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Efficient and Selective Photogeneration of Stable N-Centered Radicals via Controllable Charge Carrier Imbalance in Cesium Lead Halide Nanocrystals

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Title
Efficient and Selective Photogeneration of Stable N-Centered Radicals via Controllable Charge Carrier Imbalance in Cesium Lead Halide Nanocrystals
Author(s)
Tian Qiao; Madison E. Edwards; Xueting Tang; Xin Yan; Dong Hee Son
Publication Date
2023-07
Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.145, no.30, pp.16862 - 16871
Publisher
AMER CHEMICAL SOC
Abstract
Despite the versatility of semiconductornanocrystals (NCs) inphotoinduced chemical processes, the generation of stable radicalshas been more challenging due to reverse charge transfer or chargerecombination even in the presence of sacrificial charge acceptors.Here, we show that cesium lead halide (CsPbX3) NCs canselectively photogenerate either aminium or aminyl radicals from amines,taking advantage of the controllable imbalance of the electron andhole populations achieved by varying the solvent composition. Usingdihalomethane as the solvent, irreversible removal of the electronsfrom CsPbX3 NCs enabled by the photoinduced halide exchangebetween the NCs and the dihalomethane resulted in efficient oxidativegeneration of the aminium radical. In the absence of dihalomethanein solvent, the availability of both electrons and holes resultedin the production of an aminyl radical via sequential hole transferand reductive N-H bond dissociation. The negative charge ofthe halide ions on the NC's lattice surface appears to facilitatethe aminyl radical production, competing favorably with the reversiblecharge transfer reverting to the reactant.
URI
https://pr.ibs.re.kr/handle/8788114/13798
DOI
10.1021/jacs.3c05323
ISSN
0002-7863
Appears in Collections:
Center for Nanomedicine (나노의학 연구단) > 1. Journal Papers (저널논문)
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