Pd/Ni异结构纳米催化剂的制备及其对甲酸氧化的电催化(英文)  

Electrocatalytic Oxidation of Formic Acid on Pd/Ni Heterostructured Catalyst

作　　者：任明军[1,2] 邹亮亮[1,2] 陈举[1] 袁婷[1] 黄庆红[1] 张海峰[1] 杨辉[1] 封松林[1] 

机构地区：[1]中国科学院上海高等研究院,上海201210 [2]中国科学院研究生院,北京100039

出　　处：《电化学》2012年第6期515-520,共6页Journal of Electrochemistry

基　　金：supported by the National Basic Research Program of China(973 Program)(No.2012CB932800);the Natural Science Foundation of China(No.21073219);Shanghai Science and Technology Committee(No.11DZ1200400);the Knowledge Innovation Engineering of the CAS(No.12406,124091231)

摘　　要：通过两步还原法制备了Pd/Ni双金属催化剂.由于金属Pd原子在先行还原的Ni纳米粒子表面的外延生长以及其在Ni表面和Pd表面生长表现出的吉布斯自由能差异,最终导致了异结构Pd/Ni纳米粒子的形成.高分辨电子透射显微镜结果证实了异结构的存在,然而X射线衍射测量表明Pd/Ni纳米粒子具有类似于Pd的面心立方结构.制备的Pd/Ni纳米粒子与同等条件下合成的Pd纳米粒子相比,对甲酸氧化呈现了更高的电催化活性,而且电催化稳定性也要明显优于纯Pd纳米粒子,证明了Pd/Ni双金属催化剂是可选的直接甲酸燃料电池阳极催化剂.双金属催化剂对甲酸氧化电催化活性和稳定性增强可能是Ni原子的修饰改变了Pd粒子表面配位不饱和原子的电子结构所致.A Pd/Ni bimetallic nanostructured electrocatalyst was fabricated via a two-step reduction route.Owing to an epitaxial growth of Pd atoms on the surface of Ni nanoparticles,heterostructured Pd/Ni nanocomposites were formed and verified by high resolution transmission electron microscopy combined with energy-dispersion X-ray spectroscopy.X-ray diffraction confirmed that the as-prepared Pd/Ni nanocomposites possessed a single face-centered-cubic（fcc） Pd structure,probably due to a weaker diffraction intensity of metallic Ni and/or overlapping by that of Pd.The intrinsic catalytic activity on the Pd/Ni is higher than that on the Pd.Moreover,the durability of formic acid oxidation on the Pd/Ni was much enhanced over the Pd nanoparticles.The change in electronic structure of the surface coordination unsaturated Pd atoms and the possible dissolution of Ni species from the Pd/Ni heterostructure may account for such an improved durability for formic acid oxidation.

关 键 词：甲酸氧化 电催化 PD Ni双金属 稳定性 

分 类 号：O643.32[理学—物理化学]