Kinetic characteristics and product distribution of tar-rich coal in-situ underground pyrolysis: Influence of heterogeneous coal seam

Abstract

Tar-rich coal contains more hydrogen-rich structures such as aliphatic side chains and bridge bonds, which is a good raw material for coal to oil. In-situ underground pyrolysis of tar-rich coal has significant advantages such as environmental friendliness and high safety factor; it is an efficient, clean coal utilization technology. Due to the influence of geological structure and other factors in the formation process, underground coal seam was often heterogeneous, generally accompanied by coal gangue interlayers. Due to the coal gangue being relatively dense and has poor thermal conductivity, it is also rich in metal oxides, it would inevitably affect the pyrolysis characteristics and product distribution during the pyrolysis process of heterogeneous tar-rich coal seam. The pyrolysis characteristics of heterogeneous tar-rich coal seam with different positions and layers of coal gangue interlayer were investigated by the thermogravimetric analyzer, and related kinetic parameters were obtained by the distributed activation energy model (DAEM). Based on the fixed bed tube furnace reactor, the pyrolysis experiments of heterogeneous tar-rich coal seam with different positions and layers of coal gangue interlayer were also carried out, and the pyrolysis products were characterized and analyzed. The thermogravimetric results showed that in the pyrolysis process of heterogeneous tar-rich coal seam, the initial pyrolysis temperature and the temperature corresponding to the maximum weight loss rate shifted to the higher temperature range, and the pyrolysis characteristic index decreased significantly. Under the same conditions, the corresponding pyrolysis characteristic indexes of the upper coal gangue interlayer and 4 layers of coal gangue interlayer were lower, which were 11.69 (10−8·%·min−1·℃−3) and 11.65 (10−8·%·min−1·℃−3), respectively. Compared with homogeneous tar-rich coal seam, pyrolysis activation energies of heterogeneous coal seam generally showed the decreasing trend. Under the conditions of the upper part containing coal gangue interlayer and the upper-and-lower parts containing coal gangue interlayer, the pyrolysis activation energies were higher due to the hindrance of the cover layer of coal gangue to the volatile release, which were 555.88 kJ·mol−1 and 546.66 kJ·mol−1 respectively. The results of fixed bed pyrolysis experiments showed that compared with homogeneous tar-rich coal seam, the tar yield obtained was reduced, the degree of tar lightening was significantly improved, and the proportion of lighter tar was up to 70.00 wt%. The contents of aromatic hydrocarbons and phenolic compounds in tar increased, the contents of aliphatic hydrocarbons and oxygenated compounds decreased significantly, and the maximum reductions were nearly 4.50 wt% and 6.50 wt%, respectively. The gas yield increased, the proportions of H2 and CO2 in the gas increased, and the proportions of CO and CH4 decreased to varying degrees. The tar yields were lower under the conditions of upper gangue and 4 layers gangue, which were 6.53 wt% and 5.81 wt%, respectively, and the degrees of tar lightening were also more significant. From the relationship between pyrolysis characteristic parameters and tar properties of heterogeneous tar-rich coal seam pyrolysis, it was found that the existence of coal gangue interlayer was not conducive to the tar production, but it could promote the lightening of tar and improve the tar quality. Exploring the kinetic characteristics and pyrolysis product distribution of heterogeneous tar-rich coal seam could provide theoretical guidance for the site selection of in-situ underground pyrolysis engineering and the well arrangement.