4.7 Article

Synthesis of nitrogen-rich porous carbon nanotubes coated Co nanomaterials as efficient ORR electrocatalysts via MOFs as precursor

期刊

JOURNAL OF ALLOYS AND COMPOUNDS
卷 911, 期 -, 页码 -

出版社

ELSEVIER SCIENCE SA
DOI: 10.1016/j.jallcom.2022.165060

关键词

Metal-organic framework; carbon nanotubes; Electrocatalysis; ORR

资金

  1. National Natural Science Foundation of China [22169018, 21861035]
  2. Tianchi Hundred People Plan Project Foundation of Xinjiang Uygur Autonomous Region [TCBR202103]
  3. Key Laboratory of Oil and Gas Fine Chemicals, Ministry of Education & Xinjiang Uygur Autonomous Region

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Transition metal-based nitrogen-doped carbon nanomaterials synthesized from metal-organic frameworks exhibited excellent catalytic activity for oxygen reduction reaction (ORR). The materials showed high half-wave potential and limiting current density in both acidic and alkaline electrolytes, surpassing the performance of Pt/C. The superior ORR activity is attributed to the synergistic effects of the porous carbon nanotube structure, nitrogen-doped carbon, and Co-Nx active sites. Additionally, the optimized catalyst demonstrated better stability and methanol resistance than Pt/C.
Transition metal-based nitrogen-doped carbon materials have been proved to be a promising low-cost electrocatalyst for oxygen reduction reaction (ORR), which is a critical step in systems such as fuel batteries and zinc-air batteries. In this paper, transition metal (cobalt) N-doped carbon nanomaterials derived from metal-organic framework (MOFs) were synthesized by calcination of ZIF-67 precursors at high temperature (Co@NCNTs). Nitrogen atoms were introduced into the carbon matrix by capturing volatile CNx from di-cyandiamide, and porous carbon nanotube structures with N-doped and uniformly dispersed active sites were obtained. The effects of different carbonization temperatures and molar ratio of Co/2-MI on the catalytic activity of materials for ORR reaction were studied. It was found that the Co@NCNTs prepared at 700 degrees C with the ratio of cobalt metal to dimethylimidazole of 1: 8 shows excellent ORR activity in both acidic and alkaline electrolytes. In alkaline conditions, the half-wave potential E-1/2 = 0.81 V, initial potential E-onset = 0.89 V, and limiting current density even reaching 7.4 mA cm(-2). And in acidic electrolytes, E-1/2 = 0.66 V, while the limiting current density is 6.4 mA cm(-2), which is still better than that of Pt/C. Its excellent ORR performance is due to the synergistic effect of the porous carbon nanotube structure, N-doped carbon and Co-Nx active sites. Meanwhile, the optimum catalyst also shows better stability and methanol resistance than Pt/C in both acidic and alkaline electrolytes. (c) 2022 Published by Elsevier B.V.

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