ENERGY
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2024
·
IF 9
Yuxuan Xing,Jingchun Huang,Zhenqi Wang,Wei Hu,Minghou Xu,Yu Qiao
This study focused on the effect of oxygen (0–15 %) and 5 % CaO addition on the organic-S control and transformation behavior during pyrolysis (400–600 °C) of sludge under the conditions relevant to smoldering combustion. The results show that oxygen inhibits the total emission of gaseous sulfur (decreased by 25.6–36.9 %). At low temperatures (<500 °C), oxygen enhances the oxidation of aliphatic-S, aromatic-S/thiophene-S, and sulfide-S, leading more sulfur retains in the form of sulfone-S and sulfate-S in char products, also migrates to water-soluble products (especially sulfone-S). At high temperatures (>500 °C), the formed sulfur species in char products mainly further decompose into water-soluble sulfone-S, and partially generate SO 2 . After the addition of CaO during oxidative pyrolysis, the synergistic promotion effect on the sulfur fixation in char products is found, mainly due to the generation of more amount of stable sulfone-S and sulfate-S in char products. This leads to a decrease in gaseous sulfur by 12.4–14.6 % and an increase in sulfur content of char products by 31.3–202.9 %.
研究领域:
环境科学
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能源工程
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产品关联
DOI
高影响因子
PLoS One
·
2019
·Vol. 14
·期 1
·e0208125
·
IF 2.776
Chuanchuan Cai,Tao Ge,Mingxu Zhang
Coking coal is geologically scarce resource and most of them cannot be directly used in steel making due to their higher sulfur content. One desulfurization method that has great potential for massive application is microwave desulfurization, which removes the relatively stubborn organic sulfur under mild conditions. The dielectric properties of coals determine the efficiency of the microwave energy absorption. The key to describing the mechanism of microwave desulfurization and further improvement of the desulfurization efficiency is the dielectric response of organic sulfur compounds in coal to microwave. This study focuses on existing formand microwave response of organic sulfur components of three typical coking coal in China. Resultsshowed that the major organic sulfur in selected coals is thiophene which has a stable structure and is the most difficult to be removed. Several dielectric peaks (dielectric loss)andsignificant differencesofeach selected coal samples are observed. The microwave absorption peaks of the model sulfur compounds are identified to be within 9-11GHz. The real parts of the relative dielectric constants (hereinafter referred to as ε ′) shows a decreasing trend as: diphenyl sulfoxide > diphenyl sulfone > diphenyl sulfide > dibenzothiophene > Octadecane thiol. Response to microwaveare observed to be distinctively different between sulfur-containing and sulfur-free model compounds. The dielectric polarization of mixture (coal mixed with model sulfur compounds) is greater than pure coal. Meanwhile the higher the sulfur content of the coal, the greater the ε ′ is. Sulfur componentsin coal can significantly influence its polarization.
研究领域:
能源科学
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材料科学
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DOI
PubMed
高影响因子
FUEL
·
2023
·
IF 7.4
Qihuang Huo,Yahui Wang,Huijun Chen,Yu Feng,Lina Han,Weiren Bao,Liping Chang,Jiancheng Wang,Kechang Xie
It is a win–win strategy to prepare mercury sorbents from low-cost high-sulfur raw materials. In part 1, mercury sorbents with excellent performance were prepared from high inorganic sulfur coal through KOH activation. However, this method does not work for high organic sulfur coal. In this work, a two-step preparation method is developed to prepare mercury sorbents from high organic sulfur coal. The first step is the co-pyrolysis/carbonization of Fe 2 O 3 and coal, during which organic sulfur in coal is converted into FeS x . XPS shows that the percentage of S x 2– /S on the surface of the carbonized samples gradually increases from 5.4% to 22.2% with the m(Fe):m(S o ) ratio from 0:4 to 5:4. The second step is KOH activation, and it converts FeS x into various S species, including C-S, S 0 , S 2 2− and S 2− . Among the prepared mercury sorbents, LF+3Fe/4S-A (m(Fe):m(S o ) = 3:4) shows the best mercury removal performance, and its mercury removal efficiency remains above 84% for 120 min under N 2 +O 2 at 120 °C. The Hg-TPDD and XPS results indicate that S*, including C-S, S 0 and S 2 2− , are the major active sites for mercury removal rather than Fe element, and HgS is the main existing form of mercury on the used sorbents. Besides LF coal, this two-step process is also applicable to other high organic sulfur coals (such as LL coal, WJZ coal, and SY coal) and high-sulfur petroleum coke.
研究领域:
环境科学
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能源材料
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DOI
高影响因子
Catalysts
·
2023
·Vol. 13
·期 2
·410
·
IF 3.9
Shaokang Wang,Hang Xu
The intermediate di-[EMIM]Cl was synthesized from methyl imidazole and 1,4-dichlorobutane and then reacted with cobalt chloride at 105 °C to prepare a bi-[EMIM]CoCl3ionic liquid catalyst. The di-[EMIM]CoCl3catalyst coupled with oxone to remove sulfur-containing organics in octane. The di-[EMIM]CoCl3catalyst was characterized by HNMR, FTIR, TG, and SEM–EDS. The dibenzothiophene (DBT) was dissolved in octane to prepare a model oil with an initial sulfur content of 500 ppm. Six grams of the model oil was added. The results showed that the optimal dosages of di-[EMIM]CoCl3, oxone (20 wt%), and [BMIM]BF4extractant were 1 g, 2 g, and 2 g, respectively. At the optimum temperature of 45 °C, 100% of sulfur was removed after 40 min. After di-[EMIM]CoCl3was recycled five times, the sulfur removal percentage remained above 91%. The sulfur removal percentages for different sulfur-containing organics followed the order of dibenzothiophene (DBT) > benzothiophene (BT) > 4,6-dimethyldibenzothiophene (4,6-DMDBT). The oxidation product was determined to be DBTO2by GC–MS analysis, and the oxidation mechanism was discussed. The active oxygen atoms of oxone oxidized DBT to form DBTO, and then persulfate oxidized DBTO to DBTO2via an identical oxidation mechanism.Keywords:dicationic ionic liquids;cobalt chloride;oxone;desulfurization;catalytic oxidation
研究领域:
化学工程
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环境科学
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DOI
高影响因子
ATMOSPHERIC ENVIRONMENT
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2022
·
IF 5.755
Jingrong He,Li Li,Yunxiang Li,Mei Huang,Ying Zhu,Shihuai Deng
In this work, six aromatic organosulfates (phenyl, 2-/3-/4-methylphenyl, benzyl and phenethyl sulfates) were synthesized, with the purpose to obtain the standards and apply them to quantify the organosulfates in ambient aerosols. The purity of the synthesized organosulfates was determined by high performance liquid chromatography/ultraviolet detector (HPLC/UV). Meanwhile, the organosulfate standards and atmospheric PM 2.5 samples were measured by high performance liquid chromatography/electrospray ionization/tandem mass spectrometry (HPLC/ESI/MS/MS). The characteristic ion fragments were phenolate anion m/z 93 for phenyl sulfate, creylate anion m/z 107 for methylphenyl sulfate, sulfate radical anion ·SO 4 − ( m/z 96) for benzyl sulfate, and hydrogen sulfate anion HSO 4 − ( m/z 97) for phenethyl sulfate. The characteristic fragment ions used for quantification can improve the identification of target compounds in chromatograms, obtain lower detection limits, and will minimize analytical errors caused by the introduction of surrogates. The concentrations of phenyl, methylphenyl, benzyl and phenethyl sulfates in winter PM 2.5 in Wenjiang District of Chengdu were 0.58 ± 0.56, 2.37 ± 3.59, 1.79 ± 3.51, 0.04 ± 0.08 ng/m 3 , respectively.
研究领域:
环境科学
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分析化学
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产品关联
DOI
高影响因子
RSC Advances
·
2022
·Vol. 12
·期 18
·11262-11271
·
IF 4.036
Qiong Zhu,Jinhua Wang,Si Chen,Hongquan Fu,Juan Zhang,Hejun Gao,Yunwen Liao
By controlling the species of the organic sulfur source, CdS samples were produced with different photocatalytic performances by a low-temperature solvothermal method. Different species of the organic sulfur source were chosen as the coordination agent to control the interactions in the crystal growth process. Among them, thioacetamide was the best coordination agent. The hydrophobic chain could be good for reducing the resistance of charge transfer, and increasing the rate of surface charge transfer and the lifetime of the photoexcited electrons. Benefiting from the hydrophobic chain, CdS shows an excellent photocatalytic hydrogen evolution rate of 943.54 μmol h−1 g−1 and a rhodamine B photocatalytic degradation rate of 99.1% in 60 min, which is superior to the photocatalysis of pure CdS prepared by many other methods.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
PubMed
高影响因子
FUEL PROCESSING TECHNOLOGY
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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
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煤化工
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环境化学
·
应用化学
·
清洁燃料技术
✓ 已验证
DOI
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Jiahang Zhou,Minqiang Xia,Lingui Hu,Yunbo Li
Herein, a novel method is presented for the in situ growth of gold nanofilms with branched structures in the presence of organosulfur. The key feature in this approach is the Rayleigh instability of ultrathin gold nanowires (AuNWs) without oleylamine (OAm), which allows the ultrathin AuNWs to decompose into gold nanoparticles (AuNPs) and the AuNPs to in situ grow into branched structures for high-performance stability and electrical conductivity. The sheet resistance of the gold nanofilms initially sharply decreased, whereas it subsequently slightly increased with the concentration of CS(NH2)2 until it exceeded the optimal range. After undergoing a 10 min heat treatment at 150 °C, the sheet resistance of the nanofilms was further reduced to 18 Ω/sq, which could be maintained for more than five months. The internal structure becomes fully grown and denser, forming a branched structure after heat treatment. Only certain organosulfurs can improve the electrical properties of the gold nanofilms, and the mechanism of organosulfur in the in situ growth of gold nanofilms with branched structures has also been presented. Overall, this novel method provides a straightforward and convenient approach to obtaining gold nanomaterials with branched structures, holding great potential promise for applications in flexible electronics, catalysis, and energy fields.
研究领域:
材料科学
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纳米技术
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电子工程
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产品关联
DOI
PubMed
高影响因子
ACS Omega
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2022
·
IF 4.132
Fei Gao,Zhe Jia,Ya-fei Shan,Yifei Teng,Ying-di Li,Xin-ge Pu
The low-temperature oxidation spontaneous combustion of coal was caused by the active groups in its structure. The oxidation mechanism of carbon and oxygen functional groups in coal had been extensively studied, but there were few reports on the study of sulfur functional groups initiating the coal spontaneous combustion. To investigate the influence of organic sulfur functional groups on the spontaneous combustion of high-sulfur coal and explore its transformation characteristics, the low-temperature oxidation experimental system was used to study the spontaneous combustion tendency of coal with similar metamorphic degrees and different organic sulfur contents. The variations of element forms and organic sulfur functional groups were analyzed by X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy during low-temperature oxidation of coal and model compounds. The results showed that the forms of organic sulfur in coal mainly included mercaptans, thioethers, thiophenes, sulfones (sulfoxides), and sulfates, and the low-temperature oxidation of coal was not only related to the content of organic sulfur but also related to its type. The coal samples, which possess a low content of total sulfur and a small proportion of active organic sulfur groups such as mercaptans and thioethers, had a lower concentration of indicator gas and a smaller tendency to coal spontaneous combustion. After low-temperature oxidation, the content of mercaptan, thioether, thiophene, methyl(methylene), and pyridine in coal decreased, and the content of oxygen-containing groups such as sulfone (sulfoxide), sulfate, carboxyl, and nitrogen oxide increased. The elements of S, C, and N all changed to a high-valent state. In the oxidation reaction of model compounds, mercaptans were more reactive than thiophenes in the low-temperature region, and the oxidation of thiophene could direct form sulfone (sulfoxide), while the oxidation of mercaptan formed disulfide first. It is speculated that low-valence sulfur migrated to a high-valent state by providing sulfhydryl radicals (•SH) and sulfur radicals (C–S•) combined with active oxygen atoms. After the low-temperature oxidation reaction of model compounds, some organic sulfur existed in the form of aromatic sulfur or sulfur oxides and a small part of sulfur escaped as SO2 and H2S gases in the solid oxidation product.
研究领域:
矿业工程
·
化学工程
✓ 已验证
DOI
高影响因子
Journal of Cleaner Production
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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
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环境科学
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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
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化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2025
·
IF 8.4
Lidan Cao,Yupei Chai,Yingxing Zhang,Jielan Zhang,Junhong Wang,Rui Wu
Sulfur-containing gases produced during the utilization of petroleum fuels are the main cause of air pollution. To remove organic sulfur-containing compounds from simulated gasoline, magnetic hydrophobic Cu + -containing SBA-15 mesoporous molecular sieves (PMS-Cu + ) were prepared by magnetization of the sample, loading and reduction of copper ion and hydrophobic treatment of the sample. The composition and structure of the synthesized composites were characterized by XRD, FTIR, SEM, TEM, and XPS, which proved the successful preparation of the adsorbent PMS-Cu + . In addition, it was also investigated on the adsorption capacity of the prepared adsorbent for organic sulfur compounds in simulated gasoline and the factors affecting the desulfurization performance. Through the kinetic study of the adsorption process, it was found that the process conformed to the quasi-secondary kinetic properties, the adsorption process was dominated by chemical adsorption, and internal and external diffusion co-determined the adsorption rate. Moreover, the apparent activation energy of the adsorption process was 50.83 kJ/mol.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）