Ultrafast Reaction Mechanisms in Perovskite Based Photocatalytic C-C Coupling

Kang Wang, Haipeng Lu, Xiaolin Zhu, Yixiong Lin, Matthew Beard, Yong Yan, Xihan Chen

Research output: Contribution to journalArticlepeer-review

61 Scopus Citations

Abstract

Solar driven carbon−carbon (C−C) bond formation is a new direction in solar energy utilization. Earth abundant nanocrystal based photocatalysts are highly sought after as they can potentially eliminate expensive noble metal catalysts. A detailed understanding of the underlying reaction mechanisms could provide guidance in designing new systems that can activate a larger class of small molecules. Here, we employ transient absorption spectroscopy to study a model C−C bond formation reaction, i.e., α-alkylation of aldehydes catalyzed by colloidal CsPbBr3 nanocrystals (NCs). We find that both electrons and holes undergo ultrafast charge transfer (∼50 ps) from photoexcited perovskite NCs to reactant molecules. A charge separated state lives for more than 0.8 μs, enabling a radical mechanism to form the C−C bonds. We discuss the differences between the NCs photoredox catalysts and the molecular catalyst.

Original languageAmerican English
Pages (from-to)566-571
Number of pages6
JournalACS Energy Letters
Volume5
Issue number2
DOIs
StatePublished - 14 Feb 2020

Bibliographical note

Publisher Copyright:
© 2020 American Chemical Society.

NREL Publication Number

  • NREL/JA-5900-74533

Keywords

  • carbon-carbon bond forming
  • nanocrystal photocatalyst
  • perovskite nanocrystals

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