To overcome two obstacles in graphene functionalization—the random distribution of functional groups and substantial lattice defects,in this contribution,we rationally bypass the universal yet destructive graphene ox...To overcome two obstacles in graphene functionalization—the random distribution of functional groups and substantial lattice defects,in this contribution,we rationally bypass the universal yet destructive graphene oxide(GO)-derived methodologies and adopt reductive covalent functionalization of natural graphite.In this strategy,ultrahigh density graphene sheets with evenly distributed negative charges were intermediately yielded by potassium reduction to graphite.Subsequently,they were regioregularly and efficiently brominated by the benchmark electrophile of molecular bromine.The combined characterizations determined the graphene bromide derivative to have a molecular formula of C_(24)-Br,corresponding well with the brominated entity of the inseparable C_(24)-K^(+)graphite intercalation compounds.Due to the regular distribution of Br groups and intact hexagonal lattice of the graphene matrix,the C_(24)-Br_GBr delivers exceptional electrical properties although theπ-conjugation is partially blocked by C(sp^(3))-Br sites and greatly outperforms its counterparts derived from GO bromination.In both model applications of quickly switchable electrochromic devices and all-solid-state supercapacitors,C_(24)-Br_GBr exhibits impressive performance,which highlights the great significance and prospect of regioregular and lattice-nondestructive graphene functionalization.展开更多
基金The authors gratefully acknowledge financial support from the National Natural Science Foundation of China(no.21504080)the Natural Science Foundation of Zhejiang Province(no.LQ15B040003)the Fundamental Research Funds of Zhejiang Sci-Tech University(no.2020Q040).
文摘To overcome two obstacles in graphene functionalization—the random distribution of functional groups and substantial lattice defects,in this contribution,we rationally bypass the universal yet destructive graphene oxide(GO)-derived methodologies and adopt reductive covalent functionalization of natural graphite.In this strategy,ultrahigh density graphene sheets with evenly distributed negative charges were intermediately yielded by potassium reduction to graphite.Subsequently,they were regioregularly and efficiently brominated by the benchmark electrophile of molecular bromine.The combined characterizations determined the graphene bromide derivative to have a molecular formula of C_(24)-Br,corresponding well with the brominated entity of the inseparable C_(24)-K^(+)graphite intercalation compounds.Due to the regular distribution of Br groups and intact hexagonal lattice of the graphene matrix,the C_(24)-Br_GBr delivers exceptional electrical properties although theπ-conjugation is partially blocked by C(sp^(3))-Br sites and greatly outperforms its counterparts derived from GO bromination.In both model applications of quickly switchable electrochromic devices and all-solid-state supercapacitors,C_(24)-Br_GBr exhibits impressive performance,which highlights the great significance and prospect of regioregular and lattice-nondestructive graphene functionalization.
