外加能量场对煤中有机硫结构特性影响规律的量子化学研究

为分析煤中有机硫结构对微波的响应规律,采用密度泛函理论模拟研究了煤中几种典型含硫模型化合物的含硫键在不同外加能量场作用下的变化规律和断键特点,从而进一步理解其脱除机理。结果表明,外电场从0增加到0.054 4eV时,体系的总能量随着外电场的增强而逐渐增大,最高占据轨道能量EH、最低空轨道能量EL、能隙EG均随着外电场的增强而减小,电偶极矩随着外电场的增强而增加,表明外电场的加入使分子的活性和极性增加,分子中的S—S键长和S原子电荷数均随外加电场的增强而增大,各基团的谐振频率随外加电场的增强而减小,振动光谱强度也有所变化。因此,针对煤中的有机含硫结构在微波脱硫过程中,需要考虑外加能量场所导致的分子活性及极性等变化的影响。

Quantum chemistry investigation on influence regularity of the external energy fields to the organic sulfur structural characteristics in coal

In order to analyze the response regularity of the organic sulfur structure in coal to microwave，the change rule and bond broken characteristics of the sulfur bond in several typical sulfur model compounds in coal were studied under the different external energy fields using the density functional theory simulation，thus it can make us understand the removal mechanism furtherly.The results show that the total energy of the system increases with the electric field from 0 to 0.054 4 eV，the highest occupied orbital energy EH，the lowest empty orbital energy EL and the energy gap EG all decrease with the increase of the electric field，it indicates that the molecular activity and polarity increase with the electric field increasing for the electric dipole moment increasing with the electric field.The bond length of S—S in molecular and the charge of S atom increase with the electric field heightening，the resonance frequency of the each group decreases with the increase of applied electric field，the vibration spectrum intensity also change.It need to consider the changing influence of the molecular activity and polarity which the external electron fields lead to during the microwave desulfurization process as the organic sulfur structure in coal.