Catalyzed oxidative desulfurization of coal tar pitch with trifluoroacetic acid/choline chloride eutectic solvent

Q3 Energy

燃料化学学报 Pub Date : 2025-06-01 DOI:10.1016/S1872-5813(24)60516-5

Chenpeng ZHAO , Rui ZHANG , Chunfeng MU , Dekang LI , Dakui ZHANG , Haifeng LIU , Lijun JIN , Ying HE , Haoquan HU

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引用次数: 0

Abstract

To avoid the adverse effects of sulfur in coal tar pitch (CTP) on properties of the prepared carbon materials and environment, organic acids with different acidity and choline chloride (ChCl) were selected to prepare deep eutectic solvents (DES) by low-temperature heating, and H₂O₂ as the oxidant to compose a catalytic oxidation-extraction desulfurization system of CTP. The effects of DES composition, oxidation temperature, oxidation time, and H₂O₂ dosage on desulfurization of CTP were investigated. The results show that trifluoroacetic acid (TFA)/ChCl DES has a certain effect in catalyzing the oxidative desulfurization of CTP, and the optimal desulfurization rate of CTP reaches 38.7%. The products obtained under various reaction conditions were analyzed by means of elemental analysis, FT-IR, XRD and XPS. The results show that the oxidative desulfurization of CTP catalyzed by acidic DES not only greatly improves hydrophilicity of CTP to solvent by introducing a certain amount of oxygen-containing functional groups, but also changes surface micromorphology of CTP, resulting in cracks and small particles. All these promote oxidation of thiophene sulfur in CTP to sulfone, which is further oxidized to soluble sulfate, thereby achieving sulfur removal. At the same time, oxygen content of CTP after DES catalytic oxidation treatment is relatively low, which has little effect on crystal alignment of carbonized pitch char. This work provides a technical basis for expanding high-value utilization of high-sulfur CTP.

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三氟乙酸/氯化胆碱共熔溶剂催化煤焦油沥青氧化脱硫研究

为避免煤焦油沥青（CTP）中硫对制备的炭材料性能和环境的不利影响，选择不同酸度的有机酸和氯化胆碱（ChCl），通过低温加热制备深度共晶溶剂（DES），以H2O2为氧化剂组成CTP的催化氧化-萃取脱硫体系。考察了DES组成、氧化温度、氧化时间和H2O2用量对CTP脱硫效果的影响。结果表明，三氟乙酸(TFA)/ChCl DES对CTP的氧化脱硫有一定的催化作用，CTP的最佳脱硫率达到38.7%。采用元素分析、FT-IR、XRD、XPS等方法对不同反应条件下的产物进行了分析。结果表明，酸性DES催化CTP氧化脱硫不仅通过引入一定量的含氧官能团，大大提高了CTP对溶剂的亲水性，而且还改变了CTP的表面微观形貌，产生裂纹和小颗粒。这些都促进了CTP中噻吩硫氧化为砜，砜进一步氧化为可溶性硫酸盐，从而达到除硫的目的。同时，经过DES催化氧化处理的CTP的氧含量相对较低，对碳化沥青焦的晶体排列影响不大。为扩大高硫CTP的高价值利用提供了技术依据。

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来源期刊

燃料化学学报 Chemical Engineering-Chemical Engineering (all)

CiteScore

2.80

自引率

0.00%

发文量

5825

期刊介绍： Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.