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Few Layer g-C3N4 Dispersed Quaternary Phosphonium Ionic Liquid for Highly Efficient Catalytic Oxidative Desulfurization of Fuel
Energy & Fuels ( IF 5.2 ) Pub Date : 2020-09-22 , DOI: 10.1021/acs.energyfuels.0c02357 Suhang Xun 1 , Qiutong Ti 1 , Linlan Wu 2 , Minqiang He 2 , Chao Wang 1 , Linlin Chen 2 , Wenshu Yang 3 , Linhua Zhu 4 , Wenshuai Zhu 2 , Huaming Li 2
Energy & Fuels ( IF 5.2 ) Pub Date : 2020-09-22 , DOI: 10.1021/acs.energyfuels.0c02357 Suhang Xun 1 , Qiutong Ti 1 , Linlan Wu 2 , Minqiang He 2 , Chao Wang 1 , Linlin Chen 2 , Wenshu Yang 3 , Linhua Zhu 4 , Wenshuai Zhu 2 , Huaming Li 2
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Functionalized ionic liquids (ILs) have been considered as efficient catalysts for oxidative desulfurization (ODS), but the further industrial applications are hampered by the poor separability with oil phase after reaction and large dosage. In this work, few-layered graphitic carbon nitride (g-C3N4) with high specific surface area was prepared via thermal oxidation and employed as a carrier to construct supported ionic liquid catalyst for ODS. A functional quaternary phosphonium ionic liquid [(C6H13)3PC14H29]3PMo12O40 (abbreviated as C14PPMo) was synthesized and immobilized on g-C3N4. Then, the as-prepared samples were characterized by FT-IR, DRS, XRD, N2 adsorption–desorption isotherm, XPS, SEM, and TEM, systematically. It was found that few layer g-C3N4 had a large specific surface area (194.89 m2 g–1), which was conducive to the high dispersion of C14PPMo IL. The obtained support catalyst C14PPMo/g-C3N4 exhibited outstanding catalytic ability on the oxidation of dibenzothiophene (DBT), and the desulfurization efficiency could reach 100% with a small dosage of IL under optimal conditions. The oxidative products of DBT and 4,6-dimethyldibenzothiophene (4,6-DMDBT) were the homologous sulfones and proved by GC-MS, and the proposed reaction processes were studied, respectively. Since the supported IL was a heterogeneous catalyst and no additional solvent was added, C14PPMo IL could be separated and repossessed readily after the reaction. Moreover, the recycle ability of C14PPMo/g-C3N4 on the oxidation of both DBT and 4,6-DMDBT were investigated simultaneously, and both of the desulfurization activities could still remain above 90% after 6 times cycling.
中文翻译：
几层gC 3 N 4分散的季Ph离子液体可实现燃料的高效催化氧化脱硫
官能化离子液体（ILs）被认为是氧化脱硫（ODS）的有效催化剂，但由于反应后与油相的分离性差且用量大，阻碍了进一步的工业应用。在这项工作中，通过热氧化制备了具有高比表面积的几层石墨氮化碳（gC 3 N 4），并用作载体来构建用于ODS的负载型离子液体催化剂。功能性季phospho离子液体[（C 6 H 13）3 PC 14 H 29 ] 3 PMo 12 O 40（缩写为C 14合成PPMo）并将其固定在gC 3 N 4上。然后，通过FT-IR，DRS，XRD，N 2吸附-解吸等温线，XPS，SEM和TEM对其进行系统表征。发现很少的gC 3 N 4层具有较大的比表面积（194.89 m 2 g –1），这有助于C 14 PPMo IL的高分散性。得到的载体催化剂C 14 PPMo / gC 3 N 4对二苯并噻吩（DBT）的氧化具有出色的催化能力，并且在最佳条件下以少量IL脱硫效率可以达到100％。DBT和4,6-二甲基二苯并噻吩（4,6-DMDBT）的氧化产物是同源砜，并通过GC-MS证明，并研究了所提出的反应过程。由于负载的IL是非均相催化剂，并且不添加其他溶剂，因此在反应后，C 14 PPMo IL可以分离并重新安置。此外，C 14 PPMo / gC 3 N 4的循环能力 同时研究了DBT和4,6-DMDBT的氧化脱硫率，经过6次循环后，两种脱硫活性仍可保持在90％以上。
更新日期：2020-10-16
中文翻译：
几层gC 3 N 4分散的季Ph离子液体可实现燃料的高效催化氧化脱硫
官能化离子液体（ILs）被认为是氧化脱硫（ODS）的有效催化剂，但由于反应后与油相的分离性差且用量大，阻碍了进一步的工业应用。在这项工作中，通过热氧化制备了具有高比表面积的几层石墨氮化碳（gC 3 N 4），并用作载体来构建用于ODS的负载型离子液体催化剂。功能性季phospho离子液体[（C 6 H 13）3 PC 14 H 29 ] 3 PMo 12 O 40（缩写为C 14合成PPMo）并将其固定在gC 3 N 4上。然后，通过FT-IR，DRS，XRD，N 2吸附-解吸等温线，XPS，SEM和TEM对其进行系统表征。发现很少的gC 3 N 4层具有较大的比表面积（194.89 m 2 g –1），这有助于C 14 PPMo IL的高分散性。得到的载体催化剂C 14 PPMo / gC 3 N 4对二苯并噻吩（DBT）的氧化具有出色的催化能力，并且在最佳条件下以少量IL脱硫效率可以达到100％。DBT和4,6-二甲基二苯并噻吩（4,6-DMDBT）的氧化产物是同源砜，并通过GC-MS证明，并研究了所提出的反应过程。由于负载的IL是非均相催化剂，并且不添加其他溶剂，因此在反应后，C 14 PPMo IL可以分离并重新安置。此外，C 14 PPMo / gC 3 N 4的循环能力 同时研究了DBT和4,6-DMDBT的氧化脱硫率，经过6次循环后，两种脱硫活性仍可保持在90％以上。
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