title: Bottom-Up Fabrication of Sulfur-Doped Graphene Films Derived from Sulfur-Annulated Nanographene for Ultrahigh Volumetric Capacitance Micro-Supercapacitors.
abstract: Heteroatom doping of nanocarbon films can efficiently boost the pseudocapacitance of micro-supercapacitors (MSCs); however, wafer-scale fabrication of sulfur-doped graphene films with a tailored thickness and homogeneous doping for MSCs remains a great challenge. Here we demonstrate the bottom-up fabrication of continuous, uniform, and ultrathin sulfur-doped graphene (SG) films, derived from the peripherical trisulfur-annulated hexa-peri-hexabenzocoronene (SHBC), for ultrahigh-rate MSCs (SG-MSCs) with landmark volumetric capacitance. The SG film was prepared by thermal annealing of the spray-coated SHBC-based film, with assistance of a thin Au protecting layer, at 800 °C for 30 min. SHBC with 12 phenylthio groups decorated at the periphery is critical as a precursor for the formation of the continuous and ultrathin SG film, with a uniform thickness of ∼10.0 nm. Notably, the as-produced all-solid-state planar SG-MSCs exhibited a highly stable pseudocapacitive behavior with a volumetric capacitance of ∼582 F cm-3at 10 mV s-1, excellent rate capability with a remarkable capacitance of 8.1 F cm-3even at an ultrahigh rate of 2000 V s-1, ultrafast frequency response with a short time constant of 0.26 ms, and ultrahigh power density of ∼1191 W cm-3. It is noteworthy that these values obtained are among the best values for carbon-based MSCs reported to date.
authors.affiliation: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , 457 Zhongshan Road, Dalian 116023, China.
authors.forename: Zhong-Shuai
authors.identifier: 0000-0003-1851-4803
authors.initials: ZS
authors.lastname: Wu
authors.affiliation: State Key Laboratory for Physical Chemistry of Solid Surfaces and Department of Chemistry College of Chemistry and Chemical Engineering, Xiamen University , 422 Siming South Road, Xiamen 361005, China.
authors.forename: Yun-Zhi
authors.initials: YZ
authors.lastname: Tan
authors.affiliation: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , 457 Zhongshan Road, Dalian 116023, China.|State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , 457 Zhongshan Road, Dalian 116023, China.|University of Chinese Academy of Sciences , 19 A Yuquan Rd, Shijingshan District, Beijing 100049, China.
authors.forename: Shuanghao
authors.initials: S
authors.lastname: Zheng
authors.affiliation: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , 457 Zhongshan Road, Dalian 116023, China.|University of Chinese Academy of Sciences , 19 A Yuquan Rd, Shijingshan District, Beijing 100049, China.
authors.forename: Sen
authors.initials: S
authors.lastname: Wang
authors.affiliation: School of Chemistry, University of Manchester , Oxford Road, Manchester M13 9PL, United Kingdom.
authors.forename: Khaled
authors.initials: K
authors.lastname: Parvez
authors.affiliation: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , 457 Zhongshan Road, Dalian 116023, China.|University of Chinese Academy of Sciences , 19 A Yuquan Rd, Shijingshan District, Beijing 100049, China.
authors.forename: Jieqiong
authors.initials: J
authors.lastname: Qin
authors.affiliation: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , 457 Zhongshan Road, Dalian 116023, China.|State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , 457 Zhongshan Road, Dalian 116023, China.
authors.forename: Xiaoyu
authors.initials: X
authors.lastname: Shi
authors.affiliation: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , 457 Zhongshan Road, Dalian 116023, China.|University of Chinese Academy of Sciences , 19 A Yuquan Rd, Shijingshan District, Beijing 100049, China.
authors.forename: Chenglin
authors.initials: C
authors.lastname: Sun
authors.affiliation: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , 457 Zhongshan Road, Dalian 116023, China.|State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , 457 Zhongshan Road, Dalian 116023, China.
authors.forename: Xinhe
authors.identifier: 0000-0001-9404-6429
authors.initials: X
authors.lastname: Bao
authors.affiliation: Center for Advancing Electronics Dresden (cfaed) & Department of Chemistry and Food Chemistry, Technische Universität Dresden , Mommsenstraβe 4, 01062 Dresden, Germany.
authors.forename: Xinliang
authors.initials: X
authors.lastname: Feng
authors.affiliation: Max-Planck-Institut für Polymerforschung , Ackermannweg 10, 55128 Mainz, Germany.
authors.forename: Klaus
authors.identifier: 0000-0001-6630-8786
authors.initials: K
authors.lastname: Müllen