Pd-Ni-B/C Nanocatalysts for Electrochemical Oxidation of Ethanol in Alkaline Media

J. Ribeiro, Ronaldo S. Silva, Giancarlo Richard Salazar Banda, K. Eguiluz
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引用次数: 1

Abstract

This paper describes the synthesis of Pd0.70-Nix-By nanoparticles (x:y = 0.30:0, 0:0.30, 0.25:0.05, 0.20:0.10, 0.15:0.15, and 0.10:0.20) supported on carbon Vulcan XC-72 R by the chemical reduction method using ethylene glycol as a reducing agent for the study of the electrochemical oxidation of ethanol in alkaline media. Neither surfactants nor templates were used during the syntheses. The catalysts were physically characterized by transmission electron microscopy that showed the formation of nanoparticles with diameters of approximately 3 nm. Analyses of X-ray dispersive energy spectroscopy coupled with scanning electron microscopy identified the presence of the synthesized metals in concentrations close to the nominal ones. The electrochemical study was performed by CO-stripping, cyclic voltammetry, chronoamperometry, and steady-state polarization curves. The catalytic efficiency was also evaluated against the oxidation of CO, which is the principal intermediate adsorbed on the surface of catalysts during ethanol oxidation. The Pd0.70Ni0.15B0.15/C catalyst showed the lowest oxidation onset potentials for both CO (0.37 V) and ethanol oxidation (0.51 V) compared with the Pd/C catalyst (0.63 V and 0.64 V). Chronoamperometric tests also revealed that the Pd0.70Ni0.15B0.15/C catalyst displayed current densities four times higher than those of the Pd/C catalyst, probably because of the electronic and geometric effect that favors the removal of intermediate species from the catalyst surface. The synthesized ternary catalysts were more efficient toward the electrochemical oxidation of ethanol in alkaline media than Pd0.7Ni0.3/C and Pd/C catalysts. Thus, the synergistic effect of boron on the structure of binary nanoparticle catalysts supported on carbon for use in direct alcohol fuel cells was demonstrated for the first time.
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碱性介质中乙醇电化学氧化的Pd-Ni-B/C纳米催化剂
本文以乙二醇为还原剂,采用化学还原法制备了以Vulcan XC-72 R为载体的pd0.70 - ni - by纳米粒子(x:y = 0.30: 0,0:0.30, 0.25:0.05, 0.20:0.10, 0.15:0.15, 0.10:0.20),用于研究乙醇在碱性介质中的电化学氧化作用。合成过程中既没有使用表面活性剂,也没有使用模板。通过透射电子显微镜对催化剂进行了物理表征,结果表明催化剂形成的纳米颗粒直径约为3 nm。x射线色散能谱和扫描电镜分析表明,合成金属的浓度与标称浓度接近。通过co汽提法、循环伏安法、计时安培法和稳态极化曲线进行了电化学研究。对乙醇氧化过程中吸附在催化剂表面的主要中间体CO的氧化效果进行了评价。与Pd/C催化剂(0.63 V和0.64 V)相比,Pd0.70Ni0.15B0.15/C催化剂的CO氧化电位(0.37 V)和乙醇氧化电位(0.51 V)最低。时间电流测试还表明,Pd0.70Ni0.15B0.15/C催化剂的电流密度比Pd/C催化剂高4倍,这可能是由于电子和几何效应有利于催化剂表面中间物质的去除。合成的三元催化剂对乙醇在碱性介质中的电化学氧化效果优于Pd0.7Ni0.3/C和Pd/C催化剂。因此,硼对用于直接醇燃料电池的碳负载二元纳米颗粒催化剂结构的协同效应首次得到证实。
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