Single-Atom Fe-N4 sites promote the triplet-energy transfer process of g-C3N4 for the photooxidation
2021
Wang, Junhui | Yin, Shimin | Zhang, Qinhua | Cao, Fengliang | Xing, Yicheng | Zhao, Qingshan | Wang, Yang | Xu, Wengang | Wu, Wenting | Wu, Mingbo
Polymeric carbon nitride materials show intriguing prospects in numerous light-to-energy conversion applications, but seldom studies focus on their triplet energy transfer, leading to the insufficient lifetime for the photochemical process. Inspired by the porphyrin molecular photocatalyst, single-atom sites (Fe-N₄) as triplet sensitizing sites were fabricated in g-C₃N₄ for the preparation of Fe-g-C₃N₄, which processes a long-lived triplet emissive state (τPH = 4.93 μs). But under realistic condition for the large-scale production of catalyst, single atoms are inevitable to sinter, resulting in the formation of other metal species. Therefore, the photooxidation of 1,5-dihydroxynaphthalene (1,5-DHN) and the photocatalytic E-Z Isomerization of stilbene were selected as the model reactions to evaluate the influence of various Fe species on the triplet energy transfer. It was found that Fe-N₄ sites promote the triplet energy transfer process, while Fe nanoclusters (Fe⁰) promote the electron transfer and inhibit triplet energy transfer. This finding provides guidance for the rational design of photocatalysts to efficiently improve triplet energy transfer process and its application.
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