Electrocatalytic reduction of NO3- on palladium/copper electrodes

被引:264
作者
de Vooys, ACA [1 ]
van Santen, RA [1 ]
van Veen, JAR [1 ]
机构
[1] Eindhoven Univ Technol, Dept Inorgan Chem & Catalysis, NL-5600 MB Eindhoven, Netherlands
关键词
electrocatalytic reduction; nitrate reduction; palladium/copper; DEMS; nitrite;
D O I
10.1016/S1381-1169(99)00375-1
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
The reduction of NO3- on palladium/copper electrodes has been studied using differential electrochemical mass spectroscopy (DEMS), rotating ring-disk electrodes (RRDE) and quartz microbalance electrodes (ECQM). In acidic electrolytes, the activity increases linearly with Cu coverage, in alkaline electrolytes, a different dependence on coverage is observed. One monolayer of Cu gives a different selectivity from bulk copper. The adsorption of NO3- is competitive with SO42-, whereas Cl- adsorption blocks the reduction. Competitive adsorption lowers both the activity and the selectivity to N-2. Copper activates the first electron transfer, the role of palladium is to steer the selectivity towards N-2. The trends in activity and selectivity are explained in terms of coverage of N-species. (C) 2000 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:203 / 215
页数:13
相关论文
共 28 条
  • [1] ANION SURFACE INTERACTIONS .2. NITROUS-OXIDE REDUCTION AS A PROBE OF ANION ADSORPTION ON TRANSITION-METAL SURFACES
    AHMADI, A
    BRACEY, E
    EVANS, RW
    ATTARD, G
    [J]. JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1993, 350 (1-2) : 297 - 316
  • [2] BALZERS AG, 1991, MANUAL MASS SPECTROM
  • [3] Characterization of supported Pd-Cu bimetallic catalysts by SEM, EDXS, AES and catalytic selectivity measurements
    Batista, J
    Pintar, A
    Ceh, M
    [J]. CATALYSIS LETTERS, 1997, 43 (1-2) : 79 - 84
  • [4] VOLTAMMETRIC STUDY OF THE UNDERPOTENTIAL DEPOSITION OF COPPER ON POLYCRYSTALLINE AND SINGLE-CRYSTAL PALLADIUM SURFACES
    CHIERCHIE, T
    MAYER, C
    [J]. ELECTROCHIMICA ACTA, 1988, 33 (03) : 341 - 345
  • [5] Adsorption and reactivity of NO on Cu(111): A synchrotron infrared reflection absorption spectroscopic study
    Dumas, P
    Suhren, M
    Chabal, YJ
    Hirschmugl, CJ
    Williams, GP
    [J]. SURFACE SCIENCE, 1997, 371 (2-3) : 200 - 212
  • [6] ELECTROREDUCTION OF NITROUS-OXIDE TO NITROGEN USING A GAS-DIFFUSION ELECTRODE LOADED WITH PT CATALYST
    FURUYA, N
    YOSHIBA, H
    [J]. JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1991, 303 (1-2): : 271 - 275
  • [7] The study of NO adsorbate layers on platinized platinum in the liquid phase with cyclic voltammetry, DEMS and FTIRS
    Gootzen, JFE
    vanHardeveld, RM
    Visscher, W
    vanSanten, RA
    vanVeen, JAR
    [J]. RECUEIL DES TRAVAUX CHIMIQUES DES PAYS-BAS-JOURNAL OF THE ROYAL NETHERLANDS CHEMICAL SOCIETY, 1996, 115 (11-12): : 480 - 485
  • [8] The electrocatalytic reduction of NO3- on Pt, Pd and Pt+Pd electrodes activated with Ge
    Gootzen, JFE
    Peeters, PGJM
    Dukers, JMB
    Lefferts, L
    Visscher, W
    vanVeen, JAR
    [J]. JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1997, 434 (1-2): : 171 - 183
  • [9] Improving the selectivity of catalytic degradation of nitrate by use of mixed catalysts made of nitrate reducing PdCu/Al2O3 and nitrite reducing Pd/Al2O3 catalysts
    Hahnlein, M
    Prusse, U
    Horold, S
    Vorlop, KD
    [J]. CHEMIE INGENIEUR TECHNIK, 1997, 69 (1-2) : 90 - 93
  • [10] ROLE OF ADSORPTION PHENOMENA IN THE ELECTROCATALYTIC REDUCTION OF NITRIC-ACID AT A PLATINIZED PLATINUM-ELECTRODE
    HORANYI, G
    RIZMAYER, EM
    [J]. JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1982, 140 (02) : 347 - 366