期刊文献+

A Co-N/C hollow-sphere electrocatalyst derived from a metanilic CoAl layered double hydroxide for the oxygen reduction reaction, and its active sites in various pH media 被引量:4

A Co-N/C hollow-sphere electrocatalyst derived from a metanilic CoAl layered double hydroxide for the oxygen reduction reaction, and its active sites in various pH media
原文传递
导出
摘要 Transition-metal-coordinating nitrogen-doped carbon catalysts (M-N/C, M = Co, Fe, Mn, Ni, etc.) are considered one of the most promising nonprecious-metal electrocatalysts for the oxygen reduction reaction (ORR). However, they suffer from low ORR catalytic activity, and their active sites have not been fully identified. Herein, we report the synthesis of a porous Co-N/C hollow-sphere electrocatalyst by carbonization of metanilic anions between the layers of a Co-A1 layered double hydroxide. The as-prepared Co-N/C catalyst exhibited excellent ORR catalytic activity with a high half-wave potential and a large diffusion-limited current in alkaline and neutral solutions. The performance of the catalyst was comparable to those of commercial Pt/C electrocatalysts. Through investigating the effects of mask ions (SCN- and F-) on the ORR activity of the Co-N/C catalyst, and comparing the ORR activity before and after the destruction of Co-Nx sites in different pH media, we concluded that the Co-Nx sites act directly as the ORR active sites in acidic and neutral solutions, but have a negligible effect on the ORR activity in alkaline conditions. Transition-metal-coordinating nitrogen-doped carbon catalysts (M-N/C, M = Co, Fe, Mn, Ni, etc.) are considered one of the most promising nonprecious-metal electrocatalysts for the oxygen reduction reaction (ORR). However, they suffer from low ORR catalytic activity, and their active sites have not been fully identified. Herein, we report the synthesis of a porous Co-N/C hollow-sphere electrocatalyst by carbonization of metanilic anions between the layers of a Co-A1 layered double hydroxide. The as-prepared Co-N/C catalyst exhibited excellent ORR catalytic activity with a high half-wave potential and a large diffusion-limited current in alkaline and neutral solutions. The performance of the catalyst was comparable to those of commercial Pt/C electrocatalysts. Through investigating the effects of mask ions (SCN- and F-) on the ORR activity of the Co-N/C catalyst, and comparing the ORR activity before and after the destruction of Co-Nx sites in different pH media, we concluded that the Co-Nx sites act directly as the ORR active sites in acidic and neutral solutions, but have a negligible effect on the ORR activity in alkaline conditions.
出处 《Nano Research》 SCIE EI CAS CSCD 2017年第7期2508-2518,共11页 纳米研究(英文版)
基金 This research was supported by the National Basic Research Program of China (No. 2014CB932103), National Natural Science Foundation of China (Nos. 51272020, 21236003, and U1407118), Beijing Engineering Center for Hierarchical catalysts and Fundamental Research Funds for the Central Universities (No. YS1406).
关键词 confined space hollow carbon sphere hierarchical pore structure electrocatalysts oxygen reduction reaction confined space,hollow carbon sphere,hierarchical pore structure,electrocatalysts,oxygen reduction reaction
  • 相关文献

参考文献2

二级参考文献93

  • 1Bashyam, R.; Zelenay, P. A class of non-precious metal composite catalysts for fuel cells. Nature 2006, 443, 63-56.
  • 2Wang, X.; Lee, J. S.; Zhu, Q.; Liu, J.; Wang, Y.; Dai, S. Ammonia-treated ordered mesoporous carbons as catalytic materials for oxygen reduction reaction. Chem. Mater. 2010, 22, 2178-2180.
  • 3Jaouen, F.; Proietti, E.; Lefevre, M.; Chenitz, R.; Dodelet, J.-P.; Wu, G.; Chung, H. T.; Johnston, C. M.; Zelenay, P. Recent advances in non-precious metal catalysis for oxygen- reduction reaction in polymer electrolyte fuel cells. Energy Environ. Sci. 2011, 4, 114-130.
  • 4Chen, Z.; Higgins, D.; Yu, A.; Zhang, L.; Zhang, J. A review on non-precious metal electrocatalysts for PEM fuel cells. Energy Environ. Sci. 2011, 4, 3167-3192.
  • 5Yang, S.; Feng, X.; Wang, X.; Miallen, K. Graphene-based carbon nitride nanosheets as efficient metal-flee electrocatalysts for oxygen reduction reactions. Angew. Chem. Int. Ed. 2011, 50, 5339-5343.
  • 6Bezerra, C. W. B.; Zhang, L.; Lee, K.; Liu, H.; Marques, A. L. B.; Marques, E. P.; Wang, H.; Zhang, J. A review of Fe N/C and Co-N/C catalysts for the oxygen reduction reaction. Electrochim. Acta. 2008, 53, 4937-4951.
  • 7Wang, S.; Iyyampertmaal, E.; Roy, A.; Xue, Y.; Yu, D.; Dai L. Vertically aligned BCN nanotubes as efficient metal-free electrocatalysts for the oxygen reduction reaction: A synergetic effect by Co-doping with boron and nitrogen. Angew. Chem Int. Ed. 2011, 50, 11756-11760.
  • 8Yang, L.; Jiang, S.; Zhao, Y.; Zhu, L.; Chen, S.; Wang, X.; Wu, Q.; Ma, J.; Ma, Y.; Hu, Z. Boron-doped carbon nanotubes as metal-free electrocatalysts for the oxygen reduction reaction. Angew. Chem. Int. Ed. 2011, 50, 7132-7135.
  • 9Li, Y.; Zhou, W.; Wang, H.; Xie, L.; Liang, Y.; Wei, F.; Idrobo, J.-C.; Pennycook, S. J.; Dai, H. An oxygen reduction electrocatalyst based on carbon nanotube-graphene complexes. Nat. Nanotechnol. 2012, 7, 394-400.
  • 10Qu, L.; Liu, Y,; Back, J.-B., Dai, L. Nitrogen-doped graphene as efficient metal-free electrocatalyst for oxygen reduction in fuel cells. ACSNano 2010, 4, 1321-1326.

共引文献27

同被引文献28

引证文献4

二级引证文献24

相关作者

内容加载中请稍等...

相关机构

内容加载中请稍等...

相关主题

内容加载中请稍等...

浏览历史

内容加载中请稍等...
;
使用帮助 返回顶部