首页|Sulfur doped iron-nitrogen-hard carbon nanosheets as efficient and robust noble metal-free catalysts for oxygen reduction reaction in PEMFC
Sulfur doped iron-nitrogen-hard carbon nanosheets as efficient and robust noble metal-free catalysts for oxygen reduction reaction in PEMFC
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Transition metal-nitrogen-carbon(M-N-C)as a promising substitute for the conventional noble metal-based catalyst still suffers from low activity and durability for oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).To tackle the issue,herein,a new type of sulfur-doped iron-nitrogen-hard carbon(S-Fe-N-HC)nanosheets with high activity and durability in acid media were devel-oped by using a newly synthesized precursor of amide-based polymer with Fe ions based on copolymer-izing two monomers of 2,5-thiophene dicarboxylic acid(TDA)as S source and 1,8-diaminonaphthalene(DAN)as N source via an amination reaction.The as-synthesized S-Fe-N-HC features highly dispersed atomic FeNx moieties embedded into rich thiophene-S doped hard carbon nanosheets filled with highly twisted graphite-like microcrystals,which is distinguished from the majority of M-N-C with soft or gra-phitic carbon structures.These unique characteristics endow S-Fe-N-HC with high ORR activity and out-standing durability in 0.5 M H2S04.Its initial half-wave potential is 0.80 V and the corresponding loss is only 21 mV after 30,000 cycles.Meanwhile,its practical PEMFC performance is a maximum power output of 628.0 mW cm-2 and a slight power density loss is 83.0 mW cm-2 after 200-cycle practical operation.Additionally,theoretical calculation shows that the activity of FeNx moieties on ORR can be further enhanced by sulfur doping at meta-site near FeN4C.These results evidently demonstrate that the dual effect of hard carbon substrate and S doping derived from the precursor platform of amid-polymers can effectively enhance the activity and durability of Fe-N-C catalysts,providing a new guidance for developing advanced M-N-C catalysts for ORR.
Bin Liu、Jiawang Li、Bowen Yan、Qi Wei、Xingyu Wen、Huarui Xie、Huan He、Pei Kang Shen、Zhi Qun Tian
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Collaborative Innovation Center of Sustainable Energy Materials,School of Physical Science and Technology,Guangxi University,Guangxi Key Laboratory of Electrochemical Energy Materials,State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures,Nanning 530004,Guangxi,China
National Natural Science Foundation of ChinaGuangxi Science and Technology Project
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