异质结, S型电荷转移, 光热催化, 析氢反应, 苯甲醇氧化

Abstract:

The development of efficient bifunctional photocatalysts for simultaneous H₂ evolution and organic oxidation is impeded by the difficulty in synergizing charge separation, broad-spectrum light harvesting, and surface reaction kinetics. This challenge is addressed through the construction of a ZnCdS/Co₂SnO₄ S-scheme heterojunction, in which Co₂SnO₄ is engineered as a triple-function module. This module not only establishes an interfacial electric field for directed S-scheme charge transfer, preserving high-potential carriers, but also acts as a potent photothermal agent, converting near-infrared light into localized heat to reduce the apparent activation energy for H₂ evolution. Furthermore, its spinel surface provides intrinsic catalytic sites with a near-optimal hydrogen adsorption free energy. This triadic synergy yields exceptional concurrent production of H₂ (31.7 mmol g^-1 h^-1) and benzaldehyde (28.8 mmol g^-1 h^-1). Our work provides a paradigm of concerted light-charge-heat management for designing advanced, full-spectrum-responsive photocatalytic systems.

Key words: ZnCdS/Co₂SnO₄, S-scheme heterojunction, Photothermal catalysis, Photocatalytic hydrogen evolution, Benzyl alcohol oxidation

张晓, 王雨欣, 孙书涵, 熊贤强, 李覃, 吕康乐. 电荷-光热-催化协同提升ZnCdS/Co₂SnO₄光催化产氢与苯甲醇氧化性能[J]. 催化学报, 2026, 90: 184-196.

Xiao Zhang, Yuxin Wang, Shuhan Sun, Xianqiang Xiong, Qin Li, Kangle Lv. Charge-photothermal-catalysis synergy in ZnCdS/Co₂SnO₄ for enhanced photocatalytic hydrogen evolution and benzyl alcohol oxidation[J]. Chinese Journal of Catalysis, 2026, 90: 184-196.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65183-2

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图/表 5

Fig. 1. (a) Schematic of heterojunction preparation procedure. (b) XRD patterns of ZCS, CSO, and ZCS/CSO-x% heterojunction. TEM (c) and HRTEM (d) images of ZCS/CSO-7%. (e) Elemental mapping images of ZCS/CSO-7% composite. (f) N2 physisorption isotherms of ZCS, CSO, and ZCS/CSO-7% heterojunction.

Fig. 2. (a) Time-course profile of H2 production. (b) Production rate of H2 and BAD along with selectivity for BAD. (c) Probing the reaction pathway via in-situ DRIFTS during BA oxidation. (d) AQE across different wavelengths. (e) Benchmarking H2 evolution activity against reported ZCS composites (data in Table S2). (f) Testing the photocatalytic stability through recycling runs.

Fig. 3. Calculated work functions for CSO (a) and ZCS (b). Deduced energy band alignment (c) and charge density difference (d) for the ZCS/CSO-7% composite. High-resolution XPS and in-situ irradiated high-resolution XPS spectra of CSO, ZCS, and ZCS/CSO-7% samples: Cd 3d (e) and Sn 3d (f). 2D TA spectra (g,h) and kinetics decay traces (i) probed at 550 nm for ZCS and ZCS/CSO-7%, respectively.

Fig. 4. (a) Photocatalytic H2 generation curves at various temperatures. (b) Infrared thermal images comparing ZCS and the ZCS/CSO-7% composite under visible (Vis) and full-spectrum (Vis-NIR) irradiation during HER testing. (c) Recording the temperature evolution and distribution through thermal mapping under different light sources (Vis and Vis-NIR).

Fig. 5. (a) Presenting the DFT-calculated hydrogen adsorption free energy profile. (b) Transient photocurrent response curves of ZCS, CSO, and ZCS/CSO-7%. (c) Measuring surface wettability via contact angles. (d) EIS spectra. (e) Temperature dependence of H2 evolution rates and comparison of apparent activation energies for ZCS and ZCS/CSO-7%. (f) Illustrating the proposed synergistic photocatalytic mechanism.

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电荷-光热-催化协同提升ZnCdS/Co₂SnO₄光催化产氢与苯甲醇氧化性能

Charge-photothermal-catalysis synergy in ZnCdS/Co₂SnO₄ for enhanced photocatalytic hydrogen evolution and benzyl alcohol oxidation

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