文献类型：期刊文献

英文题名：Coupling Interfacial Charge Separation with Oxygen Vacancy Dynamics for Light-Driven Dry Reforming of Methane via 2D CeO2 Nanosheets

作者：Yao, Yuan[1]; Wang, Zhi-Qiang[2]; Dang, Zhengzheng[1]; Tang, Junying[3]; Huang, Kelei[4]; Bao, Mengyao[1]; Zhao, Tianshuo[5,6]; Wang, Yanming[7]; Meng, Xiangchao[8]; Mao, Chengliang[9]; Gong, Xue-Qing[10]; He, Yulian[1,10]

机构：[1] Global College, Shanghai Jiao Tong University, Shanghai, 200240, China; [2] State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, 200237, China; [3] School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai, 20000, China; [4] Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology, School of Chemistry and Chemical Engineering, Guangxi University, Guangxi, Nanning, 530004, China; [5] Department of Electrical & Computer Engineering, The University of Hong Kong, Hong Kong, 999077, China; [6] Materials Innovation Institute for Life Sciences and Energy [MILES], HKU-SIRI, Guangdong, Shenzhen, 518000, China; [7] Global Institute of Future Technology, Shanghai Jiao Tong University, Shanghai, 200240, China; [8] College of Chemistry and Chemical Engineering, Ocean University of China, Shandong, Qingdao, 266100, China; [9] School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China; [10] State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China

年份：2026

卷号：16

期号：15

起止页码：15187

外文期刊名：ACS Catalysis

收录：EI(收录号：20263321301797);Scopus(收录号：2-s2.0-105047259699)

语种：英文

外文关键词：Carbon dioxide - Cerium oxide - Chemical bonds - Conversion efficiency - Density functional theory - Energy efficiency - Irradiation - Oxygen - Photons - Reaction kinetics - Reforming reactions

摘要：Light-driven dry reforming of methane (LDRM) provides a feasible route for converting methane (CH4) and carbon dioxide (CO2) into synthesis gas, yet most reported systems require ultraviolet light or a high photon flux, limiting their practical deployment. Here, we show that interfacial oxygen vacancy dynamics can be regulated under mild broadband irradiation through engineered metal–support electronic coupling. In this way, Rh nanoparticles (NPs) supported on two-dimensional CeO2 nanosheets (NS) exhibit record-high Rh-specific activity under low-intensity broadband irradiation (1.20 W·cm–2, 200–800 nm) without external heating, delivering H2 and CO production rates of 681 and 832 mmol·gRh–1·h–1, respectively, together with the highest light-to-chemical energy conversion efficiency (LTCEE) reported for Rh-based LDRM catalysts under low-intensity irradiation (≤3.0 W·cm–2). In-situ characterizations, combined with density functional theory calculations, reveal a photochemical Mars–van Krevelen mechanism driven by interfacial charge separation. Photoexcited electrons transfer from CeO2-NS to Rh NPs across the Schottky junction, generating electron-rich Rhδ– species, while holes remain on CeO2-NS to induce interfacial oxygen vacancies (Ov). These vacancies serve as dynamic active sites that lower the energy barrier for CO2 dissociation, promote *CH3O oxidation, and facilitate *CO desorption. The ultrathin nanosheet architecture further lowers the Ov formation energy and improves charge separation efficiency, enabling dynamic vacancy generation under a low photon flux. This work establishes a general strategy for integrating light-induced charge separation with defect-mediated thermal chemistry to overcome kinetic limitations in thermodynamically demanding reactions, offering a pathway toward efficient solar-driven reforming. ? 2026 American Chemical Society