PtNiSnO_2/C的制备、表征及其电催化氧化乙醇活性  

Preparation and Characterization of Pt-Ni-SnO_2/C for Ethanol Oxidation Reaction

作　　者：黄明辉[1] 金碧瑶[1] 赵莲花[1] 孙世刚[2] 

机构地区：[1]延边大学理学院化学系,吉林延吉133002 [2]厦门大学固体表面物理化学国家重点实验室,福建厦门361005

出　　处：《物理化学学报》2017年第3期563-572,共10页Acta Physico-Chimica Sinica

基　　金：吉林省科技发展计划项目(20120741);厦门大学固体表面物理化学国家重点实验室开放课题(201407)资助~~

摘　　要：采用改进的B?nnemann法成功制备了Pt/C、Pt-Ni_(1/3)/C、Pt-SnO_2/C、Pt-Ni_x-SnO_2/C(x=1/4,1/3,2/3,1)阳极电催化剂。利用X射线衍射(XRD)、高分辨透射电子显微镜(HR-TEM)以及X射线光电子能谱(XPS)对催化剂晶型结构、表面形貌和表面电子结构进行了表征。运用线性扫描伏安(LSV)和电流密度-时间(j-t)曲线进行电化学测试,研究了乙醇电催化氧化(EOR)活性。并用原位红外光谱(in situ FT-IR)研究了EOR过程中产物的分布。结果表明,Pt-Ni_(1/3)-SnO_2/C是由Pt-Ni合金和SnO_2两相组成。XPS结果表明,在Pt-SnO_2中添加微量的Ni,Pt表面电子结构发生了改变。电化学结果表明,三元催化剂的EOR活性均优于二元和纯Pt,其中Pt-Ni_(1/3)-SnO_2/C的EOR活性最佳。Ni和SnO_2的加入并没有显著提高乙醇C―C键的断裂能力,但是二者的协同作用在低电位(0.1 V)下加强了乙醛的进一步氧化,生成了乙酸。A series of Pt/C, Pt-NilEC, Pt-SnOJC and Pt-Ni-SnOJC （x = 1/4, 1/3, 2/3, 1）anode electro-catalysts have been synthesized by an improved B6nnemann method. The crystal structure, surface morphology and surface electronic structure were characterizated by X-ray diffraction （XRD）, high resolution transmission electron microscope （HR-TEM） and X-ray photoelectron spectroscopy （XPS）. The electro-catalytic activities were characterizated by linear sweep voltammetry （LSV） and amperometric current density-time （j-t） curve techniques for ethanol oxidation reaction （EOR）. In sfu spectroelectrochemical studies have been used to identity adsorbed reaction intermediates and products （in situ Fourier transform infrared spectroscopy, FT-IR）. XRD and HR-TEM analysis revealed two phases in the ternary Pt-Ni-SnO2/C catalyst： Pt-Ni alloys and SnO2. XPS results show that the electronic structure of the Pt in Pt-Nil,3-SnOJC might be changed due to the addition of Ni. The activity of Pt-Ni-SnO2/C for EOR was found to be higher than that of Pt/C, Pt-Ni/C and Pt-SnOJC catalysts. The incorporation of Ni and SnO2 did not significantly improve C--C bond breaking for complete oxidation of ethanol, but the synergy under the low potential （0.1 V） to strengthen the further oxidation of acetaldehyde, generate the acetic acid.

关 键 词：铂 镍 二氧化锡 乙醇电氧化 

分 类 号：O643.36[理学—物理化学]