Methanol Oxidation at Diamond-Supported Pt Nanoparticles: Effect of the Diamond Surface Termination
Methanol Oxidation at Diamond-Supported Pt Nanoparticles: Effect of the Diamond Surface Termination
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金刚石负载的 Pt 纳米粒子的甲醇氧化：金刚石表面终止的影响
DOI：
10.1021/jp4039804
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发表时间：
2013
期刊：
影响因子：
--
通讯作者：
Celorrio V
中科院分区：
文献类型：
--
作者：
Celorrio V
用差示电化学质谱(DEM)研究了高温高压金刚石颗粒负载的铂纳米粒子对吸附CO、甲醇和甲酸氧化的电催化活性。金刚石颗粒被用作尺寸稳定的电催化剂载体，其表面处理导致材料的表面主要具有氢(HDP)或氧基官能团(ODP)。采用浸渍法制备了平均直径小于5 nm的铂纳米粒子。与吸附CO氧化有关的伏安响应似乎不受金刚石载体表面终止的影响。然而，在酸性溶液中甲醇的氧化表现出很大的不同，铂/HDP产生的电流密度比铂/ODP型和商用铂催化剂(Pt/E-TEK)要小。DEM研究表明，铂/丙二醛和铂/E-TEK具有较高的CO2转化效率，而铂/HDP的转化效率约为90%。在所有催化剂上都有甲酸作为中间产物生成的证据。与甲酸氧化相关的电流密度也有显著差异，铂/HDP也提供了最低的电流密度。实验数据表明，吸附的HCOO2物种是甲醇氧化的关键中间体，其后续的氧化为CO2强烈地受到金刚石载体表面有效终止的影响。
The electrocatalytic reactivity of Pt nanoparticles supported on high-pressure, high-temperature diamond particles toward adsorbed CO, methanol, and formic acid oxidation is investigated employing differential electrochemical mass spectrometry (DEMS). Surface treatment of diamond particles, employed as dimensionally stable electrocatalyst supports, leads to materials with surfaces featuring mainly hydrogen (HDP) or oxygen-based functional groups (ODP). Pt nanoparticles with average diameter below 5 nm were generated by impregnation of the modified diamond particles. The voltammetric responses associated with the oxidation of adsorbed CO appeared unaffected by the surface termination of the diamond support. However, significant differences were observed for methanol oxidation in acid solutions, with Pt/HDP producing smaller current densities than Pt/ODP and a commercially available Pt catalyst (Pt/E-TEK). DEMS studies show higher conversion efficiencies to CO2for Pt/ODP and Pt/E-TEK, while Pt/HDP exhibited values of approximately 90%. Evidence of formic acid generation as intermediate during methanol oxidation was obtained on all catalysts. Significant differences in the current density associated with the oxidation of formic acid were also observed, with Pt/HDP also providing the lowest current densities. The ensemble of the experimental data suggests that adsorbed HCOOadsspecies is the key intermediate in methanol oxidation, and its subsequent oxidation to CO2is strongly affected by the effective surface termination of the diamond support.
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