Electro-Oxidation of Ethylene Glycol on a Pt-Film Electrode Studied by Combined in Situ Infrared Spectroscopy and Online Mass Spectrometry

被引:50
作者
Schnaidt, J. [1 ]
Heinen, M. [1 ]
Jusys, Z. [1 ]
Behm, R. J. [1 ]
机构
[1] Univ Ulm, Inst Surface Chem & Catalysis, D-89069 Ulm, Germany
关键词
SINGLE-CRYSTAL ELECTRODES; TIME FTIR SPECTROSCOPY; ELECTROCATALYTIC OXIDATION; PLATINUM-ELECTRODES; ELECTROCHEMICAL OXIDATION; CO ADSORPTION; CARBON-MONOXIDE; ACID; ETHANOL; SURFACE;
D O I
10.1021/jp208162q
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Adsorption and oxidation of ethylene glycol (EG) on a Pt thin film electrode was investigated in a combined spectro-electrochemical approach under continuous flow conditions, including potentiodynamic, potentiostatic, as well as adsorbate-stripping experiments. During the adsorption/electrooxidation of EG, the potential-dependent development of the EG adlayer was followed by highly surface sensitive, in situ attenuated total reflection Fourier transform infrared spectroscopy, while the volatile products were simultaneously monitored by online differential electrochemical mass spectrometry. For the assignment of the detected IR bands, comparative experiments following the adsorption/oxidation of the possible reaction intermediates/products (glycolaldehyde, glycolic acid, glyoxal, glyoxylic acid oxalic acid) were performed. The data show that (i) during the adsorption/oxidation of EG, COad is formed in the potential range between 0.1 and 0.7 V-RHE, which can be oxidized further to CO2 at potentials above 0.5 V. (ii) In addition to COad, adsorbed 2-hydroxyacetyl and glycolate were detected, where (iii) 2-hydroxyacetyl is a precursor to form adsorbed CO, and (iv) adsorbed glycolate exists in equilibrium with glycolic acid in solution.
引用
收藏
页码:2872 / 2883
页数:12
相关论文
共 66 条
[31]  
Iwasita T., 2003, HDB FUEL CELLSFUNFAM, V2, P603
[32]   ELECTROOXIDATION OF ETHYLENE-GLYCOL ON BISMUTH-MODIFIED PT(111) [J].
JIANG, XD ;
CHANG, SC ;
WEAVER, MJ .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1993, 89 (02) :223-228
[33]   ELECTROCATALYTIC OXIDATION OF ETHYLENE-GLYCOL .1. BEHAVIOR OF PLATINUM AD-ATOM ELECTRODES IN ACID-MEDIUM [J].
KADIRGAN, F ;
BEDEN, B ;
LAMY, C .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1982, 136 (01) :119-138
[34]   MECHANISTIC STUDY OF THE ELECTROOXIDATION OF ETHYLENE-GLYCOL ON GOLD AND ADATOM-MODIFIED GOLD ELECTRODES IN ALKALINE-MEDIUM [J].
KADIRGAN, F ;
BOUHIERCHARBONNIER, E ;
LAMY, C ;
LEGER, JM ;
BEDEN, B .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1990, 286 (1-2) :41-61
[35]   ELECTROCHEMICAL AND ADSORPTION BEHAVIOR OF ETHYLENE-GLYCOL AND ITS OXIDATIVE DERIVATIVES AT PLATINUM-ELECTRODES .1. ADSORPTION AND CHEMISORPTION PROCESSES [J].
KAZARINOV, VE ;
VASSILIEV, YB ;
ANDREEV, VN ;
HORANYI, G .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1983, 147 (1-2) :247-261
[36]   CATALYSIS OF ETHYLENE-GLYCOL OXIDATION ON A PT ELECTRODE MODIFIED BY FOREIGN METAL AD-ATOMS [J].
KOKKINIDIS, G ;
JANNAKOUDAKIS, D .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1982, 133 (02) :307-315
[37]   A THEORETICAL-ANALYSIS OF THE VIBRATIONAL-SPECTRUM OF CARBON-MONOXIDE ON PLATINUM METAL-ELECTRODES [J].
KORZENIEWSKI, C ;
PONS, S ;
SCHMIDT, PP ;
SEVERSON, MW .
JOURNAL OF CHEMICAL PHYSICS, 1986, 85 (07) :4153-4160
[38]   Role of crystalline defects in electrocatalysis: CO adsorption and oxidation on stepped platinum electrodes as studied by in situ infrared spectroscopy [J].
Lebedeva, NP ;
Rodes, A ;
Feliu, JM ;
Koper, MTM ;
van Santen, RA .
JOURNAL OF PHYSICAL CHEMISTRY B, 2002, 106 (38) :9863-9872
[39]   REAL-TIME FTIR SPECTROSCOPY AS A QUANTITATIVE KINETIC PROBE OF COMPETING ELECTROOXIDATION PATHWAYS FOR SMALL ORGANIC-MOLECULES [J].
LEUNG, LWH ;
WEAVER, MJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1988, 92 (14) :4019-4022
[40]   INFLUENCE OF ADSORBED CARBON-MONOXIDE ON THE ELECTROCATALYTIC OXIDATION OF SIMPLE ORGANIC-MOLECULES AT PLATINUM AND PALLADIUM ELECTRODES IN ACIDIC SOLUTION - A SURVEY USING REAL-TIME FTIR SPECTROSCOPY [J].
LEUNG, LWH ;
WEAVER, MJ .
LANGMUIR, 1990, 6 (02) :323-333