4.6 Article

Robust copper nanocrystal/nitrogen-doped carbon monoliths as carbon monoxide-resistant electrodes for methanol oxidation reaction

Journal

JOURNAL OF ENERGY CHEMISTRY
Volume 58, Issue -, Pages 247-255

Publisher

ELSEVIER
DOI: 10.1016/j.jechem.2020.10.020

Keywords

Copper nanocrystal; Methanol oxidation reaction; Non-noble metal-based electrocatalysts; Poison-resistant electrocatalysts; Nitrogen-doped carbon

Funding

  1. National Natural Science Foundation of China [21722406, 21975240, 21676258]
  2. Fundamental Research Funds for the Central Universities [WK2060190102]
  3. Central Leading Local Science and Technology Development Special Fund Project [YDZX20191400002636]
  4. Scientific and Technologial Innovation Programs of Higher Education Institutions in Shanxi [STIP 2020L0695]

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This research presents a simple strategy to synthesize copper nanocrystal/nitrogen-doped carbon monoliths as active and stable electrodes for methanol oxidation reaction. These Cu/N-C monoliths exhibit high electrical conductivity and mechanical robustness, allowing them to be used directly as electrodes for MOR without the need for substrates or additives.
Noble metal-based electrocatalysts present high activities for methanol oxidation reaction (MOR), but are limited by their high cost, low stability and poor resistance to carbon monoxide (CO) poisoning. The development of active and stable non-noble metal electrocatalysts for MOR is desired, but remains a challenge. Herein, we report a simple strategy to make copper nanocrystal/nitrogen-doped carbon (Cu/N-C) monoliths, which can serve as active and robust electrodes for MOR. Copper nanocrystals were electrochemically deposited onto a conductive polyaniline hydrogel and calcined to form Cu/N-C monolith, where the active copper nanocrystals are protected by nitrogen-doped carbon. Owing to their extremely high electrical conductivity (1.25 x 10(5) S cm(-1)) and mechanical robustness, these Cu/N-C monoliths can be directly used as electrodes for MOR, without using substrates or additives. The optimal Cu/N-C (FT)@500 monolith shows a high MOR activity of 189 mA cm(-2) at 0.6 V vs. SCE in alkaline methanol solution, superior to most of reported Cu-based MOR catalysts. Cu/N-C (FT)@500 also presents a better stability than Pt/C catalyst in the long-term MOR test at high current densities. Upon carbon monoxide (CO) poisoning, Cu/N-C (FT)@500 retains 96% of its MOR activity, far exceeding the performance of Pt/C catalyst (61% retention). Owing to its facile synthesis, outstanding activity, high stability and mechanical robustness, Cu/N-C (FT)@500 monolith is promising as a low-cost, efficient and CO-resistant electrocatalyst for MOR. (C) 2020 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.

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