Characteristics of Graphene Growth at Different Temperatures from the Benzene Ring Structure in Coal Tar

Abstract

A large number of aromatic substances can be found in so-called coal tar (containing >10,000 individual compounds), which is a mixture of heavy liquid fractions (dense viscous black liquor, tended to solidification) obtained after the pyrolysis of coal (solid product—coke, gas products, and light liquid products are also produced during the process). Volatile monocyclic aromatic hydrocarbons, which are naturally occurring in coal tar, can be exploited as premium raw materials for the production of graphene by chemical vapor deposition (CVD). Moreover, aromatic chemicals (compounds with benzene rings) can produce graphene at lower temperatures than other small-molecule gas feedstocks (for graphene growth via methane gas, the temperature must be at least 900 °C). The intermediate reaction mechanism involved in the creation of graphene from various temperature ranges of monocyclic aromatic hydrocarbons in benzene ring structures has long been a fascinating enigma. Accordingly, in this paper, we analyze the graphene growth pattern of benzene at different temperatures from 300 to 900 °C. For graphene synthesis in the lower temperature range (300~600 °C), analytical experiments show that benzene rings (almost) do not crack during the gas phase process. Thus, the structure of the benzene ring is directly coupled into graphene in the above temperature range. When benzene is more thoroughly transformed into tiny molecules that are deposited on the surface of copper foil at higher temperatures (700~900 °C), graphene is formed by a complex mixture of carbon sources, including gaseous small molecules (methane and ethane) and benzene. Based on the process above, we provide an alternative solution for the large-scale industrial preparation of graphene, with low energy consumption, via low-temperature synthesis of graphene by the CVD method using the coal tar carbon source at 500 °C, which is the optimal growth temperature of the benzene ring.