AlHumaidan Faisal S, Rana Mohan S, Vinoba Mari, AlSheeha Hanadi M, Ali Afnan A, Navvamani R
Petroleum Research Center, Kuwait Institute for Scientific Research Kuwait
RSC Adv. 2023 Mar 8;13(12):7766-7779. doi: 10.1039/d2ra07481h.
A method for synthesizing graphene derivatives from asphaltene is proposed in this work. The graphene derivatives are mainly composed of few-layer graphene-like nano-sheets of randomly distributed heteroatoms; mainly sulfur and nitrogen. The proposed method is based on a thermal treatment in which asphaltene is carbonized in a rotating quartz-tube furnace under an inert atmosphere at a temperature in the range of 400-950 °C. Asphaltenes from different origins were employed to verify the synthesis method. The results indicate that graphene derivatives obtained at high carbonization temperature have similar structural parameters, despite the evident differences in parent asphaltenes structures and compositions. The transformation of asphaltene to graphene derivatives mainly occurred due to three factors: the reduction in the average number of aromatic layers (), the expansion in aromatic sheet diameter ( ), and the elimination of alkyl side chains. The reduction in the number of aromatic sheets per stack is primarily ascribed to thermal exfoliation, while the increase in the aromatic sheet diameter is attributed to secondary reactions in the aromatic core of asphaltene. The elimination of side chains, on the other hand, is mainly credited to thermal cracking. The quantification of defect density ( ) in the graphene derivatives suggests an association between defects and heteroatoms presence.
本工作提出了一种由沥青质合成石墨烯衍生物的方法。石墨烯衍生物主要由随机分布杂原子(主要是硫和氮)的几层类石墨烯纳米片组成。所提出的方法基于一种热处理过程,即在惰性气氛下,于旋转石英管炉中在400 - 950℃的温度范围内将沥青质碳化。采用了不同来源的沥青质来验证该合成方法。结果表明,尽管母体沥青质的结构和组成存在明显差异,但在高碳化温度下获得的石墨烯衍生物具有相似的结构参数。沥青质向石墨烯衍生物的转变主要归因于三个因素:芳香层平均数量的减少()、芳香片直径的增大()以及烷基侧链的消除。每堆叠芳香片数量的减少主要归因于热剥离,而芳香片直径的增大则归因于沥青质芳香核中的二次反应。另一方面,侧链的消除主要归因于热裂解。石墨烯衍生物中缺陷密度()的量化表明缺陷与杂原子的存在之间存在关联。