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

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          Abstract

          Surface plasmon assisted catalysis (SPAC) reactions of 4-aminothiophenol (4ATP) to and back from 4,4′-dimercaptoazobenzene (DMAB) have been investigated 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 O 2 (as an electron acceptor) is essential and H 2O (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 H 2O (or H 2) acts as the hydrogen source. More interestingly, the cyclic redox between 4ATP and DMAB by SPAC approach has been demonstrated. This SPAC methodology presents a unique platform for studying chemical reactions that are not possible under standard synthetic conditions.

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          Singlet oxygen: there is indeed something new under the sun.

          Peter Ogilby (2010)
          Singlet oxygen, O(2)(a(1)Delta(g)), the lowest excited electronic state of molecular oxygen, has been known to the scientific community for approximately 80 years. It has a characteristic chemistry that sets it apart from the triplet ground state of molecular oxygen, O(2)(X(3)Sigma), and is important in fields that range from atmospheric chemistry and materials science to biology and medicine. For such a "mature citizen", singlet oxygen nevertheless remains at the cutting-edge of modern science. In this critical review, recent work on singlet oxygen is summarized, focusing primarily on systems that involve light. It is clear that there is indeed still something new under the sun (243 references).
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            Catalytic processes monitored at the nanoscale with tip-enhanced Raman spectroscopy.

            Evelien van Schrojenstein Lantman, Tanja Deckert-Gaudig, Arjan Mank … (2012)
            Heterogeneous catalysts play a pivotal role in the chemical industry, but acquiring molecular insights into functioning catalysts remains a significant challenge. Recent advances in micro-spectroscopic approaches have allowed spatiotemporal information to be obtained on the dynamics of single active sites and the diffusion of single molecules. However, these methods lack nanometre-scale spatial resolution and/or require the use of fluorescent labels. Here, we show that time-resolved tip-enhanced Raman spectroscopy can monitor photocatalytic reactions at the nanoscale. We use a silver-coated atomic force microscope tip to both enhance the Raman signal and to act as the catalyst. The tip is placed in contact with a self-assembled monolayer of p-nitrothiophenol molecules adsorbed on gold nanoplates. A photocatalytic reduction process is induced at the apex of the tip with green laser light, while red laser light is used to monitor the transformation process during the reaction. This dual-wavelength approach can also be used to observe other molecular effects such as monolayer diffusion.
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              When the signal is not from the original molecule to be detected: chemical transformation of para-aminothiophenol on Ag during the SERS measurement.

              Yi-Fan Huang, Hong-Ping Zhu, Guo-Kun Liu … (2010)
              Surface-enhanced Raman spectroscopy (SERS) has long been considered as a noninvasive technique that can obtain the fingerprint vibrational information of surface species. We demonstrated in this paper that a laser with a power level considered to be low in the traditional SERS measurement can already lead to a significant surface reaction. para-Aminothiophenol, an important probe molecule in SERS, was found to be oxidized to form 4,4'-dimercaptoazobenzene (DMAB) on a roughened silver surface during the SERS measurement. The assumption was confirmed experimentally by surface mass spectroscopy and SERS as well as electrochemistry of the synthesized DMAB, which agrees well with theoretical calculations. A defocusing method was used to avoid the laser induced surface reaction and perform reliable SERS characterization and identification, which can effectively avoid erroneous interpretation of the distorted experimental result.
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                Author and article information

                Journal
                Journal ID (nlm-ta): Sci Rep
                Journal ID (iso-abbrev): Sci Rep
                Title: Scientific Reports
                Publisher: Nature Publishing Group
                ISSN (Electronic): 2045-2322
                Publication date (Electronic): 21 October 2013
                Publication date Collection: 2013
                Volume: 3
                Electronic Location Identifier: 2997
                Affiliations
                [1 ]Department of Chemistry, Harbin Institute of Technology , Harbin 150001, People's Republic of China
                [2 ]Chemistry Division, Physical Chemistry and Applied Spectroscopy , Los Alamos National Laboratory, Los Alamos, NM 87545, United States of America
                [3 ]Department of Chemistry, University of Florida , Gainesville, FL 32611, United States of America
                Author notes
                Article
                Publisher Item ID: srep02997
                DOI: 10.1038/srep02997
                PMC ID: 3801115
                PubMed ID: 24141289
                SO-VID: 236795f1-0530-4a0c-a673-dc474606a29f
                Copyright © Copyright © 2013, Macmillan Publishers Limited. All rights reserved
                License:

                This work is licensed under a Creative Commons Attribution-NonCommercial-ShareALike 3.0 Unported License. To view a copy of this license, visit http://creativecommons.org/licenses/by-nc-sa/3.0/

                History
                Date received : 03 June 2013
                Date accepted : 02 October 2013
                Categories
                Subject: Article

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