The development of nitrogen-rich biomass- derived carbon catalysts provides an attractive perspective to substitute for Pt-based electrocatalysts for oxygen reduction reaction （ORR）. We here report a facile strategy...The development of nitrogen-rich biomass- derived carbon catalysts provides an attractive perspective to substitute for Pt-based electrocatalysts for oxygen reduction reaction （ORR）. We here report a facile strategy for synthesis of a nitrogen-doped biocarbon/graphene-like composite electrocatalyst by pyrolyzing a solid-state mixture of coprinus comatus biomass and melamine under nitrogen protection. The graphtic carbon nitride formed by polycondensation of melamine at 600 ℃ acts as a self-sacrificing template to generate the nitrogen-doped graphene-like sheet, which can function as an inserting agent and self-generating support. The composite catalyst exhibits the most promising catalytic activity towards the four-electron ORR with a half-wave potential of around 0.83 V （vs. RHE）, and more excellent stability and tolerance to methanol/ethanol compared to the commercial Pt/C catalyst. It is interestingly found that both a higher content of nitrogen and a larger ratio of graphitic-nitrogen species, which may derive from self-addition of graphene-like support into the catalyst, can effectively improve theelectrocatalytic activity. The planar N group may be the nitrogen functionality that is most responsible for main-taining the ORR activity in alkaline medium. This study can largely encourage the exploration of high-performance carbon-based catalysts from economical and sustainable fungus biomass.展开更多
基金supported by the Basic and Frontier Research Program of Chongqing Municipality (cstc2015jcyj A50032, cstc2014jcyj A50038)the Scientific and Technological Research Program of Chongqing Municipal Education Commission (KJ1501118)+1 种基金the Talent Introduction Project of Chongqing University of Arts and Sciences (R2014CJ02)the National Natural Science Foundation of China (21273292)
文摘The development of nitrogen-rich biomass- derived carbon catalysts provides an attractive perspective to substitute for Pt-based electrocatalysts for oxygen reduction reaction （ORR）. We here report a facile strategy for synthesis of a nitrogen-doped biocarbon/graphene-like composite electrocatalyst by pyrolyzing a solid-state mixture of coprinus comatus biomass and melamine under nitrogen protection. The graphtic carbon nitride formed by polycondensation of melamine at 600 ℃ acts as a self-sacrificing template to generate the nitrogen-doped graphene-like sheet, which can function as an inserting agent and self-generating support. The composite catalyst exhibits the most promising catalytic activity towards the four-electron ORR with a half-wave potential of around 0.83 V （vs. RHE）, and more excellent stability and tolerance to methanol/ethanol compared to the commercial Pt/C catalyst. It is interestingly found that both a higher content of nitrogen and a larger ratio of graphitic-nitrogen species, which may derive from self-addition of graphene-like support into the catalyst, can effectively improve theelectrocatalytic activity. The planar N group may be the nitrogen functionality that is most responsible for main-taining the ORR activity in alkaline medium. This study can largely encourage the exploration of high-performance carbon-based catalysts from economical and sustainable fungus biomass.
