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

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

Research output: Contribution to journalArticlepeer-review

50 Scopus Citations

Abstract

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.

Original languageAmerican English
Pages (from-to)11361-11369
Number of pages9
JournalJournal of the American Chemical Society
Volume143
Issue number30
DOIs
StatePublished - 4 Aug 2021

Bibliographical note

Publisher Copyright:
©

NREL Publication Number

  • NREL/JA-5900-79390

Keywords

  • metal halide perovskite
  • nanocrystals
  • photocatalysis

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