A Nanocrystal Catalyst Incorporating a Surface Bound Transition Metal to Induce Photocatalytic Sequential Electron Transfer Events

Autor:	Xianghua Zeng, Matthew C. Beard, Jovan San Martin, Yanfa Yan, Collin Miller, Chuang Han, Nobuyuki Yamamoto, Yixiong Lin, Xiaoming Wang, Yong Yan, Xihan Chen, Sadegh Yazdi
Rok vydání:	2021
Předmět:	Chemistry General Chemistry Inner sphere electron transfer Photochemistry Heterogeneous catalysis Biochemistry Catalysis Electron transfer Colloid and Surface Chemistry Nanocrystal Transition metal Chemical bond Photocatalysis
Zdroj:	Journal of the American Chemical Society. 143:11361-11369
ISSN:	1520-5126 0002-7863
DOI:	10.1021/jacs.1c00503
Popis:	Heterogeneous photocatalysis is less common but can provide unique avenues for inducing novel chemical transformations and can also be utilized for energy transductions, i.e., the energy in the photons can be captured in chemical bonds. Here, we developed a novel heterogeneous photocatalytic system that employs a lead-halide perovskite nanocrystal (NC) to capture photons and direct photogenerated holes to a surface bound transition metal Cu-site, resulting in a N-N heterocyclization reaction. The reaction starts from surface coordinated diamine substrates and requires two subsequent photo-oxidation events per reaction cycle. We establish a photocatalytic pathway that incorporates sequential inner sphere electron transfer events, photons absorbed by the NC generate holes that are sequentially funneled to the Cu-surface site to perform the reaction. The photocatalyst is readily prepared via a controlled cation-exchange reaction and provides new opportunities in photodriven heterogeneous catalysis.
Databáze:	OpenAIRE
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