杂多酸离子液体催化燃油萃取氧化脱硫性能研究（英文）  

Extraction and Oxidative Desulfurization of Fuels Catalyzed by Polyoxometalate- Based Ionic Liquids

作　　者：张薇[1] 丁永萍[2] 张宇[1] 陈霞[1] 宋溪明[1] 

机构地区：[1]辽宁大学化学院绿色合成与先进材料制备化学辽宁省重点实验室,沈阳110036 [2]包头师范学院化学学院,包头014030

出　　处：《化学通报》2015年第4期330-336,共7页Chemistry

基　　金：国家自然科学基金(21203082;51273087);辽宁省科技厅自然科学基金项目(201102084)资助

摘　　要：本文首次将一系列含有不同酸性咪唑阳离子和不同杂多酸阴离子的杂多酸离子液体[C4mim]3PW12O40、[COOH-Cmim]3PW12O40、[SO3H-C3mim]3PW12O40、[SO3H-C3mim]3PMo12O40和[SO3H-C3mim]4SiW 12O40作为催化剂,乙腈为萃取剂,H2O2为氧化剂,用于催化含二苯并噻吩、苯并噻吩及噻吩模型油的萃取氧化脱硫研究中。实验结果显示,杂多酸离子液体催化燃油脱硫性能不仅与阳离子的酸性强弱有关,而且与阴离子结构密切相关。阳离子的催化活性顺序为:[SO3H-C3mim]+>[COOH-Cmim]+>[C4mim]+;阴离子的催化活性顺序为PW3-12O3-40>PMo12O40>SiW 12O4-40。其中[SO3H-C3mim]3PW12O40催化活性最高,在60℃反应40min的条件下,二苯并噻吩的转化率约为100%,催化不同硫化物的转化率为:二苯并噻吩>苯并噻吩>噻吩。此外,该杂多酸离子液体循环使用5次催化活性仅略有下降。A series of polyoxometalate-based ionic liquids( POM-ILs) [C4mim]3PW12O40, [COOHCmim]3PW12O40,[SO3H-C3mim]3PW12O40,[SO3H- C3mim]3PMo12O40and [SO3H-C3mim]4SiW 12O40 were applied as catalysts for the removal of dibenzothiophene( DBT),benzothiophene( BT) and thiophene( T) in model oil with H2O2 as oxidant and acetonitrile as extractant. The results showed that the acidity of cations and the type of anions of the POM-ILs all played key roles in catalyzing desulfurization reaction. The catalytic activity sequence of the cations was [SO3H-C3mim]+>[COOH-Cmim]+> [C4mim]+,while the order of anions was PW12O3-40> PMo12O3-40>SiW 12O4-40. Under the optimized conditions,the catalyst [SO3H-C3mim]3PW12O40showed the highest activity with DBT conversion of about 100% at 60℃ for 40 min. The selectivity sequence of sulfur removal for S-compounds was DBT > BT > T. Additionally,the catalyst can be recycled five times with a slight decrease in activity.

关 键 词：萃取 氧化脱硫 杂多酸离子液体 催化 

分 类 号：TQ517[化学工程] TQ203.2