Journal
NANO RESEARCH
Volume 11, Issue 12, Pages 6260-6269Publisher
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-018-2149-y
Keywords
single-atom catalyst; heteroatom codoping; porous materials; oxygen reduction; electrocatalysis
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Funding
- China Ministry of Science and Technology [2016YFA (0202801)]
- National Natural Science Foundation of China [21521091, 21390393, U1463202, 21573119, 21590792, 21501004]
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We developed a strategy based on coordination polymer to synthesize singleatom site Fe/N and S-codoped hierarchical porous carbon (Fe-1/N, S-PC). The as-obtained Fe-1/N, S-PC exhibited superior oxygen reduction reaction (ORR) performance with a half-wave potential (E-1/2, 0.904 V vs. RHE) that was better than that of commercial Pt/C (E-1/2, 0.86 V vs. RHE), single-atom site Fe/N-doped hierarchical porous carbon (Fe-1/N-PC) without S-doped (E-1/2, 0.85 V vs. RHE), and many other nonprecious metal catalysts in alkaline medium. Moreover, the Fe-1/N,S-PC revealed high methanol tolerance and firm stability. The excellent electrocatalytic activity of Fe-1/N,S-PC is attributed to the synergistic effects from the atomically dispersed porphyrin-like Fe-N-4 active sites, the heteroatom codoping (N and S), and the hierarchical porous structure in the carbon materials. The calculation based on density functional theory further indicates that the catalytic performance of Fe-1/N,S-PC is better than that of Fe-1/N-PC owing to the sulfur doping that yielded different rate-determining steps.
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