Metal-free oxidative desulfurization with molecular oxygen by using N-enriched porous carbons derived from ionic liquid-loaded covalent-organic polymer

共价键 聚合物 多孔性 化学 氧化磷酸化 氧气 离子液体 分子氧 烟气脱硫 金属 化学工程 离子键合 高分子化学 有机化学 材料科学 催化作用 离子 工程类 生物化学
作者
Imteaz Ahmed,Chul‐Ung Kim,Sung Hwa Jhung
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:450: 138416-138416 被引量:9
标识
DOI:10.1016/j.cej.2022.138416
摘要

• A microporous triazine polymer was prepared and firstly loaded with a N-containing ionic liquid. • N-enriched carbonaceous materials (ICDCs) were derived via pyrolysis of the composites. • ICDCs were applied as a metal-free catalyst for the aerobic oxidative desulfurization (ODS). • ICDC(8), with high N content, showed a remarkable result in ODS with a very low E a of 23.7 kJ/mol. • A plausible reaction mechanism with •O 2 - could be set via radical scavenger and ESR experiments. A microporous triazine polymer (MCTP) was prepared and loaded, for the first time, with an N-containing ionic liquid (IL) through a ship-in-a-bottle method. The composite material, IL@MCTP, was pyrolyzed under high temperature to get N-enriched carbonaceous materials. The obtained carbons (denoted ICDCs) were utilized as a metal-free catalyst for the aerobic oxidative desulfurization (ODS) of organic sulfur compounds like dibenzothiophene from a model fuel. The reactivity of ICDCs in ODS was dependent on the nitrogen content and porosity of the carbons. One selected material (ICDC(8)), because of high nitrogen content and adequate porosity, showed a remarkable performance in ODS or removal of dibenzothiophene with a very low activation energy of 23.7 kJ/mol. Radical scavenger experiments and ESR analysis revealed the important role of superoxide anion radicals (•O 2 - ) in oxidation. A plausible reaction mechanism to suggest an important role of nitrogen species in ICDCs to activate O 2 (via adsorption on C with a partial positive charge) was proposed. The ODS also can be carried out with air, and the catalyst was reusable for up to the fifth cycle by simple solvent washing. The ICDCs can be a competitive and environment-friendly (metal-free) ODS catalyst, especially using cheap oxidants like air or O 2 .
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