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Application of CO atmosphere in the liquid phase synthesis as a universal way to control the microstructure and electrochemical performance of Pt/C electrocatalysts
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2018-01-08 , DOI: 10.1016/j.apcatb.2018.01.013
Anastasia A. Alekseenko , Evgenia A. Ashihina , Svetlana P. Shpanko , Vadim A. Volochaev , Olga I. Safronenko , Vladimir E. Guterman

A number of new platinum-based catalysts with Pt loading from 15.2% to 17.3% was obtained by wet chemical synthesis. Ethylene glycol, formaldehyde, and formic acid were used as reducing agents. The synthesis was performed both at ambient conditions and when the solution was saturated with carbon monoxide.

It was shown that the catalysts obtained in the CO environment possess a larger electrochemical active surface area (EСSA), 140–146 m2 g−1 (Pt), compared to the analogues that have been made at ambient conditions, 72–120 m2 g−1(Pt). This could be explained by a smaller platinum NPs average size as well as a very narrow distribution of their size. In contrast to the materials synthesized at ambient conditions, the ECSA values of the catalysts, obtained in the CO-saturated media, in fact, do not depend on the type of reducing agent and the synthesis conditions. Such catalysts demonstrate the best mass-activity in ORR, which is higher than that of the commercial Pt/C catalyst HiSPEC 3000 (20% of Pt loading) and the analogues obtained at ambient conditions.

Distinctive features of the nanoparticles nucleation/growth and their structure were determined and studied when formic acid was applied as a reducing agent. Absorption processes of the CO molecules on the surface of platinum nuclei are a plausible explanation for the CO influence on nucleation/growth and, therefore, on the microstructure and EСSA, as well as other functional characteristics of Pt/C-catalysts.



中文翻译:

CO气氛在液相合成中的应用作为控制Pt / C电催化剂微观结构和电化学性能的通用方法

通过湿化学合成获得了许多新型的铂基催化剂,其铂负载量为15.2%至17.3%。乙二醇,甲醛和甲酸用作还原剂。合成是在环境条件下和溶液用一氧化碳饱和时进行的。

结果表明,与在环境条件下制备的类似物72–120 m相比,在CO环境中获得的催化剂具有更大的电化学活性表面积(EСSA)140–146 m 2  g -1(Pt)。2 克-1(铂)。这可以通过较小的铂NP平均尺寸以及其尺寸的非常窄的分布来解释。与在环境条件下合成的材料相反,在CO饱和介质中获得的催化剂的ECSA值实际上不取决于还原剂的类型和合成条件。这类催化剂在ORR中表现出最佳的质量活性,高于商业化的Pt / C催化剂HiSPEC 3000(Pt负载的20%)和在环境条件下获得的类似物。

当使用甲酸作为还原剂时,确定并研究了纳米颗粒成核/生长的独特特征及其结构。铂原子核表面上CO分子的吸收过程是CO对成核/生长,因此对微结构和EСSA以及Pt / C催化剂的其他功能特性的影响的合理解释。

更新日期:2018-01-08
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