Ultrafast Reaction Mechanisms in Perovskite Based Photocatalytic C–C Coupling
[2];
[3];
[2];
[3];
[2]
- Xiamen Univ. (China). State Key Lab. of Physical Chemistry of Solid Surfaces; National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemistry and Nano Science Center
- National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemistry and Nano Science Center
- San Diego State Univ., CA (United States)
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., a-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.
- Research Organization:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Organization:
- National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- AC36-08GO28308
- OSTI ID:
- 1660087
- Report Number(s):
- NREL/JA-5900-74533; MainId:6641; UUID:987c4031-35b6-e911-9c24-ac162d87dfe5; MainAdminID:14068
- Journal Information:
- ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 2 Vol. 5; ISSN 2380-8195
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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