In Situ Mass Spectrometric Monitoring of the Dynamic Electrochemical Process at the Electrode-Electrolyte Interface : a SIMS Approach
The in situ molecular characterization of reaction intermediates and products at electrode-electrolyte interfaces is central to mechanistic studies of complex electrochemical processes, yet a great challenge. The coupling of electrochemistry (EC) and mass spectrometry (MS) has seen rapid development and found broad applicability in tackling challenges in analytical and bioanalytical chemistry. However, few truly in situ and real-time EC-MS studies have been reported at electrode-electrolyte interfaces. An innovative EC-MS coupling method named in situ liquid secondary ion mass spectrometry (SIMS) was recently developed by combining SIMS with a vacuum compatible microfluidic electrochemical device. Using this novel capability, we report the first in situ elucidation of the electro-oxidation mechanism of a biologically significant organic compound, ascorbic acid (AA), at the electrode-electrolyte interface. The short-lived radical intermediate was successfully captured, which had not been detected directly before. Moreover, we demonstrated the power of this new technique in real-time monitoring of the formation and dynamic evolution of electrical double layers at the electrode-electrolyte interface. This work suggests further promising applications of in situ liquid SIMS in studying more complex chemical and biological events at the electrode-electrolyte interface.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2017 |
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| Erschienen: |
2017 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:89 |
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| Enthalten in: |
Analytical chemistry - 89(2017), 1 vom: 03. Jan., Seite 960-965 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Wang, Zhaoying [VerfasserIn] |
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| Links: |
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| Themen: |
Ascorbic Acid |
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| Anmerkungen: |
Date Completed 05.11.2018 Date Revised 05.11.2018 published: Print-Electronic Citation Status MEDLINE |
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| doi: |
10.1021/acs.analchem.6b04189 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM266987923 |
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| 500 | |a Date Completed 05.11.2018 | ||
| 500 | |a Date Revised 05.11.2018 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status MEDLINE | ||
| 520 | |a The in situ molecular characterization of reaction intermediates and products at electrode-electrolyte interfaces is central to mechanistic studies of complex electrochemical processes, yet a great challenge. The coupling of electrochemistry (EC) and mass spectrometry (MS) has seen rapid development and found broad applicability in tackling challenges in analytical and bioanalytical chemistry. However, few truly in situ and real-time EC-MS studies have been reported at electrode-electrolyte interfaces. An innovative EC-MS coupling method named in situ liquid secondary ion mass spectrometry (SIMS) was recently developed by combining SIMS with a vacuum compatible microfluidic electrochemical device. Using this novel capability, we report the first in situ elucidation of the electro-oxidation mechanism of a biologically significant organic compound, ascorbic acid (AA), at the electrode-electrolyte interface. The short-lived radical intermediate was successfully captured, which had not been detected directly before. Moreover, we demonstrated the power of this new technique in real-time monitoring of the formation and dynamic evolution of electrical double layers at the electrode-electrolyte interface. This work suggests further promising applications of in situ liquid SIMS in studying more complex chemical and biological events at the electrode-electrolyte interface | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a Research Support, Non-U.S. Gov't | |
| 650 | 4 | |a Research Support, U.S. Gov't, Non-P.H.S. | |
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| 700 | 1 | |a Zhang, Yanyan |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Bingwen |e verfasserin |4 aut | |
| 700 | 1 | |a Wu, Kui |e verfasserin |4 aut | |
| 700 | 1 | |a Thevuthasan, Suntharampillai |e verfasserin |4 aut | |
| 700 | 1 | |a Baer, Donald R |e verfasserin |4 aut | |
| 700 | 1 | |a Zhu, Zihua |e verfasserin |4 aut | |
| 700 | 1 | |a Yu, Xiao-Ying |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Fuyi |e verfasserin |4 aut | |
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