A Comparison of Photocatalytic Activities of Gold Nanoparticles Following Plasmonic and Interband Excitation and a Strategy for Harnessing Interband Hot Carriers for Solution Phase Photocatalysis
Abstract
© 2017 American Chemical Society. Light driven excitation of gold nanoparticles (GNPs) has emerged as a potential strategy to generate hot carriers for photocatalysis through excitation of localized surface plasmon resonance (LSPR). In contrast, carrier generation through excitation of interband transitions remains a less explored and underestimated pathway for photocatalytic activity. Photoinduced oxidative etching of GNPs with FeCl 3 was investigated as a model reaction in order to elucidate the effects of both types of transitions. The quantitative results show that interband transitions more efficiently generate hot carriers and that those carriers exhibit higher reactivity as compared to those generated solely by LSPR. Further, leveraging the strong -acidic character of the resulting photogenerated Au + hole, an interband transition induced cyclization reaction of alkynylphenols was developed. Notably, alkyne coordination to the Au + hole intercepts the classic oxidation event and leads to the formation of the catalytically active gold clusters on subnanometer scale.
- Authors:
- Publication Date:
- Research Org.:
- University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1356866
- Alternate Identifier(s):
- OSTI ID: 1361541; OSTI ID: 1379860
- Grant/Contract Number:
- DEAC02-05CH11231; AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- ACS Central Science
- Additional Journal Information:
- Journal Name: ACS Central Science; Journal ID: ISSN 2374-7943
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Zhao, Jie, Nguyen, Son C., Ye, Rong, Ye, Baihua, Weller, Horst, Somorjai, Gábor A., Alivisatos, A. Paul, and Toste, F. Dean. A Comparison of Photocatalytic Activities of Gold Nanoparticles Following Plasmonic and Interband Excitation and a Strategy for Harnessing Interband Hot Carriers for Solution Phase Photocatalysis. United States: N. p., 2017.
Web. doi:10.1021/acscentsci.7b00122.
Zhao, Jie, Nguyen, Son C., Ye, Rong, Ye, Baihua, Weller, Horst, Somorjai, Gábor A., Alivisatos, A. Paul, & Toste, F. Dean. A Comparison of Photocatalytic Activities of Gold Nanoparticles Following Plasmonic and Interband Excitation and a Strategy for Harnessing Interband Hot Carriers for Solution Phase Photocatalysis. United States. https://doi.org/10.1021/acscentsci.7b00122
Zhao, Jie, Nguyen, Son C., Ye, Rong, Ye, Baihua, Weller, Horst, Somorjai, Gábor A., Alivisatos, A. Paul, and Toste, F. Dean. Mon .
"A Comparison of Photocatalytic Activities of Gold Nanoparticles Following Plasmonic and Interband Excitation and a Strategy for Harnessing Interband Hot Carriers for Solution Phase Photocatalysis". United States. https://doi.org/10.1021/acscentsci.7b00122.
@article{osti_1356866,
title = {A Comparison of Photocatalytic Activities of Gold Nanoparticles Following Plasmonic and Interband Excitation and a Strategy for Harnessing Interband Hot Carriers for Solution Phase Photocatalysis},
author = {Zhao, Jie and Nguyen, Son C. and Ye, Rong and Ye, Baihua and Weller, Horst and Somorjai, Gábor A. and Alivisatos, A. Paul and Toste, F. Dean},
abstractNote = {© 2017 American Chemical Society. Light driven excitation of gold nanoparticles (GNPs) has emerged as a potential strategy to generate hot carriers for photocatalysis through excitation of localized surface plasmon resonance (LSPR). In contrast, carrier generation through excitation of interband transitions remains a less explored and underestimated pathway for photocatalytic activity. Photoinduced oxidative etching of GNPs with FeCl 3 was investigated as a model reaction in order to elucidate the effects of both types of transitions. The quantitative results show that interband transitions more efficiently generate hot carriers and that those carriers exhibit higher reactivity as compared to those generated solely by LSPR. Further, leveraging the strong -acidic character of the resulting photogenerated Au + hole, an interband transition induced cyclization reaction of alkynylphenols was developed. Notably, alkyne coordination to the Au + hole intercepts the classic oxidation event and leads to the formation of the catalytically active gold clusters on subnanometer scale.},
doi = {10.1021/acscentsci.7b00122},
journal = {ACS Central Science},
number = ,
volume = ,
place = {United States},
year = {Mon May 15 00:00:00 EDT 2017},
month = {Mon May 15 00:00:00 EDT 2017}
}
https://doi.org/10.1021/acscentsci.7b00122
Web of Science
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