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Insight into stable, concentrated radicals from sulfur-functionalized alkyne-rich crystalline frameworks and application in solar-to-vapor conversion
Jian-Rong Li, Jieying Hu , Lai-Hon Chung, Jilong Zhou, Parijat Borah, Zhiqing Lin, Yuan-Hui Zhong, Hua-Qun Zhou, Xianghua Yang, Zhengtao Xu*, Jun He*
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Water reduction by an organic single-chromophore photocatalyst

Kun Tang, Yu-Wu Zhong*

Chin. J. Struct. Chem., 2024, 43: 100376. DOI: 10.1016/j.cjsc.2024.100376

August 15, 2024

ABSTRACT

Up to date, the most common reactive intermediate for water reduction is metal hydride. The PyH intermediate proposed and manifested in this work offers a new perspective for the mechanism understanding of known photocatalytic systems and the design of new photocatalysts. The PyH intermediate is generated from the pyridine reaction centers via the light-induced PCET process, which is directly involved for the subsequent H−H bond formation via the hemolytic elimination of two PyH units. Recent theoretical investigations suggest that pyridinic nitrogen atoms of π-conjugated polymers may also act as the hydrogen-adsorbing sites for hydrogen evolution. It is of great interest to investigate that whether similar heterocycle-hydrogen radical intermediate is generated and involved in the water reduction catalyzed by carbon nitride and COF materials. The clarification of the reaction site and mechanism of these photocatalysts will be of great insignificance for the development of the next-generation simpler, greener, and low-cost photocatalysts.

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