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Title: Mechanistic understanding of surface plasmon assisted catalysis on a single particle: cyclic redox of 4-aminothiophenol

We investigate surface plasmon assisted catalysis (SPAC) reactions of 4-aminothiophenol (4ATP) to and back from 4,4'-dimercaptoazobenzene (DMAB) by single particle surface enhanced Raman spectroscopy, using a self-designed gas flow cell to control the reductive/oxidative environment over the reactions. Conversion of 4ATP into DMAB is induced by energy transfer (plasmonic heating) from surface plasmon resonance to 4ATP, where O2 (as an electron acceptor) is essential and H2O (as a base) can accelerate the reaction. In contrast, hot electron (from surface plasmon decay) induction drives the reverse reaction of DMAB to 4ATP, where H2O (or H2) acts as the hydrogen source. More interestingly, the cyclic redox between 4ATP and DMAB by SPAC approach has been demonstrated. Finally, this SPAC methodology presents a unique platform for studying chemical reactions that are not possible under standard synthetic conditions.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [2] ;  [3]
  1. Harbin Inst. of Technology (China); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Harbin Inst. of Technology (China)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  4. Univ. of Florida, Gainesville, FL (United States)
Publication Date:
OSTI Identifier:
1321733
Report Number(s):
LA-UR--13-26155
Journal ID: ISSN 2045-2322
Grant/Contract Number:
AC52-06NA25396
Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 3; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Research Org:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY catalytic mechanisms; photocatalysis; raman spectroscopy; SERS