Please use this identifier to cite or link to this item:
https://hdl.handle.net/10356/139338
Title: | Donor-acceptor fluorophores for energy-transfer-mediated photocatalysis | Authors: | Lu, Jingzhi Pattengale, Brian Liu, Qiuhua Yang, Sizhuo Shi, Wenxiong Li, Shuzhou Huang, Jier Zhang, Jian |
Keywords: | Engineering::Materials | Issue Date: | 2018 | Source: | Lu, J., Pattengale, B., Liu, Q., Yang, S., Shi, W., Li, S., . . . Zhang, J. (2018). Donor–acceptor fluorophores for energy-transfer-mediated photocatalysis. Journal of the American Chemical Society, 140(42), 13719-13725. doi:10.1021/jacs.8b07271 | Journal: | Journal of the American Chemical Society | Abstract: | Triplet-triplet energy transfer (EnT) is a fundamental activation pathway in photocatalysis. In this work, we report the mechanistic origins of the triplet excited state of carbazole-cyanobenzene donor-acceptor (D-A) fluorophores in EnT-based photocatalytic reactions and demonstrate the key factors that control the accessibility of the 3LE (locally excited triplet state) and 3CT (charge-transfer triplet state) via a combined photochemical and transient absorption spectroscopic study. We found that the energy order between 1CT (charge transfer singlet state) and 3LE dictates the accessibility of 3LE/3CT for EnT, which can be effectively engineered by varying solvent polarity and D-A character to depopulate 3LE and facilitate EnT from the chemically more tunable 3CT state for photosensitization. Following the above design principle, a new D-A fluorophore with strong D-A character and weak redox potential is identified, which exhibits high efficiency for Ni(II)-catalyzed cross-coupling of carboxylic acids and aryl halides with a wide substrate scope and high selectivity. Our results not only provide key fundamental insight on the EnT mechanism of D-A fluorophores but also establish its wide utility in EnT-mediated photocatalytic reactions. | URI: | https://hdl.handle.net/10356/139338 | ISSN: | 0002-7863 | DOI: | 10.1021/jacs.8b07271 | Schools: | School of Materials Science & Engineering | Rights: | © 2018 American Chemical Society. All rights reserved. | Fulltext Permission: | none | Fulltext Availability: | No Fulltext |
Appears in Collections: | MSE Journal Articles |
SCOPUSTM
Citations
5
165
Updated on Mar 24, 2024
Web of ScienceTM
Citations
5
144
Updated on Oct 25, 2023
Page view(s)
226
Updated on Mar 27, 2024
Google ScholarTM
Check
Altmetric
Items in DR-NTU are protected by copyright, with all rights reserved, unless otherwise indicated.