物理化学学报 >> 2017, Vol. 33 >> Issue (3): 563-572.doi: 10.3866/PKU.WHXB201612072

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PtNiSnO2/C的制备、表征及其电催化氧化乙醇活性

黄明辉1,金碧瑶1,赵莲花1,*(),孙世刚2   

  1. 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
  • 收稿日期:2016-10-12 发布日期:2017-03-07
  • 通讯作者: 赵莲花 E-mail:zhaolianhua@ybu.edu.cn
  • 基金资助:
    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)

Preparation and Characterization of Pt-Ni-SnO2/C for Ethanol Oxidation Reaction

Ming-Hui HUANG1,Bi-Yao JIN1,Lian-Hua ZHAO1,*(),Shi-Gang SUN2   

  1. 1 Department of Chemistry, College of Science, Yanbian University, Yanji 133002, Jilin Province, P. R. China
    2 State Key Laboratory of Physical Chemistry of Solid Surfaces of Xiamen University, Xiamen 361005, Fujian Province, P. R. China
  • Received:2016-10-12 Published:2017-03-07
  • Contact: Lian-Hua ZHAO E-mail:zhaolianhua@ybu.edu.cn
  • Supported by:
    The project was supported by the Jilin Provincial Science and Technology Project of China(20120741);Opening Foundation of State KeyLaboratory of Physical Chemistry of Solid Surface of Xiamen University, China(201407)

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摘要：

采用改进的B?nnemann法成功制备了Pt/C、Pt-Ni1/3/C、Pt-SnO2/C、Pt-Nix-SnO2/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-Ni1/3-SnO2/C是由Pt-Ni合金和SnO2两相组成。XPS结果表明，在Pt-SnO2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-Ni1/3-SnO2/C的EOR活性最佳。Ni和SnO2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。

关键词: 铂, 镍, 二氧化锡, 乙醇电氧化

Abstract:

A series of Pt/C, Pt-Ni1/3/C, Pt-SnO2/C and Pt-Nix-SnO2/C (x=1/4, 1/3, 2/3, 1) anode electro-catalysts have been synthesized by an improved B?nnemann 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 situ 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-Ni1/3-SnO2/C 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-SnO2/C 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.

Key words: Platinum, Nickel, Stannic oxide, Ethanol electricoxidation