Chen Linghan, Han Jiuhui, Ito Yoshikazu, Fujita Takeshi, Huang Gang, Hu Kailong, Hirata Akihiko, Watanabe Kentaro, Chen Mingwei
WPI Advanced Institute for Materials Research, Tohoku University, Sendai, 980-8577, Japan.
Institute of Applied Physics, Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba, 305-8573, Japan.
Angew Chem Int Ed Engl. 2018 Oct 1;57(40):13302-13307. doi: 10.1002/anie.201809315. Epub 2018 Sep 7.
Heavy chemical doping and high electrical conductivity are two key factors for metal-free graphene electrocatalysts to realize superior catalytic performance toward hydrogen evolution. However, heavy chemical doping usually leads to the reduction of electrical conductivity because the catalytically active dopants give rise to additional electron scattering and hence increased electrical resistance. A hierarchical nanoporous graphene, which is comprised of heavily chemical doped domains and a highly conductive pure graphene substrate, is reported. The hierarchical nanoporous graphene can host a remarkably high concentration of N and S dopants up to 9.0 at % without sacrificing the excellent electrical conductivity of graphene. The combination of heavy chemical doping and high conductivity results in high catalytic activity toward electrochemical hydrogen production. This study has an important implication in developing multi-functional electrocatalysts by 3D nanoarchitecture design.
重化学掺杂和高电导率是无金属石墨烯电催化剂实现优异析氢催化性能的两个关键因素。然而，重化学掺杂通常会导致电导率降低，因为催化活性掺杂剂会引起额外的电子散射，从而增加电阻。本文报道了一种由重化学掺杂域和高导电纯石墨烯基底组成的分级纳米多孔石墨烯。这种分级纳米多孔石墨烯可以容纳高达9.0 at %的高浓度氮和硫掺杂剂，而不会牺牲石墨烯优异的导电性。重化学掺杂和高导电性的结合导致了对电化学产氢的高催化活性。这项研究对于通过三维纳米结构设计开发多功能电催化剂具有重要意义。
