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Title: A completely precious metal–free alkaline fuel cell with enhanced performance using a carbon-coated nickel anode

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
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  1. College of Chemistry and Molecular Sciences, Hubei Key Lab of Electrochemical Power Sources, Wuhan University, Wuhan 430072, China
  2. Department of Chemistry and Chemical Biology, Cornell University, Ithaca, NY 14853
  3. Department of Chemical &, Biological Engineering, University of Wisconsin-Madison, Madison, WI 53706
  4. College of Chemistry and Molecular Sciences, Hubei Key Lab of Electrochemical Power Sources, Wuhan University, Wuhan 430072, China, The Institute for Advanced Studies, Wuhan University, Wuhan 430072, China
  5. School of Applied and Engineering Physics, Cornell University, Ithaca, NY 14853, Kavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, NY 14853

Alkaline fuel cells enable the use of earth-abundant elements to replace Pt but are hindered by the sluggish kinetics of the hydrogen oxidation reaction (HOR) in alkaline media. Precious metal–free HOR electrocatalysts need to overcome two major challenges: their low intrinsic activity from too strong a hydrogen-binding energy and poor durability due to rapid passivation from metal oxide formation. Here, we designed a Ni-based electrocatalyst with a 2-nm nitrogen-doped carbon shell (Ni@CNx) that serves as a protection layer and significantly enhances HOR kinetics. A Ni@CNx anode, paired with a Co−Mn spinel cathode, exhibited a record peak power density of over 200 mW/cm2 in a completely precious metal–free alkaline membrane fuel cell. Ni@CNx exhibited superior durability when compared to a Ni nanoparticle catalyst due to the enhanced oxidation resistance provided by the CNx layer. Density functional theory calculations suggest that graphitic carbon layers on the surface of the Ni nanoparticles lower the H binding energy to Ni, bringing it closer to the previously predicted value for optimal HOR activity, and single Ni atoms anchored to pyridinic or pyrrolic N defects of graphene can serve as the HOR active sites. The strategy described here marks a milestone in electrocatalyst design for low-cost hydrogen fuel cells and other energy technologies with completely precious metal–free electrocatalysts.

Research Organization:
Cornell Univ., Ithaca, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Key Research and Development Program; National Natural Science Foundation of China (NSFC); Wuhan University Innovation Team; Central Universities; National Science Foundation (NSF)
Grant/Contract Number:
SC-0019445; AC02-05CH11231; AC02-06CH11357; SC0019445; 2018YFB1502300; 21991154; 21991150; 22122204; 21872108; 2042017kf0232; 2042019kf0270; DMR-1719875
OSTI ID:
1862883
Alternate ID(s):
OSTI ID: 1904762
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Vol. 119 Journal Issue: 13; ISSN 0027-8424
Publisher:
Proceedings of the National Academy of SciencesCopyright Statement
Country of Publication:
United States
Language:
English

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