Citation: Li Danqin, Zhang Zhiqi, Zang Pengyuan, Ma Yanwen, Wu Qiang, Yang Lijun, Chen Qiang, Wang Xizhang, Hu Zheng. Alloyed Pt–Ru Nanoparticles Immobilized on Mesostructured Nitrogen-Doped Carbon Nanocages for Efficient Methanol Electrooxidation[J]. Acta Chimica Sinica, ;2016, 74(7): 587-592. doi: 10.6023/A16040196 shu

Alloyed Pt–Ru Nanoparticles Immobilized on Mesostructured Nitrogen-Doped Carbon Nanocages for Efficient Methanol Electrooxidation

Li Danqin ^a,b ,
Zhang Zhiqi ^a,b ,
Zang Pengyuan ^a,b ,
Ma Yanwen ^a,b ,
Wu Qiang ^a,b ,
Yang Lijun ^a,b ,
Chen Qiang ^a,b ,
Wang Xizhang ^a,b,*,, ,
Hu Zheng ^a,b

a.
Jiangsu Provincial Lab for Nanotechnology, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
b.
High-Tech Research Institute of Nanjing University (Suzhou), Suzhou, Jiangsu 215123

Corresponding author: Wang Xizhang, wangxzh@nju.edu.cn
Received Date: 20 April 2016

Fund Project: Changzhou Technology Support Program CE20130032National Natural Science Foundation of China 51232003National Natural Science Foundation of China 21473089National Natural Science Foundation of China 21573107Suzhou Science and Technology Project ZXG2013025National Natural Science Foundation of China 51571110National Natural Science Foundation of China 21373108the National Basic Research Program of China (973 Program, 2013CB932902

Figures(4)

Direct methanol fuel cells (DMFC) have attracted extensive attention as ideal candidates for automotive and portable applications owing to the fascinating advantages such as high conversion efficiency, environmental friendliness, safety, wide sources of methanol, and simple cell structure. Electrocatalysts are one of crucial factors limiting the performance of DMFC. Nowadays, precious Pt-based catalyst, in spite of costliness and scarcity, is the most popular catalyst for methanol oxidation reaction (MOR) at anode due to the much better performances than those of the non-Pt catalysts. But there exists some shortcomings such as poor CO-tolerance and durability. Pt alloying with other metals, e.g. Ru, is an effective strategy to improve the catalytic performance. In addition, the support with a large specific surface area (SSA), high conductivity and suitable porous structure, such as sp² carbon, could lead to high dispersion, high utilization and stability of Pt-based nanoparticles, also favorable for MOR. Recently, by in situ MgO template method, we reported the unique 3D hierarchical carbon-based nanocages featured with ultrahigh SSA, micro-meso-macro-pore coexistence, good conductivity and easy doping, which exhibited excellent electrochemical performances. Herein, taking the advantages of nitrogen-dopant anchoring function and unique mesostructures of hierarchical N-doped carbon nanocages (hNCNC), we report the Pt-Ru electrocatalysts immobilized on hNCNC (Pt-Ru/hNCNC) prepared via modified microwave-assisted ethylene glycol (EG) reduction method. The so-constructed Pt-Ru/hNCNC catalysts with ca. 30 wt% loading and tunable atomic ratio of Pt to Ru have a highly homogeneous dispersion of metal nanoparticles with the average size of ca. 3 nm. The alloying Pt-Ru/hNCNC catalysts demonstrate good CO-tolerance, high MOR activity and durability, superior to those of the counterparts of Pt/hNCNC and commercial PtRu/C. The good electrochemical performance can be ascribed to the synergistic effects of the bifunctional effect due to introduction of Ru, small size and high dispersion of metal nanoparticles induced by the large SSA and nitrogen participation of hNCNC, and multi-scaled hierarchical pore structures beneficial to the mass transportation. These results proposed a potential strategy to develop the high-performance Pt-based MOR catalysts based on the novel mesostructured hNCNC.
- direct methanol fuel cell,
- electrocatalyst,
- mesostructured,
- nitrogen-doped carbon nanocages,
- Pt-Ru alloy nano-particles,
- methanol oxidation
1. [1]
  Chen, A.; Holt-Hindle, P. Chem. Rev. 2010, 110, 3767. doi: 10.1021/cr9003902
2. [2]
  Kakati, N.; Maiti, J.; Lee, S. H.; Jee, S. H.; Viswanathan, B.; Yoon, Y. S. Chem. Rev. 2014, 114, 12397. doi: 10.1021/cr400389f
3. [3]
  Gasteiger, H. A.; Markovic, N.; Ross, P. N.; Cairns, E. J. J. Phys. Chem. 1994, 98, 617. doi: 10.1021/j100053a042
4. [4]
  Liu, Z. L.; Guo, B.; Hong, L.; Lim, T. H. Electrochem. Commun. 2006, 8, 83. doi: 10.1016/j.elecom.2005.10.019
5. [5]
  Pereira, L. G. S.; dos Santos, F. R.; Pereira, M. E.; Paganin, V. A.; Ticianelli, E. A. Electrochim. Acta 2006, 51, 4061. doi: 10.1016/j.electacta.2005.11.025
6. [6]
  Sun, J.; Ma, H.; Jiang, H.; Dang, L.; Lu, Q.; Gao, F. J. Mater. Chem. 2015, 3, 15882. doi: 10.1039/C5TA01613D
7. [7]
  Mylswamy, S.; Wang, C. Y.; Liu, R. S.; Lee, J. F.; Tang, M. J.; Lee, J. J.; Weng, B. J. Chem. Phys. Lett. 2005, 412, 444. doi: 10.1016/j.cplett.2005.07.035
8. [8]
  Watanabe, M.; Motoo, S. J. Electroanal. Chem. Interfacial Electrochem. 1975, 60, 267. doi: 10.1016/S0022-0728(75)80261-0
9. [9]
  Yue, B.; Ma, Y. W.; Tao, H. S.; Yu, L. S.; Jian, G. Q.; Wang, X. Z.; Wang, X. S.; Lu, Y. N.; Hu, Z. J. Mater. Chem. 2008, 18, 1747. doi: 10.1039/b718283j
10. [10]
  Jiang, S.; Zhu, L.; Ma, Y.; Wang, X.; Liu, J.; Zhu, J.; Fan, Y.; Zou, Z.; Hu, Z. J. Power Sources 2010, 195, 7578. doi: 10.1016/j.jpowsour.2010.06.025
11. [11]
  Feng, H.; Ma, J.; Hu, Z. J. Mater. Chem. 2010, 20, 1702. doi: 10.1039/b915667d
12. [12]
  Joo, S. H.; Kwon, K.; You, D. J.; Pak, C.; Chang, H.; Kim, J. M. Electrochim. Acta 2009, 54, 5746. doi: 10.1016/j.electacta.2009.05.022
13. [13]
  Guerrero-Ruiz, A.; Badenes, P.; Rodriguez-Ramos, I. Appl. Catal. A: Gen. 1998, 173, 313. doi: 10.1016/S0926-860X(98)00187-2
14. [14]
  Kuang, Y.; Cui, Y.; Zhang, Y.; Yu, Y.; Zhang, X.; Chen, J. Chem. Eur. J. 2012, 18, 1522. doi: 10.1002/chem.v18.5
15. [15]
  Che, G.; Lakshmi, B. B.; Fisher, E. R.; Martin, C. R. Nature 1998, 393, 346. doi: 10.1038/30694
16. [16]
  Lin, M. L.; Huang, C. C.; Lo, M. Y.; Mou, C. Y. J. Phys. Chem. C 2008, 112, 867. doi: 10.1021/jp076748m
17. [17]
  Liu, Z.; Su, F.; Zhang, X.; Tay, S. W. ACS Appl. Mater. Interfaces 2011, 3, 3824. doi: 10.1021/am2010515
18. [18]
  Yu, J. S.; Kang, S.; Yoon, S. B.; Chai, G. J. Am. Chem. Soc. 2002, 124, 9382. doi: 10.1021/ja0203972
19. [19]
  Li, F.; Chan, K.-Y.; Yung, H.; Yang, C.; Ting, S. W. Phys. Chem. Chem. Phys. 2013, 15, 13570. doi: 10.1039/c3cp00153a
20. [20]
  Cong, H.-P.; Ren, X.-C.; Yu, S.-H. ChemCatChem 2012, 4, 1555. doi: 10.1002/cctc.v4.10
21. [21]
  Bin, D.; Ren, F.; Wang, H.; Zhang, K.; Yang, B.; Zhai, C.; Zhu, M.; Yang, P.; Du, Y. RSC Adv. 2014, 4, 39612. doi: 10.1039/C4RA07742C
22. [22]
  La-Torre-Riveros, L.; Guzman-Blas, R.; Méndez-Torres, A. E.; Prelas, M.; Tryk, D. A.; Cabrera, C. R. ACS Appl. Mater. Interfaces 2012, 4, 1134. doi: 10.1021/am2018628
23. [23]
  Jiang, S.; Ma, Y.; Jian, G.; Tao, H.; Wang, X.; Fan, Y.; Lu, Y.; Hu, Z.; Chen, Y. Adv. Mater. 2009, 21, 4953. doi: 10.1002/adma.v21:48
24. [24]
  Chen, S.; Bi, J.; Zhao, Y.; Yang, L.; Zhang, C.; Ma, Y.; Wu, Q.; Wang, X.; Hu, Z. Adv. Mater. 2012, 24, 5593. doi: 10.1002/adma.201202424
25. [25]
  Xie, K.; Qin, X.; Wang, X.; Wang, Y.; Tao, H.; Wu, Q.; Yang, L.; Hu, Z. Adv. Mater. 2012, 24, 347. doi: 10.1002/adma.201103872
26. [26]
  Jiang, Y.; Yang, L.; Sun, T.; Zhao, J.; Lyu, Z.; Zhuo, O.; Wang, X.; Wu, Q.; Ma, J.; Hu, Z. ACS Catal. 2015, 5, 6707. doi: 10.1021/acscatal.5b01835
27. [27]
  Lyu, Z.; Xu, D.; Yang, L.; Che, R.; Feng, R.; Zhao, J.; Li, Y.; Wu, Q.; Wang, X.; Hu, Z. Nano Energy 2015, 12, 657. doi: 10.1016/j.nanoen.2015.01.033
28. [28]
  Zhao, J.; Lai, H.; Lyu, Z.; Jiang, Y.; Xie, K.; Wang, X.; Wu, Q.; Yang, L.; Jin, Z.; Ma, Y.; Liu, J.; Hu, Z. Adv. Mater. 2015, 27, 3541. doi: 10.1002/adma.v27.23
29. [29]
  Lyu, Z.; Feng, R.; Zhao, J.; Fan, H.; Xu, D.; Wu, Q.; Yang, L.; Chen, Q.; Wang, X.; Hu, Z. Acta Chim. Sinica 2015, 73, 1013.
30. [30]
  Feng, R.; Wang, L.; Lyu, Z.; Wu, Q.; Yang, L.; Wang, X.; Hu, Z. Acta Chim. Sinica 2014, 72, 653. doi: 10.6023/A14030227
31. [31]
  Prabhuram, J.; Zhao, T. S.; Liang, Z. X.; Chen, R. Electrochim. Acta 2007, 52, 2649. doi: 10.1016/j.electacta.2006.09.027
32. [32]
  Roth, C.; Benker, N.; Theissmann, R.; Nichols, R. J.; Schiffrin, D. J. Langmuir 2008, 24, 2191. doi: 10.1021/la7015929
33. [33]
  Bock, C.; Paquet, C.; Couillard, M.; Botton, G. A.; MacDougall, B. R. J. Am. Chem. Soc. 2004, 126, 8028. doi: 10.1021/ja0495819
34. [34]
  Giorgi, L.; Pozio, A.; Bracchini, C.; Giorgi, R.; Turtù, S. J. Appl. Electrochem. 2001, 31, 325. doi: 10.1023/A:1017595920726
35. [35]
  Wang, Z.-C.; Ma, Z.-M.; Li, H.-L. Appl. Surf. Sci. 2008, 254, 6521. doi: 10.1016/j.apsusc.2008.04.017
36. [36]
  Liu, S.-H.; Yu, W.-Y.; Chen, C.-H.; Lo, A.-Y.; Hwang, B.-J.; Chien, S.-H.; Liu, S.-B. Chem. Mater. 2008, 20, 1622. doi: 10.1021/cm702777j
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