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

Zhao, Jie; Nguyen, Son C.; Ye, Rong; Ye, Baihua; Weller, Horst; Somorjai, Gábor A.; Alivisatos, A. Paul; Toste, F. Dean

doi:10.1021/acscentsci.7b00122

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

Journal Article · Mon May 15 00:00:00 EDT 2017 · ACS Central Science

DOI:https://doi.org/10.1021/acscentsci.7b00122· OSTI ID:1356866

Zhao, Jie;

; Ye, Rong; Ye, Baihua;

;

; Alivisatos, A. Paul;

© 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.

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Research Organization:: University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: DEAC02-05CH11231; AC02-05CH11231

OSTI ID:: 1356866

Alternate ID(s):: OSTI ID: 1361541; OSTI ID: 1379860

Journal Information:: ACS Central Science, Journal Name: ACS Central Science; ISSN 2374-7943

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 155 works

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