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

Martin, Jovan San; Zeng, Xianghua; Chen, Xihan; Miller, Collin; Han, Chuang; Lin, Yixiong; Yamamoto, Nobuyuki; Wang, Xiaoming; Yazdi, Sadegh; Yan, Yanfa; Beard, Matthew C.; Yan, Yong

doi:10.1021/jacs.1c00503

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

Journal Article · Wed Jul 21 00:00:00 EDT 2021 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.1c00503· OSTI ID:1811835

Martin, Jovan San ^[1]; Zeng, Xianghua ^[2]; ^[3]; Miller, Collin ^[1]; Han, Chuang ^[1]; Lin, Yixiong ^[1]; Yamamoto, Nobuyuki ^[1]; ^[4]; ^[5]; ^[4]; ^[3]; ^[1]

San Diego State Univ., CA (United States). Dept. of Chemistry and Biochemistry
San Diego State Univ., CA (United States). Dept. of Chemistry and Biochemistry; Jiaxing Univ. (China). College of Biological, Chemical Science and Engineering
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Univ. of Toledo, OH (United States). Dept. of Physics and Astronomy; Univ. of Toledo, OH (United States). Wright Center for Photovoltaics Innovation and Commercialization (PVIC)
Univ. of Colorado, Boulder, CO (United States). Renewable & Sustainable Energy Institute

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.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1811835

Report Number(s):: NREL/JA--5900-79390; MainId:33616; UUID:41b27c19-7463-4339-b030-3914d0dd3115; MainAdminID:25835

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 30 Vol. 143; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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