Journal
NANO RESEARCH
Volume 12, Issue 7, Pages 1651-1657Publisher
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-019-2415-7
Keywords
non-precious metal; oxygen reduction reaction; Fe2N nanoparticle; FeNx moiety; proton exchange membrane fuel cell
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Funding
- National Key Research and Development Program of China [2017YFA0206500]
- National Natural Science Foundation of China [21802161, 21673275, 21533005]
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Replacing Pt-based electrocatalysts for the oxygen reduction reaction (ORR) with high performance and low-cost non-precious metal catalysts is crucial for the commercialization of fuel cells. Herein, we present a highly efficient Fe-N-C porous ORR electrocatalyst with FeN(x)moieties promoted by Fe2N nanoparticles derived from Fe-doped zeolitic imidazolate framework. The best-performing Fe-N-C/HPC-NH(3)catalyst exhibits a superior ORR activity with an onset (E-0) and half-wave (E-1/2) potential of 0.945 and 0.803 V (RHE), respectively, which is comparable to those of the commercial Pt/C in acidic media. Probing and acid-leaching experiments prove that FeNx moieties play an important role in the ORR and the Fe2N can further improve the ORR activity. Density functional theory calculation reveals a synergistic effect that the existence of Fe2N weakens the adsorption of ORR intermediates on active sites and lowers the reaction free energy of the potential limiting step, thus facilitating the ORR. Both experimental evidence and theoretical analysis for the enhancement of ORR activity by Fe2N decoration in Fe-N-C catalyst might inspire a new strategy for rational design of high performance non-precious metal catalysts.
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