Adsorptive Denitrogenation of Fuel over Metal Organic Frameworks: Effect of N-Types and Adsorption Mechanisms
Adsorptive Denitrogenation of Fuel over Metal Organic Frameworks: Effect of N-Types and Adsorption Mechanisms
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DOI：
10.1021/jp5045817
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发表时间：
2014-09
影响因子：
3.7
通讯作者：
Ying Wu;Jing Xiao;Luoming Wu;M. Chen;Hongxia Xi;Zhong Li;Haihui Wang
中科院分区：
文献类型：
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作者：
Ying Wu;Jing Xiao;Luoming Wu;M. Chen;Hongxia Xi;Zhong Li;Haihui Wang
本工作研究吸附脱氮（ADN）的燃料在金属有机框架使用相结合的实验/计算方法。MIL-101（Cr）在低浓度下显示出高的ADN容量，这归因于MIL-101（Cr）上提供最强吸附的位点。MIL-101（Cr）对碱性喹啉的吸附能力高于非碱性吲哚，因为喹啉的吸附强度（−61.31 kJ/mol）大于吲哚（−38.33 kJ/mol）。燃料中各种化合物的吸附选择性遵循有机氮>有机硫>萘的顺序，与吸附强度的顺序为BEN（−62 <$−34 kJ/mol）< BES（−32 <$−24 kJ/mol）< BENap（−21.65 kJ/mol）一致，表明MIL-101（Cr）是ADN的高选择性吸附剂。多环芳烃对ADN的影响很小，而四氢呋喃对ADN的吸附有不同程度的抑制作用，这取决于N型吸附剂（包括N基吸附剂）对ADN吸附机理的影响。
This work investigates adsorptive denitrogenation (ADN) of fuels over metal organic frameworks using a combined experimental/computational approach. MIL-101(Cr) shows high ADN capacities at low concentrations, ascribing to the sites on MIL-101(Cr) offering the strongest adsorption. Adsorption capacity of MIL-101(Cr) is higher for basic quinoline than that for nonbasic indole due to a greater adsorption strength of quinoline (−61.31 kJ/mol) than indole (−38.33 kJ/mol). Adsorption selectivity of various types of compounds in fuels follows the order of organonitrogen ≫ organosulfur > naphthalene, in good agreement with the order of adsorption strength as BEN (−62 ∼ −34 kJ/mol) < BES (−32 ∼ −24 kJ/mol) < BENap (−21.65 kJ/mol), suggesting MIL-101(Cr) is a highly selective adsorbent for ADN. ADN is negligibly affected by polyaromatic hydrocarbons, but suppressed by oxygenate cosolvent, that is, tetrahydrofuran to varied extents, depending on the varied adsorption mechanisms affected by N-types, including N-basi...