1. Unveiling the key role of excited-state hydrogen bonding in homogeneous photocatalytic CO2 reduction.
- Author
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Zhang, Naitian, Li, Yuehui, Shang, Wenzhe, Liu, Wei, Cheng, Xusheng, Song, Suchan, Song, Xuedan, Shi, Yantao, and Hao, Ce
- Subjects
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HYDROGEN bonding , *PHOTOREDUCTION , *CARBON dioxide reduction , *STRUCTURE-activity relationships , *IRRADIATION , *ROSE bengal , *CHARGE exchange - Abstract
In this paper, we investigated the role of excited-state hydrogen bonding in the photocatalytic carbon dioxide reduction reaction (CO2RR) utilizing Rose Bengal as a catalyst, through a combined experimental and theoretical approach. Experiments validated the successful conversion of CO2 to CO in a homogeneous aqueous solution system under light irradiation, without additional photosensitizers or sacrificial agents. Theoretically, the DFT/TDDFT calculations modeled the catalyst-reactants as a hydrogen-bonded complex (HBC), understanding the energy, hydrogen, and electron transfer mechanisms induced by excited-state hydrogen bonding. Combining the photophysical and photochemical insights revealed the complete catalytic cycle, identifying the water oxidation process as the rate-limiting step in the entire photocatalytic CO2RR process. Experimental and computational results provide molecular-level insights into the structure–activity relationships. This work enhances comprehension of the pivotal role of excited-state hydrogen bonding and holds significant reference value for enhancing the conversion efficiency in the photocatalytic CO2RR. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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