• 文献标题:   Efficient synthesis of amine-functionalized graphene oxide by ultrasound-assisted reactions and density functional theory mechanistic insight
  • 文献类型:   Article
  • 作  者:   SIERRA U, CUARA E, MERCADO A, DIAZBARRIGA E, BAHENA A, CORTES A, MARTINEZ JP, SOLA M, FERNANDEZ S
  • 作者关键词:   graphite oxide, graphene oxide, amine, ultrasound, density functional theory
  • 出版物名称:   APPLIED NANOSCIENCE
  • ISSN:   2190-5509 EI 2190-5517
  • 通讯作者地址:  
  • 被引频次:   4
  • DOI:   10.1007/s13204-021-01798-4 EA APR 2021
  • 出版年:   2021

▎ 摘  要

Herein described is a facile preparation protocol by which amino-alcohol derivatives of graphene oxide (GO) can be conveniently synthesized in high yield and short time by an ultrasound treatment of ethanol-graphite-oxide suspensions and amines. Linear primary amines of different chain length rapidly react with graphite oxides prepared from powder and flakes, leading to the formation of GO amino-alcohol derivatives. Characterization of the amine-modified materials by XRD, TGA, FTIR, and Raman spectroscopy demonstrates the proposed derivatization; the findings are corroborated by SEM and TEM observations. Additionally, quantum-chemical investigations shed additional light on the reaction, suggesting an alcohol-accelerated S(N)2 mechanism where the initial step, the simultaneous formation of a C-N bond (GO-amine) and rupture of an epoxide bond in GO, is rate-determining. Energy barriers lower than 8 kcal/mol are estimated, which can be overcome with the energy supplied by the sonotrode tip (ca. 2 kcal) and the use of ethanol to facilitate it.