摘要
采用密度泛函理论方法比较了DBT/DBTO2和[BMIM]+[PF6]-/[BMIM]+[BF4]-的相互作用。对最稳定的[BMIM]+[PF6]-、[BMIM]+[PF6]--DBT、[BMIM]+[PF6]--DBTO2、[BMIM]+[BF4]-、[BMIM]+[BF4]--DBT、[BMIM]+[BF4]--DBTO2进行了NBO和AIM分析。结果表明,DBT和[BMIM]+[PF6]-/[BMIM]+[BF4]-中的咪唑环彼此相互平行,NBO和AIM分析表明它们之间发生了!-!相互作用。H1'和H9'形成的F…H氢键有利于!-!堆积作用的形成。DBTO2倾向于趋近C2-H2和甲基基团形成O…H相互作用;DBTO2优先吸附在[BMIM]+[PF6]-/[BMIM]+[BF4]-。在模拟油中,[BMIM]+[PF6]-和[BMIM]+[BF4]-离子液体对DBTO2的萃取能力大于DBT,其原因是可能是DBTO2具有较大的极性和O…H与F…H的氢键作用。
The interactions between sulfur-containing compounds of dibenzothiophene （DBT） and dibenzothiophene sulfone （ DBTO2 ） and ionic liquids of 1-butyl-3-methylimidazolium hexafluorophosphate （ [ BMIM] ＋ [ PF6 ] - ） and 1-butyl-3- methylimidazolium tetrafluoroborate （ E BMIM] ＊[ BF4 ]-） were comparatively studied by using density functional theory. The most stable structures of EBMIM]＋EPF6]-, ~BMIM~＋EPF6] -DBT, EBMIM]＋EPF6]--DBTO2, EBMIM~＋~BF4] , [BMIM]＋IBF4] -DBT, and [BMIM]＋EBF4]--DBTO2 systems were obtained by natural bond orbitais （NBO） and atoms in molecules （AIM） analyses. The results indicated that DBT and [BMIM] rings of IBMIM]＋~PF6] /EBMIM]＋EBF4]- are parallel to each other. There is a strong rc-r~ interaction between them in terms of NBO and AIM analyses. The HI＇ and H9＇ involved F-.. H hydrogen bonding interactions may favor the formation of 7r-~ stacking interactions. The DBTO2 preferentially locates near the C2-H2 and methyl group of [ BMIM] ＋ to form O..-H interactions. The predicted geometries and interaction energies imply the preferential adsorption of DBTO2 on [ BMIM] ＋ [ PF6 ] -/E BMIM] ~ I BF4 ] -. The [ BMIM~ ＋ [ PF6 ] -/[ BF4 ] - have better extracting ability to remove DBTO2 than DBT, possibly due to the larger polarity of DBTOz and stronger interactions between I BMIM]~ [ PF6 ] -/[ BF4 ]- and DBTO2.
出处
《燃料化学学报》
EI
CAS
CSCD
北大核心
2012年第12期1444-1453,共10页
Journal of Fuel Chemistry and Technology
