管径对碳纳米管负载铂催化剂氧还原的影响

引用本文: 于景华, 李文文, 朱红. 管径对碳纳米管负载铂催化剂氧还原的影响[J]. 物理化学学报, 2017, 33(9): 1838-1845. doi: 10.3866/PKU.WHXB201705052 shu

Citation: YU Jing-Hua, LI Wen-Wen, ZHU Hong. Effect of the Diameter of Carbon Nanotubes Supporting Platinum Nanoparticles on the Electrocatalytic Oxygen Reduction[J]. Acta Physico-Chimica Sinica, 2017, 33(9): 1838-1845. doi: 10.3866/PKU.WHXB201705052 shu

管径对碳纳米管负载铂催化剂氧还原的影响

北京化工大学理学院, 化工资源有效利用国家重点实验室, 北京 100029
基金项目:
北京市科技计划（Z171100000917019），国家重点基础研究发展计划（2016YFB0101203），国家自然科学基金（21376022，21476020），国际科技合作项目（2013DFA51860）和中央高校基本科研业务费（JC1504）资助

摘要: 采用微波辅助乙二醇法制备了一系列酸处理后的不同管径（8-15，20-30，30-50，>50 nm）的碳纳米管（CNT）负载铂（Pt）催化剂（Pt/CNT）。通过X射线光电子能谱（XPS）、X射线衍射（XRD）、热重分析仪（TGA）、透射电子显微镜（TEM）对所制得催化剂进行结构表征；采用循环伏安法（CV）和线性扫描伏安法（LSV）对其催化性能进行测试。结果表明，不同管径的碳纳米管对Pt的粒径、载量和分散性有一定程度影响；然而，不同CNT管径的催化剂表现出明显不同的催化氧还原反应（ORR）活性。采用管径为8-15 nm的CNT作为载体制备的催化剂（Pt/CNT₈）的Pt载量最高，表现出有很好的催化活性和稳定性。Pt/CNT₈在0.9 V时Pt的质量活性为0.188 A·mg^-1，是商业催化剂（JM Pt/C）的2倍。经扫描5000圈稳定性测试之后，Pt/CNT₈的半波电位负移（~7 mV）远远小于商业JM Pt/C半波电位的负移（~32 mV），表现出优越的催化ORR稳定性。

关键词:

English

Effect of the Diameter of Carbon Nanotubes Supporting Platinum Nanoparticles on the Electrocatalytic Oxygen Reduction

State Key Laboratory of Chemical Resource Engineering, School of Science, Beijing University of Chemical Technology, Beijing 100029, P. R. China
Received Date: 23 March 2017
Revised Date: 24 April 2017
Available Online: 05 May 2017
Fund Project:
The project was supported by the Beijing Municipal Science and Technology Program, China (Z171100000917019), the National Key Research and Development Program of China (2016YFB0101203), the National Natural Science Foundation of China (21376022, 21476020), International S&T Cooperation Program of China (2013DFA51860), and Fundamental Research Funds for the Central Universities, China (JC1504).

Abstract: A series of nanocatalysts consisting of acid treated carbon nanotubes (CNTs) with different diameters (8-15, 20-30, 30-50, >50 nm) supporting platinum (Pt) nanoparticles (Pt/CNTs) were synthesized via a microwave-assisted ethylene glycol method. The as-synthesized catalysts were characterized by X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), thermogravimetric analysis (TGA), and transmission electron microscopy (TEM). Their catalytic performances in the oxygen reduction reaction (ORR) were evaluated by cyclic voltammetry (CV) and linear sweep voltammetry (LSV). The experimental results showed that the diameter of the CNTs influences the particle size, loading, and dispersion of Pt NPs. Furthermore, the Pt/CNTs having different CNT diameters displayed different catalytic activities in the ORR. The catalyst Pt/CNT₈, which was prepared by using CNTs with diameters ranging between 8-15 nm as the support, exhibited the highest Pt loading, catalytic activity, and stability in the ORR. The mass activity of Pt/CNT₈ was determined to be 0.188 A·mg^-1 at 0.9 V, which is folds higher than that of the commercially available JM Pt/C catalyst. After testing the stability for 5000 potential cycles, the negative shift (~7 mV) of the half-wave potential for Pt/CNT₈ was found to be significantly lesser than that for the JM Pt/C catalyst (~32 mV), indicating superior catalytic stability.

Key words:

1. [1]
  (1) Frederick, T. W.; Balasubramanian, L.; Mark, F. M. J. Phys. Chem. Lett. 2010, 1, 2204. doi: 10.1021/jz100553m
2. [2]
  (2) Debe, M. K. Nature 2012, 486, 43. doi: 10.1038/nature11115
3. [3]
  (3) Yi, B. L. Fuel Cells—Principle technologies and applications.Chemical Industry Press: Beijing, 2003. [衣宝廉. 燃料电池: 原理·技术·应用. 北京: 化学工业出版社, 2003.]
4. [4]
  (4) Li, W. Z.; Liang, C. H.; Zhou, W. J. J. Phys. Chem. B 2003, 107, 6292. doi: 10.1021/jp022505c
5. [5]
  (5) Stoyanova, A.; Naldenov, V.; Petrov, K.; Nikolov, I.; Vitanov, T.; Budevski, E. J. Appl. Electrochem. 1999, 29, 1197. doi: 10.1023/A:1003482613323
6. [6]
  (6) Aricò, A.S.; Stassi, A.; Modica, E.; Ornelas, R.; Gatto, I.; Passalacqua, E.; Antonucci, V. J. Power Sources 2008, 178, 525. doi: 10.1016/j.jpowsour.2007.10.005
7. [7]
  (7) Wang, J. J.; Yin, G. P.; Shao, Y. Y.; Zhang, S.; Wang, Z. B.; Gao, Y. Z. J. Power Sources 2007, 171, 331. doi: 10.1016/j.jpowsour.2007.06.084
8. [8]
  (8) Zhang, C. L.; Wang, S. Y.; Peng, Z. M. J. Mater. Chem. A 2014, 2, 19778. doi: 10.1039/C4TA04728A
9. [9]
  (9) Stamenkovic, V. R.; Mun, B. S.; Arenz, M.; Mayrhofer, K. J.; Lucas, C. A.; Wang, G.; Ross, P. N.; Markovic, N. M. Nat. Mater. 2007, 6, 241. doi: 10.1038/nmat1840
10. [10]
  (10) Huang, H. X.; Chen, S. X.; Yuan, C. J. Power Sources 2008, 175, 166. doi: 10.1016/j.jpowsour.2007. 08.107
11. [11]
  (11) Sun, Z. P.; Zhang, X. G.; Liang, Y. Y.; Tong, H.; Xue, R. L.; Yang, S.D.; Li, H. L. Electrochim. Acta 2009, 633, 1. doi: 10.1016/j.jelechem.2009.04.013
12. [12]
  (12) Ahn, S. H.; Kwon, O. J.; Kim, S. K.; Choi, I.; Kim, J. J. Int. J. Hydrogen Energy 2010, 35, 13309. doi: 10.1016/j.ijhydene.2010.09.035
13. [13]
  (13) Wan, K.; Long, G.; Liu, M.; Du, L.; Liang, Z.; Tsiakaras, P. Appl. Catal. B: Environm. 2015, 165, 566. doi: 10.1016/j.apcatb.2014.10.054
14. [14]
  (14) Viva, F. A.; Bruno, M. M.; Franceschini, E. A.; Thomas, Y. R. J.; Ramos S. G.; Solorza-Feria, O.; Corti, H. R. Int. J. Hydrogen Energy 2014, 39, 8821. doi: 10.1016/j.ijhydene.2013.12.027
15. [15]
  (15) Madhu, S. S.; Mohammad, N. B.; Zhang, Y.; Li, R. Y.; Sun X. L.; Cai, M.; Frederick, T. W. J. Power Sources 2009, 192, 330. doi: 10.1016/j.jpowsour.200 9.02.087
16. [16]
  (16) Tong, H.; Li, H. L.; Zhang, X. G. Carbon 2007, 45, 2424. doi: 10.1016/j.carbon.2007.06.028
17. [17]
  (17) Walid, M. D.; Toyoko, I. J. Experim. Nanosci. 2015, 10, 392. doi: 10.1080/17458080.2013.838703
18. [18]
  (18) Zhang, Y.; Hu, J. S.; Wei, Z. D.; Wan L. J. ACS Catal. 2015, 5, 2903. doi: 10.1021/acscatal.5b00117
19. [19]
  (19) Guo, L.; Chen, S. G.; Wei, Z. D. J. Power Sources 2014, 255, 387. doi: org/10.1016/j.jpowsour.2014.01.040
20. [20]
  (20) Gong, K.; Du, F.; Xia, Z.; Durstock, M.; Dai, L. Science 2009, 323, 760. doi: 10.1126/science.1168049
21. [21]
  (21) Guo, L.; Chen, S. G.; Li, L.; Wei, Z. D. J. Power Sources 2014, 247, 360. doi: org/10.1016/j.jpowsour.2013.08.102
22. [22]
  (22) Wang, X.; Li, W. Z.; Chen, Z. W.; Wa, J. M.; Yan, Y. S. J. Power Sources 2006, 158, 154. doi: 10.1016/j.jpowsour.2005.09.039
23. [23]
  (23) Wu, G.; Xu, B. Q.; J. Power Sources 2007, 174, 148. doi: 10.1016/j.jpowsour.2007.08.024
24. [24]
  (24) Zhao, Y. C.; Lan, H. X.; Deng, B. B.; Tian, J. N.; Yang, X. L.; Wang, F. Y. Acta Phys. -Chim. Sin. 2010, 26, 2255. [赵彦春, 兰黄鲜, 邓彬彬, 田建袅, 杨秀林, 王凤阳. 物理化学学报, 2010, 26, 2255.]doi: 10.3866/PKU.WHXB20100829
25. [25]
  (25) Chen, Y.; Tang, Y. W.; Kong L. Y.; LIU, C. P.; XING, W.; LU, T. H. Acta Phys. -Chim. Sin. 2006, 22, 119. [陈煜, 唐亚文, 孔令涌, 刘长鹏, 邢巍, 陆天虹. 物理化学学报, 2006, 22, 119.]doi: 10.3866/PKU.WHXB20060124
26. [26]
  (26) Hsieh, C. T.; Gu, J. L.; Tzou, D. Y.; Chu, Y. C.; Chen, Y. C. Int. J. Hydrogen Energy 2013, 38, 10345. doi: 10.1016/j.ijhydene.2013.05.146
27. [27]
  (27) He, D. P.; Zeng, C.; Xu, C.; Cheng N. C.; Li, H. G.; Mu, S. C.; Pan, M. Langmuir 2011, 27, 5582. doi: 10.1021/la2003589
28. [28]
  (28) Li, X. G.; Hsing, I. Electrochim. Acta 2006, 51, 5250. doi: 10.1016/j.electacta.2006.01.046
29. [29]
  (29) Tao, L.; Dou, S.; Ma, Z. L; Wang, S. Y. Electrochimica. Acta 2015, 157, 46. doi: 10.1016/j.electacta.2015.01.054
30. [30]
  (30) Fang, B. Z.; Kim, M. S.; Kim, J. H.; Song, M. Y.; Wang Y. J.; Wang, H. J.; Wilkinson, D. P.; Yu J. S. J. Mater. Chem. 2011, 21, 8066 doi:10.1039/C1JM10847F
31. [31]
  (31) Kong, B. S.; Jung, D. H.; Oh, S. K.; Han, C. S.; Jung, H. T. J . Phys. Chem. C 2007, 111, 8377. doi: 10.1021/jp071297r
32. [32]
  (32) Nie, Y.; Li, L.; Wei, Z. D. Chem. Soc. Rev. 2015, 44, 2168. doi:10.1039/C4CS00484A
33. [33]
  (33) Yu, R. Q; Chen, L. W.; Liu Q. Q.; Lin J. Y.; Tan, K. Lee.; Siu, C. N.; Chan, H. S. O.; Xu G. Q.; Hor, T. S. A. Chem. Mater 1998, 10, 718. doi: 10.1021/cm970364z
34. [34]
  (34) Star, A.; Liu, Y.; Grant, K.; Ridvan, L.; Stoddart, J. F.; Steuerman, D.W.; Diehl, M. R.; Boukai, A.; Heath, J. R. Macromolecules 2003, 36, 553. doi: 10.1021/ma021417n
35. [35]
  (35) Soin, N.; Roy, S. S.; Karlsson, L.; McLaughlin, J. A. Diamond RelatMater 2010, 19, 595. doi: 10.1016/j.diamond.2009.10.029
36. [36]
  (36) He, D. P.; Mu, S. C; Pan, M. Carbon 2011, 49, 82. doi: 10.1016/j.carbon.2010.08.045
37. [37]
  (37) Mu, Y.; Liang, H.; Hu, J.; Jiang, L.; Wan, L. J. J. Phys. Chem. B 2005, 109, 22212. doi: 10.1021/jp0555448
38. [38]
  (38) Liu, Z. L.; Lin, X. H.; Lee, J. Y.; Zhang, W.; Han, M.; Gan, L. M. Langmuir 2002, 18, 4054. doi: 10.1021/la0116903
39. [39]
  (39) Kongkanand, A.; Kuwabata, S.; Girishkumar, G.; Kamat, P. Langmuir 2006, 22, 2392. doi: 10.1021/la052753a
40. [40]
  (40) Liu, J. B.; Yuan, Y.; Bashir, S. Energies 2013, 12, 6476. doi:10.3390/en6126476
41. [41]
  (41) Zhao, Y. C.; Yang, X. L.; Tian, J. N. Electrochim. Acta 2009, 54, 7114. doi: 10.1016/j.electacta.2009.07.021
42. [42]
  (42) Yu, H.; Zeng, K.; Fu, X. B.; Zhang, Yan.; Peng, F.; Wang, H. J.; Yang, J. J. Phys. Chem. C 2008, 112, 11875. doi: 10.1021/jp804003g
43. [43]
  (43) Hussain, S.; Pal, A. K. Mater. Lett. 2008, 62, 1874. doi:10.1016/j.matlet.2007.10.021
44. [44]
  (44) Luo, M. C.; Wei, L. L.; Wang, F. W.; Han, K. F.; Zhu, H. J. Power Sources 2014, 270, 34. doi: 10.1016/j.jpowsour.2014.07.102
45. [45]
  (45) Zhu, H.; Luo, M. C.; Zhang, S.; Wei, L. L.; Wang, F. W.; Wang, Z. G.; Wei, Y. S.; Han, K. F. Int. J. Hydrogen Energy 2013, 38, 3323. doi: 10.1016/j.ijhydene.2012.12.12

扫一扫看文章

计量

PDF下载量: 2
文章访问数: 843
HTML全文浏览量: 110

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

管径对碳纳米管负载铂催化剂氧还原的影响

English

Effect of the Diameter of Carbon Nanotubes Supporting Platinum Nanoparticles on the Electrocatalytic Oxygen Reduction

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

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

管径对碳纳米管负载铂催化剂氧还原的影响

English

Effect of the Diameter of Carbon Nanotubes Supporting Platinum Nanoparticles on the Electrocatalytic Oxygen Reduction

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

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs