CAJ | 학술논문

粘土矿已经被广泛用来去除有机物,修复和净化被石油碳氢化合物污染的土壤和地下水。我们选择高岭石作为研究对象,构造了Si6O18H12和Al6O24H30两个团簇模型分别代表高岭石的硅氧层表面和铝氧层表面,在MP2/6-31G(d,p)//B3LYP/6-31G(d,p)的理论水平上系统地研究了气态下苯分子和高岭石团簇模型的相互作用。并进一步分析了苯分子和高岭石表面相互作用的各种气态性质,比如：优化的几何构型、结构参数、吸附能、自然键轨道电荷分布、振动频率变化、静电势、电子密度性质(次级氢键的电子密度和拉普拉斯算符值)和电子密度差分等。优化的几何构型表明苯分子吸附在高岭石表面的本质可能是次级氢键的形成。其他性质的结果进一步验证了次级氢键的存在,并指出苯更倾向于吸附在高岭石的铝氧层表面,且苯环和铝氧层表面形成近似90°的夹角。
점토광이경피엄범용래거제유궤물,수복화정화피석유탄경화합물오염적토양화지하수。아문선택고령석작위연구대상,구조료Si6O18H12화Al6O24H30량개단족모형분별대표고령석적규양층표면화려양층표면,재MP2/6-31G(d,p)//B3LYP/6-31G(d,p)적이론수평상계통지연구료기태하분분자화고령석단족모형적상호작용。병진일보분석료분분자화고령석표면상호작용적각충기태성질,비여：우화적궤하구형、결구삼수、흡부능、자연건궤도전하분포、진동빈솔변화、정전세、전자밀도성질(차급경건적전자밀도화랍보랍사산부치)화전자밀도차분등。우화적궤하구형표명분분자흡부재고령석표면적본질가능시차급경건적형성。기타성질적결과진일보험증료차급경건적존재,병지출분경경향우흡부재고령석적려양층표면,차분배화려양층표면형성근사90°적협각。
Clay minerals are used to remove organics and to remediate soils and groundwater contaminated with petroleum hydrocarbons. Cluster models of Si6O18H12 and Al6O24H30 for the tetrahedral (Si-O) and octahedral (Al-O) surfaces of kaolinite were set up to mimic kaolinite surfaces. The interactions of benzene molecule and the kaolinite cluster models were systematical y studied at the MP2/6-31G(d,p)//B3LYP/6-31G(d,p) level. The gas-state adsorption properties of benzene on the kaolinite surfaces, such as the optimized structures, structural parameters, adsorption energies, natural bond orbital charge distributions, vibration frequencies, electrostatic potential maps, electron density characteristics (the ρ and ▽2ρ values of secondary hydrogen-bonds), and electron density difference, were analyzed in this work. The optimized structures indicate that the adsorption of benzene molecule on the kaolinite surfaces may be caused by formation of secondary hydrogen-bonds. The results for the other properties further confirmed the existence of secondary hydrogen-bonds. Benzene molecule is more likely to be adsorbed on the Al-O surface than on the Si-O surface. The adsorption angle between the benzene ring plane and the kaolinite Al-O surface is about 90°.