Identification of Fleeting Electrochemical Reaction Intermediates Using Desorption Electrospray Ionization Mass Spectrometry

被引：103

作者：

Brown, Timothy A. ^{[1
]}

Chen, Hao ^{[2
,3
]}

Zare, Richard N. ^{[1
]}

机构：

[1] Stanford Univ, Dept Chem, Stanford, CA 94305 USA

[2] Ohio Univ, Dept Chem & Biochem, Ctr Intelligent Chem Instrumentat, Athens, OH 45701 USA

[3] Ohio Univ, Edison Biotechnol Inst, Athens, OH 45701 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2015年 / 137卷 / 23期

基金：

美国国家科学基金会;

关键词：

THIN-LAYER SPECTROELECTROCHEMISTRY; SONIC-SPRAY IONIZATION; URIC-ACID; REACTION-MECHANISMS; CYCLIC VOLTAMMETRY; REACTION-PRODUCTS; OXIDATION; ONLINE; INSTRUMENTATION; SPECTROSCOPY;

D O I：

10.1021/jacs.5b03862

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

We report a new method; for the mass spectrometric detection of fleeting reaction intermediates in electrochemical reactions utilizing a "waterwheel" working electrode setup. This Setup takes inspiration from desorption electrospray ionization. (DESI) mass spectrometry, where the sampling time is on the order of milliseconds, to sample directly from the surface of a working electrode for mass spectrometric analysis. We present data that show the formation of a diimine intermediate of the electrochemical oxidation of uric acid that has a lifetime in solution of 23 ms as well as data that provide evidence for the formation of a similar diimine species from the electrooxidation of xanthine, which has not been previously observed.

引用

页码：7274 / 7277

页数：4

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