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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

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:
; ORCiD logo; ; ; ORCiD logo; ORCiD logo; ; ORCiD logo
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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acscentsci.7b00122

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Works referenced in this record:

How to deal with the loss in plasmonics and metamaterials
journal, January 2015


Plasmon-induced hot carrier science and technology
journal, January 2015

  • Brongersma, Mark L.; Halas, Naomi J.; Nordlander, Peter
  • Nature Nanotechnology, Vol. 10, Issue 1
  • DOI: 10.1038/nnano.2014.311

Highly Active Heterogeneous Palladium Nanoparticle Catalysts for Homogeneous Electrophilic Reactions in Solution and the Utilization of a Continuous Flow Reactor
journal, December 2010

  • Huang, Wenyu; Liu, Jack Hung-Chang; Alayoglu, Pinar
  • Journal of the American Chemical Society, Vol. 132, Issue 47
  • DOI: 10.1021/ja108898t

Effect of Au surface plasmon nanoparticles on the selective CO2 photoreduction to CH4
journal, November 2015


Metal Nanoparticles Catalyzed Selective Carbon–Carbon Bond Activation in the Liquid Phase
journal, June 2016

  • Ye, Rong; Yuan, Bing; Zhao, Jie
  • Journal of the American Chemical Society, Vol. 138, Issue 27
  • DOI: 10.1021/jacs.6b03977

Hybrid single nanoreactor for in situ SERS monitoring of plasmon-driven and small Au nanoparticles catalyzed reactions
journal, January 2015

  • Li, Pan; Ma, Bingbing; Yang, Liangbao
  • Chemical Communications, Vol. 51, Issue 57
  • DOI: 10.1039/C5CC03792A

Photocatalytic Conversion of CO 2 to Hydrocarbon Fuels via Plasmon-Enhanced Absorption and Metallic Interband Transitions
journal, July 2011

  • Hou, Wenbo; Hung, Wei Hsuan; Pavaskar, Prathamesh
  • ACS Catalysis, Vol. 1, Issue 8
  • DOI: 10.1021/cs2001434

Plasmonic Harvesting of Light Energy for Suzuki Coupling Reactions
journal, April 2013

  • Wang, Feng; Li, Chuanhao; Chen, Huanjun
  • Journal of the American Chemical Society, Vol. 135, Issue 15
  • DOI: 10.1021/ja310501y

Selective etching of gold nanorods by ferric chloride at room temperature
journal, January 2009

  • Zou, Renxian; Guo, Xia; Yang, Jian
  • CrystEngComm, Vol. 11, Issue 12
  • DOI: 10.1039/b911902g

High-Temperature Organic Reactions at Room Temperature Using Plasmon Excitation: Decomposition of Dicumyl Peroxide
journal, January 2011

  • Fasciani, Chiara; Alejo, Carlos J. Bueno; Grenier, Michel
  • Organic Letters, Vol. 13, Issue 2
  • DOI: 10.1021/ol1026427

Reduction of Nitroaromatic Compounds on Supported Gold Nanoparticles by Visible and Ultraviolet Light
journal, November 2010

  • Zhu, Huaiyong; Ke, Xuebin; Yang, Xuzhuang
  • Angewandte Chemie International Edition, Vol. 49, Issue 50
  • DOI: 10.1002/anie.201003908

Visible‐Light‐Driven Oxidation of Organic Contaminants in Air with Gold Nanoparticle Catalysts on Oxide Supports
journal, July 2008

  • Chen, Xi; Zhu, Huai‐Yong; Zhao, Jin‐Cai
  • Angewandte Chemie, Vol. 120, Issue 29
  • DOI: 10.1002/ange.200800602

The case for plasmon-derived hot carrier devices
journal, January 2015


Relativistic effects in homogeneous gold catalysis
journal, March 2007


Study of Heat Transfer Dynamics from Gold Nanorods to the Environment via Time-Resolved Infrared Spectroscopy
journal, January 2016


Hot Electrons Do the Impossible: Plasmon-Induced Dissociation of H 2 on Au
journal, December 2012

  • Mukherjee, Shaunak; Libisch, Florian; Large, Nicolas
  • Nano Letters, Vol. 13, Issue 1
  • DOI: 10.1021/nl303940z

Light-Concentrating Plasmonic Au Superstructures with Significantly Visible-Light-Enhanced Catalytic Performance
journal, April 2015

  • Yang, Jinhu; Li, Ying; Zu, Lianhai
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 15
  • DOI: 10.1021/acsami.5b01078

Theory and computation of hot carriers generated by surface plasmon polaritons in noble metals
journal, June 2015

  • Bernardi, Marco; Mustafa, Jamal; Neaton, Jeffrey B.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8044

Gold Nanoparticles Located at the Interface of Anatase/Rutile TiO 2 Particles as Active Plasmonic Photocatalysts for Aerobic Oxidation
journal, April 2012

  • Tsukamoto, Daijiro; Shiraishi, Yasuhiro; Sugano, Yoshitsune
  • Journal of the American Chemical Society, Vol. 134, Issue 14
  • DOI: 10.1021/ja2120647

Visible light-induced photocatalytic reaction of gold-modified titanium(iv) oxide particles: action spectrum analysis
journal, January 2009

  • Kowalska, Ewa; Abe, Ryu; Ohtani, Bunsho
  • Chem. Commun., Issue 2
  • DOI: 10.1039/B815679D

Small Gold Clusters Formed in Solution Give Reaction Turnover Numbers of 107 at Room Temperature
journal, December 2012

  • Oliver-Meseguer, J.; Cabrero-Antonino, J. R.; Dominguez, I.
  • Science, Vol. 338, Issue 6113
  • DOI: 10.1126/science.1227813

A Pt-Cluster-Based Heterogeneous Catalyst for Homogeneous Catalytic Reactions: X-ray Absorption Spectroscopy and Reaction Kinetic Studies of Their Activity and Stability against Leaching
journal, August 2011

  • Li, Yimin; Liu, Jack Hung-Chang; Witham, Cole A.
  • Journal of the American Chemical Society, Vol. 133, Issue 34
  • DOI: 10.1021/ja204191t

Growing gold nanoprisms with light
journal, July 2016


Limits of localized heating by electromagnetically excited nanoparticles
journal, September 2006

  • Keblinski, Pawel; Cahill, David G.; Bodapati, Arun
  • Journal of Applied Physics, Vol. 100, Issue 5
  • DOI: 10.1063/1.2335783

Photocatalytic Enhancements to the Reduction of 4-Nitrophenol by Resonantly Excited Triangular Gold–Copper Nanostructures
journal, July 2015

  • Hajfathalian, Maryam; Gilroy, Kyle D.; Yaghoubzade, Ali
  • The Journal of Physical Chemistry C, Vol. 119, Issue 30
  • DOI: 10.1021/acs.jpcc.5b04618

In Situ IR and X-ray High Spatial-Resolution Microspectroscopy Measurements of Multistep Organic Transformation in Flow Microreactor Catalyzed by Au Nanoclusters
journal, February 2014

  • Gross, Elad; Shu, Xing-Zhong; Alayoglu, Selim
  • Journal of the American Chemical Society, Vol. 136, Issue 9
  • DOI: 10.1021/ja412740p

Mechanism of supported gold nanoparticles as photocatalysts under ultraviolet and visible light irradiation
journal, January 2009

  • Zhu, Huaiyong; Chen, Xi; Zheng, Zhanfeng
  • Chemical Communications, Issue 48
  • DOI: 10.1039/b917052a

Gold photosensitized SrTiO3 for visible-light water oxidation induced by Au interband transitions
journal, January 2014

  • Liu, Lequan; Li, Peng; Adisak, Boonchun
  • Journal of Materials Chemistry A, Vol. 2, Issue 25
  • DOI: 10.1039/c4ta01988a

Control of selectivity in heterogeneous catalysis by tuning nanoparticle properties and reactor residence time
journal, September 2012

  • Gross, Elad; Liu, Jack Hung-Chang; Toste, F. Dean
  • Nature Chemistry, Vol. 4, Issue 11
  • DOI: 10.1038/nchem.1465

Nanogold plasmonic photocatalysis for organic synthesis and clean energy conversion
journal, January 2014

  • Wang, Changlong; Astruc, Didier
  • Chem. Soc. Rev., Vol. 43, Issue 20
  • DOI: 10.1039/C4CS00145A

Atomically Precise Colloidal Metal Nanoclusters and Nanoparticles: Fundamentals and Opportunities
journal, September 2016


Ligand Effects and Ligand Design in Homogeneous Gold(I) Catalysis
journal, March 2012

  • Wang, Weibo; Hammond, Gerald B.; Xu, Bo
  • Journal of the American Chemical Society, Vol. 134, Issue 12
  • DOI: 10.1021/ja3011397

Ligand Effects in Homogeneous Au Catalysis
journal, August 2008

  • Gorin, David J.; Sherry, Benjamin D.; Toste, F. Dean
  • Chemical Reviews, Vol. 108, Issue 8
  • DOI: 10.1021/cr068430g

Effect of aqueous and ambient atmospheric environments on plasmon-driven selective reduction reactions
journal, June 2015

  • Ding, Qianqian; Chen, Maodu; Li, Yuanzuo
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep10269

Facile in situ synthesis of visible-light plasmonic photocatalysts M@TiO2 (M = Au, Pt, Ag) and evaluation of their photocatalytic oxidation of benzene to phenol
journal, January 2011

  • Zheng, Zhaoke; Huang, Baibiao; Qin, Xiaoyan
  • Journal of Materials Chemistry, Vol. 21, Issue 25
  • DOI: 10.1039/c1jm10983a

Polymer-Encapsulated Metallic Nanoparticles as a Bridge Between Homogeneous and Heterogeneous Catalysis
journal, November 2014


Identification of Active Gold Nanoclusters on Iron Oxide Supports for CO Oxidation
journal, September 2008


Controlling the Selectivity of the Surface Plasmon Resonance Mediated Oxidation of p -Aminothiophenol on Au Nanoparticles by Charge Transfer from UV-excited TiO 2
journal, April 2015

  • Wang, Jiale; Ando, Romulo A.; Camargo, Pedro H. C.
  • Angewandte Chemie International Edition, Vol. 54, Issue 23
  • DOI: 10.1002/anie.201502077

Gold(I)-Catalyzed Activation of Alkynes for the Construction of Molecular Complexity
journal, April 2015

  • Dorel, Ruth; Echavarren, Antonio M.
  • Chemical Reviews, Vol. 115, Issue 17
  • DOI: 10.1021/cr500691k

Photochemical transformations on plasmonic metal nanoparticles
journal, May 2015

  • Linic, Suljo; Aslam, Umar; Boerigter, Calvin
  • Nature Materials, Vol. 14, Issue 6
  • DOI: 10.1038/nmat4281

Converting homogeneous to heterogeneous in electrophilic catalysis using monodisperse metal nanoparticles
journal, November 2009

  • Witham, Cole A.; Huang, Wenyu; Tsung, Chia-Kuang
  • Nature Chemistry, Vol. 2, Issue 1
  • DOI: 10.1038/nchem.468

Asymmetric Catalysis at the Mesoscale: Gold Nanoclusters Embedded in Chiral Self-Assembled Monolayer as Heterogeneous Catalyst for Asymmetric Reactions
journal, March 2013

  • Gross, Elad; Liu, Jack H.; Alayoglu, Selim
  • Journal of the American Chemical Society, Vol. 135, Issue 10
  • DOI: 10.1021/ja310640b