期刊
CHEMISTRY-AN ASIAN JOURNAL
卷 15, 期 3, 页码 432-439出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/asia.201901616
关键词
FeNC catalyst; graphene; metal-organic frameworks; non-noble catalyst; oxygen reduction reaction
资金
- National Natural Science Foundation of China [21601106, 21675099]
- Higher Educational Science and Technology Program of Shandong Province, China [J15LC04]
- Major Basic Research Program of Natural Science Foundation of Shandong Province, P. R. China [ZR2018ZC0129]
- Key Research and Development Plan of Shandong Province [2018GGX104108]
- Fundamental Research Funds for the Central Universities [18CX02068A]
High-performance non-noble electrocatalysts for oxygen reduction reaction (ORR) are the prerequisite for large-scale utilization of fuel cells. Herein, a type of sandwiched-like non-noble electrocatalyst with highly dispersed FeNx active sites embedded in a hierarchically porous carbon/graphene heterostructure was fabricated using a bottom-up strategy. The in situ ion substitution of Fe3+ in a nitrogen-containing MOF (ZIF-8) allows the Fe-heteroatoms to be uniformly distributed in the MOF precursor, and the assembly of Fe-doped ZIF-8 nano-crystals with graphene-oxide and in situ reduction of graphene-oxide afford a sandwiched-like Fe-doped ZIF-8/graphene heterostructure. This type of heterostructure enables simultaneous optimization of FeNx active sites, architecture and interface properties for obtaining an electron-catalyst after a one-step carbonization. The synergistic effect of these factors render the resulting catalysts with excellent ORR activities. The half-wave potential of 0.88 V vs. RHE outperforms most of the none-noble metal catalyst and is comparable with the commercial Pt/C (20 wt %) catalyst. Apart from the high activity, this catalyst exhibits excellent durability and good methanol-tolerance. Detailed investigations demonstrate that a moderate content of Fe dopants can effectively increase the intrinsic activities, and the hybridization of graphene can enhance the reaction kinetics of ORR. The strategy proposed in this work gives an inspiration towards developing efficient noble-metal-free electrocatalysts for ORR.
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