AICHE JOURNAL
·
2019
·Vol. 65
·期 8
·e16625
·
IF 3.463
Zhen Song,Xutao Hu,Yageng Zhou,Teng Zhou,Zhiwen Qi,Kai Sundmacher
Although double salt ionic liquids (DSILs) offer significant advantages over classical two-ion ionic liquids as separation solvents, relevant studies are still scarce and a systematic DSIL selection method is thus highly desirable. In this contribution, a rational method for designing DSILs as extraction solvents is proposed and exemplified by the thiophene/ n -octane separation. The effects of additional degrees of freedom for DSIL design (i.e., double cations and/or anions and the ion ratio) on the thermodynamic properties are first analyzed by COSMO-RS. Then, a multilevel DSIL design method combining the prediction of infinite dilution thermodynamic properties, the estimation of physical properties, the evaluation of phase equilibrium behavior, and the experimental validation is proposed. By applying this method, [C 2 MIm][OAc] x [NO 3 ] 1- x ( x = [0, 1]) and [C 2 MIm][OAc] x [SCN] 1- x ( x = [0.70, 1]) are identified as promising DSIL solvents for the thiophene/ n -octane separation. Correspondingly, the liquid–liquid equilibria of {DSILs + thiophene + n -octane} with the designed DSILs are experimentally studied.
研究领域:
化学工程
·
分离科学
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2016
·
IF 2.567
Jing Chen,Bo Zhang,Guangw Miao,Jun Men
SiO2–NiO aerogels with different molar ratios of Si/Ni (n(Si/Ni)) were prepared by a sol–gel method and atmospheric pressure drying technology. The morphology and structure of SiO2–NiO aerogels were characterized by XRD, BET, XRF, and SEM methods. The equilibrium adsorption performance of thiophene or benzothiophene on the SiO2–NiO aerogels were studied at three different adsorption temperatures (298, 313, 333 K). The adsorption equilibrium data of thiophene on SiO2–NiO aerogels were more in line with the Temkin model at the lower temperature, while they were well fitted with both Langmuir and Temkin isotherms at the higher temperature. The maximum saturation adsorption capacities obtained by the Langmuir isotherms at different temperature decreased in the order qm(298 K) > qm(313 K) ≈ qm(333 K). The maximum saturation adsorption capacities of thiophene or benzothiophene on SiO2–NiO aerogels with different n(Si/Ni) values at 298 K decreased in the order SiO2–NiO-23 > SiO2–NiO-74 > SiO2–NiO-6. The maximum saturation adsorption capacities of thiophene and benzothiophene on SiO2–NiO-23 aerogels are 6.4564 and 2.1316 mgS/g, respectively. Both the amount of adsorption active sites and the textural structure of aerogels could significantly affect the adsorption performance. The higher the nickel content, specific surface area, pore volume, and larger pore size of the aerogel, the larger the adsorption capacity. The absolute value of adsorption heat of thiophene on SiO2–NiO aerogels increased gradually with the increase of n(Si/Ni) (the reduction of the Ni content).
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
INORGANICA CHIMICA ACTA
·
2022
·
IF 3.118
Mingyan Chen,Dehua Zhang,Ziying Wang,Yao Zhang,Yucheng Liu
UiO-66 loading carboxyl and phosphotungstic acid has a good affinity to thiophene (TH). The synthesized catalyst, changed its original structure, which can increase its reactive site and enhance the interaction with thiophene (TH) in order to improve the adsorption performance. Then the structural changes were analyzed by XRD, FT-IR, SEM, BET, EDS and other characterization methods. Through static experiments of adsorption desulfurization, it is found that when the adsorption time is 240 min, the adsorption temperature is 30 ℃ and the oil-to-agent ratio is 100:1, the adsorption effect: UiO-66-(COOH) 2 (UC2) > UiO-66, the highest adsorption capacity can reach 89.99 mg/g; while PTA@UiO-66 (PAU) can reach adsorption equilibrium at 210 min, it has better desulfurization performance than UiO-66. After being recycled for 5 times, the adsorption effect is only slightly decreased: the adsorption capacity of UC2 was still 78.02% of the initial adsorption capacity, while that of PAU was 76.07% of the initial adsorption capacity. According to the adsorption kinetics, the adsorption process of thiophene on the adsorbent UC2 is more consistent with W-M model, and the adsorption of PAU is more in line with the pseudo-first order kinetic equation. In addition, it also includes the process of intraparticle diffusion and liquid film diffusion.
研究领域:
化学工程
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材料科学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 11
·6605-6614
·
IF 3.108
Ce Gao,Qingda An,Zuoyi Xiao,Shangru Zhai
Nowadays, processing of ultra-low sulfur fuel oil has been a hot topic of research all over the world; hence, an efficient adsorption process to tackle this issue is eliciting increasing attention. However, the preparation of high-performance adsorbents is still a challenge. Herein, zirconium-substituted mesoporous SBA-15 with highly dispersed active Cu(I) species has been successfully synthesized by our group at 493 K via a mild vapor-reduction method. The as-prepared material was characterized by powder X-ray diffraction (XRD), nitrogen adsorption and desorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and UV-vis diffuse reflectance (DRUV) spectroscopy. All characterization methods demonstrated that the Cu(I) species were highly dispersed in an ordered mesoporous framework with short channels rather than piled on the surface. The as-prepared materials also exhibited an excellent adsorption capacity for thiophene (up to 29.86 mg g−1 at 323 K). Pseudo-second-order kinetics model and Freundlich isotherm can well describe the adsorption kinetics and isotherm data, respectively. More remarkably, an ultrasound-assisted treatment can be effectively employed to regenerate adsorbent, with only a slight reduction in the adsorption capacity after five cycles.
研究领域:
材料科学
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能源化学
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环境工程
✓ 已验证
DOI
高影响因子
FUEL
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2015
·
IF 3.52
Fuping Tian,Zhikai Fu,Huan Zhang,Jianjun Zhang,Yongying Chen,Cuiying Jia
Adsorption desulfurization is one of the most promising ways to reduce the sulfur content of gasoline at deeper level. In this work, thiophene (TP) adsorption capacity in cyclohexane onto [Cu 3 (BTC) 2 (H 2 O) 3 ] (HKUST-1) was measured by batch method, and the effect of cyclohexene and toluene on sulfur capacity was investigated. Adsorption isotherms of TP, cyclohexene, and toluene in cyclohexane onto HKUST-1 were conducted at 298.15–313.15 K to explicate the different extent of influence by cyclohexene or toluene addition. The results showed that, compared with cyclohexene, the addition of toluene in model gasoline led to a moderate decline in sulfur capacity of HKUST-1. The isotherm data of TP adsorption were well-correlated using Langmuir equation, while those of cyclohexene or toluene adsorption fitted Freundlich model, indicating different adsorption mechanisms between TP and competitors. The adsorption capacities followed the order of toluene < cyclohexene ≪TP at the same equilibrium concentrations, implying the order of the adsorption affinities, which is in good agreement with the different extent of influence by cyclohexene and toluene. The excellent regeneration performance of HKUST-1 in TP adsorption benefits from the physical adsorption mechanism, which was hinted by the enthalpy of TP adsorption (−37.31 ± 2.04 kJ mol −1 ) and no detection of new sulfur species.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2015
·
IF 4.642
Yawei Shi,Xiangwen Zhang,Guozhu Liu
Activated carbons derived from hydrothermal carbonization of sucrose and subsequent KOH activation have been prepared and tested for the adsorptive removal of refractory thiophenic compounds. Textural and chemical properties of the carbons and their corresponding impacts on adsorption rates and capacities were discussed in detail. The optimum carbon possessed high adsorption capacity (41.5 mgS/g for 300 ppmwS model oil), fast adsorption rate (97% saturated within 5 min) as well as relatively good selectivity for the adsorption of thiophenic compounds due to the abundant small micropores, suitable mesopore fraction and various oxygen functionalities present in the carbon. Combined with the economic and environmental merits of the preparation procedure, the sucrose-derived activated carbons are promising candidates for potential practical applications.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Zhiheng Wang,Yanyan Liu,Xin Li,Ruiyao Gao,Jiong Sun,Jiankun Liu,Songdong Yao
This study utilized the swelling properties of superabsorbent polymers (SAP) to adsorb zeolite sols and slurries to construct C-HY composites. The synthesized C-HY composites proved to be effective supports for NiMo catalysts in the hydrodesulfurization (HDS) of dibenzothiophene ( DBT ) and 4,6-dimethyl-dibenzothiophene (4,6-DMDBT). XRD , BET, SEM, TG, NH 3 -TPD, FTIR, H 2 -TPR, TEM and XPS were used to characterization the texutural structure, acidity and metal distribution of prepared NiMo/C-HY catalysts. By combining zeolite slurries with SAPs, HY can be efficiently incorporated into carbon substrate structure in three dimensions (3D), thereby changing the structural characteristics, morphology, acidity, and metal distribution of HDS catalysts. The conversion of DBT decreases sequentially: NiMo/C-HY-s > NiMo/C-HY-h > NiMo/C-HY-p > NiMo/C-HY-c, and the conversion of 4,6-DMDBT decreased sequentially: NiMo/C-HY-s > NiMo/C-HY-p > NiMo/C-HY-h ≫ NiMo/C-HY-c. The introduction of HY into the carbon support can increase the HDS reaction rate of NiMo/C by more than 1.2–1.5 times. The intrinsic reaction activity of NiMo/C-HY-s can even exceed that of traditional NiMo/Al 2 O 3 catalysts. Based on the same Mo loading amount, the HDS activity of NiMo/C-HY-s is twice that of NiMo/Al 2 O 3 in DBT HDS and 1.1–1.5 times that of NiMo/Al 2 O 3 in 4,6-DMDBT HDS. It is thought that HY in carbon composites promotes C–S bond cleavage of sulfur-containing molecules in DBT HDS. The unique dispersion of Mo species induced by HY favors the formation of highly stacked NiMoS active phases, which may be the crucial in 4,6-DMDBT HDS.
研究领域:
催化化学
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材料科学
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能源化工
✓ 已验证
产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2022
·Vol. 16
·期 12
·1735-1742
·
IF 4.803
Yu Guojia,Jin Dongyu,Li Xinyu,Zhang Fan,Tian Shichao,Qu Yixin,Zhou Zhiyong,Ren Zhongqi
A nitrogen-containing ionic liquid was synthesized using an aromatic nitrogen-containing heterocyclic and an amino acid, and applied to the extractive desulfurization process to remove benzothiophene, dibenzothiophene, and 4,6-dimethyldibenzothiphene from a model fuel oil. Chemical characterizations and simulation using Gaussian 09 software confirmed the rationality of an ionic liquid structure. Classification of non-covalent interactions between the ionic liquid and the three sulfur-containing contaminants was studied by reduced density gradient analysis. The viscosity of the ionic liquid was adjusted by addition of polyethylene glycol. Under extraction conditions of the volume of ionic liquid to oil as 1:1 and temperature as room temperature, the desulfurization selectivity of ionic liquid followed the order of 4,6-dimethyldibenzothiphene (15 min) < benzothiophene (15 min) ≈ dibenzothiophene (10 min). Addition of p -xylene and cyclohexene to the fuel oil had little effect. The extractant remained stable and effective after multiple regeneration cycles.
研究领域:
化学
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环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2020
·
IF 2.369
Feifan Chen,Bo Zhang,Luxia Yin,Yongkang Lu,Wanhui Gong,Jianguang Gao,Zekai Zhang,Wensheng Ning
Amine-modified SiO2 hybrid aerogel desulfurization adsorbents with varied Si/N molar ratios (SiO2-NH2-n) were prepared via the sol–gel method followed by the atmospheric drying technique. SiO2-NH2-n aerogels were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), in situ Fourier transform infrared (FT-IR), and N2 adsorption–desorption. The desulfurization performances of SiO2-NH2-n were studied by the batch and breakthrough adsorption experiments. SiO2-NH2-n exhibited an obvious improvement in adsorption capacity for thiophenics compared with SiO2 aerogel due to the hydrogen bonding between thiophenics and amino groups. Among them, SiO2-NH2-8 had the best performance, and the adsorption capacities for thiophene, benzothiophene, and dibenzothiophene were 6.8, 9.5, and 10.2 mg S/gads, respectively. No effect of toluene and cyclohexene on the adsorption of SiO2-NH2-8 for thiophene was observed. The equilibrium adsorption data of SiO2-NH2-8 for thiophene were well fitted by the Freundlich model, indicating that multilayer adsorption occurred on the heterogenetic surface of SiO2-NH2-8. The kinetic adsorption data of SiO2-NH2-8 for thiophene could correlate properly with the pseudo-second-order kinetic model, suggesting that the rate-controlling steps involve surface adsorption. The saturated SiO2-NH2-8 could be regenerated completely via heating at 393 K for 12 h, and the regenerated SiO2-NH2-8 afforded 100% breakthrough adsorption capacity for thiophene.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 52
·32671-32679
·
IF 3.361
Hailian Bao,Xiaodi Chen,Rui Yuan,Chao Zhang,Shiai Xu
A surface heterojunction catalyst of g-C3N4–PEDOT/P3HT with P3HT and PEDOT as the polymer sensitizer and hole transport pathway is successfully prepared. The as constructed g-C3N4–PEDOT/P3HT composite exhibits a photocatalyst H2 evolution rate up to 427703.3 μmol h−1 g−1 which is 1059 times higher than that of g-C3N4, 118 times higher than that of g-C3N4–PEDOT with ascorbic acid as sacrificial reagents. What's more, the g-C3N4–PEDOT/P3HT can even show an obviously enhanced photocatalytic H2 evolution rate which is 6.1 times higher than that of pure g-C3N4 in pure water without any sacrificial reagent. Combining the experimental results and molecular dynamic (MD) simulation results, a possible mechanism can be drawn that the existed PEDOT possesses relatively higher hole mobility and can be used as a hole conductor between g-C3N4 and P3HT. Then, the photogenerated holes migration can be accelerated by PEDOT from the VB of g-C3N4 to the VB of P3HT. All those factors may benefit the synergy among g-C3N4, PEDOT and P3HT, which finally facilitates the rapid migration of photoinduced electron–hole pairs and eventually improves the photocatalytic H2 activity process of g-C3N4–PEDOT/P3HT with visible light. The present work may provide useful insights for designing a surface heterojunction composite photocatalyst with high photocatalytic activity for H2 production.
研究领域:
材料科学
·
化学
·
光催化
·
可再生能源
✓ 已验证
DOI
高影响因子
MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2021
·Vol. 222
·期 10
·2000418
·
IF 2.527
Haoting Zheng,Kun Wu,Weilong Chen,Bingfei Nan,Zhencai Qu,Mangeng Lu
A series of copolymers of poly3-alkylthiophene (PTm) with different side chain lengths and copolymers of 3-butylthiophene and 3-butoxythiophene (PTDx) with different ratios are synthesized by oxidative polymerization. As the length of the side chain decreases, WAXD patterns of PTm show an increase in crystallinity. An increment of 50% in thermal conductivity is observed and the maximum thermal conductivity reaches to 0.320 Wm –1 K –1 . For PTDx, as the proportion of 3-butoxythiophene increases, the UV spectrum appears red-shifted, indicating an enhanced degree of p-π conjugation. The thermal conductivity of PTDx is increased from 0.340 to 0.374 Wm –1 K –1 , which is around twice that of traditional thermoplastics. Molecular dynamics (MD) is used to simulate the changes in the volume and dihedral angle overlap of the polymer at different temperatures, and achieves the same result as the experiment. MD simulations and experimental measurements have shown that reducing steric hindrance and enhancing p-π conjugation can increase the thermal conductivity of the polymer. Young's modulus of PTDx (around 1.86 GPa) is lower than that of conventional plastics, and its flexibility makes it more versatile.
研究领域:
材料科学
·
物理学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Mingxian Duan,Yeshuang Wang,Huiling Fan,Zhelin Su,Chao Yang,Jiawei Kou,Ju Shangguan
Thiophene (C 4 H 4 S) removal from coke oven gas is critical to its subsequent high valuable utilization but remains a challenge. MOF-199 was considered as a promising candidate for C 4 H 4 S adsorption removal owing to its nature of enriched opened Cu sites. However, the presence of mixed valence of Cu(II) and Cu(I) in MOF-199 makes it puzzling to their respective contribution to the removal of C 4 H 4 S. Herein, a series of MOF-199 with different Cu(I) contents were synthesized using different methods, including hydrothermal, solution diffusion, and ultrasonic, and their C 4 H 4 S adsorption performance were investigated. The respective contributions of Cu(II) and Cu(I) to the C 4 H 4 S removal was systematically discussed. The collected results indicated that although the samples prepared with different methods present a remarkable difference in textural characters, the latter was found to have a negligible influence on the C 4 H 4 S removal owing to MOF-199(H) affording an inferior surface area and pore volumes but performing the best C 4 H 4 S removal capacity of 53.7 mg S/g. The co-adsorption results of CH 3 SCH 3 and C 4 H 4 S indicated that the excellent performance of MOF-199(H) mainly attributed to the presence of Cu(I), which provides active sites for C 4 H 4 S adsorption through π complex coordination. Cu(II) species was also found to the C 4 H 4 S adsorption via soft-acid-base coordinated interaction, but its contribution is 8.3 mg S/g, only accounting for 15.5 %. Additionally, the adsorption of C 4 H 4 S on MOF-199(H) was found to follow the intra-particle diffusion model and the Langmuir models. Moreover, MOF-199(H) also exhibited an excellent regeneration performance due to the weak interaction between C 4 H 4 S and their opened Cu sites, the C 4 H 4 S adsorption capacity still reaches 50.6 mg S/g after three regeneration cycles, about 94 % of its initial value. The results collected in this study will provide new insights for the manipulation of performance of C 4 H 4 S adsorption on the MOF-199.
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
危险品化学品经营许可证（带存储）