• 文献标题:   Direct Observation of Spatially Heterogeneous Single-Layer Graphene Oxide Reduction Kinetics
  • 文献类型:   Article
  • 作  者:   MCDONALD MP, ELTOM A, VIETMEYER F, THAPA J, MOROZOV YV, SOKOLOV DA, HODAK JH, VINODGOPAL K, KAMAT PV, KUNO M
  • 作者关键词:   graphene oxide, reduced graphene oxide, photolysi, reduction, photobrightening, fluorescence intermittency
  • 出版物名称:   NANO LETTERS
  • ISSN:   1530-6984 EI 1530-6992
  • 通讯作者地址:   Univ Notre Dame
  • 被引频次:   28
  • DOI:   10.1021/nl402057j
  • 出版年:   2013

▎ 摘  要

Graphene oxide (GO) is an important precursor in the production of chemically derived graphene. During reduction, GO's electrical conductivity and band gap change gradually. Doping and chemical functionalization are also possible, illustrating GO's immense potential in creating functional devices through control of its local hybridization. Here we show that laser-induced photolysis controllably reduces individual single-layer GO sheets. The reaction can be followed in real time through sizable decreases in GO's photoluminescence efficiency along with spectral blueshifts. As-produced reduced graphene oxide (rGO) sheets undergo additional photolysis, characterized by dramatic emission enhancements and spectral redshifts. Both GO's reduction and subsequent conversion to photobrightened rGO captured through movies of their photoluminescence kinetics. Rate maps illustrate sizable spatial and temporal heterogeneities in sp(2) domain growth and reveal how reduction "flows" across GO and rGO sheets. The observed heterogeneous reduction kinetics provides mechanistic insight into GO's conversion to chemically derived graphene and highlights opportunities for overcoming its dynamic, chemical disorder.