Abstract
The hydrocarbons (HCs) are typical air pollutants causing photochemical smog or greenhouse effect. With the aim of producing new electrocatalysts for the butane oxidation reaction, and possibly other electrochemical oxidation processes, we have investigated the preparation and characterization of novel systems electrocatalysts for the oxydation of butane to produce less contaminant. Due to the feasibility to control the size and distribution of particles, the underpotential deposition was used. This method is very effective for the preparation of Mo-Ni Zr-Ni, Mo-Sn and Mo-Ni-Sn systems supported on the glass carbon (GC) at room temperature. The study of the codeposition process and the catalytic evaluation of different systems was performed in a thermostated three-electrode cell (T=22?C), using a microcomputer-controlled potentiostat/galvanostat Autolab with PGSTAT30 equip?ment and GPES software. Codeposits were prepared on glass carbon - based substrates (surface area 1 cm2). The reference electrode was an Ag/AgCl /1 mol dm-3 KCl electrode mounted in a Luggin capillary. The counterelectrode was a graphite rod . All solutions were prepared using reagent-grade chemicals [(NH4)2 Mo O4, 99.5 %, BDH), ( NiSO4.6H2O, 99%, Sigma), ( SnCl2.2H2O, 99%, BDH), (ZrOCl2.8H2O, 99%, Merck) (H3PO4 , p.a. Merck ) and ultrapure water (18.0 MQ cm-1) Milli-Q system. The n-butane (Matheson C.P., 99.99%) oxidative reaction was carried out with saturation in aqueous 0.5 M phosphoric acid solution, at 22?C. The n-butane is inert on GC under the experimental conditions of this work. Electrolytic phase formation of different systems on glassy carbon electrode was investigated using cyclic voltammetry and potential step techniques. Analysis of the current-time transients obtained for each alloys, indicated that distinct mechanisms of nucleation are involved during the early stages of codeposits (1). Detailed analysis of these mechanisms will be presented. Evaluation of electrocatalytic activity for butane oxidation in 0.5 M H3PO4 solution showed interesting performance for Mo (29,9 %)-Ni (2,7%)-Sn(67,4%) / GC and Ni (28,97%)-Zr (71,03%)/GC. The calculated exchange current density (io) were 1.2 x 10-12 and 5.13 x 10-9 A.cm-2 , respectively. This fact is highly significant and promising for other HCs.
Author(s): M. Choy M., J. M Ortega, M. Gonzalez, Z. Puentes.