Issue

Vol. 19 (2027)

Elucidating the Respective Roles of Photochemical and Photothermal Effects in Photocatalytic Methanol Decomposition

https://doi.org/10.1007/s40820-026-02305-6
Qichen Liu
National Synchrotron Radiation Laboratory (NSRL), University of Science and Technology of China, Hefei 230029, Anhui, People’s Republic of China
Yida Zhang
College of Chemical Engineering, Inner Mongolia University of Technology, Hohhot 010051, Inner Mongolia, People’s Republic of China
Limin Liu
National Synchrotron Radiation Laboratory (NSRL), University of Science and Technology of China, Hefei 230029, Anhui, People’s Republic of China
Zixiang Huang
National Synchrotron Radiation Laboratory (NSRL), University of Science and Technology of China, Hefei 230029, Anhui, People’s Republic of China
Jiawei Zheng
National Synchrotron Radiation Laboratory (NSRL), University of Science and Technology of China, Hefei 230029, Anhui, People’s Republic of China
Shiqin Jian
School of Physics and Mechanics, Wuhan University of Technology, Wuhan 430070, Hubei, People’s Republic of China
Haibin Pan
National Synchrotron Radiation Laboratory (NSRL), University of Science and Technology of China, Hefei 230029, Anhui, People’s Republic of China
Chi Cao
National Synchrotron Radiation Laboratory (NSRL), University of Science and Technology of China, Hefei 230029, Anhui, People’s Republic of China
Hongliang Li
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, Anhui, People’s Republic of China
Qing Yang
College of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, Anhui, People’s Republic of China
Yu Bai
Experimental Center for Engineering and Materials Science, University of Science and Technology of China, Hefei 230027, Anhui, People’s Republic of China
Xusheng Zheng
National Synchrotron Radiation Laboratory (NSRL), University of Science and Technology of China, Hefei 230029, Anhui, People’s Republic of China

Corresponding Author: Xusheng Zheng

zxs@ustc.edu.cn

Nano-Micro Letters, Vol. 19 (2027), Article Number: 2

Abstract

Photocatalytic reactions can be driven by both photochemical and photothermal processes. However, their individual contributions and synergistic effect remain to be clarified. Herein, we investigated the respective roles of these effects using a Cu–TiO2/Ti model catalyst that integrated photochemical and photothermal functionalities within a single photocatalytic system. Employing photocatalytic methanol decomposition as a model reaction, the Cu–TiO2/Ti catalyst achieved a high H2 yield rate of 0.511 mmol h−1 with selectivity of 96.6% toward HCHO among oxidation products, attributed to the cooperative action of photochemical and photothermal processes. In situ resonant Auger electron spectroscopy (RAS), together with in situ Cu K-edge X-ray absorption fine structure and excited-state density functional theory calculations, revealed the accumulation of photogenerated electrons at Cu sites from TiO2, suggests the possible formation of an electron transfer pathway from TiO2 to Cu, which promotes stepwise methanol dehydrogenation to HCHO and H2. Simultaneously, the photothermal contribution from Ti enhanced catalytic activity by accelerating reaction kinetics and promoting the desorption of HCHO, thereby suppressing its overoxidation to CO.


Highlights:
1 A rationally engineered Cu-TiO2/Ti model catalyst enables the distinction of photochemical and photothermal effects, revealing their distinct roles in enhancing CH3OH dehydrogenation and suppressing HCHO overoxidation, thus achieving high H2 production, excellent HCHO selectivity, and long-term stability in a non-noble metal system.
2 The integration of in situ resonant Auger electron spectroscopy with in situ diffuse reflectance infrared Fourier transform spectroscopy, in situ Synchrotron radiation photoelectron spectroscopy, and molecular dynamics simulations enable direct visualization of charge transfer pathways and elucidates how the photothermal effect promotes HCHO desorption while preventing overoxidation.

Keywords

Photochemical effect Photothermal effect Electron transfer Synchrotron radiation H2 production
Liu, Qichen, Yida Zhang, Limin Liu, Zixiang Huang, Jiawei Zheng, Shiqin Jian, Haibin Pan, Chi Cao, Hongliang Li, Qing Yang, Yu Bai, and Xusheng Zheng. 2026. “Elucidating the Respective Roles of Photochemical and Photothermal Effects in Photocatalytic Methanol Decomposition”. Nano-Micro Letters 19 (July):2. https://doi.org/10.1007/s40820-026-02305-6.
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