Coprinus comatus-derived nitrogen-containing biocarbon electrocatalyst with the addition of self-generating graphene-like support for superior oxygen reduction reaction  

作　　者：Chaozhong Guo Wenli Liao Zhongbin Li Lingtao Sun Haibo Ruan Qingshan Wu Qinghong Luo Jie Huang Changguo Chen 

机构地区：[1]Research Institute for New Materials Technology, Chongqing University of Arts and Sciences [2]School of Chemistry and Chemical Engineering, Chongqing University [3]School of Materials and Chemical Engineering, Chongqing University of Arts and Sciences

出　　处：《Science Bulletin》2016年第12期948-958,共11页科学通报（英文版）

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);the Talent Introduction Project of Chongqing University of Arts and Sciences (R2014CJ02);the National Natural Science Foundation of China (21273292)

摘　　要：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.The development of nitrogen-rich biomassderived 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 °C acts as a selfsacrificing 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 fourelectron 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 the electrocatalytic activity. The planar N group may be the nitrogen functionality that is most responsible for maintaining 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.

关 键 词：Coprinus comatus N-doped carbon ELECTROCATALYSIS Oxygen reduction Active site 

分 类 号：O643.36[理学—物理化学]