FUEL PROCESSING TECHNOLOGY
·
2018
·
IF 3.956
Longfei Tang,Songjiang Chen,Shiwei Wang,Xiuxiang Tao,Huan He,Lei Zheng,Chenyan Ma,Yidong Zhao
The present work investigated the feasibility of heterocyclic sulfur (HS) removal for coal utilizing potassium tert-butoxide and hydrosilane system. Changes of sulfur forms with treatment time in Xinyu (XY) coal were determined by XANES . Results showed that reductions of total sulfur and organic sulfur for XY coal were 55% and 53%, respectively. >85% sulfoether and thiophene sulfur were removed after treated for 4 h, suggesting that the HS could be removed to a high extent from coal. However, contents of sulfonate and sulfonic ester increased with treatment time due to the hydrolysis and oxidation of intermediate products containing Si S bands. Furthermore, it indicated that the HS could be removed selectively from coal without destroying the macromolecular structure of coal based on analysis of desulfurization mechanism. These findings suggested that the desulfurization of refractory HS in coal could be obtained using the potassium tert-butoxide/hydrosilane reductive system, which provided a reference for desulfurization of high organic sulfur coal .
研究领域:
能源化学
·
煤化工
·
环境化学
·
应用化学
·
清洁燃料技术
✓ 已验证
DOI
高影响因子
Journal of Cleaner Production
·
2020
·
IF 7.246
Yongliang Xu,Yang Liu,Yunchuan Bu,Menglei Chen,Lanyun Wang
A large amount of SOx will be produced in the combustion process of coal without desulfurization , which is the main factor causing air pollution, environmental damage and PM2.5 increase. Here, desulfurization of coal by chemical agents are summarized. Acid/alkali desulfurization and occur mainly through the chemical reaction of an acid/alkali with a metal oxide or sulfate (such as calcium oxide and ferric sulfate) to remove sulfur from coal, which can only remove a small amount of inorganic sulfur and organic sulfur. Moreover, the combination of an organic solvent with an acid/alkali for desulfurization can transform the organic sulfur molecule into an inorganic sulfur salt in an acid/alkali environment due to cyclic polar compounds containing oxygen or nitrogen that react with coal molecules and dissolve part of the coal molecules. Furthermore, microwave combined with chemical reagents for desulfurization shows better desulfurization efficiency and economy, but most of them were aimed at the removal of oil and model sulfur, and there were few studies on sulfur removal from coal. In view of the advantages of low volatility and high recycling rate of ionic liquids (ILs), the research progress and mechanism of action of ionic liquids in coal desulfurization are reviewed. It is found that acidic ionic liquids can be combined with hydrogen in coal to effectively dissolve organic sulfur. While the acidic ionic liquid was applied in combination with the oxidant hydrogen peroxide, the desulfurization effect appears more significant. The –SH and -S-S- functional groups in coal could be better oxidized by hydrogen peroxide to sulfone and sulfoxide, which was due to the oxidation promoted by acidic ionic liquids.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Yuqing Wang,Tao Ge,Chuanchuan Cai,Jingyao Xu
Screening suitable ionic liquids（ILs） for removing organic sulfur compounds from coal and discovering new, effective and environmentally friendly coal desulfurization additives is crucial. The solubility properties (SP) of six organic sulfur model compounds (OSMCs) in imidazole ILs were calculated based on the COSMO-SAC model. The results showed that 2-thiophenecarboxylic acid and 2-aminophenyl phenyl sulfone exhibited favorable solubility properties in certain ILs. The solubility properties of partial imidazole ILs consisting of [Cl] - were significantly better than other anions. Through the σ -profiles analysis of ILs anions, cations and OSMCs, it showed that [Cl]- had a higher tendency to be hydrogen bond acceptor than other anions. The polar groups in OSMCs increased the hydrogen bond donor or acceptor sites for interactions with ILs, while extended the optional range of ILs for hydrogen bond interactions with OSMCs. The extraction efficiencies of 2-thiophenecarboxylic acid by ILs were above 25%, with [DMIM][Cl] displaying the highest efficiency at 47.5%. Meanwhile, [DMIM][Cl] was the most effective extractant for removing all OSMCs except benzothiophene, which was basically consistent with the calculation results. Electrostatic potential analysis was used to obtain the sites where OSMCs are the most likely to form hydrogen bond interactions with [DMIM][Cl]. And characterization of hydrogen bond formation between ILs and OSMCs was obtained by FTIR analysis. The hydrogen bond formed by p-thiocresol with [DMIM][Cl] is weak, and the hydrogen bonds formed by 2-thiophenecarboxylic acid, 2-aminophenyl phenyl sulfone with [DMIM][Cl] are relatively strong. The analysis of intermolecular hydrogen bond interactions verified the mechanism underlying the excellent extraction performance for specific OSMCs by the selected ILs.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2017
·
IF 3.752
Longfei Tang,Shiwei Wang,Jifeng Guo,Xiuxiang Tao,Huan He,Li Feng,Songjiang Chen,Ning Xu
The removal mechanism of sulfoether in coal by microwave with peroxyacetic acid, was determined by evaluating changes in sulfur containing compounds after desulfurization by XANES and GC/MS. The highest occupied molecular orbital composition , the electrostatic potential distribution, and the sulfur containing bond dissociation energy (BDE) of model compounds molecules were also determined to support the experimental results. Results showed that sulfoether was easily oxidized to corresponding sulfoxide or sulfone in treated samples. Although benzyl sulfides were more readily oxidized than disulfides , the latter was easier to remove due to the higher breaking probability of the S S bond. The sulfur atoms within sulfur ether in coal are the active sites for electrophilic reaction . As sulfur atoms were oxidized, the sulfur containing BDEs decreased considerably and the dipole moments of sulfoether molecules increased. These findings suggest that the removal efficiency of sulfoether in coal may be improved by moderate and selective oxidation under microwave treatment.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Asia-Pacific Journal of Chemical Engineering
·
2023
·Vol. 18
·期 4
·e2908
·
IF 1.8
Tao Ge,Yuqing Wang,Jingyao Xu,Dinghao Liu,Yulu Wei,Zhaohui Wang
The microwave absorption properties of dielectrics determine the promotion degree of microwave energy to chemical reaction. The wave-absorbing characteristics of organic sulfur compounds in high-sulfur coking coal need to be studied to improve the efficiency of microwave desulfurization of coal. In this study, the imaginary part of complex dielectric constants ( ε′′ ) and dielectric loss tangent (tan σ ) of benzene mercaptan, difurfuryl disulfide, and benzothiophene were characterized. The dipole moment, molecular configuration, and frontier molecular orbital energy of organic sulfur compounds were simulated and calculated under the different external energy fields. The migration law of mercaptan, sulfide, and thiophene in coal in microwave field were analyzed. The results show that the ε'′ and tan σ of benzothiophene slightly changed with the change in microwave frequency in the frequency range of 500–2500 MHz, and the microwave absorption properties are weaker than those of benzene mercaptan and difurfuryl disulfide. Therefore, difurfuryl disulfide and benzene mercaptan molecules are more active in the microwave field than benzothiophene. The sulfur components in benzene mercaptan and difurfuryl disulfide can dissociate in the form of small inorganic sulfur molecules of carbon sulfides and disulfides, respectively. After microwave irradiation, the relative content of mercaptan and thioether in coal was decreased, whereas the relative content of thiophene remained almost unchanged.
研究领域:
能源化学
·
量子化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2024
·
IF 5.3
Tao Ge,Bingyi Zhou,Jingyao Xu,Yulu Wei
Ionic liquids (ILs) were selected and applied to investigate the best coal desulfurization through orthogonal tests. FTIR, XPS, SEM and contact angle tests were used to characterize the effect on the physical and chemical structures in coal for revealing the coal desulfurization mechanism by ILs-H 2 O 2 system. The orthogonal test results showed that reaction temperature and reaction time were the main influencing factors for the desulfurization rates of coal in the ILs-H 2 O 2 system, and the ILs synergy could effectively improve the desulfurization rates of H 2 O 2 . The maximum coal desulfurization rates of [BMIM][HSO 4 ], [BMIM][OTF], and [BMIM][BF 4 ] ionic liquids were 30.7%, 30%, and 33.2%, respectively. The results indicated that the alkyl groups in coal were oxidized and the contents of oxygen-containing functional groups such as hydroxyl and carbonyl increased. Coal surface underwent swelling, the internal pores increased and new pores and cracks were generated. The wettability of coal improved substantially. In addition, the physical structures changes in coal facilitated the contact between the extractant and the sulfur-containing structures. The contents of thiols and sulfides in coal significantly decreased and were oxidized to sulfoxides and sulfones, with some further oxidized to soluble sulfites or sulfates. Thus achieving removal from coal.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）