U.S. Army Engineer Research and Development Center, 3909 Halls Ferry Road, Vicksburg, Mississippi 39180, USA.
Langmuir. 2012 Sep 18;28(37):13307-17. doi: 10.1021/la3027286. Epub 2012 Sep 4.
The adsorption of benzene, polycyclic aromatic hydrocarbons (PAHs), and nitroaromatic compounds (NACs) on the carbonaceous surfaces from the gas phase and water solution was investigated. Several different levels of theory were applied, including DFT-, MP2-, and CCSD(T)-based methods, to find an approach that is computationally inexpensive and can provide accurate thermodynamic parameters for studied adsorption phenomena. The methods and techniques used (including cluster and periodic approximations) were evaluated on the basis of comparison with available experimental data. The optimized structures of calculated complexes are obtained, and the interaction energies and Gibbs free energies are predicted. Good agreement was revealed for the theoretical and experimental adsorption energies of benzene and PAHs adsorbed on the carbon surfaces. The adsorption of benzene, PAHs, and NACs on carbon is suggested to be effective from the gas phase for all studied compounds and for PAHs and NACs also from water solution at room temperature.
研究了气相和水溶液中碳质表面对苯、多环芳烃 (PAHs) 和硝基芳烃化合物 (NACs) 的吸附。应用了几种不同的理论水平，包括 DFT、MP2 和 CCSD(T) 方法，以找到一种计算成本低廉且能为研究的吸附现象提供准确热力学参数的方法。所使用的方法和技术（包括簇和周期性近似）是基于与可用实验数据的比较进行评估的。计算得到了优化的配合物结构，并预测了相互作用能和吉布斯自由能。苯和 PAHs 吸附在碳表面的理论和实验吸附能之间显示出良好的一致性。对于所有研究的化合物，从气相到室温下的水溶液，苯、PAHs 和 NACs 在碳上的吸附被认为是有效的。
