Nitrate reduction on single-crystal platinum electrodes

被引:161
作者
Dima, GE [1 ]
Beltramo, GL [1 ]
Koper, MTM [1 ]
机构
[1] Eindhoven Univ Technol, Schuit Inst Catalysis, Inorgan Chem & Catalysis Lab, NL-5600 MB Eindhoven, Netherlands
关键词
nitrate reduction; platinum single-crystal electrodes; nitric oxide; FTIR; electrocatalysis;
D O I
10.1016/j.electacta.2005.02.093
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
The structure sensitivity of the reduction of nitrate has been studied on a series of single-crystal platinum electrodes by cyclic voltammmetry and in situ FTIRAS in sulfuric and perchloric acid solutions. The nitrate reduction is a structure-sensitive reaction on single-crystal platinum electrodes. However, this structure sensitivity is essentially controlled by other species (hydrogen, sulfate) that interact strongly with the electrode surface rather than by a structure-sensitive nitrate adsorption, dissociation or reduction. Voltammetric and spectroscopic data point to adsorbed nitric oxide (NO) as the main stable intermediate of the nitrate reduction to ammonia. No evidence for the formation of N2O was found. On surfaces with sufficiently wide (111) terraces in the absence of specifically adsorbed sulfate, an oxidizable nitrate reduction product is detected voltammetrically, which may tentatively be attributed to the formation of a small amount of hydroxylamine earlier during the voltammetric scan. (C) 2005 Elsevier Ltd. All rights reserved.
引用
收藏
页码:4318 / 4326
页数:9
相关论文
共 26 条
[1]   ANION SURFACE INTERACTIONS .2. NITROUS-OXIDE REDUCTION AS A PROBE OF ANION ADSORPTION ON TRANSITION-METAL SURFACES [J].
AHMADI, A ;
BRACEY, E ;
EVANS, RW ;
ATTARD, G .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1993, 350 (1-2) :297-316
[2]   ANION-SURFACE INTERACTIONS .3. N2O REDUCTION AS A CHEMICAL PROBE OF THE LOCAL POTENTIAL OF ZERO TOTAL CHARGE [J].
ATTARD, GA ;
AHMADI, A .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1995, 389 (1-2) :175-190
[3]   VOLTAMMETRIC BEHAVIOR OF NO3- IONS AT PLATINIZED PLATINUM-ELECTRODES (ELECTROCATALYTIC ACTIVITY OF ELECTRODES WITH (100) PREFERRED ORIENTATION) [J].
BAKOS, I ;
HORANYI, G .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1994, 370 (1-2) :309-313
[4]   Nitric oxide reduction and oxidation on stepped pt[n(111)x(111)] electrodes [J].
Beltramo, GL ;
Koper, MTM .
LANGMUIR, 2003, 19 (21) :8907-8915
[5]   ELECTROCHEMICAL ADSORPTION BEHAVIOR OF PLATINUM STEPPED SURFACES IN SULFURIC-ACID-SOLUTIONS [J].
CLAVILIER, J ;
ARMAND, D ;
SUN, SG ;
PETIT, M .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1986, 205 (1-2) :267-277
[6]  
DACUHNA MCM, 1996, J ELECTROANAL CHEM, V441, P163
[7]   CVD preparation of catalytic membranes for reduction of nitrates in water [J].
Daub, K ;
Wunder, VK ;
Dittmeyer, R .
CATALYSIS TODAY, 2001, 67 (1-3) :257-272
[8]   The influence of nitrate concentration and acidity on the electrocatalytic reduction of nitrate on platinum [J].
de Groot, MT ;
Koper, MTM .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2004, 562 (01) :81-94
[9]   Mechanistic study of the nitric oxide reduction on a polycrystalline platinum electrode [J].
de Vooys, ACA ;
Koper, MTM ;
van Santen, RA ;
van Veen, JAR .
ELECTROCHIMICA ACTA, 2001, 46 (06) :923-930
[10]   Electrocatalytic reduction of nitrate at low concentration on coinage and transition-metal electrodes in acid solutions [J].
Dima, GE ;
de Vooys, ACA ;
Koper, MTM .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2003, 554 :15-23