Chen Sheng-pei, Huang Tao, Zhen Chun-hua, Zhang Qi, Gong Hui, Sun Shi-gang
State Key Laboratory for Physical Chemistry of Solid Surfaces, Department of Chemistry, Institute of Physical Chemistry, Xiamen University, Xiamen 361005, China.
Guang Pu Xue Yu Guang Pu Fen Xi. 2003 Apr;23(2):273-5.
Electrocatalytic properties of three electrodes for formic acid oxidation were studied by using electrochemical in situ FTIR spectroscopy and cyclic voltammetry in this paper. It is demonstrated that the electrocatalytical mechanism of formic acid oxidation on platinum-dispersed carbon(Pt/GC) is similar to that on massive platinum, which involves two paths, i.e. one way through active intermediate and the other through poison intermediate to CO2. The Pt/GC exhibits higher catalytivity than pure platinum. The electrode of Pt/GC modified by Sb (Sb-Pt/GC) was also prepared in the work. It was observed that the onset potential (Ei) for formic acid oxidation on Sb-Pt/GC was shift negatively for 0.20 V. The peak potential (Ep) was observed to shifted negatively to 0.34 V and the value of oxidation current (jp) was enhanced nearly 7.28 times. Similar results were also observed on surface alloy/GC prepared. In this case, Ei and Ep were -0.12 and 0.32 V, respectively, jp was enhanced about 8.15 times, and FWHM (full width at half maximum) was 0.50 V. It is indicated that Sb-Pt/GC and surface alloy/GC can not only effectively restrain the formation of poison intermediate CO, but also significantly increase the electrocatalytic activities for oxidation of active intermediates.
本文采用电化学原位傅里叶变换红外光谱和循环伏安法研究了三种电极对甲酸氧化的电催化性能。结果表明,甲酸在铂分散碳(Pt/GC)上的电催化氧化机理与在块状铂上相似,涉及两条路径,即一条通过活性中间体,另一条通过中毒中间体生成二氧化碳。Pt/GC表现出比纯铂更高的催化活性。工作中还制备了用Sb修饰的Pt/GC电极(Sb-Pt/GC)。观察到Sb-Pt/GC上甲酸氧化的起始电位(Ei)负移了0.20 V。峰电位(Ep)负移至0.34 V,氧化电流值(jp)提高了近7.28倍。在制备的表面合金/GC上也观察到了类似结果。在这种情况下,Ei和Ep分别为-0.12和0.32 V,jp提高了约8.15倍,半高宽(FWHM)为0.50 V。结果表明,Sb-Pt/GC和表面合金/GC不仅能有效抑制中毒中间体CO的形成,还能显著提高活性中间体氧化的电催化活性。