期刊
ACS NANO
卷 12, 期 6, 页码 5674-5683出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.8b01502
关键词
monomicelle assembly; two-dimensional architecture; sandwich-like composite; iron- and nitrogen-doped carbon; oxygen reduction
类别
资金
- Australian Research Council (ARC) Future Fellow [FT150100479]
- JSPS KAKENHI [17H05393, 17K19044]
- Qingdao University of Science and Technology
- Suzuken Memorial Foundation
- Japan Society for the Promotion of Science International Research Fellows (JSPS) [17F17080]
Triblock copolymer micelles coated with melamine-formaldehyde resin were self-assembled into closely packed two-dimensional (2D) arrangements on the surface of graphene oxide sheets. Carbonizing these structures created a 2D architecture composed of reduced graphene oxide (rGO) sandwiched between two monolayers of sub-40 nm diameter hollow nitrogen-doped carbon nano spheres (N-HCNS). Electrochemical tests showed that these hybrid structures had better performance for oxygen reduction compared to physically mixed rGO and N-HCNS that were not chemically bonded together. Further impregnation of the sandwich structures with iron (Fe) species followed by carbonization yielded Fe/(1.6)-N-HCNS/rGO-900 with a high specific surface area (968.3 m(2) g(-1)), a high nitrogen doping (6.5 at%), and uniformly distributed Fe dopant (1.6 wt %). X-ray absorption fine structure analyses showed that most of the Fe in the nitrogen doped carbon framework is composed of single Fe atoms each coordinated to four N atoms. The best Fe-1.6-N-HCNS/rGO-900 catalyst performed better in electrocatalytic oxygen reduction than 20 wt % Pt/C catalyst in alkaline medium, with a more positive half-wave potential of 0.872 V and the same limiting current density. Bottom-up soft-patterning of regular carbon arrays on free-standing 2D surfaces should enable conductive carbon supports that boost the performance of electrocatalytic active sites.
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