Wang Xu, Wang Weimiao, Liu Yang, Ren Mengmeng, Xiao Huining, Liu Xiangyang
State Key Laboratory of Polymer Materials Engineering, College of Polymer Science and Engineering, Sichuan University, Chengdu, Sichuan 610065, P. R. China.
Department of Chemical Engineering, University of New Brunswick, Fredericton, NB E3B 5A3, Canada.
Phys Chem Chem Phys. 2016 Jan 28;18(4):3285-93. doi: 10.1039/c5cp06914a.
The effect of solvent on the chemical structure and properties of fluorinated graphene (FG) was particularly investigated in this work. It is found that the reduction of FG and the weakening of strong covalent C-F bonding take place under the action of some dipolar solvents even at room temperature. The rate of the C-F bond rupture reaction is positively influenced by the dipole moment of solvent and fluorine coverage of FG sheets. Meanwhile, defluorination of FG is controllable through the time and temperature of solvent treatment. These solvents function as the nucleophilic catalysts, promoting chemical transformation, which leads to a series of changes in the structure and properties of FG, such as a decline of fluorine concentration of about 40% and the reduction of thermal stability and band gap from 3 to 2 eV. After the treatment with dipolar solvent N-methyl-2-pyrrolidinone, FG maintained a capacity of 255 mA h g(-1) and a power density of 2986 W kg(-1) at a high discharge rate, while the pristine FG could not be discharged at all. This is called the "solvent activation" effect on the electrochemical performance of FG. The finding may draw attention to the effect of various external factors on the chemical structure and properties of FG, which is of great importance for the realization of the FG's potential.
本工作特别研究了溶剂对氟化石墨烯(FG)化学结构和性能的影响。研究发现,即使在室温下,在某些偶极溶剂的作用下,FG也会发生还原以及强共价C-F键的减弱。C-F键断裂反应的速率受到溶剂偶极矩和FG片层氟覆盖率的正向影响。同时,FG的脱氟可通过溶剂处理的时间和温度来控制。这些溶剂起到亲核催化剂的作用,促进化学转化,这导致FG的结构和性能发生一系列变化,例如氟浓度下降约40%,热稳定性和带隙从3 eV降低到2 eV。用偶极溶剂N-甲基-2-吡咯烷酮处理后,FG在高放电率下保持了255 mA h g(-1)的容量和2986 W kg(-1)的功率密度,而原始FG根本无法放电。这被称为对FG电化学性能的“溶剂活化”效应。该发现可能会引起人们对各种外部因素对FG化学结构和性能影响的关注,这对于实现FG的潜力具有重要意义。