S型CdS/MnO<sub>2</sub>异质结的合理构建用于高附加值甲苯光热协同催化选择性氧化

引用本文: 李振, 张素娟, 王中辽, 张金锋, 陈高礼, 陈士夫. S型CdS/MnO₂异质结的合理构建用于高附加值甲苯光热协同催化选择性氧化[J]. 物理化学学报, 2026, 42(4): 100179. doi: 10.1016/j.actphy.2025.100179 shu

Citation: Zhen Li, Sujuan Zhang, Zhongliao Wang, Jinfeng Zhang, Gaoli Chen, Shifu Chen. Rational design of S-scheme CdS/MnO₂ heterojunctions for high-value photothermal synergistic catalytic oxidation of toluene[J]. Acta Physico-Chimica Sinica, 2026, 42(4): 100179. doi: 10.1016/j.actphy.2025.100179 shu

S型CdS/MnO₂异质结的合理构建用于高附加值甲苯光热协同催化选择性氧化

绿色与精准合成化学及应用教育部重点实验室; 淮北师范大学化学与化工学院, 安徽淮北 235000

通讯作者: Email: zhangsujuancgl@163.com (张素娟); gaolichen@chnu.edu.cn (陈高礼); chshifu@chnu.edu.cn (陈士夫); Tel: +86-561-3802061 (陈士夫); Fax: +86-561-3802061 (陈士夫)

摘要: 甲苯的选择性氧化制备高附加值产物一直是催化科学中的重大挑战。为解决传统光催化效率较低的问题，本工作提出了一种光热协同策略，构筑了新型S型CdS/MnO₂异质结催化剂。通过将CdS纳米颗粒负载于具有本征光热活性的MnO₂上，形成致密的S型异质结结构，该结构可产生内建电场，有效促进光生载流子的快速分离并抑制其复合。同时，CdS的引入对MnO₂的电子能带结构进行了调控，从而提升产物选择性。得益于上述协同效应，优化后的25% CdS/MnO₂催化剂表现出优异的催化性能，在150 ℃和氧气气氛下，实现了14.1 mmol g⁻¹ h⁻¹的甲苯氧化速率，且对苯甲醇和苯甲醛的选择性高达90%。机理研究表明，电子顺磁共振和傅立叶变换红外光谱结果验证了光热协同效应在促进氧化过程中的关键作用。本研究不仅提出了构筑高效光热异质结的有效策略，也为温和条件下甲苯的选择性氧化提供了新的思路。

关键词:

English

Rational design of S-scheme CdS/MnO₂ heterojunctions for high-value photothermal synergistic catalytic oxidation of toluene

Key Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education; School of Chemistry and Chemical Engineering, Huaibei Normal University, Huaibei 235000, Anhui Province, China

Corresponding author: Email: zhangsujuancgl@163.com (Sujuan Zhang); gaolichen@chnu.edu.cn (Gaoli Chen); chshifu@chnu.edu.cn (Shifu Chen); Tel: +86-561-3802061 (Shifu Chen); Fax: +86-561-3802061 (Shifu Chen)

Received Date: 27 July 2025
Accepted Date: 02 September 2025
Revised Date: 01 September 2025
Available Online: 15 April 2026

Abstract: The targeted partial oxidation of toluene to valuable products continues to present a significant hurdle in catalytic science. To address the low efficiency of conventional photocatalysis, we developed a photothermal synergistic strategy by constructing a novel S-scheme CdS/MnO₂ heterojunction catalyst. CdS nanoparticles were anchored onto MnO₂, a material with intrinsic photothermal activity, forming a compact S-scheme heterojunction. This architecture generates an intrinsic electric field that markedly accelerates the segregation of light-induced charge carriers and inhibits their recombination. Moreover, CdS incorporation modulates the electronic band structure of MnO₂, thereby improving product selectivity. Owing to these synergistic effects, the optimized 25% CdS/MnO₂ catalyst demonstrated excellent catalytic performance, attaining a toluene oxidation rate of 14.1 mmol g⁻¹ h⁻¹ with an impressive 90% selectivity toward benzyl alcohol and benzaldehyde under an oxygen atmosphere at 150 ℃. Mechanistic investigations via Electron Paramagnetic Resonance and Fourier Transform Infrared Spectroscopy analyses revealed the pivotal role of photothermal synergy in promoting the oxidation process. This work not only provides an effective strategy for designing advanced photothermal heterojunctions but also presents new insights into the selective oxidation of toluene under mild conditions.

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沈阳化工大学材料科学与工程学院沈阳 110142

S型CdS/MnO₂异质结的合理构建用于高附加值甲苯光热协同催化选择性氧化

通讯作者: Email: zhangsujuancgl@163.com (张素娟); gaolichen@chnu.edu.cn (陈高礼); chshifu@chnu.edu.cn (陈士夫); Tel: +86-561-3802061 (陈士夫); Fax: +86-561-3802061 (陈士夫)

English

Rational design of S-scheme CdS/MnO₂ heterojunctions for high-value photothermal synergistic catalytic oxidation of toluene

Corresponding author: Email: zhangsujuancgl@163.com (Sujuan Zhang); gaolichen@chnu.edu.cn (Gaoli Chen); chshifu@chnu.edu.cn (Shifu Chen); Tel: +86-561-3802061 (Shifu Chen); Fax: +86-561-3802061 (Shifu Chen)

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S型CdS/MnO2异质结的合理构建用于高附加值甲苯光热协同催化选择性氧化

通讯作者: Email: zhangsujuancgl@163.com (张素娟); gaolichen@chnu.edu.cn (陈高礼); chshifu@chnu.edu.cn (陈士夫); Tel: +86-561-3802061 (陈士夫); Fax: +86-561-3802061 (陈士夫)

English

Rational design of S-scheme CdS/MnO2 heterojunctions for high-value photothermal synergistic catalytic oxidation of toluene

Corresponding author: Email: zhangsujuancgl@163.com (Sujuan Zhang); gaolichen@chnu.edu.cn (Gaoli Chen); chshifu@chnu.edu.cn (Shifu Chen); Tel: +86-561-3802061 (Shifu Chen); Fax: +86-561-3802061 (Shifu Chen)

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

S型CdS/MnO₂异质结的合理构建用于高附加值甲苯光热协同催化选择性氧化

Rational design of S-scheme CdS/MnO₂ heterojunctions for high-value photothermal synergistic catalytic oxidation of toluene

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs