研究论文

Nb2O5·nH2O-PtRu/C 的制备及其对甲醇氧化的催化作用

  • 李伟伟 ,
  • 张向军 ,
  • 卢世刚
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  • a. 北京有色金属研究总院 动力电池研究中心 北京 100088;
    b. 新乡学院化学与化工学院 河南新乡 453000

收稿日期: 2011-09-28

  修回日期: 2011-12-17

  网络出版日期: 2012-01-14

基金资助

国家高技术研究发展计划(863 计划)(No. 2007AA03Z245)资助项目.

Preparation and Activity of Nb2O5·nH2O-PtRu/C for Methanol Oxidation

  • Li Weiwei ,
  • Zhang Xiangjun ,
  • Lu Shigang
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  • a. R&D Centre for Vehicle Battery and Energy Storage, General Research Institute for Nonferrous Metals, Beijing 100088;
    b. College of Chemistry and Chemical Engineering of Xinxiang University, Xinxiang 453000, Henan

Received date: 2011-09-28

  Revised date: 2011-12-17

  Online published: 2012-01-14

Supported by

Project supported by the National High Technology Research and Development Program (No. 2007AA03Z245).

摘要

采用沉淀法制备了甲醇氧化电催化剂10%Nb2O5·nH2O-20%Pt10%Ru/C, 并在Ar 气氛下对它进行了热处理. 用X射线衍射(XRD), 透射电子显微镜(TEM)和X 射线光电子谱(XPS)研究了热处理对催化剂的结构和形貌的影响, 用循环伏安法和计时电流法研究了热处理对催化剂的电化学性能的影响. 结果表明: 催化剂中看不到Ru 的衍射峰存在, Pt 晶粒以面心立方体结构存在, Nb2O5·nH2O 对Pt 的结合能基本无影响; 与20%Pt10%Ru/C 相比, 同温度热处理的条件下,10%Nb2O5·nH2O-20%Pt10%Ru/C 催化剂中Pt, Ru 合金化程度较差, 活性组分颗粒较小、分散均匀, 而且催化甲醇氧化性能和抗“CO”毒化性能较好, 700 ℃热处理的10%Nb2O5·nH2O-20%Pt10%Ru/C 的性能最好. Nb2O5·nH2O 不仅能抑制热处理过程中活性颗粒的长大和Pt, Ru 的合金化, 还能促进氢离子的传递, 提供活性“-OH”, 使甲醇及其氧化中间体更容易吸附-脱附.

本文引用格式

李伟伟 , 张向军 , 卢世刚 . Nb2O5·nH2O-PtRu/C 的制备及其对甲醇氧化的催化作用[J]. 化学学报, 2012 , 70(9) : 1073 -1080 . DOI: 10.6023/A1103286

Abstract

10%Nb2O5·nH2O-20%Pt10%Ru/C electro-catalyst for methanol oxidation was prepared by deposition method, followed with heat treatment in Ar atmosphere. The effect of heat treatment on morphology, structure and electrochemistry performance of the product was characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), cyclic voltammetry and chronoamperograms. No diffraction peaks of Ru were observed in the XRD patterns, while all the peaks of Pt were in accordance with the face centered cubic crystal structure. The binding energy of Pt was not affected by Nb2O5·nH2O. Compared with 20%Pt10%Ru/C, in 10%Nb2O5·nH2O-20%Pt10%Ru/C samples, the activated particles were uniformly dispersed, and the performances of methanol oxidation and resistance to “CO” were better. The results indicated that the introduction of Nb2O5·nH2O inhibited the growth of active particles, and decreased the alloying degree of Pt-Ru during heat treatment. Besides, Nb2O5·nH2O also provided active “-OH” and improved H+ transfer, leading to easier adsorption-desorption of methanol and its oxidation intermediates.

参考文献

1 Bai, Z.-Y.; Yang, L.; Zhang, J.-S.; Li, L.; Hu, C.-G.; Lv, J.; Guo, Y.-M. J. Power Sources 2010, 195, 2653.  

2 Diaz, V. M.; Ohanian, C. F. Int. J. Hydrogen Energy 2010,15, 10539.

3 Sakthivel, M.; Schlange, A.; Kunz, U.; Turek, T. J. Power Sources 2010, 195, 7083.  

4 Wang, J.-S.; Guo, X.; Song, C.-Y. Acta Phys.-Chim. Sin.2009, 25, 767 (in Chinese). (王建设, 郭勋, 宋成盈, 物理化学学报, 2009, 25, 767.)

5 Esteban, A. F.; Gabriel, A. P.; Federico, J. W. J. Power Sources 2011, 196, 172.

6 Ma, L.; Zhao, X.; Si, F.-Z.; Liu, C.; Liang, L. Electrochim. Acta 2010, 55, 9105.  

7 Katlin, I. B. E.; Geoffroy, R. P. M.; Marilia, M. S. P.; Giancarlo, R. S. B.; Luis, A. A. Energy Fuels 2010, 24,4012.  

8 Sun, H.-J.; Ding, L.-X.; Chen, Y. Chinese J. Inorg. Chem.2010, 26, 25 (in Chinese). (孙翰君, 丁良鑫, 陈煜, 无机化学学报, 2010, 26, 25.)

9 Chen, W.-M.; Sun, G..-Q.; Liang, Z.-X.; Mao, Q.; Li, H.-Q.; Wang, G.-X.; Xin, Q.; Chang, H.; Pak, C.; Seung, D. J. Power Sources 2006, 160, 933.  

10 Thomas, M. A.; Badri, S.; Jamie, S. L.; Nagappan, R.; David, E. B.; David, E. R.; Sanjeev, M. J. Phys. Chem. C2010, 114, 1028.  

11 Ma, J.-H.; Feng, Y.-Y.; Zhang, G.-R.; Wang, A.-J.; Xu, B.-Q. Chin. J. Catal. 2010, 31, 521 (in Chinese). (马俊红, 冯媛媛, 张贵荣, 王安杰, 徐柏庆, 催化学报,2010, 31, 521.)

12 Zhu, S.; Wang, S.-L.; Gao, Y.; Jiang, L.-H.; Sun, H.-G.; Sun, Q. Int. J. Hydrogen Energy 2010, 35, 11254.  

13 Li. L.; Wang, H.-X.; Xu, B.-Q.; Li, J.-L.; Lu, T.-H.; Mao, Z.-Q. Acta Chim. Sinica 2003, 61, 818 (in Chinese). (李莉, 王恒秀, 徐柏庆, 李晋鲁, 陆天虹, 毛宗强, 化学学报, 2003, 61, 818.)

14 Xiong, L.-P.; Hu, S.; Ren, X.-B.; Luo, Y.-M. J. Inorg Mater.2010, 25, 279 (in Chinese). (熊亮萍, 胡胜, 任兴碧, 罗阳明, 无机材料学报, 2010,25, 279.)  

15 Xu, B.-Q.; Li, L. Acta Phys.-Chim. Sin. 2003, 19, 342 (in Chinese). (徐柏庆, 李莉, 物理化学学报, 2003, 19, 342.)  

16 Camara, G. A.; Giz, M. J.; Paganin, V. A.; Ticianelli, E. A. J. Electroanal. Chem. 2002, 537, 21.  

17 Liu, Z.-L.; Lee, J.-Y.; Chen, W.-X.; Han, M.; Gan, L.-M. Langmuir 2004, 20, 181.  

18 Hu, S.; Xiong, L.-P.; Gu, M.; Xiao, C.-J.; Ren, X.-B.; Liu, J.; Luo, Y.-M. Atomic Energy Science and Technology 2009,43, 294 (in Chinese). (胡胜, 熊亮萍, 古梅, 肖成建, 任兴碧, 刘俊, 罗阳明, 原子能科学技术, 2009, 43, 294.)

19 Frances, J. S.; Sanjeev, M.; David, E. R. J. Phys. Chem. C2010, 114, 442.  

20 Yan, S.-Y.; Sun, G.-Q.; Qi, J.; Gao, Y.; Xin, Q. Chin. J. Catal. 2009, 30, 1109 (in Chinese). (闫世友, 孙公权, 齐静, 高妍, 辛勤, 催化学报, 2009,30, 1109.)

21 Wang, X.-G.; Su, Y.; Liu, C.- P.; Liao, J.-H.; Xing, W.; Lu, T.-H. Chem. J. Chin. Univ. 2009, 30, 1819 (in Chinese). (王晓刚, 苏怡, 刘长鹏, 廖建辉, 邢巍, 陆天虹, 高等学校化学学报, 2009, 30, 1819.)

22 Wei, Y.-C.; Liu, C.-W.; Chang, W.-J.; Wang, K.-W. J. Alloys Compd. 2011, 509, 535.  

23 Sun, Q.; Fu, Y.-C.; Yang, H.-X.; Auroux, A.; Shen, J. J. Mol. Catal. A: Chem. 2007, 275, 183.  

24 Adzic, R.; Zhang, J.-L.; Sasaki, K.; Vukmirovic, M.; Shao, M.; Wang, J. FY 2006 Annual Progress Report, DE-AC02-98CH10886.  

25 Cha, Q.-X. Introduction to Electrodes Kinetics, 3th ed., Science Press, Beijing, 2002, p. 275 (in Chinese). (查全性, 电极过程动力学导论, 第三版, 科学出版社, 北京, 2002, p. 275.)
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