Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 32, Issue 18, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202111396
Keywords
coupling site; electrocatalysis; endogenous metal oxide; N-doped carbon; oxygen reduction
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Funding
- National Natural Science Foundation of China [51772332, 51972345]
- Hunan Provincial Science and Technology Plan Project [2018RS3008, 2017TP1001]
- Natural Science Foundation of Hunan Province [2021JJ30790]
- innovation project of graduate student in Hunan province [2021zzts0065]
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A novel synthesis strategy for fabricating metal-free carbon with nitrogen dopants and carbon defects is reported, which exhibits outstanding activity and stability in the oxygen reduction reaction. The strategy involves the conversion of metal-nitrogen moieties to endogenous metal oxides during pyrolysis, resulting in the formation of abundant coupling sites between nitrogen dopants and carbon defects.
Coupling sites of nitrogen dopants and intrinsic carbon defects (N/DC) in metal-free carbon are highly active toward electrocatalytic oxygen reduction reaction (ORR), and yet they are hard to be effectively constructed. Here, a novel synthesis strategy for fabrication of N/DC-enriched metal-free carbon from precursors containing metal-nitrogen moieties (M-N-x) is reported. During pyrolysis of the precursors, the M-N-x is in situ converted to endogenous metal oxides (MOx) via a halide-mediated bait and switch mechanism to realize a domain-confined etching of the carbon matrix around the nitrogen dopants, forming abundant N/DC coupling sites in the final carbon products. The optimized N/DC-enriched carbon exhibits an outstanding ORR activity and stability with a half-wave potential of 0.903 V (versus RHE) in 0.1 m KOH solution, outperforming most of the reported metal-free carbon catalysts. Experimental investigations and theoretical calculations demonstrate an improved electron-donating ability and optimized binding energies of the N/DC coupling sites toward the ORR intermediates, which are primarily responsible for such an excellent ORR activity. This domain-confined endogenous MOx etching strategy is also widely applicable to different M-N-x-containing precursors as well as different halide mediators, which opens up new possibilities to fabricate metal/nonmetal doped carbon materials enriched with various coupling sites of desired synergistic properties.
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