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Single-Molecular Catalysis Identifying Activation Energy of the Intermediate Product and Rate-Limiting Step in Plasmonic Photocatalysis
Li, W; Miao, JJ; Peng, TH; Lv, H; Wang, JG; Li, K; Zhu, Y; Li, D
2020
Source PublicationNANO LETTERS
ISSN1530-6984
Volume20Issue:4Pages:2507-2513
Subtype期刊论文
AbstractPlasmon-mediated photocatalysis provides a novel strategy for harvesting solar energy. Identification of the rate-determining step and its activation energy in plasmon-mediated photocatalysis plays critical roles for understanding the contribution of hot carriers, which facilitates rational designation of catalysts with integrated high photochemical conversion efficiency and catalytic performance. However, it remains a challenge due to a lack of research tools with spatiotemporal resolution that are capable of capturing intermediates. In this work, we used a single-molecule fluorescence approach to investigate a localized surface plasmon resonance (LSPR)-enhanced photocatalytic reaction with subturnover resolution. By introducing variable temperature as an independent parameter in plasmonic photocatalysis, the activation energies of tandem reaction steps, including intermediate generation, product generation, and product desorption, were clearly differentiated, and intermediate generation was found to be the rate-limiting step. Remarkably, the cause of the plasmon-enhanced catalysis performance was found to be its ability of lowering the activation energy of intermediate generation. This study gives new insight into the photochemical energy conversion pathways in plasmon-enhanced photocatalysis and sheds light on designing high- performance plasmonic catalysts.
KeywordCROSS-COUPLING REACTIONS HOT-ELECTRONS SOLAR-ENERGY REVEALS KINETICS CARRIER NANOSTRUCTURES CONVERSION PALLADIUM DYNAMICS
DOI10.1021/acs.nanolett.9b05255
Indexed BySCI
Language英语
Citation statistics
Cited Times:20[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/33142
Collection中科院上海应用物理研究所2011-2020年
Affiliation1.East China Normal Univ, Sch Chem & Mol Engn, Shanghai 200241, Peoples R China
2.Chinese Acad Sci, Div Phys Biol, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201800, Peoples R China
3.Chinese Acad Sci, Bioimaging Ctr, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201800, Peoples R China
4.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
5.Shanghai Ocean Univ, Coll Food Sci & Technol, Shanghai 201306, Peoples R China
6.Hunan Univ, Coll Chem & Chem Engn, State Key Lab Chemo Biosensing & Chemometr, Hunan Prov Key Lab Biomacromol Chem Biol, Changsha 410082, Hunan, Peoples R China
7.Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
Recommended Citation
GB/T 7714
Li, W,Miao, JJ,Peng, TH,et al. Single-Molecular Catalysis Identifying Activation Energy of the Intermediate Product and Rate-Limiting Step in Plasmonic Photocatalysis[J]. NANO LETTERS,2020,20(4):2507-2513.
APA Li, W.,Miao, JJ.,Peng, TH.,Lv, H.,Wang, JG.,...&Li, D.(2020).Single-Molecular Catalysis Identifying Activation Energy of the Intermediate Product and Rate-Limiting Step in Plasmonic Photocatalysis.NANO LETTERS,20(4),2507-2513.
MLA Li, W,et al."Single-Molecular Catalysis Identifying Activation Energy of the Intermediate Product and Rate-Limiting Step in Plasmonic Photocatalysis".NANO LETTERS 20.4(2020):2507-2513.
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