title: Self-Size-Limiting Nanoscale Perforation of Graphene for Dense Heteroatom Doping.
abstract: A scalable and controllable nanoscale perforation method for graphene is developed on the basis of the two-step thermal activation of a graphene aerogel. Different resistance to the thermal oxidation between graphitic and defective domains in the weakly reduced graphene oxide is exploited for the self-limiting nanoscale perforation in the graphene basal plane via selective thermal degradation of the defective domains. The resultant nanoporous graphene with a narrow pore-size distribution addresses the long-standing challenge for the high-level doping of graphene with lattice-mismatched large-size heteroatoms (S and P). Noticeably, this novel heteroatom doping strategy is demonstrated to be highly effective for oxygen reduction reaction (ORR) catalysis. Not only the higher level of heteroatom doping but also favorable spin and charge redistribution around the pore edges leads to a strong ORR activity as supported by density functional theory calculations.
authors.affiliation: National Creative Research Initiative Center for Multi-Dimensional Directed Nanoscale Assembly, Department of Materials Science & Engineering, KAIST , 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea.|Department of Physics, Indian Institute of Technology Guwahati (IITG) , Guwahati 781039, Assam, India.
authors.forename: Uday Narayan
authors.initials: UN
authors.lastname: Maiti
authors.affiliation: SRM Research Institute, SRM University , Kattankulathur 603 203, Tamil Nadu, India.
authors.forename: Ranjit
authors.initials: R
authors.lastname: Thapa
authors.affiliation: National Creative Research Initiative Center for Multi-Dimensional Directed Nanoscale Assembly, Department of Materials Science & Engineering, KAIST , 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea.
authors.forename: Joonwon
authors.initials: J
authors.lastname: Lim
authors.affiliation: National Creative Research Initiative Center for Multi-Dimensional Directed Nanoscale Assembly, Department of Materials Science & Engineering, KAIST , 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea.
authors.forename: Dong Jun
authors.initials: DJ
authors.lastname: Li
authors.affiliation: Department of Materials Science & Engineering, Pusan National University , Pusan 609-735, Republic of Korea.
authors.forename: Kwang Ho
authors.initials: KH
authors.lastname: Kim
authors.affiliation: National Creative Research Initiative Center for Multi-Dimensional Directed Nanoscale Assembly, Department of Materials Science & Engineering, KAIST , 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea.
authors.forename: Sang Ouk
authors.initials: SO
authors.lastname: Kim
keywords: density functional theory; doping; graphene; oxygen reduction reaction; perforation