Electrocatalytic Oxidation of Formic Acid on Pd/Ni Heterostructured Catalyst

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表面及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.This work was 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) and the Knowledge Innovation Engineering of the CAS (No. 12406, 124091231).This work was 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) and the Knowledge Innovation Engineering of the CAS (No. 12406, 124091231).作者联系地址：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 100039Author's Address: 1. Shanghai Advanced Research Institute, Chinese Academy of Sciences CAS, Shanghai 201210, China; 2. Graduate School of the CAS, Beijing 100039, China通讯作者E-mail：[email protected] & [email protected]

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