Yu Song, Bo Jiang, Wu Li
Key Laboratory of Coal bed Methane Resource & Reservoir Formation Process, Ministry of Education, China University of Mining & Technology, Xuzhou 221116, China.
Phys Chem Chem Phys. 2017 Jul 21;19(27):17773-17788. doi: 10.1039/c7cp02993d. Epub 2017 Jun 28.
The competitive adsorptions of CH/CO/HO on coal vitrinite (DV-8, CHON) were computed based on density function theory (DFT) and grand canonical Monte Carlo (GCMC). The adsorption process reaches the saturation state after adsorbing 17 CHs, 22 COs, and 35 HOs per CHON respectively. The optimal configurations of CH-vitrinite, CO-vitrinite, and HO-vitrinite respectively manifest as aromatic/T/rT (1 adsorption location, 2 adsorption sites and T here represents sites above the carbon atom and the heteroatom, 3 adsorption orientation and rT here means the orientations of three hydrogen atoms pointing to vitrinite), aromatic/T/v (v represents the orientations perpendicular to the plane of vitrinite), and aromatic/rV/T (rV represents an oxygen atom pointing to the vitrinite surface). The GCMC results show that high temperature is not conducive to the vitrinite's adsorption of adsorbates and the adsorption capacity order is HO > CO > CH (263-363 K) in the one-component, binary, and ternary adsorbate systems. The optimal configurations of vitrinite are similar to graphite/graphene, while ΔE is significantly lower than graphite/graphene. Simulation data are in good agreement with the experimental results.
基于密度泛函理论（DFT）和巨正则蒙特卡罗（GCMC）方法，计算了CH/CO/HO在煤镜质体（DV-8，CHON）上的竞争吸附情况。吸附过程中，每个CHON分别吸附17个CH、22个CO和35个HO后达到饱和状态。CH-镜质体、CO-镜质体和HO-镜质体的最优构型分别表现为芳香族/T/rT（1个吸附位置，2个吸附位点，T表示碳原子和杂原子上方的位点，3个吸附取向，rT表示三个氢原子指向镜质体的取向）、芳香族/T/v（v表示垂直于镜质体平面的取向）和芳香族/rV/T（rV表示一个氧原子指向镜质体表面）。GCMC结果表明，高温不利于镜质体对吸附质的吸附，在单组分、二元和三元吸附质体系中，吸附容量顺序为HO > CO > CH（263 - 363 K）。镜质体的最优构型与石墨/石墨烯相似，但ΔE显著低于石墨/石墨烯。模拟数据与实验结果吻合良好。
