Enhancing Catalytic Activity and Selectivity by Plasmon-Induced Hot Carriers

Enhancing Catalytic Activity and Selectivity by Plasmon-Induced Hot Carriers

Summary: Plasmon-assisted chemical transformation holds great potential for solar energy conversion. However, simultaneous enhancement of reactivity and selectivity is still challenging and the mechanism remains mysterious. Herein, we elucidate the localized surface plasmon resonance (LSPR)-induced...

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Main Authors: Xiao-Qing Liu, Fei-Fei Meng, Xing Chen, Yu-Hang Li, Hao Yang, Feng Peng, Xi-Hong Lu, Ye-Xiang Tong, Zhong-Qun Tian, Jian-Feng Li, Ping-Ping Fang
Format: Article
Language:English
Published: Elsevier 2020-05-01
Series:iScience
Subjects:
Inorganic Chemistry
Catalysis
Materials Science
Online Access:http://www.sciencedirect.com/science/article/pii/S2589004220302923
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spelling doaj-c2fe34733541462d9a46f8274196f1f92020-11-25T03:23:37ZengElsevieriScience2589-00422020-05-01235Enhancing Catalytic Activity and Selectivity by Plasmon-Induced Hot CarriersXiao-Qing Liu0Fei-Fei Meng1Xing Chen2Yu-Hang Li3Hao Yang4Feng Peng5Xi-Hong Lu6Ye-Xiang Tong7Zhong-Qun Tian8Jian-Feng Li9Ping-Ping Fang10MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, The Key Lab of Low-carbon Chem & Energy Conservation of Guangdong Province, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, ChinaMOE Key Laboratory of Bioinorganic and Synthetic Chemistry, The Key Lab of Low-carbon Chem & Energy Conservation of Guangdong Province, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, ChinaState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen 361005, ChinaGuangzhou Key Laboratory for New Energy and Green Catalysis, School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou 510006, ChinaMOE Key Laboratory of Bioinorganic and Synthetic Chemistry, The Key Lab of Low-carbon Chem & Energy Conservation of Guangdong Province, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, ChinaGuangzhou Key Laboratory for New Energy and Green Catalysis, School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou 510006, ChinaMOE Key Laboratory of Bioinorganic and Synthetic Chemistry, The Key Lab of Low-carbon Chem & Energy Conservation of Guangdong Province, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, ChinaMOE Key Laboratory of Bioinorganic and Synthetic Chemistry, The Key Lab of Low-carbon Chem & Energy Conservation of Guangdong Province, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, ChinaState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen 361005, ChinaState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen 361005, China; Corresponding authorMOE Key Laboratory of Bioinorganic and Synthetic Chemistry, The Key Lab of Low-carbon Chem & Energy Conservation of Guangdong Province, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, China; Corresponding authorSummary: Plasmon-assisted chemical transformation holds great potential for solar energy conversion. However, simultaneous enhancement of reactivity and selectivity is still challenging and the mechanism remains mysterious. Herein, we elucidate the localized surface plasmon resonance (LSPR)-induced principles underlying the enhanced activity (∼70%) and selectivity of photoelectrocatalytic redox of nitrobenzene (NB) on Au nanoparticles. Hot carriers selectively accelerate the conversion rate from NB to phenylhydroxylamine (PHA) by ∼14% but suppress the transformation rate from PHA to nitrosobenzene (NSB) by ∼13%. By adding an electron accepter, the as-observed suppression ratio is substantially enlarged up to 43%. Our experiments, supported by in situ surface-enhanced Raman spectroscopy and density functional theory simulations, reveal such particular hot-carrier-induced selectivity is conjointly contributed by the accelerated hot electron transfer and the corresponding residual hot holes. This work will help expand the applications of renewable sunlight in the directional production of value-added chemicals under mild conditions.http://www.sciencedirect.com/science/article/pii/S2589004220302923Inorganic ChemistryCatalysisMaterials Science
collection DOAJ
language English
format Article
sources DOAJ
author Xiao-Qing Liu
Fei-Fei Meng
Xing Chen
Yu-Hang Li
Hao Yang
Feng Peng
Xi-Hong Lu
Ye-Xiang Tong
Zhong-Qun Tian
Jian-Feng Li
Ping-Ping Fang
spellingShingle Xiao-Qing Liu
Fei-Fei Meng
Xing Chen
Yu-Hang Li
Hao Yang
Feng Peng
Xi-Hong Lu
Ye-Xiang Tong
Zhong-Qun Tian
Jian-Feng Li
Ping-Ping Fang
Enhancing Catalytic Activity and Selectivity by Plasmon-Induced Hot Carriers
iScience
Inorganic Chemistry
Catalysis
Materials Science
author_facet Xiao-Qing Liu
Fei-Fei Meng
Xing Chen
Yu-Hang Li
Hao Yang
Feng Peng
Xi-Hong Lu
Ye-Xiang Tong
Zhong-Qun Tian
Jian-Feng Li
Ping-Ping Fang
author_sort Xiao-Qing Liu
title Enhancing Catalytic Activity and Selectivity by Plasmon-Induced Hot Carriers
title_short Enhancing Catalytic Activity and Selectivity by Plasmon-Induced Hot Carriers
title_full Enhancing Catalytic Activity and Selectivity by Plasmon-Induced Hot Carriers
title_fullStr Enhancing Catalytic Activity and Selectivity by Plasmon-Induced Hot Carriers
title_full_unstemmed Enhancing Catalytic Activity and Selectivity by Plasmon-Induced Hot Carriers
title_sort enhancing catalytic activity and selectivity by plasmon-induced hot carriers
publisher Elsevier
series iScience
issn 2589-0042
publishDate 2020-05-01
description Summary: Plasmon-assisted chemical transformation holds great potential for solar energy conversion. However, simultaneous enhancement of reactivity and selectivity is still challenging and the mechanism remains mysterious. Herein, we elucidate the localized surface plasmon resonance (LSPR)-induced principles underlying the enhanced activity (∼70%) and selectivity of photoelectrocatalytic redox of nitrobenzene (NB) on Au nanoparticles. Hot carriers selectively accelerate the conversion rate from NB to phenylhydroxylamine (PHA) by ∼14% but suppress the transformation rate from PHA to nitrosobenzene (NSB) by ∼13%. By adding an electron accepter, the as-observed suppression ratio is substantially enlarged up to 43%. Our experiments, supported by in situ surface-enhanced Raman spectroscopy and density functional theory simulations, reveal such particular hot-carrier-induced selectivity is conjointly contributed by the accelerated hot electron transfer and the corresponding residual hot holes. This work will help expand the applications of renewable sunlight in the directional production of value-added chemicals under mild conditions.
topic Inorganic Chemistry
Catalysis
Materials Science
url http://www.sciencedirect.com/science/article/pii/S2589004220302923
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AT yexiangtong enhancingcatalyticactivityandselectivitybyplasmoninducedhotcarriers
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