Chen, Enqi; Wang, Chao; Xiong, Lunqiao; Zheng, Yaxuan; Tian, Jingyin; Li, Xiyi; Lan, Yang; Chen, Enqi; Wang, Chao; Xiong, Lunqiao; Zheng, Yaxuan; Tian, Jingyin; Li, Xiyi; Lan, Yang; Tang, Junwang; - view fewer (2025) Infrared and Thermo Co-Driven Catalysis for CO2 Conversion to Valuable Chemicals. Advanced Materials , Article e12626. 10.1002/adma.202512626. (In press).

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Abstract

Conversion of CO2 into high value chemicals presents a promising pathway for CO2 mitigation and utilisation. The direct synthesis of dimethyl carbonate from CO2 and methanol is one of such carbon-neutral pathways. However, thermal catalytic processes for direct dimethyl carbonate synthesis have reached a performance bottleneck at elevated temperatures. This work explores the synergy of photon and thermal energy to enhance the dimethyl carbonate production rate to 30 mmol/g/h, together with 100% selectivity, thanks to a defect-modified and noble-metal free cerium oxide catalyst. Fundamentally, it is found that the defects in cerium oxide can provide energy levels that enable IR light absorption and generate holes with a moderate oxidation potential, so avoiding the unfavorable overoxidation pathway and enhancing the production rate of dimethyl carbonate. The thermal energy has been proved to remarkably facilitate the relaxation of IR-induced charge carriers and to enhance the dimethyl carbonate formation process. This work introduces a strategy of IR photons and thermo co-driven catalysis and achieves a breakthrough in dimethyl carbonate formation.

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