Ran Liu , Chang Wang , Qiang Yang , Jing-Ran Yang , Chen Liu , Liberty Mguni , Xin-Ying Liu , Ya-Li Yao , Fa-Tang Li
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The investigation results of four DILs prepared from different metal chlorides ([HSO<sub>3</sub>C<sub>3</sub>NEt<sub>3</sub>]Cl-MnCl<sub>n</sub>, MnCl<sub>n</sub> = AlCl<sub>3</sub>, ZnCl<sub>2</sub>, CuCl<sub>2</sub>, FeCl<sub>3</sub>) in oxidative desulfurization showed that [HSO<sub>3</sub>C<sub>3</sub>NEt<sub>3</sub>]Cl–AlCl<sub>3</sub> had an outstanding catalytic effect and significantly promoted the oxidation of sulfides. With a 0.2 g [HSO<sub>3</sub>C<sub>3</sub>NEt<sub>3</sub>]Cl–AlCl<sub>3</sub>, the removal rate of dibenzothiophene (DBT) reached 100% in 10 mL model oil under mild conditions at 55 °C for 20 min. The key is its ability to induce the dismutation of superoxide anions (•O<sub>2</sub><sup>−</sup>), which facilitates the generation of singlet oxygen (<sup>1</sup>O<sub>2</sub>). The efficient oxidation of DBT is accomplished through a predominantly <sup>1</sup>O<sub>2</sub>-mediated non-radical mechanism. [HSO<sub>3</sub>C<sub>3</sub>NEt<sub>3</sub>]Cl-AlCl<sub>3</sub> serves as a favorable medium for contact to be made between <sup>1</sup>O<sub>2</sub> and sulfides, which indicates an efficient catalytic-adsorption synergy.</div></div>","PeriodicalId":19938,"journal":{"name":"Petroleum Science","volume":"22 1","pages":"Pages 492-507"},"PeriodicalIF":6.1000,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Exceptional functionalized dual-acidic ionic liquid: High-efficiency catalytic reaction medium for oxidation desulfurization\",\"authors\":\"Ran Liu , Chang Wang , Qiang Yang , Jing-Ran Yang , Chen Liu , Liberty Mguni , Xin-Ying Liu , Ya-Li Yao , Fa-Tang Li\",\"doi\":\"10.1016/j.petsci.2024.07.012\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The development of highly active functionalized ionic liquids (ILs) as both extractants and catalysts for use in achieving deep desulfurization continues to pose challenges. In this study, a highly efficient oxidative desulfurization system was constructed, composed of dual-acidic ionic liquids (DILs) and H<sub>2</sub>O<sub>2</sub>-AcOH. The investigation results of four DILs prepared from different metal chlorides ([HSO<sub>3</sub>C<sub>3</sub>NEt<sub>3</sub>]Cl-MnCl<sub>n</sub>, MnCl<sub>n</sub> = AlCl<sub>3</sub>, ZnCl<sub>2</sub>, CuCl<sub>2</sub>, FeCl<sub>3</sub>) in oxidative desulfurization showed that [HSO<sub>3</sub>C<sub>3</sub>NEt<sub>3</sub>]Cl–AlCl<sub>3</sub> had an outstanding catalytic effect and significantly promoted the oxidation of sulfides. With a 0.2 g [HSO<sub>3</sub>C<sub>3</sub>NEt<sub>3</sub>]Cl–AlCl<sub>3</sub>, the removal rate of dibenzothiophene (DBT) reached 100% in 10 mL model oil under mild conditions at 55 °C for 20 min. The key is its ability to induce the dismutation of superoxide anions (•O<sub>2</sub><sup>−</sup>), which facilitates the generation of singlet oxygen (<sup>1</sup>O<sub>2</sub>). 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引用次数: 0
摘要
高活性功能化离子液体(ILs)作为萃取剂和催化剂用于实现深度脱硫仍然面临挑战。本研究构建了由双酸性离子液体(DILs)和H2O2-AcOH组成的高效氧化脱硫体系。对不同金属氯化物([HSO3C3NEt3]Cl-MnCln、MnCln = AlCl3、ZnCl2、CuCl2、FeCl3)制备的四种dil进行氧化脱硫的研究结果表明,[HSO3C3NEt3] Cl-AlCl3具有突出的催化作用,显著促进了硫化物的氧化。用0.2 g [HSO3C3NEt3] Cl-AlCl3在10 mL模型油中,在55℃的温和条件下,作用20 min,二苯并噻吩(DBT)的去除率达到100%。关键是它能诱导超氧阴离子(•O2−)的突变,促进单线态氧(1O2)的生成。DBT的有效氧化主要通过o2介导的非自由基机制完成。[HSO3C3NEt3]Cl-AlCl3作为1O2与硫化物接触的良好介质,表现出高效的催化吸附协同作用。
Exceptional functionalized dual-acidic ionic liquid: High-efficiency catalytic reaction medium for oxidation desulfurization
The development of highly active functionalized ionic liquids (ILs) as both extractants and catalysts for use in achieving deep desulfurization continues to pose challenges. In this study, a highly efficient oxidative desulfurization system was constructed, composed of dual-acidic ionic liquids (DILs) and H2O2-AcOH. The investigation results of four DILs prepared from different metal chlorides ([HSO3C3NEt3]Cl-MnCln, MnCln = AlCl3, ZnCl2, CuCl2, FeCl3) in oxidative desulfurization showed that [HSO3C3NEt3]Cl–AlCl3 had an outstanding catalytic effect and significantly promoted the oxidation of sulfides. With a 0.2 g [HSO3C3NEt3]Cl–AlCl3, the removal rate of dibenzothiophene (DBT) reached 100% in 10 mL model oil under mild conditions at 55 °C for 20 min. The key is its ability to induce the dismutation of superoxide anions (•O2−), which facilitates the generation of singlet oxygen (1O2). The efficient oxidation of DBT is accomplished through a predominantly 1O2-mediated non-radical mechanism. [HSO3C3NEt3]Cl-AlCl3 serves as a favorable medium for contact to be made between 1O2 and sulfides, which indicates an efficient catalytic-adsorption synergy.
期刊介绍:
Petroleum Science is the only English journal in China on petroleum science and technology that is intended for professionals engaged in petroleum science research and technical applications all over the world, as well as the managerial personnel of oil companies. It covers petroleum geology, petroleum geophysics, petroleum engineering, petrochemistry & chemical engineering, petroleum mechanics, and economic management. It aims to introduce the latest results in oil industry research in China, promote cooperation in petroleum science research between China and the rest of the world, and build a bridge for scientific communication between China and the world.