RSC Advances p. 39178 - 39184 (2017)
Update date:2022-08-18
Topics:
Shao, Zonggui
Tong, Lei
Qian, Yasheng
Dun, Rongmin
Li, Wenmu
The development of non-precious metal (NPM) catalysts with superior performance to replace Pt/C is critical for the wide application of proton-exchange membrane fuel cells. In this work, a three-dimensional crosslinked polymer with highly dispersed iron-nitrogen (Fe-N) coordination units and a mechanically robust framework is designed, synthesized and used as the sole precursor to obtain Fe-coordinated nitrogen-doped carbon (Fe-Nx/C) oxygen reduction reaction (ORR) catalysts. After optimization of the pyrolysis conditions and the use of SiO2 templates to modify the catalyst nanostructure, a highly active catalyst of T-FeNC-800R is obtained, which exhibits a high half-wave potential of 751 mV in 0.1 M HClO4. Besides, the T-FeNC-800R catalyst has an excellent ORR activity with onset and half-wave potentials of 1030 and 873 mV in 0.1 M KOH, respectively, which are higher than those of Pt/C (onset and half-wave potentials are 1009 and 855 mV vs. RHE, respectively). Moreover, this catalyst exhibits an almost four electron transfer process, high long-term stability, and better methanol tolerance than Pt/C catalyst in acidic media. The excellent oxygen reduction reaction performance of T-FeNC-800R can be attributed to the mesoporous structure, high specific surface area and a large number of exposed active sites. Moreover, the effects of the SiO2 template, secondary pyrolysis and iron element on the catalytic performance are systematically discussed.
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