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FUEL PROCESSING TECHNOLOGY · 2015 · IF 3.352

Adsorption of benzothiophene from fuels on modified NaY zeolites

Hui-Ying Sun,Lin-Ping Sun,Fei Li,Long Zhang

The adsorption of benzothiophene from fuels on NaY zeolites modified with 0.09   M NaOH aqueous solution was investigated. The sulfur removal reached to 99.9%, and the adsorption capacity was 1.65   mg   benzothiophene/g of the modified adsorbent. The results of the scanning electron microscopy, X-ray diffraction, X-ray fluorescence, and N 2 adsorption–desorption isotherms analyses show that mesopores appeared on the surface of NaY-0.09 adsorbent and the intrinsic crystallinity was preserved after the modification. Py-IR and NH 3 -TPD analyses indicated that the adsorption of benzothiophene occurred on the weak Lewis acid sites on the adsorbent. Both an increase in the number of the weak Lewis acid sites and the formation of mesopores on NaY-0.09 adsorbent improved its desulfurization activity.

研究领域: 化学工程 · 材料科学
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FUEL PROCESSING TECHNOLOGY · 2014 · IF 3.019

Acylation desulfurization of heavy cracking oil as a supplementary oil upgrading pathway

Xing-Yu Chen,Jia-Jun Gao,Ying-Zhou Lu,Hong Meng,Chun-Xi Li

Acylation reaction is used to enhance the basicity and polarity of the thiophenes and thus promote their adsorptive removability by Lewis acid, forming an acylation desulfurization (ADS) process for the refractory sulfurs. The ADS performance of six acylating reagents (ARs) was assessed for heavy cracking oil and light oil at 303   K with AlCl 3 as the catalyst, and the influence of ADS on the oil quality was also studied. The results show that ADS is efficient to remove the thiophenes, but less efficient for the removal of mercaptans and thioethers in light oil. S-removal rate of 90.9% was achieved for heavy cracking oil with acetyl bromide (AB)-AlCl 3 (AB/S   =   2/1; AlCl 3 /S   =   5/1) in 0.5   h. The coexistent olefins and aromatics can slightly deteriorate the ADS performance and influence the oil properties. ADS might be used as a promising sulfur separating strategy for the cracking oil.

研究领域: 化学工程 · 石油加工
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JOM · 2020 ·Vol. 72 ·期 9 ·3195-3203 · IF 2.054

Recovery of Lead from Spent Lead Paste by Pre-desulfurization and Low-Temperature Reduction Smelting

Xie Boyi,Yang Tianzu,Liu Weifeng,Zhang Duchao,Chen Lin

The treatment of spent lead paste is essential for the recycling of spent lead-acid batteries. In this study, we propose a facile route for the recovery of lead from spent lead paste by pre-desulfurization followed by low-temperature reduction smelting. The effects of two desulfurization methods, i.e., high-pressure and normal-pressure processes, on the desulfurization efficiency of spent lead paste were compared. The high-pressure process was found to be more effective than the normal-pressure process; 99.1% of sulfur was removed under the high pressure conditions with NaOH excess of 1.1 at 150°C for 30 min. Moreover, a part of PbO 2 reacted with PbO to form Pb 3 O 4 . Afterwards, the desulfurized residue, mainly consisting of Pb 3 O 4 and PbO 2 , was directly used in low-temperature reduction smelting, and the optimum smelting conditions were determined to be: starch/Pb-residue mass ratio = 1/6.3; Na 2 O/Pb-residue mass ratio = 1/15; B 2 O 3 /Pb-residue mass ratio = 1/7.5; smelting temperature 700°C; and smelting duration 90 min. The lead recovery under the optimum conditions was as high as 93%. Scanning electron microscope images of the smelting slag showed that the smelting slag mainly consisted of PbO x and Na 2 O.

CAS / MDL: 1303-86-2
研究领域: 环境科学 · 冶金工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2019 · IF 5.107

An environment-friendly process of lead recovery from spent lead paste

Tianzu Yang,Boyi Xie,Weifeng Liu,Duchao Zhang,Lin Chen

Spent lead paste, an important secondary resource, calls for recycling at the request of both environmental protection and the sustainable development of lead industry. An environment-friendly process to recover lead from spent lead paste was proposed. The impurities Sb, Ca, Fe and Cu in spent lead paste were firstly removed by H 2 SO 4 at the leaching rate of 92.22%, 86.43%, 87.89% and 94.04%, respectively. And then, 99.9% of PbO 2 in spent lead paste was reduced to PbO by the hydrothermal reduction process with glucose as the reductant. In the process of hydrothermal desulfurization by NaOH, 99.46% of S in the reduced lead paste was removed and then the lead paste was converted into a single phase of 3PbO·H 2 O. Finally, metallic lead, with a purity of 99.978%, was obtained from the single-phase lead paste by a low-temperature reduction smelting process with starch as the reductant under the conditions of Na 2 O/B 2 O 3  = 1/2, PbO/B 2 O 3  = 5/1, starch/PbO = 1/7.5, smelting temperature 700 °C, and smelting duration 90 min, and the lead recovery is high up to 95.53%. Compared with the traditional lead smelting technology, the smelting temperature was reduced from 1200 °C to 700 °C, helping greatly reduce the energy consumption. The process proposed in this paper guides a new development direction for the utilization of spent lead paste.

CAS / MDL: 1303-86-2
研究领域: 冶金工程 · 环境科学
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International Journal of Coal Preparation and Utilization · 2023 · IF 2.1

Exploration of the sulfur removal mechanism of diphenyl sulfone loaded on activated carbon during Fe-assisted pyrolysis

Xuexia Wang,Wencheng Xia,Yaoli Peng,Guangyuan Xie

Iron-assisted pyrolysis (Fe-assisted pyrolysis) is a high-efficiency technique to remove sulfur from low-rank coal. However, the sulfur removal mechanism of Fe-assisted pyrolysis did not compressively address. For filling this gap, this study explored the sulfur removal mechanism of diphenyl sulfone during Fe-assisted pyrolysis based on the factor optimization of desulfurization performance. The iron powder under the optimal conditions of Fe-assisted pyrolysis was characterized with X-ray diffractometer (XRD) and X-ray photoelectron spectroscopy (XPS), showing that FeS and some FeS2 were formed on the surface of post-pyrolysis iron powder. Gas chromatography (GC) analysis manifested that the addition of iron powder in the pyrolysis process could considerably reduce the SO2 emission. GC and Fourier transform infrared spectrometer (FTIR) analyses demonstrated that there was C–S bond broken in the diphenyl sulfone structure during Fe-assisted pyrolysis. From the results of thermogravimetry-mass spectrometry (TG-MS), the addition of iron powder in the pyrolysis process could enhance the reaction rate and reduce the temperature required for the reaction. We believe that the results of the present study provided a theoretical basis for a profound understanding of the desulfurization mechanism of Fe-assisted pyrolysis.

研究领域: 能源科学 · 环境科学
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HYDROMETALLURGY · 2020 · IF 3.338

Promotion of manganese extraction and flue gas desulfurization with manganese ore by iron in the anodic solution of electrolytic manganese

Lu Yao,Guangzhi Xin,Pengyan Pu,Lin Yang,Xia Jiang,Zhicheng Jiang,Wenju Jiang

In this work, Mn ore was mixed with the wastewater anode solution of electrolytic Mn (ASEM, instead of water) and utilized as the desulfurizer for simultaneous SO 2 removal from flue gas and Mn extraction. The effects of Fe 2+ and Fe 3+ on Mn leaching and flue gas desulfurization were investigated. For MnO 2 and Mn 2 O 3 (mixed with ASEM), the introduction of Fe 2+ could simultaneously increase Mn extraction efficiency and flue gas desulfurization efficiency when MnO 2 and Mn 2 O 3 mixed with ASEM was used. Fe 3+ addition could improve desulfurization efficiency obviously for MnCO 3 . Fe 2+ could react with MnO 2 and H + to form Mn 2+ and Fe 3+ . This reaction further improved Mn extraction and simultaneously decreased the acidity of ASEM, thus promoting SO 2 removal. The introduced Fe 3+ could react with SO 2 , when MnO 2 was absent from the desulfurizer slurry. The resulting Fe 2+ was then oxidized by O 2 to form Fe 3+ , which underwent a Fe 3+ ↔ Fe 2+ cycle to promote flue gas desulfurization. Thus, the introduction of Fe ions, especially Fe 2+ , could promote simultaneous Mn leaching and flue gas desulfurization with Mn ore. This work provided not only a new way for effective SO 2 removal from flue gas and Mn extraction but also for recycling ASEM.

研究领域: 环境科学 · 冶金工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

An insight into mineral waste pulp for sulfur dioxide removal: A novel synergy-coordination mechanism involving surfactant

Zimeng Nie,Chen Li,Senlin Tian,Ping Ning,Dian Yang,Yingjie Li

Desulfurization by ore pulp has proved to be an attractive pathway, by which sulfur dioxide (SO 2 ) removal from fuel gas and mineral acid leaching can be realized simultaneously in hydrometallurgy. However, the weak reaction between alkalescent ore pulp and the weak acid SO 2 aqueous solution, and large mass transfer resistance caused by the heterogeneity of pulp seriously impeded their applications. Increasing the dispersion and surface tension of pulp by surfactants is an effective way, which has been rarely reported. Herein, the influence of the representative cationic, anionic and nonionic surfactants on desulfurization performance by ore pulp containing electrolytic manganese residue (EMR), phosphate ores (PO), and copper tailings (CT) were investigated systematically. Due to the high performance of anionic surfactant in enhancing the dispersion of ore pulp, reducing the surface tension of pulp, and increasing foaming, the desulfurization efficiency of EMR, PO, and CT was increased by 21.56 ± 3.25%, 23.13 ± 4.09%, and 20.54 ± 1.01%, respectively. However, the charge neutralization of cationic surfactant and the non-dissociation of nonionic surfactant made their promotion lower than the anionic one. Further, the co-ions and counter-ions in pulp affected the performance of surfactants in desulfurization. Besides, transition metal ions catalyzed the oxidation of SO 2 and promoted the formation of H 2 SO 4 .

研究领域: 冶金学 · 环境科学
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FUEL PROCESSING TECHNOLOGY · 2021 · IF 7.033

Hydro-upgrading of algal bio-oil in tetralin for the production of high-quality liquid fuel: Process intensification

Lei Chen,Zhi-Cong Wang,Dabo Chen,Lin-Xin Yin,Pei-Gao Duan

We report a new process to realize the deep removal of N, O, and S from the bio-oil when using a batch reactor to do the hydro-upgrading experiments. That is, within a fixed reaction time, hydro-upgrading of the bio-oil was carried out in several stages. After each stage reaction was finished, the reactor was cooled, and the gas in the reactor was replaced with fresh hydrogen, and then the reaction continued until the total reaction time was complete. A bio-oil produced from hydrothermal liquefaction of microalgae mixed with tetralin at a mass ratio of 1:1 was used as the feedstock . The experiments were performed at different temperatures (300–480 °C) and time (1–8 h) with fixed addition of 10 wt% Pt/C and 8 MPa H 2 . Higher treated bio-oil yield was always achieved if the reaction was performed in several stages. The N-, O-, and S- containing compounds in the gaseous products mainly consisted of C 2 H 4 N, C 3 H 7 N, C 6 H 7 N, NH 3 , (SCN) 2 , SO 2 , and H 2 O. The removal of these gas products avoided their secondary reactions with the bio-oil and slowed down the catalyst poisoning , and thus breaking through the equilibrium limitations of denitrogenation, desulfurization , and deoxygenation and prolonging the activity of the catalyst.

CAS / MDL: 119-64-2
研究领域: 能源生物学 · 化学工程
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ENERGY & FUELS · 2016 · IF 2.835

Adsorptivity of a Hyper Cross-Linked Ionic Polymer Poly(vinyl imidazole)-1,4-bis(chloromethyl)benzene for Thiophenic Sulfurs in Model Oil

Jing Zhang,Hui-hui Xu,Ying-zhou Lu,Hong Meng,Chun-xi Li,Biao-hua Chen,Zhi-gang Lei

A hyper cross-linked ionic polymer (HCIP) PVimBCmBn was synthesized through free radical polymerization of 1-vinylimidazole (Vim) and quaternized cross-linking with 1,4-bis(chloromethyl) benzene (BCmBn). Its composition, structure, morphology, specific area, porous structure and thermal stability were characterized, and the desulfurization performance was investigated. The results show that the HCIP prepared with stoichiometric ratio of PVim and BCmBn are ultrafine powders with specific area of 99.6 m2·g–1 and average pore size of 16.1 nm, being micro/mesoporous materials. The S-removability of HCIP is superior to its precursor (ethyl imidazole) and the imidazolium-based ionic liquids (ILs), which manifests the importance of the available micropores for the accommodation of sulfur molecules with less energy barrier. The adsorption isotherms of PVimBCmBn follow the Langmuir equation with its saturated adsorbance being 7.0, 5.2, and 4.1 mgS·g–1, respectively, for dibenzothiophene, benzothiophene, and thiophene in model oil at 293 K. However, its adsorptive removal ability for DBT in diesel oil is quite low due to its limited S-selectivity with respect to the abundant confused ring aromatics wherein.

研究领域: 化学工程 · 材料科学
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FUEL · 2022 · IF 8.035

Symbiosis of 1 T and 2H phases in the basal plane of defective MoS2 nanoflowers for efficient hydrodesulfurization

Zhe Bai,Luyao Wang,Hongwei Cao,Xiangwen Zhang,Guozhu Li

Hydrodesulfurization (HDS) is an effective way to reduce sulfur content in oil for the enforcement of more stringent environmental regulations. MoS 2 has been widely used as an effective component for catalyzing HDS, and needs to be extensively studied in depth. Herein, MoS 2 nanoflowers with the symbiosis of 1T-2H phases in the basal planes and coexistence of S and Mo vacancies are prepared via the assembly of many nanosheets by a one-pot solvothermal method. The morphology, crystal phase structure and defects of these 1T-2H MoS 2 samples were well characterized. The 1T/2H ratio and the state of vacancies were effectively tuned by changing the solvothermal conditions. Active and stable 1T-2H mixed MoS 2 nanoflowers with high content of 1T phase and moderate S and Mo vacancies were obtained by the regulation of oxalic acid in the mixture of ethanol and water. In the HDS of dibenzothiophene at 300 °C and 4 MPa, the optimal catalyst of MoS 2 -water–ethanol-OA exhibited a substrate conversion of 89.3% in 10 h. Moreover, the activity of MoS 2 -water–ethanol-OA was well retained without any decrease in the recycling experiment.

CAS / MDL: 12054-85-2
研究领域: 催化 · 材料科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Enhanced SO2, NO, and Cr (VI) removal by lignin-derived high N-doped activated carbon through one-pot strategy: Structure development, structure–performance relationship and mechanism insight

Huirong Zhang,Lin Luo,Zixiong Zhao,Yi Shen,Jinglei Cui,Xiaokai Shi,Xiaoliang Han

The production of high-performance activated carbon (AC) is recognized as an essential strategy for the effective utilization of lignin resources. In this work, the N-doped AC was successfully prepared by blending sodium lignosulfonate (SL) and different ratios of FeCl 3 through one-pot strategy. The AC structure evolution and performance were obtained by a series of characterization and tests. The results showed that, during the activation process, FeCl 3 first complexed with urea and catalyzed the depolymerization of SL, and the rapid pore development was mainly caused by the template, including formed FeCl 2 , Na 2 Fe 3 Cl 8 and Na 6 FeCl 8 . The ratio of FeCl 3 /SL adjusts the AC physicochemical texture. AC-3 processed a super total specific surface area and pore volume, respectively up to 2048 m 2 /g and 1.47 cm 3 /g. Meanwhile, AC-2 showed a higher nitrogen content of 11.4 %. The as-prepared AC shows super desulfurization, denitrification and Cr (Ⅵ) removal ability. AC-2 displayed maximum sulfur capacity and NO conversion, up to 199.1 mg/g and 42.4 %. This enhanced performance is primarily attributed to the pore structure induced by FeCl 3 activation, which provides a foundation for adsorption and catalytic processes, further augmented by the increased active sites due to nitrogen doping. AC-3 achieved an extremely high Cr (VI) adsorption capacity, up to 386.2 mg/g, which was primarily attributed to the redox effect of N-containing and O-containing groups on Cr (VI), in addition, the effect of physical adsorption including pore structure is not neglectable. This study highlights the significant potential of environmentally friendly lignin-based porous carbon materials for removing contaminants in both gas and liquid phases.

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Synergistic effect of dual Brønsted acidic deep eutectic solvents for oxidative desulfurization of diesel fuel

Wei Jiang,Kun Zhu,Hongping Li,Linhua Zhu,Mingqing Hua,Jin Xiao,Chao Wang,Zhenzhen Yang,Guangying Chen,Wenshuai Zhu,Huaming Li,Sheng Dai

Deep eutectic solvents (DESs) are generally used as attractive solvents or extractants rather than catalysts in the field of synthesis and separation. Herein, dual Brønsted acidic DESs were prepared by mixing sulfonated quaternary ammonium and oxalic acid as extractants and catalysts for deep oxidative desulfurization. Compared to the DESs with single acidic group, the dual acidic DESs exhibited much higher catalytic activity likely due to the synergistic effect. The 1 H NMR study indicated that the weak interaction between DES and sulfur compounds led to a low extraction capacity. However, the sulfur removal could reach 97.7% under optimized reaction conditions. Density functional theory (DFT) calculations demonstrated that sulfonic group and carboxylic group are of equal importance to desulfurization performance. Further, the desulfurization efficiency was also strongly affected by the viscosity of DESs. Here, we put forward a new strategy that the reaction time could be sharply shortened to 40 min and 100 min by adding low viscous acetonitrile and polyethylene glycol into DES to form mixing reaction system, respectively.

研究领域: 化学工程 · 催化 · 环境化学 · 燃料科学
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