Citation: Jianan Hong, Chenyu Xu, Yan Liu, Changqi Li, Menglin Wang, Yanwei Zhang. Decoding the interfacial competition between hydrogen evolution and CO₂ reduction via edge-active-site modulation in photothermal catalysis[J]. Acta Physico-Chimica Sinica, ;2025, 41(9): 100099. doi: 10.1016/j.actphy.2025.100099 shu

Decoding the interfacial competition between hydrogen evolution and CO₂ reduction via edge-active-site modulation in photothermal catalysis

State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang Province, China

Corresponding author: Chenyu Xu, mrxcy@zju.edu.cn Yanwei Zhang, zhangyw@zju.edu.cn
Received Date: 22 March 2025
Revised Date: 19 April 2025
Accepted Date: 28 April 2025

Fund Project: the Zhejiang Provincial Natural Science Foundation of China LDT23E06014E06the National Natural Science Foundation of China 52341602the Zhejiang Provincial Natural Science Foundation of China LQ24E060001the National Key Research and Development Project 2023YFC3710800the Fundamental Research Funds for the Central Universities 2022ZFJH04

Solar-driven photothermal catalytic CO₂ conversion with H₂O is a promising approach to produce sustainable fuels and chemicals. However, the competition between hydrogen evolution reaction (HER) and CO₂ reduction reaction (CO₂RR) results in unsatisfactory product selectivity. Noble metal nanoparticles (NMNPs) are widely used cocatalysts to introduce active sites on semiconductors, with unique active sites at the metal-semiconductor interfacial edges playing a critical role in the competitive mechanisms. Herein, we prepared a series of NMNPs loaded on Al-doped SrTiO₃ with abundant interfacial edge sites for continuous photothermal catalytic CO₂ and H₂O conversion. Different NMNPs demonstrated distinct CO₂-induced effects on hydrogen evolution. The key intermediate interactions were investigated by in situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations. The results revealed that bidentate carbonate (b-CO₃²⁻) tended to occupy the edge sites at the metal-semiconductor interfaces, competitively consuming the active sites for *H adsorption and altering the energy barrier of hydrogen evolution. The predominant site-blocking effect of b-CO₃²⁻ on Rh-loaded catalysts was verified through establishing a simplified geometric model to quantify the correlation of particle sizes, active site proportions and CO₂-induced hydrogen production variations. Controlling Rh nanoparticle size can tune the proportion of edge sites, which involves a trade-off between *H coverage and CO₂ activation and promotes the CO₂RR process toward methane production. This work initially unravels the interfacial competitive mechanism between HER and CO₂RR via edge-active-site modulation, hoping to provide valuable insights for the rational catalyst design and offer potential strategies to enhance CO₂ conversion efficiency.
- Photothermal catalysis,
- Hydrogen evolution,
- CO₂ reduction,
- Active site,
- Interfacial competition
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Decoding the interfacial competition between hydrogen evolution and CO2 reduction via edge-active-site modulation in photothermal catalysis

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通讯作者: 陈斌, bchen63@163.com

Decoding the interfacial competition between hydrogen evolution and CO₂ reduction via edge-active-site modulation in photothermal catalysis