CMK-5负载Pt-Ni合金催化剂及其甲醇电化学氧化性能

引用本文: 丁晓春, 陈秀, 周建华, 王涛, 孙盾, 何建平. CMK-5负载Pt-Ni合金催化剂及其甲醇电化学氧化性能[J]. 物理化学学报, 2011, 27(03): 711-716. doi: 10.3866/PKU.WHXB20110327 shu

Citation: DING Xiao-Chun, CHEN Xiu, ZHOU Jian-Hua, WANG Tao, SUN Dun, HE Jian-Ping. Pt-Ni Catalyst Supported on CMK-5 for the Electrochemical Oxidation of Methanol[J]. Acta Physico-Chimica Sinica, 2011, 27(03): 711-716. doi: 10.3866/PKU.WHXB20110327 shu

CMK-5负载Pt-Ni合金催化剂及其甲醇电化学氧化性能

基金项目:
国家自然科学基金(50871053)资助项目 (50871053)

摘要:

采用NaBH₄还原法将不同原子比的铂镍负载于CMK-5(由SBA-15模板所得的碳载体)表面. X射线衍射(XRD)和X射线光电子能谱(XPS)测试结果表明, 所得催化剂是以铂镍合金的形式存在, 相对于Pt/CMK-5而言, 这种合金化的催化剂中Pt表现出更多的金属态. 电化学测试结果显示, 在催化剂中主要以化合态存在的镍(包括NiO、Ni(OH)₂和NiOOH)可能更有利于甲醇的吸附和氧化产物从催化剂表面的脱附. 另外, 从循环伏安测试结果可知, Pt-Ni/CMK-5 (5:1)(原子比)具有较大的比表面活性, 其电化学活性面积高达63.9 m²·g^-1, 且与Pt/CMK-5相比抗CO中毒能力有明显改善.

关键词:

English

Pt-Ni Catalyst Supported on CMK-5 for the Electrochemical Oxidation of Methanol

1.
College of Material Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, P. R. China
Received Date: 27 October 2010
Available Online: 03 March 2011
Fund Project:
国家自然科学基金(50871053)资助项目

Abstract:

Pt-Ni alloy catalysts with different atomic ratios were deposited on CMK-5 (carbon replicated from SBA-15 silica) by NaBH₄ reduction. X-ray diffraction (XRD) suggests alloy formation between Pt and Ni. X-ray photoelectron spectroscopy (XPS) shows that Pt-Ni/CMK-5 (5:1) has more detectable oxidized Ni. More metallic Pt is present on Pt-Ni/CMK-5 (5:1) (atomic ratio) than on Pt/CMK-5. Oxidized Ni species, such as NiO, Ni(OH)₂， and NiOOH, favor the adsorption of methanol and the dissociation of methanol from the surface of Pt. Cyclic voltammetry shows that Pt-Ni/CMK-5 (5:1) has the highest specific activity among the as-made catalysts and its electrochemical active area is 63.9 m²·g^-1. It has more resistance to CO poisoning than Pt/CMK-5.

Key words:

1. [1]
  
  (1) Liu, X.; Chen, J.; Liu, G.; Zhang, L.; Zhang, H. M.; Yia, B. L. J. Power Sources 2010, 195, 4098.
  (1) Liu, X.; Chen, J.; Liu, G.; Zhang, L.; Zhang, H. M.; Yia, B. L. J. Power Sources 2010, 195, 4098.
2. [2]
  (2) Li, W. Z.; Zhou, W. J.; Li, H. Q.; Zhou, Z. H.; Zhou, B.; Sun, G. Q.; Xin, Q. Electrochim. Acta 2004, 49, 1045.(2) Li, W. Z.; Zhou, W. J.; Li, H. Q.; Zhou, Z. H.; Zhou, B.; Sun, G. Q.; Xin, Q. Electrochim. Acta 2004, 49, 1045.
3. [3]
  (3) Yang, C. W.; Wang, D. L.; Hu, X. G.; Dai, C. S.; Liang, Z. J. Alloy. Compd. 2008, 448, 109.(3) Yang, C. W.; Wang, D. L.; Hu, X. G.; Dai, C. S.; Liang, Z. J. Alloy. Compd. 2008, 448, 109.
4. [4]
  (4) Wang, X. M.; Li, N.; Pfefferle, L. D.; Haller, G. L. J. Phys. Chem., C 2010, 114, 16996.(4) Wang, X. M.; Li, N.; Pfefferle, L. D.; Haller, G. L. J. Phys. Chem., C 2010, 114, 16996.
5. [5]
  (5) Tang, H.; Chen, J. H.; Nie, L. H.; Liu, D. Y.; Deng, W.; Kuang, Y. F.; Yao, S. Z. J. Colloid Interface Sci. 2004, 269, 26.(5) Tang, H.; Chen, J. H.; Nie, L. H.; Liu, D. Y.; Deng, W.; Kuang, Y. F.; Yao, S. Z. J. Colloid Interface Sci. 2004, 269, 26.
6. [6]
  (6) Steigerwalt, E. S.; Deluga, G. A.; Lukehart, C. M. J. Nanosci. Nanotechnol. 2003, 3, 247.(6) Steigerwalt, E. S.; Deluga, G. A.; Lukehart, C. M. J. Nanosci. Nanotechnol. 2003, 3, 247.
7. [7]
  (7) Yen, C. H.; Shimizu, K.; Lin, Y. Y.; Bailey, F.; Cheng, I. F.; Wai, C. M. Energy Fuels 2007, 21, 2268.(7) Yen, C. H.; Shimizu, K.; Lin, Y. Y.; Bailey, F.; Cheng, I. F.; Wai, C. M. Energy Fuels 2007, 21, 2268.
8. [8]
  (8) Shimazaki, Y.; Hayasaka, S.; Koyama, T,; Nagao, D.; Kobayashi, Y.; Konno, M. J. Colloid Interface Sci. 2010, 350, 580.(8) Shimazaki, Y.; Hayasaka, S.; Koyama, T,; Nagao, D.; Kobayashi, Y.; Konno, M. J. Colloid Interface Sci. 2010, 350, 580.
9. [9]
  (9) Zhao, Y.; Yifeng, E.; Fan, L. Z.; Qiu, Y. F.; Yang, S. H. Electrochim. Acta 2007, 52, 5873.(9) Zhao, Y.; Yifeng, E.; Fan, L. Z.; Qiu, Y. F.; Yang, S. H. Electrochim. Acta 2007, 52, 5873.
10. [10]
  (10) Do, J. S.; Chen, Y. T.; Lee, M. H. J. Power Sources 2007, 172, 623.(10) Do, J. S.; Chen, Y. T.; Lee, M. H. J. Power Sources 2007, 172, 623.
11. [11]
  (11) Choi, J. H.; Park, K. W.; Kwon, B. K.; Sung, Y. E. J. Electrochem. Soc. 2003, 150, 773.(11) Choi, J. H.; Park, K. W.; Kwon, B. K.; Sung, Y. E. J. Electrochem. Soc. 2003, 150, 773.
12. [12]
  (12) Liu, F.; Lee, J. Y.; Zhou, W. J. J. Phys. Chem. B 2004, 108, 17959.(12) Liu, F.; Lee, J. Y.; Zhou, W. J. J. Phys. Chem. B 2004, 108, 17959.
13. [13]
  (13) Jeon, T. Y.; Yoo, S. J.; Cho, Y. H.; Lee, K. S.; Kang, S. H.; Sung, Y. E. J. Phys. Chem. C 2009, 113, 19732.(13) Jeon, T. Y.; Yoo, S. J.; Cho, Y. H.; Lee, K. S.; Kang, S. H.; Sung, Y. E. J. Phys. Chem. C 2009, 113, 19732.
14. [14]
  (14) Jiang, S. J.; Ma, Y. W.; Tao, H. S.; Jian, G. Q.; Wang, X. Z.; Fan, Y. N.; Zhu, J. M.; Hu, Z. J. Nanosci. Nanotechnol. 2010, 10, 3895.(14) Jiang, S. J.; Ma, Y. W.; Tao, H. S.; Jian, G. Q.; Wang, X. Z.; Fan, Y. N.; Zhu, J. M.; Hu, Z. J. Nanosci. Nanotechnol. 2010, 10, 3895.
15. [15]
  (15) Yano, H.; Kataoka, M.; Yamashita, H.; Uchida, H.; Watanabe, M. Langmuir 2007, 23, 6438.(15) Yano, H.; Kataoka, M.; Yamashita, H.; Uchida, H.; Watanabe, M. Langmuir 2007, 23, 6438.
16. [16]
  (16) He, C. Z.; Kunz, H. R.; Fenton, J. M. J. Electrochem. Soc. 2003, 150, A1071.(16) He, C. Z.; Kunz, H. R.; Fenton, J. M. J. Electrochem. Soc. 2003, 150, A1071.
17. [17]
  (17) Mathiyarasu, J.; Remona, A. M.; Mani, A.; Phani, K. L. N.; Yegnaraman, V. J. Solid State Electrochem. 2004, 8, 968.(17) Mathiyarasu, J.; Remona, A. M.; Mani, A.; Phani, K. L. N.; Yegnaraman, V. J. Solid State Electrochem. 2004, 8, 968.
18. [18]
  (18) Liu, Z. L.; Ling, X. Y.; Su, X. D.; Lee, J. Y. J. Phys. Chem. B 2004, 108, 8234.(18) Liu, Z. L.; Ling, X. Y.; Su, X. D.; Lee, J. Y. J. Phys. Chem. B 2004, 108, 8234.
19. [19]
  (19) Wang, Z. B.; Yin, G. P.; Shi, P. F. J. Electrochem. Soc. 2005, 153, A2406.(19) Wang, Z. B.; Yin, G. P.; Shi, P. F. J. Electrochem. Soc. 2005, 153, A2406.
20. [20]
  (20) Park, K. W.; Choi, J. H.; Ahn, K. S.; Sung, Y. E. J. Phys. Chem. B 2004, 108, 5989.(20) Park, K. W.; Choi, J. H.; Ahn, K. S.; Sung, Y. E. J. Phys. Chem. B 2004, 108, 5989.
21. [21]
  (21) Sun, D.; He, J. P.; Zhou, J. H.; Wang, T.; Di, Z. Y.; Ding, X. C. Acta Phys.-Chim. Sin. 2010, 26, 1219.(21) Sun, D.; He, J. P.; Zhou, J. H.; Wang, T.; Di, Z. Y.; Ding, X. C. Acta Phys.-Chim. Sin. 2010, 26, 1219.
22. [22]
  [孙盾, 何建平, 周建华, 王涛, 狄志勇, 丁晓春.. 物理化学学报, 2010, 26, 1219.][孙盾, 何建平, 周建华, 王涛, 狄志勇, 丁晓春.. 物理化学学报, 2010, 26, 1219.]
23. [23]
  (22) Lu, A. H.; Li, W. C.; Schmidt, W. G.; Schuth, F. Microporous Mesoporous Mat. 2005, 80, 117.(22) Lu, A. H.; Li, W. C.; Schmidt, W. G.; Schuth, F. Microporous Mesoporous Mat. 2005, 80, 117.
24. [24]
  (23) Antolini, E.; Salgado, J. R. C.; nzalez, E. R. J. Electroanal. Chem. 2005, 580, 145.(23) Antolini, E.; Salgado, J. R. C.; nzalez, E. R. J. Electroanal. Chem. 2005, 580, 145.
25. [25]
  (24) Zhou, J. H.; He, J. P.; Dang, W. J.; Zhao, G. W.; Zhang, C. X.; Mei, T. Q. Electrochem. Solid-State Lett. 2007, 10, B191.(24) Zhou, J. H.; He, J. P.; Dang, W. J.; Zhao, G. W.; Zhang, C. X.; Mei, T. Q. Electrochem. Solid-State Lett. 2007, 10, B191.
26. [26]
  (25) Pozio, A.; Francesco, D. M.; Cemmi, A. J. Power Sources 2002, 105, 13.(25) Pozio, A.; Francesco, D. M.; Cemmi, A. J. Power Sources 2002, 105, 13.
27. [27]
  (26) Yang, R. Z.; Iiu X. P.; Zhang, H. R. Carbon 2005, 43, 11.(26) Yang, R. Z.; Iiu X. P.; Zhang, H. R. Carbon 2005, 43, 11.
28. [28]
  (27) Zhou, J. H.; He, J. P.; Dang, W. J.; Zhao, G. W.; Zhang, C. X. Electrochem. Solid-State Lett. 2007, 10, B191.(27) Zhou, J. H.; He, J. P.; Dang, W. J.; Zhao, G. W.; Zhang, C. X. Electrochem. Solid-State Lett. 2007, 10, B191.
29. [29]
  (28) Park, K. W.; Choi, J. H.; Kwon, B. K.; Lee, S. A.; Sung, Y. E. J. Phys. Chem. B 2002, 106, 1869.(28) Park, K. W.; Choi, J. H.; Kwon, B. K.; Lee, S. A.; Sung, Y. E. J. Phys. Chem. B 2002, 106, 1869.
30. [30]
  (29) jkovic, S. L.; Vidakovic, T. R.; Durovic, D. R. Electrochim. Acta 2003, 48, 3607.(29) jkovic, S. L.; Vidakovic, T. R.; Durovic, D. R. Electrochim. Acta 2003, 48, 3607.
31. [31]
  (30) Radmilovic, V.; Gasteiger, H. A.; Ross, P. N. J. Catal. 1995, 154, 98.(30) Radmilovic, V.; Gasteiger, H. A.; Ross, P. N. J. Catal. 1995, 154, 98.
32. [32]
  (31) Geng, D. S.; Lu, G. X. J. Phys. Chem. C 2007, 111, 11897.(31) Geng, D. S.; Lu, G. X. J. Phys. Chem. C 2007, 111, 11897.
33. [33]
  (32) Liu, F.; Lee, J. Y.; Zhou, W. J. Small 2006, 2, 121.(32) Liu, F.; Lee, J. Y.; Zhou, W. J. Small 2006, 2, 121.
34. [34]
  (33) Watanabe, M.; Uchida, M.; Motoo, S. J. Electroanal. Chem. 1987, 229, 395.(33) Watanabe, M.; Uchida, M.; Motoo, S. J. Electroanal. Chem. 1987, 229, 395.
35. [35]
  (34) Park, K. W.; Choi, J. H.; Sung, Y. E. J. Phys. Chem. B 2003, 107, 5851.(34) Park, K. W.; Choi, J. H.; Sung, Y. E. J. Phys. Chem. B 2003, 107, 5851.
36. [36]
  (35) Lin, Y.; Cui, X.; Yen, C.; Wai, C. M. J. Phys. Chem. B 2005, 109, 14410.
  (35) Lin, Y.; Cui, X.; Yen, C.; Wai, C. M. J. Phys. Chem. B 2005, 109, 14410.

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

CMK-5负载Pt-Ni合金催化剂及其甲醇电化学氧化性能

English

Pt-Ni Catalyst Supported on CMK-5 for the Electrochemical Oxidation of Methanol

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

CMK-5负载Pt-Ni合金催化剂及其甲醇电化学氧化性能

English

Pt-Ni Catalyst Supported on CMK-5 for the Electrochemical Oxidation of Methanol

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

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