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The Role of Electrodeposited Pd Catalyst Loading on the Mechanisms of Formic Acid Electro-Oxidation

机译:电沉积钯催化剂负载量对甲酸电氧化机理的影响

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This work addresses the effects of Pd nanoparticle loading and dispersion on the mechanisms of formic acid (FA) electro-oxidation. For this purpose, different levels of Pd nanoparticle loading (0.10-0.98 mg cm~(-2)) with similar size (~10-13 nm) were electrodeposited on the carbon cloth via square wave pulse technique. The mechanisms of FA oxidation in 0.5 M HCOOH+0.5 M H2SO4 solution were studied and identified using cyclic voltammetry (CV) together with Fourier transform infrared spectroscopy (FTIR). Based on the obtained results, it was found that the electrochemical active surface area and Tafel slopes are independent of Pd loading levels, but both the shape and peak potential of the voltammograms are significantly affected by the Pd loading levels. The results of CV and FTIR showed that the different levels of Pd loading changes the FA oxidation pathway, which is attributed to the fact that the higher Pd loading results in the closer distribution of Pd nanoparticles. It was suggested that, at high Pd loading, the Pd-HCOO_(ads) formation is not the only available pathway for FA oxidation process and the Pd-CO_(ads) formation pathway also exists, which is oxidized to CO2 at more anodic potentials.
机译:这项工作解决了Pd纳米粒子负载和分散对甲酸(FA)电氧化机理的影响。为此,通过方波脉冲技术在碳布上电沉积了大小相似(〜10-13 nm)的不同水平的Pd纳米粒子负载量(0.10-0.98 mg cm〜(-2))。利用循环伏安法(CV)和傅立叶变换红外光谱法(FTIR)研究并鉴定了FA在0.5 M HCOOH + 0.5 M H2SO4溶液中的氧化机理。基于获得的结果,发现电化学活性表面积和Tafel斜率与Pd负载水平无关,但是伏安图的形状和峰值电势均受Pd负载水平显着影响。 CV和FTIR的结果表明,不同水平的Pd负载改变了FA氧化途径,这归因于较高的Pd负载导致Pd纳米颗粒分布更紧密。有人提出,在高Pd负载下,Pd-HCOO_(ads)的形成不是FA氧化过程的唯一可用途径,并且还存在Pd-CO_(ads)的形成途径,它在更多的阳极电势下被氧化成CO2。 。

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