Quantifying hot carrier and thermal contributions in plasmonic photocatalysis

Photocatalysis based on optically active, "plasmonic" metal nanoparticles has emerged as a promising approach to facilitate light-driven chemical conversions under far milder conditions than thermal catalysis. However, an understanding of the relation between thermal and electronic excitat...

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Published in	Science (American Association for the Advancement of Science) Vol. 362; no. 6410; pp. 69 - 72
Main Authors	Zhou, Linan, Swearer, Dayne F, Zhang, Chao, Robatjazi, Hossein, Zhao, Hangqi, Henderson, Luke, Dong, Liangliang, Christopher, Phillip, Carter, Emily A, Nordlander, Peter, Halas, Naomi J
Format	Journal Article
Language	English
Published	United States The American Association for the Advancement of Science 05.10.2018
Subjects	Activation Ammonia Catalysis Catalysts Copper base alloys Current carriers Decomposition Decomposition reactions Energy efficiency Light Light effects Luminous intensity Nanoparticles Nitrogen atoms Optical activity Organic chemistry Photocatalysis Photocatalysts Photochemistry Reduction Ruthenium Surface temperature Wavelengths
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Abstract	Photocatalysis based on optically active, "plasmonic" metal nanoparticles has emerged as a promising approach to facilitate light-driven chemical conversions under far milder conditions than thermal catalysis. However, an understanding of the relation between thermal and electronic excitations has been lacking. We report the substantial light-induced reduction of the thermal activation barrier for ammonia decomposition on a plasmonic photocatalyst. We introduce the concept of a light-dependent activation barrier to account for the effect of light illumination on electronic and thermal excitations in a single unified picture. This framework provides insight into the specific role of hot carriers in plasmon-mediated photochemistry, which is critically important for designing energy-efficient plasmonic photocatalysts.
AbstractList	Photocatalysis based on optically active, "plasmonic" metal nanoparticles has emerged as a promising approach to facilitate light-driven chemical conversions under far milder conditions than thermal catalysis. However, an understanding of the relation between thermal and electronic excitations has been lacking. We report the substantial light-induced reduction of the thermal activation barrier for ammonia decomposition on a plasmonic photocatalyst. We introduce the concept of a light-dependent activation barrier to account for the effect of light illumination on electronic and thermal excitations in a single unified picture. This framework provides insight into the specific role of hot carriers in plasmon-mediated photochemistry, which is critically important for designing energy-efficient plasmonic photocatalysts. Plasmonic catalysts can generate hot charge carriers that can activate reactants and, in turn, reduce the overall barrier to a reaction. Zhou et al. studied the decomposition of ammonia to hydrogen on a copper alloy nanostructure that absorbed light and generated electrons that activated nitrogen atoms on ruthenium surface atoms (see the Perspective by Cortés). By measuring reaction rates at different wavelengths, light intensities, and catalyst surface temperatures, the light-induced reduction of the apparent activation barrier was quantified. Science , this issue p. 69 ; see also p. 28 A Ru-Cu alloy plasmonic photocatalyst substantially reduced the thermal activation barrier for ammonia decomposition. Photocatalysis based on optically active, “plasmonic” metal nanoparticles has emerged as a promising approach to facilitate light-driven chemical conversions under far milder conditions than thermal catalysis. However, an understanding of the relation between thermal and electronic excitations has been lacking. We report the substantial light-induced reduction of the thermal activation barrier for ammonia decomposition on a plasmonic photocatalyst. We introduce the concept of a light-dependent activation barrier to account for the effect of light illumination on electronic and thermal excitations in a single unified picture. This framework provides insight into the specific role of hot carriers in plasmon-mediated photochemistry, which is critically important for designing energy-efficient plasmonic photocatalysts. Hot carriers reducing thermal barriersPlasmonic catalysts can generate hot charge carriers that can activate reactants and, in turn, reduce the overall barrier to a reaction. Zhou et al. studied the decomposition of ammonia to hydrogen on a copper alloy nanostructure that absorbed light and generated electrons that activated nitrogen atoms on ruthenium surface atoms (see the Perspective by Cortés). By measuring reaction rates at different wavelengths, light intensities, and catalyst surface temperatures, the light-induced reduction of the apparent activation barrier was quantified.Science, this issue p. 69; see also p. 28Photocatalysis based on optically active, “plasmonic” metal nanoparticles has emerged as a promising approach to facilitate light-driven chemical conversions under far milder conditions than thermal catalysis. However, an understanding of the relation between thermal and electronic excitations has been lacking. We report the substantial light-induced reduction of the thermal activation barrier for ammonia decomposition on a plasmonic photocatalyst. We introduce the concept of a light-dependent activation barrier to account for the effect of light illumination on electronic and thermal excitations in a single unified picture. This framework provides insight into the specific role of hot carriers in plasmon-mediated photochemistry, which is critically important for designing energy-efficient plasmonic photocatalysts.
Author	Christopher, Phillip Carter, Emily A Dong, Liangliang Nordlander, Peter Robatjazi, Hossein Zhang, Chao Zhao, Hangqi Zhou, Linan Halas, Naomi J Henderson, Luke Swearer, Dayne F
Author_xml	– sequence: 1 givenname: Linan orcidid: 0000-0002-2989-1535 surname: Zhou fullname: Zhou, Linan organization: Department of Chemistry, Rice University, Houston, TX 77005, USA – sequence: 2 givenname: Dayne F orcidid: 0000-0003-0274-4815 surname: Swearer fullname: Swearer, Dayne F organization: Department of Chemistry, Rice University, Houston, TX 77005, USA – sequence: 3 givenname: Chao orcidid: 0000-0001-5619-341X surname: Zhang fullname: Zhang, Chao organization: Department of Electrical and Computer Engineering, Rice University, Houston, TX 77005, USA – sequence: 4 givenname: Hossein orcidid: 0000-0002-5101-263X surname: Robatjazi fullname: Robatjazi, Hossein organization: Department of Electrical and Computer Engineering, Rice University, Houston, TX 77005, USA – sequence: 5 givenname: Hangqi orcidid: 0000-0002-9422-3875 surname: Zhao fullname: Zhao, Hangqi organization: Department of Electrical and Computer Engineering, Rice University, Houston, TX 77005, USA – sequence: 6 givenname: Luke orcidid: 0000-0003-3114-531X surname: Henderson fullname: Henderson, Luke organization: Department of Chemistry, Rice University, Houston, TX 77005, USA – sequence: 7 givenname: Liangliang orcidid: 0000-0003-3848-1439 surname: Dong fullname: Dong, Liangliang organization: Department of Chemistry, Rice University, Houston, TX 77005, USA – sequence: 8 givenname: Phillip surname: Christopher fullname: Christopher, Phillip organization: Department of Chemical Engineering, University of California, Santa Barbara, Santa Barbara, CA, 93106-5080, USA – sequence: 9 givenname: Emily A orcidid: 0000-0001-7330-7554 surname: Carter fullname: Carter, Emily A organization: School of Engineering and Applied Science, Princeton University, Princeton, NJ 08544-5263, USA – sequence: 10 givenname: Peter orcidid: 0000-0002-1633-2937 surname: Nordlander fullname: Nordlander, Peter email: nordland@rice.edu, halas@rice.edu organization: Department of Physics and Astronomy, Rice University, Houston, TX 77005, USA – sequence: 11 givenname: Naomi J orcidid: 0000-0002-8461-8494 surname: Halas fullname: Halas, Naomi J email: nordland@rice.edu, halas@rice.edu organization: Department of Physics and Astronomy, Rice University, Houston, TX 77005, USA
BackLink	https://www.ncbi.nlm.nih.gov/pubmed/30287657$$D View this record in MEDLINE/PubMed
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Snippet	Photocatalysis based on optically active, "plasmonic" metal nanoparticles has emerged as a promising approach to facilitate light-driven chemical conversions... Plasmonic catalysts can generate hot charge carriers that can activate reactants and, in turn, reduce the overall barrier to a reaction. Zhou et al. studied... Hot carriers reducing thermal barriersPlasmonic catalysts can generate hot charge carriers that can activate reactants and, in turn, reduce the overall barrier...
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SubjectTerms	Activation Ammonia Catalysis Catalysts Copper base alloys Current carriers Decomposition Decomposition reactions Energy efficiency Light Light effects Luminous intensity Nanoparticles Nitrogen atoms Optical activity Organic chemistry Photocatalysis Photocatalysts Photochemistry Reduction Ruthenium Surface temperature Wavelengths
Title	Quantifying hot carrier and thermal contributions in plasmonic photocatalysis
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