| 张薇,丁永萍,张宇,陈霞,宋溪明.化学通报,2015,78(4):330-336. |
| 杂多酸离子液体催化燃油萃取氧化脱硫性能研究 |
| Extraction and Oxidative Desulfurization of Fuels Catalyzed by Polyoxometalate-Based Ionic Liquids |
| 投稿时间：2014-09-16 修订日期：2014-11-05 |
| DOI： |
| 中文关键词: 萃取 氧化脱硫 杂多酸离子液体 催化 |
| 英文关键词:Extraction, Oxidative desulfurization, Polyoxometalate-based ionic liquids, Catalysis |
| 基金项目:国家自然科学基金(21203082, 51273087)和辽宁省科技厅自然科学基金项目(201102084)资助 |
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| 中文摘要: |
| 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]4SiW12O40，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、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PW12O403- > PMo12O403- > SiW12O404-。其中[SO3H-C3mim]3PW12O40催化活性最高，在60oC反应40 min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。 |
| 英文摘要: |
| A series of polyoxometalate-based ionic liquids (POM-ILs) [C4mim]3PW12O40, [COOH-Cmim]3PW12O40, [SO3H-C3mim]3PW12O40, [SO3H- C3mim]3PMo12O40 and [SO3H-C3mim]4SiW12O40 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 experimental results showed that the acidity of cations and the type of anions of the POM-ILs all played key roles for catalyzing desulfurization reaction. The catalytic activities of the cations followed the order of [SO3H-C3mim] > [COOH-Cmim] > [C4mim] and the order of anions was PW12O403- > PMo12O403- > SiW12O404-. Under the optimized conditions, the catalyst [SO3H-C3mim]3PW12O40 showed the highest activity with DBT conversion of about 100% at 60 oC for 40 min. And its sulfur removal selectivity for S-compounds followed the order of DBT > BT > T. Additionally, the catalyst can be recycled five times with a slight decrease in activity. |
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