JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2019
·
IF 2.298
Wenliang Cui,Jilong Wang,Yueyang Xu,Zijia Cao,Yongping Zeng
Faujasite (FAU) zeolites with low Si/Al ratios (e.g., X-type zeolites) have much more exchangeable cation sites than those with high Si/Al ratios (Y-type zeolites) for Cu(I), which could improve the adsorption performance via π-complexation. However, the structure of Cu-exchanged X-type zeolites was unstable during autoreduction at high temperatures as reported [Takahashi; et. al., Ind. Eng. Chem. Res., 2002, 41, 2487−2496]. Here, we proposed a scheme of Cu-exchanged X-type zeolites in copper–ammonia solution to improve the stability of the zeolite structure during autoreduction. Therefore, it makes us be able to study the adsorption properties of thiophenic compounds in Cu(I)-exchanged FAU zeolites from low to high Si/Al ratios. The modified zeolites were characterized by X-ray diffraction, high-resolution transmission electron microscopy, inductively coupled plasma spectroscopy, X-ray fluorescence, and Brunauer–Emmett–Teller analysis and tested by adsorption desulfurization experiments in model fuels. The results indicate that the modified zeolites with various Si/Al ratios show different adsorption properties for thiophene and benzothiophene. The adsorption capacity for thiophene decreased in the order Cu(I)Y-5.30 > Cu(I)X-1.23 > Cu(I)Y-2.30. For benzothiophene, the adsorption capacity decreased in the order Cu(I)Y-2.30 > Cu(I)Y-5.30 > Cu(I)X-1.23.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Ning Gu,Yueyang Xu,Yan Yin,Xuzhao Gao,Yongping Zeng
SO x released from the combustion of sulfur-containing compounds in fuels pollute the environment and have a serious impact on human health. Adsorption desulfurization is an effective and environmentally friendly technique for removing sulfur-containing compounds from fuels. Metal-organic frameworks (MOFs) have high specific surface areas and can be easily modified and functionalized, making them excellent candidates for adsorption desulfurization in fuels. In this work, the precursor MIL-100(Fe)-SA was prepared using the hydrothermal method , and the adsorbent Ni@MIL-100(Fe)-SA was obtained by doping Ni 2+ into the resulting MIL-100(Fe)-SA using the impregnation method. FT-IR, X-ray diffraction, scanning electron microscopy, transmission electron microscopy and nitrogen adsorption-desorption isotherms were used to analyze the samples. The results indicated that Ni 2+ was successfully loaded onto MIL-100(Fe)-SA, and the MOF's structure remained stable. The adsorption performance of benzothiophene and thiophene was evaluated through batch adsorption experiments. The adsorption capacities of Ni@MIL-100(Fe)-SA for thiophene and benzothiophene were 23.68 mg S/g and 49.58 mg S/g, respectively. These observations could be ascribed to the π-complexation interactions between Ni 2+ of the framework and thiophenic compounds. The regeneration experiments demonstrated that the spent 11Ni@MIL-100(Fe)-SA-1.5 reach 86% of the adsorption capacity of fresh adsorbent after four cycles. Additionally, the regenerated adsorbent maintained good crystallinity after recycling.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Konglu Guo,Yueyang Xu,Yan Yin,Yongping Zeng
Adsorption desulfurization can effectively remove thiophene-containing compounds in fuels. UiO-66 is a potential candidate for adsorption desulfurization due to the excellent chemical stability and resistances to acids and alkali. However, the adsorption capacity is relatively low for the big molecules of sulfide (such as thiophenes) because of the pore size in the microporous structure. We used Zn 4 O(BC) 6 as a template to synthesize a new π-complexation adsorbent (H-UiO-66-SO 3 Cu(I)) via ion-exchange and steam-induced reduction, with hierarchical porous (microporous and mesoporous) structure. The adsorbent was characterized by FT-IR, XRD , SEM , TEM and N 2 adsorption-desorption isotherms. The results show that H-UiO-66-SO 3 Cu(I) has the stable structural properties with the new mesopores . H-UiO-66-SO 3 Cu(I) has a good adsorption performance for thiophene and benzothiophene in the model fuel. The regeneration results show that H-UiO-66-SO 3 Cu(I) can be recycled four times and still has good adsorption performance.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Energies
·
2021
·Vol. 14
·期 1
·234
·
IF 3.004
Yu Ji,Qiang Yao,Weihong Cao,Yueying Zhao
To probe the possibility of thiophenolate as an origin of dibenzothiophenes (DBTs) and establish the detailed chemical transformations from thiophenolate to DBTs, the thermal degradation of thiophenolate has been carried out at various temperatures. The characterizations of both gaseous products and solid residues indicate that DBTs together with benzene, diphenyl sulfide, and diphenyl disulfide are the major degradation products. The presence of benzene supports that the thermal degradation of thiophenolate begins with the homolysis of Ar‒H bonds. The subsequent hydroarylation followed by the elimination and cyclization reactions facilely generates DBTs. The transformation of thiophenolate to DBTs is chemically simple and highly geochemically feasible. It readily unifies the chemical pathways involved in the generation of DBTs from thiophenolate and that of dibenzofurans from phenolate in nature.Keywords:thiophenolate;dibenzothiophene;phenyldibenzothiophene;homolysis;hydroarylation;aromatic sulfur heterocyclics
研究领域:
化学
·
地质化学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Hao Zhang,Guang-Ren Qian,Hong Liu
Alumina composites containing microporous ZSM-5 (Z-5) and mesoporous ZSM-5 (MZ-5), corresponding to x ZA and x MZA, were developed by incorporating Z-5 and MZ-5 into γ - Al 2 O 3 , respectively. The two series of NiMoS/ x MZA and NiMoS/ x ZA catalysts were prepared with these two composites as supports, respectively, and were used for the simultaneous hydrodesulfurization (HDS) of thiophene (T) and benzothiophene (BT). The results show that NiMoS/ x MZA series catalysts exhibit higher HDS activity than that of NiMoS/ x ZA and NiMoS/γ-Al 2 O 3 , and the HDS activity of NiMoS/ x MZA catalysts increases with the increase of MZ-5. The high HDS activity can be mainly attributed to the synergistic effects of the efficient diffusing pore channels, high dispersion of type II NiMoS phases, suitable acidity, and moderate Mo-support interaction. Moreover, the product distribution of HDS shows that the NiMoS/ x MZA catalysts possess the dominant direct desulfurization (DDS) selectivity and the selectivity increases with the increase of MZ-5 content due to more corner sites and suitable Brønsted (B) acid sites, whereas the NiMoS/ x ZA catalysts perform more excellent hydrogenation (HYD) selectivity, and the selectivity increases with the increase of Z-5 content because of the existence of more edge sites. Based on this, the possible reaction network for T and BT hydrodesulfurization over the catalysts are proposed.
研究领域:
催化化学
·
能源化工
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2020
·
IF 5.065
Hong Li,Yuhao Zhang,Dexin Sun,Liang Zhao,Jinsen Gao,Chunming Xu
In order to investigate the ability of N -methyl-2-pyrrolidone (NMP) to extract aromatics (benzene, toluene) and sulfides (3-methylthiophene, thiophene) from n-hexane, the liquid-liquid equilibrium (LLE) data of n-hexane + {benzene, toluene, thiophene or 3-methylthiophene} + NMP systems were determined at 293.15 K under 101.3 kPa. The Othmer-Tobias and Hand equations were applied to validate the reliability of the obtained LLE data, and the correlation coefficients ( R 2 ) are close to unity. It was found that sulfides could be successfully extracted from n-hexane by NMP solvent companying with the extraction of aromatics. However, the separation factors and distribution coefficients of the sulfides are greater than those of aromatics, indicating that the sulfides are more easily extracted by NMP. Furthermore, the separation energies of the sulfides are greater than that of aromatics, which is also a piece of evidence for easier separation of sulfides. In order to extend those results to other extraction processes involving those sulfides, aromatics and solvent, the binary interaction parameters of the NRTL and UNIQUAC thermodynamic models were calculated by correlating the LLE data. The RMSD values were all <0.0070, and a graphical user interface based on the Gibbs tangent plane test was also applied to validate the coherent consistency of the parameters. The results show that the obtained binary interaction parameters could be reliable adopted in the design and optimization of the related extraction/separation process in industry.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
ORGANIC GEOCHEMISTRY
·
2025
·
IF 2.5
Yili Mao,Ke Du,Xiaofeng Xia,Zhiwei Gao,Qilin Xiao,Quan Shi,Yongge Sun
Benzothiophenes (BTs) and dibenzothiophenes (DBTs) are an important organic sulfur compounds (OSCs) in crude oils, primarily as proxies for thermal maturity and secondary alteration, though their biological sources and depositional environments remain debated. Compound-specific stable carbon isotopic measurements could provide new insights into their origins. In this study, we employed improved methylation/demethylation reactions for selective separation of thiophenic and sulfidic compounds from crude oils to measure the stable carbon isotopic compositions of individual BTs and DBTs. Experiments with model compounds show no significant isotopic fractionation of BTs and DBTs through entire procedure, while small fractionation occurs for sulfidic compounds. Pre-removal of alkanes and additional purification by alumina column chromatography effectively reduced co-elution interference, enhancing the accuracy of isotopic measurements. To demonstrate the method’s applicability, two crude oils from Chinese petroliferous basins were analyzed, integrating δ 34 S values of individual DBTs. In the low maturity, non-biodegraded lacustrine oil, the DBTs exhibit highly 13 C-depleted values (av., −35.2 ‰) compared to oil fractions and non-sulfurized individual organic compounds. With the exception of 1-methyldibenzothiophene (−29.1 ‰), the BTs are enriched in 13 C relative to DBTs by up to ∼5.5 ‰, suggesting the distinct organic sources. In the biodegraded marine oil, although a small discrepancy in δ 13 C values (∼1 ‰) remains, similar δ 13 C values of oil components indicate a shared source, as shown by δ 13 C values of pristane (–33.0 ‰) and phytane (–33.7 ‰). δ 34 S values of individual DBTs (21–23 ‰) suggest a common source for organic sulfur given its moderate maturity (equivalent vitrinite reflectance of ∼0.9 % R equ ). While OSCs formation in oils from the Tarim Basin is attributed to the incorporation of TSR-H 2 S into labile compounds in biodegraded oils, we propose that OSCs in these oils form mainly from sulfur re-incorporation, followed by cyclization and/or aromatization into functionalized aromatic and alkyl cyclohexane compounds at the early stage of diagenesis. This leads to similar carbon and sulfur signatures in BTs and DBTs. Therefore, successful carbon isotope measurements of individual BTs and DBTs could provide new insights into their sources and formation pathways, and application limitations. Future studies on samples from diverse geological settings could further demonstrate the methods potentials.
研究领域:
地球化学
·
石油地质学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2014
·
IF 2.235
Nan Li,Fang Wang,Zhiqing Zhang,Huihui Nie,Chengcheng Ren,Mei Cui
Polymeric 1-vinyl-3-ethylimidazolium tetrafluoroborate ionic liquids modified microspheres of silica gel were prepared by free radical polymerization in toluene. Characterization with Fourier transform infrared (FTIR), elemental analysis, scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), gel permeation chromatography (GPC), thermogravimetric analysis (TGA), and 13C, 29Si magic angle spinning (MAS) nuclear magnetic resonance (NMR) demonstrated that 1-vinyl-3-ethylimidazolium tetrafluoroborate had successfully loaded on the surface of silica gel and formed a stable polymer coating. Furthermore, to detect the potential desulfurization performance, a series of experiments of model fuel desulfurization with polymeric ionic liquid modified silica gel had been carried out. The desulfurization efficiency of modified silica gel was investigated by removing 2-methylthiophene, benzothiophene, and dibenzothiophene from model fuel (n-heptane/2-methylthiophene, benzothiophene, and dibenzothiophene) under tested conditions. It was shown that the modified silica gel exhibited remarkable desulfurization capacity for aromatic S-containing compounds and the sulfur removal selectivity followed the order of 2-methylthiophene < benzothiophene < dibenzothiophene due to the different density aromatic π-electrons.
研究领域:
材料科学
·
环境化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Guojia Yu,Dongyu Jin,Fan Zhang,Shichao Tian,Zhiyong Zhou,Zhongqi Ren
Porous liquids (PLs) combine the advantages of porous solid materials and the fluidity of liquids, and show great potential for applications. Based on the interactions between sulfides in fuel oil and nitrogen-containing heterocyclic ionic liquid (ILs), dicationic imidazole-based ILs with different alkyl side chains and linkage chains, and benzyl-grafted DBU amidinocyclic IL were used as sterically hindered solvents to enhance the extractivity, and the microporous structure of metal–organic framework MIL-53(Al) improve the adsorption performance. Several novel functionalized PLs with dual roles of extraction and adsorption were synthesized under electrostatic interaction between the two. The results showed it had good extraction-adsorption coupled desulfurization performance of fuel oil. Under optimal conditions, the removal efficiencies reached to 67.67 %, 85.5 % and 84.34 % for thiophene, benzothiophene and dibenzothiophene with initial sulfur concentration of 5000 ppm, respectively. Quantitative calculation and visualization analysis revealed the mechanism of desulfurization process, it is subject to the dual action of microporous structure and ILs. Due to the π-π stacking and van der Waals (VDW) forces between sulfides and ILs, thiophene-like sulfides is first extracted into the ILs phase, then diffuses to the two-phase interface between the ILs and MIL-53(Al), after screening by the window size, it enters into the pore and is firmly adsorbed under the effect of electrostatic interaction, Lewis acidic sites, π-π force, etc. The porous liquids provide a new direction for fuel desulfurization process, and is a new functionalized solvent with great application potential and research value.
研究领域:
化学工程
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Polymers
·
2023
·Vol. 15
·期 8
·1856
·
IF 5
Wen Wang,Jie Cao,Jiawen Yu,Fajuan Tian,Xiaoyu Luo,Yiting Hao,Jiyan Huang,Fucheng Wang,Weiqiang Zhou,Jingkun Xu,Ximei Liu,Hanjun Yang
Supercapacitors are widely used in various fields due to their high power density, fast charging and discharging speeds, and long service life. However, with the increasing demand for flexible electronics, integrated supercapacitors in devices are also facing more challenges, such as extensibility, bending stability, and operability. Despite many reports on stretchable supercapacitors, challenges still exist in their preparation process, which involves multiple steps. Therefore, we prepared stretchable conducting polymer electrodes by depositing thiophene and 3-methylthiophene on patterned 304 stainless steel (SS 304) through electropolymerization. The cycling stability of the prepared stretchable electrodes could be further improved by protecting them with poly(vinyl alcohol)/sulfuric acid (PVA/H2SO4) gel electrolyte. Specifically, the mechanical stability of the polythiophene (PTh) electrode was improved by 2.5%, and the stability of the poly(3-methylthiophene (P3MeT) electrode was improved by 7.0%. As a result, the assembled flexible supercapacitors maintained 93% of their stability even after 10,000 cycles of strain at 100%, which indicates potential applications in flexible electronics.
研究领域:
材料科学
·
电子工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2024
·
IF 5.9
Wen-shuo Zhang,Ying Li,Xian Zhang,Jun Shen,Yu-gao Wang,Yan-xia Niu,Gang Liu,Qing-bai Xu
During the hot mixing process of road-paving asphalt, odorous substances are released, primarily consisting of sulfur-containing compounds that are regarded as atmospheric pollutants, negatively impacting both human quality of life and the eco-environment. In the paper, a kind of simulated asphalt solution was designed with two sulfur-containing compounds, dibenzothiophene (DBT) and benzothiophene (BT), as well as n-eicosane dissolved in cyclohexane. DBT and BT were extracted with deep eutectic solvent (DES) of tetrabutylammonium bromide and polyethylene glycol (TBAB/PEG). The effects of different molecular weight of PEG as donor on desulfurization efficiency were investigated. The effects of DES donor/receptor ratio, extraction temperature and time, solvent oil ratio, mixing speed, recycling performance of DES on desulfurization efficiency were also studied and optimized. The results indicated that the maximum desulfurization efficiency of BT reached 89.40 % at room temperature with a ratio of agent to oil of 2:1, reaction time of 30 min, and mixing speed of 600 rpm. Similarly, the desulfurization efficiency of DBT achieved 95.54 % when the ratio of agent to oil was 3.5:1, with reaction time of 30 min and mixing speed of 600 rpm. After being recycled eight times, the extraction efficiencies of DBT and BT remained at 85.3 % and 65.2 %, respectively. Under optimized conditions, the extraction efficiency of petroleum asphalt exceeded 23 %. Fourier Transform Infrared (FTIR) analysis indicated that the sulfur-containing compounds found in the saturates and aromatics of road-paving asphalt were extracted by DESs, which are generally more volatile than those found in asphaltenes during hot-mixing. Additionally, minimal changes were observed in the structural composition of the four fractions of desulfurized asphalt.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Reaction Chemistry & Engineering
·
2023
·Vol. 8
·期 12
·3124-3132
·
IF 3.9
Chenhua Shu,Min Zhao,Hua Cheng,Yajie Deng,Pierre Stiernet,Niklas Hedin,Jiayin Yuan
A type-III porous liquid based on zeolitic imidazolate framework-8 (ZIF-8) and an ionic liquid trihexyltetradecylphosphonium bis(trifluoromethylsulfonyl)imide ([THTDP][BTI]) was synthesized and used for the desulfurization of model diesel. The desulfurization effect by ZIF-8/[THTDP][BTI] combined both the adsorptive desulfurization by ZIF-8 and the extraction desulfurization by [THTDP][BTI]. The removal of the three chosen aromatic organic sulfides by the ZIF-8/[THTDP][BTI] porous liquid followed the order of dibenzothiophene (73.1%) > benzothiophene (70.0%) > thiophene (61.5%). It was further found that deep desulfurization could be realized by ZIF-8/[THTDP][BTI] through triple desulfurization cycles and ZIF-8/[THTDP][BTI] can be regenerated readily. The desulfurization mechanism was explored further in detail by conformation search and density functional theory calculations. Calculations supported that the large molecular volume of [THTDP][BTI] excluded itself from the cavities of ZIF-8, making the pores of ZIF-8 in the porous liquid unoccupied and accessible by other guest species, here the studied organic sulfides. These calculations indicate that the van der Waals interactions were the main interactions between ZIF-8/[THTDP][BTI] and specifically benzothiophene. This work supports that the porous liquid ZIF-8/[THTDP][BTI] could potentially be used for desulfurization of diesel in industry.
研究领域:
化学工程
·
材料科学
·
环境化学
✓ 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）