具有高活性和突出的抗中毒性能的Pt 修饰Ru/C催化剂的制备和表征

doi:10.3866/PKU.WHXB20101214

物理化学学报 >> 2010, Vol. 26 >> Issue (12): 3193-3198.doi: 10.3866/PKU.WHXB20101214

具有高活性和突出的抗中毒性能的Pt 修饰Ru/C催化剂的制备和表征

高海丽, 廖世军, 曾建皇, 梁振兴, 谢义淳

华南理工大学化学与化工学院, 广州510641

收稿日期:2010-05-25 修回日期:2010-09-29 发布日期:2010-12-01
通讯作者: 廖世军 E-mail:chsjliao@scut.edu.cn
基金资助:
国家自然科学基金(20673040, 20876062)和国家高技术研究发展计划项目(863) (2009AA05Z119)资助

Preparation and Characterization of Platinum-Decorated Ru/C Catalyst with High Performance and Superior Poison Tolerance

GAO Hai-Li, LIAO Shi-Jun, ZENG Jian-Huang, LIANG Zhen-Xing, XIE Yi-Chun

School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, P. R. China

Received:2010-05-25 Revised:2010-09-29 Published:2010-12-01
Contact: LIAO Shi-Jun E-mail:chsjliao@scut.edu.cn
Supported by:
The project was supported by the National Natural Science Foundation of China (20673040, 20876062) and National High-Tech Research and Development Program of China (863) (2009AA05Z119).

摘要/Abstract

摘要：

采用两步浸渍-还原法制备了一种具有高Pt 利用效率, 高性能的Pt 修饰的Ru/C催化剂(Ru@Pt/C). 对于甲醇的阳极氧化反应, 该催化剂的单位质量铂的催化活性分别为Pt/C、自制PtRu/C 和商业JM PtRu/C 催化剂的1.9、1.5和1.4倍; 其电化学活性比表面积分别为Pt/C 和自制PtRu/C的1.6和1.3倍. 尤为重要的是该催化剂对甲醇氧化中间体具有很好的去除能力, 其正向扫描的氧化峰的峰电流密度(I_f)与反向扫描氧化峰的峰电流密度(I_b)之比可高达2.4, 为Pt/C 催化剂的I_f/I_b的2.7 倍, 表明催化剂具有很好的抗甲醇氧化中间体毒化的能力.另外, Ru@Pt/C催化剂的稳定性也高于Pt/C、自制PtRu/C 和商业JM PtRu/C 催化剂的稳定性. 采用X射线衍射(XRD)、透射电镜(TEM)和X射线光电子能谱(XPS)对催化剂进行了表征, Pt 在Ru表面的包覆结构得到了印证. Ru@Pt/C的高铂利用效率、高性能和高抗毒能力使其有望成为一种理想的直接甲醇燃料电池电催化剂.

关键词: 直接甲醇燃料电池, Pt修饰Ru/C, 电催化剂, 甲醇氧化, 抗中毒能力

Abstract:

A platinum-decorated Ru/C catalyst with high platinum utilization efficiency, high performance, and high poisoning tolerance was prepared using a two-stage impregnation reduction method. We found that for anodic methanol oxidation the catalyst activity in terms of the Pt load was 1.9 and 1.5 times as that of Pt/C and PtRu/C alloy catalysts, respectively. These values are also higher than that of the commercial JM PtRu/C catalyst. The electrochemically active surface area of Ru@Pt/C was found to be 1.6 and 1.3 times as those of Pt/C and PtRu/C alloy catalysts, respectively. Furthermore, we found that the ratio of the forward peak current density (I_f) to the backward peak current density (I_b) reached 2.4, which was 2.7 times as that of the Pt/C catalyst. This implies that the Pt-decorated Ru/C catalyst possesses a high tolerance for the intermediate poisoning species. In addition, the stability of Ru@Pt/C was higher than that of Pt/C, PtRu/ C alloy and JM PtRu/C. The catalyst was characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The core-shell structure of the catalyst was determined by XRD and TEM. The high performance and high poisoning tolerance of Ru@Pt/C during the anodic oxidation of methanol make it a promising electrocatalyst for direct methanol fuel cells.

Key words: Direct methanol fuel cell, Platinum-decorated Ru/C, Electrocatalyst, Methanol oxidation, Poison tolerance

高海丽, 廖世军, 曾建皇, 梁振兴, 谢义淳. 具有高活性和突出的抗中毒性能的Pt 修饰Ru/C催化剂的制备和表征[J]. 物理化学学报, 2010, 26(12): 3193-3198.

GAO Hai-Li, LIAO Shi-Jun, ZENG Jian-Huang, LIANG Zhen-Xing, XIE Yi-Chun. Preparation and Characterization of Platinum-Decorated Ru/C Catalyst with High Performance and Superior Poison Tolerance[J]. Acta Phys. -Chim. Sin., 2010, 26(12): 3193-3198.

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB20101214

https://www.whxb.pku.edu.cn/CN/Y2010/V26/I12/3193

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具有高活性和突出的抗中毒性能的Pt 修饰Ru/C催化剂的制备和表征

Preparation and Characterization of Platinum-Decorated Ru/C Catalyst with High Performance and Superior Poison Tolerance

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