ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2023
·Vol. 415
·期 10
·1889-1896
·
IF 4.3
Li Shuofan,Wu Jianxun,Zhang Weilai,Jiang Yue,Hu Miao,Chung Keng H.,Shi Quan
Thiophenes and sulfides are the dominant sulfur-containing compounds in petroleum and have been widely of concern in the fields of petroleum refining and geochemistry. In this study, a novel approach was developed for selective separation and characterization of petroleum-derived thiophenic and sulfide compounds. Thiophenic compounds were selectively converted to sulfonates in the presence of vitriolic acid and can be characterized by negative ion electrospray mass spectrometry. Thiophenic sulfonates were further separated from the oil by silica chromatography and enabled the molecular characterization of sulfides in the residual oil. Various model sulfur compounds and a vacuum gas oil were used to validate the method; thiophenic and sulfide biomarker compounds in a well-documented crude oil were selectively characterized. The results indicate that the approach is feasible for molecular characterization of thiophenic and sulfide compounds, which is complementary to recently developed methods for separation and/or ionization of sulfur compounds in petroleum. Graphical Abstract
研究领域:
化学
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地质学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2021
·
IF 6.609
Guang Miao,Peng Chong,Cuiting Yang,Zewei Liu,Hao Yu,Lei Dong,Guoqing Li,Jing Xiao
The demand for heterocyclic sulfur compounds is increasingly in fine chemical industry, where the thiophenic sulfur impurities in fuels can be a potential recyclable feedstock. In this work, the catalytic upgrading of thiophenic sulfur compounds over a silver-modified MoO 3 catalyst under ambient conditions was reported. Br 2 and H 2 O 2 /HBr were used to convert thiophenic compounds in alkane and alcohol solutions. The conversion of various thiophenic compounds (thiophene, benzothiophene and dibenzothiophene) to the corresponding bromides reached up to 81.6 ~ 99.8%. The bromination path undergoes electrophilic substitution mechanism, and the transformation of mono- to dibromides is identified as the rate-determining step. The introduction of MoAg 2 O 4 phase on MoO 3 is rationalized to boost the conversion of mono-bromothiophene, which results in the selectivity of 2,5-dibromothiophene increased from 10% to over 50%. The optimized silver loading was 10% due to its high thiophene conversion and selectivity of dibromides. Silver modification of MoO 3 rods not only stabilized the textural property of catalysts but also improved its bromination activity compared to the bulk MoO 3 indicated by SEM and FTIR characterization. Density functional theory (DFT) calculation suggested that the formation of 2-bromothiphene and 2,5-dibromothiophene were preferred on the MoO 3 (111) and MoAg 2 O 4 (111) sites, respectively. The catalytic upgrading approach paves the way for the efficient utilization of thiophenic sulfur impurities in fuels to their value-added under mild conditions.
研究领域:
化学工程
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2022
·Vol. 139
·期 26
·e52431
·
IF 3.057
Haohao Ding,Zhonglin Luo,Biaobing Wang
A phosphorus/sulfur-containing compound (sulfonylbis(3,1-phenylene) bis(diphenyl-phosphinate), named as SBPDPP) is designed and synthesized by nucleophilic substitution reaction between diphenylphosphinyl chloride and 4,4-dihydroxydiphenylsulfone, and its chemical structure is verified by Fourier transform infrared, 1 H and 31 P nuclear magnetic resonance. The incorporation of SBPDPP accelerates the curing process but decreases the glass transition temperature and the crosslinking density of the epoxy resin (EP). The cured EP with 6 wt% SBPDPP passes UL-94 V0 rating and gives limited oxygen index value of 38.8%, meanwhile maintaining 90% of the transmittance of the pure EP. Its peak heat release rate, total heat release, total smoke production, and total smoke rate are reduced by 40.8%, 42.0%, 26.3%, and 21.9% in comparison with the pure EP, demonstrating that the SBPDPP improved simultaneously the fire safety and smoke suppression. The comprehensive analysis of the char residues after cone calorimeter test and the volatile gasses during the pyrolysis demonstrates that the SBPDPP exerted dual flame retardant effect in the gas and condensed phase. The cured FREPs have promising applications that requiring flame retardancy and maintaining transparency.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
PLoS Pathogens
·
2024
·Vol. 20
·期 7
·e1012410
·
IF 5.5
Xiaojun Zhong,Fuwen Liu,Tianqi Liang,Ranran Lu,Mengting Shi,Xiujuan Zhou,Menghua Yang
One of the greatest challenges encountered by enteric pathogens is responding to rapid changes of nutrient availability in host. However, the mechanisms by which pathogens sense gastrointestinal signals and exploit available host nutrients for proliferation remain largely unknown. Here, we identified a two-component system in Vibrio parahaemolyticus , TtrRS, which senses environmental tetrathionate and subsequently activates the transcription of the ttrRS - ttrBCA-tsdBA gene cluster to promote V. parahaemolyticus colonization of adult mice. We demonstrated that TsdBA confers the ability of thiosulfate oxidation to produce tetrathionate which is sensed by TtrRS. TtrRS autoregulates and directly activates the transcription of the ttrBCA and tsdBA gene clusters. Activated TtrBCA promotes bacterial growth under micro-aerobic conditions by inducing the reduction of both tetrathionate and thiosulfate. TtrBCA and TsdBA activation by TtrRS is important for V. parahaemolyticus to colonize adult mice. Therefore, TtrRS and their target genes constitute a tetrathionate-responsive genetic circuit to exploit the host available sulfur compounds, which further contributes to the intestinal colonization of V. parahaemolyticus .
Access to host nutrients is regarded as a critical step for the pathogen infection. However, the human gastrointestinal tract is colonized by an enormous number of microbes, which limits pathogens’ access to nutrient supplies. Sulfur is one of the most abundant elements on Earth and is also essential to all living organisms. The mechanisms by which bacteria, especially intestinal pathogens, regulate the bioavailability of utilizable sulfur in the host are poorly understood. Here, we characterized a tetrathionate-responsive genetic circuit, which was involved in the utilization of sulfur compounds including tetrathionate and thiosulfate in V. parahaemolyticus , and thus contributed to the bacterial intestinal colonization. Our study provides new insight into the ability of bacterial pathogens to sense gastrointestinal signals and exploit host nutrients for their colonization, which contributes to a better understanding of the pathogenesis of enteric pathogens.
研究领域:
微生物学
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病原生物学
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分子生物学
✓ 已验证
DOI
PubMed
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2012
·Vol. 109
·期 9
·3492-3497
·
IF 9.681
Xufang Duan,Eric Block,Zhen Li,Timothy Connelly,Jian Zhang,Zhimin Huang,Xubo Su,Yi Pan,Lifang Wu,Qiuyi Chi,Siji Thomas,Shaozhong Zhang,Minghong Ma,Hiroaki Matsunami,Guo-Qiang Chen,Hanyi Zhuang
Odorant receptors (ORs) in olfactory sensory neurons (OSNs) mediate detection of volatile odorants. Divalent sulfur compounds, such as thiols and thioethers, are extremely potent odorants. We identify a mouse OR, MOR244-3, robustly responding to (methylthio)methanethiol (MeSCH2SH; MTMT) in heterologous cells. Found specifically in male mouse urine, strong-smelling MTMT [human threshold 100 parts per billion (ppb)] is a semiochemical that attracts female mice. Nonadjacent thiol and thioether groups in MTMT suggest involvement of a chelated metal complex in MOR244-3 activation. Metal ion involvement in thiol–OR interactions was previously proposed, but whether these ions change thiol-mediated OR activation remained unknown. We show that copper ion among all metal ions tested is required for robust activation of MOR244-3 toward ppb levels of MTMT, structurally related sulfur compounds, and other metal-coordinating odorants (e.g., strong-smelling trans-cyclooctene) among >125 compounds tested. Copper chelator (tetraethylenepentamine, TEPA) addition abolishes the response of MOR244-3 to MTMT. Histidine 105, located in the third transmembrane domain near the extracellular side, is proposed to serve as a copper-coordinating residue mediating interaction with the MTMT–copper complex. Electrophysiological recordings of the OSNs in the septal organ, abundantly expressing MOR244-3, revealed neurons responding to MTMT. Addition of copper ion and chelator TEPA respectively enhanced and reduced the response of some MTMT-responding neurons, demonstrating the physiological relevance of copper ion in olfaction. In a behavioral context, an olfactory discrimination assay showed that mice injected with TEPA failed to discriminate MTMT. This report establishes the role of metal ions in mammalian odor detection by ORs.
研究领域:
神经科学
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分子生物学
✓ 已验证
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2013
·
IF 2.853
Qianli Wang,Lecheng Lei,Jingke Zhu,Bin Yang,Zhongjian Li
In this work, three 4-dimethylaminopyridinium-based ionic liquids (ILs), N-ethyl-4-dimethylaminopyridinium dicyanamide ([C24DMAPy][N(CN)2]), N-butyl-4-dimethylaminopyridinium dicyanamide ([C44DMAPy][N(CN)2]) and N-hexyl-4-dimethylaminopyridinium dicyanamide ([C64DMAPy][N(CN)2]), were synthesized and then demonstrated to be efficient for aromatic sulfur compounds extraction from fuels. The mutual solubility evaluating results indicated that 4-dimethylaminopyridinium-based ILs hardly dissolved in the fuels, while the solubility of 97# gasoline in ILs varies from 7.0 wt % for [C24DMAPy][N(CN)2] to 12.4 wt % for [C64DMAPy][N(CN)2] and the solubility of 0# diesel in ILs varies from 6.7 wt % for [C24DMAPy][N(CN)2] to 9.7 wt % for [C64DMAPy][N(CN)2]. Also, the sulfur partition coefficient was evaluated. In the case of model gasoline, the thiophene (TS) partition coefficient in model gasoline varies from 0.885 for [C24DMAPy][N(CN)2] to 1.218 for [C64DMAPy][N(CN)2]. In the case of model diesel, 4-dimethylaminopyridinium-based ILs exhibit a relatively higher sulfur partition coefficient, compared to alkyl modified pyridinium-based ILs. 1H NMR results confirmed that the high aromatic π-electron density of the dimethylaminopyridinium cation was the main reason for the good extraction performance. 1H NMR results also confirmed the KN sequence for each IL ([C24DMAPy][N(CN)2] < [C44DMAPy][N(CN)2] < [C64DMAPy][N(CN)2]) is mainly due to the sulfur compounds and ILs structures. Furthermore, the extractive selectivity results indicated a more preferable extraction of TS than toluene with 4-dimethylaminopyridinium-based ILs. To have a better evaluation of the overall sulfur extraction performance, the three 4-dimethylaminopyridinium-based ILs were compared to other typical ILs (e.g., pyridinium-based ILs and imidazolium-based ILs), which suggested our synthesized 4-dimethylaminopyridinium-based ILs exhibited good balance between mutual solubility and the sulfur partition coefficient. ILs after use were regenerated by a water dilution process. Based on these results, 4-dimethylaminopyridinium-based ILs can be used as potential extractants for EDS processes.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
SEPARATION SCIENCE AND TECHNOLOGY
·
2015
·
IF 1.171
Jessica Juweriah Ibrahim,Shurong Gao,Ahmed A. Abdeltawab,Salem S. Al-Deyab,Liang Yu,Guangren Yu,Xiaochun Chen,Xingyue Yong
The inability of traditional hydrodesulfurization (HDS) to effectively remove aromatic sulfur compounds such as thiophene (TS) and dibenzothiophene (DBT) has called for alternative methods to be studied, among which extractive desulfurization using ionic liquids (ILs) has attracted increasing interest. In this work, we prepared a new IL, 1-butyl-3-methylimidazolium dicyano(nitroso)methanide ([C4mim][dcnm]), and investigated its extractive desulfurization for both model oils and real FCC gasoline, where model diesel fuel was composed of n-hexane and droplets of DBT and model gasoline was composed of n-hexane, toluene and droplets of TS. Other three [dcnm]-based ILs, 1-ethyl-3-methylimidazolium dicyano(nitroso)methanide ([C2min][dcnm]), N-ethyl-N-methylpyrrolidinium dicyano(nitroso)methanide ([C2mpyr][dcnm]), and N-butyl-N-methylpyrrolidinium dicyano(nitroso)methanide ([C4mpyr][dcnm]), were also comparatively investigated. These [dcnm]-based ILs have low viscosity which favors the mass transfer and reduces the extractive equilibrium time, also are fluorine-free which avoids the corrosion by hydrogen fluoride from anion decomposition that occurs generally in fluorine-containing ILs. The desulfurization ability follows the order [C4min][dcnm] > [C4mpyr][dcnm] > [C2min][dcnm] > [C2mpyr][dcnm]. Typically, [C4min][dcnm] is capable of removing 66% DBT and 53% TS from their respective model oils after one cycle (initial 500 ppm S, 25°C, 15 min, mass ratio of IL:oil 1:1), and < 10 ppm S-content can be obtained after 4 cycles. It was observed interestingly that the S-content in real FCC gasoline can be reduced from initial 250 ppm to < 30 ppm after 6 cycles using [C4min][dcnm] as extractive reagent, which is better than some previous results for real feedstocks. Mutual solubility, extractive temperature, IL:oil mass ratio, multiple extraction, initial S-content, and regeneration were also studied. These dcnm-based ILs are competitive extractive reagents compared with some other ILs to remove those aromatic S-compounds from fuel oils.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Asia-Pacific Journal of Chemical Engineering
·
2020
·Vol. 16
·期 1
·e2581
·
IF 1.06
Tao Ge,Fen Li,Yang Li
The present study aims to reveal the influence mechanism of organic sulfur structures and microwave frequency on its dielectric property and establish the relationship between the dielectric properties of organic sulfur components in coal and the efficiency of microwave desulfurization. Results showed that the different polarization mechanisms of organic sulfur compounds lead to the real part of complex permittivity decreased initially and then increased with increasing frequency. At the same time, the real parts of the complex permittivity of mercaptan and thioether compounds were higher than that of thiophene, which were caused by their different structures. As the frequency increased, the loss tangent, microwave penetration depth, and absorption index showed decline in oscillation. The loss tangent was mainly related to the polarization mechanism; both polarization mechanism and microwave wavelength had effect on the changes of microwave penetration depth and absorption index. Mercaptan and thioether compounds were more effective at converting microwave energy into heat energy. After microwave processing, the relative content of mercaptan (thioether) in GZ, CQ, and SX coals decreased from 37.38%, 36.93%, and 40.02% to 27.34%, 29.26%, and 26.67% and of thiophene increased from 47.61%, 53.35%, and 49.54% to 58.76%, 59.09%, and 60.38%.
研究领域:
能源科学
·
化学工程
✓ 已验证
DOI
高影响因子
Foods
·
2021
·Vol. 10
·期 7
·1444
·
IF 4.35
Lulu Ma,Cheng Yang,Xin Jiang,Qun Wang,Jian Zhang,Lianfu Zhang
The effects of some sulfur-containing compounds on the isomerization and degradation of lycopene, phytofluene, and phytoene under different thermal treatment conditions were studied in detail. Isothiocyanates such as allyl isothiocyanate (AITC) and polysulfides like dimethyl trisulfide (DMTS) had the effect on the configuration of PTF (phytofluene), PT (phytoene), and lycopene. The proportion of their naturally occurringZ-isomers (Z1,2-PTF and 15-Z-PT) decreased and transformed into other isomers including all-trans configuration, whileZ-lycopene increased significantly after thermal treatment, especially for 5-Z-lycopene. The results showed that increase in heating temperature, time, and the concentration of DMTS and AITC could promote the isomerization reaction effectively to some extent. In addition, 15-Z-PT and the newly formedZ4-PTF were the predominant isomers in tomato at the equilibrium. Unlike the lycopene, which degraded significantly during heat treatment, the isomers of PTF and PT were stable enough to resist decomposition. Moreover, the isomerization of three carotenoids was enhanced, and the bioaccessibility of lycopene increased significantly with the addition of shii-take mushroom containing sulfur compounds, while there was no positive effect observed in that of PTF and PT.
研究领域:
植物学
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食品科学
·
营养学
✓ 已验证
DOI
高影响因子
JOURNAL OF INSECT SCIENCE
·
2015
·Vol. 15
·期 1
·
IF 1.025
Shi Jizhe,Liu Xinchao,Li Zhen,Zheng Yuanyuan,Zhang Qingwen,Liu Xiaoxia
The aim of this research was to evaluate acute toxicity of the essential oil of leaves of Chinese chives, Allium tuberosum Rottler ex Spreng (Asparagales: Alliaceae) and its major constituents against Apolygus lucorum Meyer-Dür (Hemiptera: Miridae). The essential oil of A. tuberosum leaves was obtained by hydrodistillation and analyzed by gas chromatography and gas chromatography-mass spectrometry. The major constituents of the oil were sulfur-containing compounds, including allyl methyl trisulfide (36.24%), diallyl disulfide (27.26%), diallyl trisulfide (18.68%), and dimethyl trisulfide (9.23%). The essential oil of A. tuberosum leaves exhibited acute toxicity against Ap. lucorum with an LD 50 value of 20.03 μg per adult. Among the main compounds, diallyl trisulfide (LD 50 = 10.13 μg per adult) showed stronger acute toxicity than allyl methyl trisulfide (LD 50 = 21.10 μg per adult) and dimethyl trisulfide (LD 50 = 21.65 μg per adult). The LD 50 value of diallyl disulfide against Ap. lucorum was 28.10 μg per adult. The results indicated that the essential oil of A. tuberosum and its major constituents may have a potential to be developed as botanical insecticides against Ap. lucorum.
研究领域:
植物学
·
昆虫学
·
农药科学
✓ 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
PROCEEDINGS OF THE COMBUSTION INSTITUTE
·
2014
·
IF 3.828
Shuai Liu,Mengmeng Wei,Yu Qiao,Zhenle Yang,Ben Gui,Yun Yu,Minghou Xu
This study reports the release of five sulfur-containing odorants (H 2 S, SO 2 , COS, CS 2 and CH 3 SH) during the pyrolysis of sewage sludge. Pyrolysis experiments using both raw sewage sludge and seven sludge samples loaded with various organic sulfur compounds were performed to determine the effects of the type of organic sulfur on the release of sulfur-containing gases. It was observed that the formation of H 2 S, the predominant odorant, significantly increases at temperatures above 150 °C. Aliphatic and aromatic sulfur compounds were found to be the two main organic sulfur sources for the release of sulfur-containing gases. The release of sulfur-containing gases from aliphatic sulfur greatly increases at 250 °C, whereas significant sulfur-containing gases are released from aromatic sulfur at relatively high temperatures of 350–450 °C. It was also observed that the presence of sulphonic acid and thiophene in sludge does not significantly affect the release of sulfur-containing gases.
研究领域:
环境科学
·
能源工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）