NEW JOURNAL OF CHEMISTRY
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2015
·Vol. 39
·期 10
·8158-8164
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IF 3.086
Dongshun Deng,Guoqiang Han,Yaotai Jiang
Efficient and reversible absorption of SO2 in six new deep eutectic solvents (DESs) composed of levulinic acid (LA) and quaternary ammonium salts (choline chloride, CC; choline acetyl chloride, CAC; tetraethylammonium chloride, TEAC; tetraethylammonium bromide, TEAB; tetrabutylammonium chloride, TBAC; tetrabutylammonium bromide, TBAB) was systematically investigated. The molar ratio of LA to quaternary ammonium salt was fixed at 3 : 1. The results showed that all DESs possessed satisfactory performance for SO2 absorption, with the maximum absorption capacity of 0.625 g SO2 per g DES of LA–TEAC at 293.15 K under ambient pressure. The absorbed SO2 was easily released by bubbling N2 at 323.15 K and the regenerated DES was recycled five times without obvious loss of absorption performance. The solubility of SO2 in DES of LA–CC at T = 293.15, 303.15, 313.15, and 323.15 K under subatmospheric pressures was also determined. The relative thermodynamic parameters, i.e., absorption enthalpy, absorption entropy, and absorption Gibbs free energy, were further calculated, giving results with small negative values. The influence of water content on the SO2 absorption was also investigated. According to NMR and FTIR analyses, the absorption of SO2 in DES was a physical process. Moreover, all the DESs exhibited high selectivity for SO2/CO2. The present DESs are promising absorbents for SO2 because of their high absorption capacity and good reversibility.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
·
IF 13.6
Lurui Wan,Kai Wang,Yuan Chen,Zhiyong Xu,Wenbo Zhao
Wet flue gas desulfurization is widely used for its high efficiency, however, the low absorption capacity, high viscosity and poor thermal stability of absorbents remains an open question. Herein, a low viscosity and high thermal stability SO 2 absorbent with dual interacting sites was synthesized by introducing phenyl into organic silicon . The thermal stability of 1,5-bis (diethylamino)− 1,1,5,5-tetramethyl-3,3-diphenyltrisiloxane (BADPS) is comparable to ILs , while its viscosity is much lower than that of ILs . For the first time, we use a variant of the pseudo-first-order reaction rate equation obtained the reaction rate constant and the saturation absorption capacity. In addition, the optimal absorption and desorption temperatures were obtained based on an objective function. Mostly importantly, the absorption enthalpy change (ΔH) and entropy change (ΔS) of BADPS absorption reaction show the highest absolute values of SO 2 absorbents reported so far. These results indicated that the prepared amine alkyl organosilicon could serve as a promising desulfurizing agent with low-energy consumption.
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2014
·
IF 4.331
Shidong Tian,Yucui Hou,Weize Wu,Shuhang Ren,Jianguo Qian
The capture of SO 2 by ionic liquids (ILs) has drawn much attention all over the world. However, ILs can absorb not only SO 2 but also water from flue gas. The removal of water from ILs is necessary for reusing the absorbent. In order to reduce the energy costs of removing water, it would be helpful to weaken the interactions between ILs and water. In this work, two kinds of hydrophobic task-specific ILs, 1-(2-diethyl-aminoethyl)-3-methylimidazolium hexafluorophosphate ([Et 2 NEmim] [PF 6 ]) and 1-(2-diethyl-aminoethyl)-1-methylpyrrolidinium hexafluorophosphate ([Et 2 NEmpyr][PF 6 ]), were designed and synthesized. Thermal stability and physical properties of the ILs were studied. Furthermore, the application of the ILs for the capture of SO 2 and the absorption mechanism were systematically investigated. It has been found that both of the ILs are immiscible with water, and [Et 2 NEmim][PF 6 ] has much lower viscosity, much higher thermal stability and much higher SO 2 absorption rate than [Et 2 NEmpyr][PF 6 ]. [Et 2 NEmim][PF 6 ] shows high SO 2 absorption capacities up to 2.11 mol SO 2 per mole IL (pure SO 2 ) and 0.94 mol SO 2 per mole IL (3% SO 2 ) under hydrous conditions at 30 °C. The result suggests that [Et 2 NEmim][PF 6 ] is a promising recyclable absorbent for the capture of SO 2 .
研究领域:
化学工程
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环境科学
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产品关联
DOI
PubMed
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2015
·
IF 3
Shidong Tian,Yucui Hou,Weize Wu,Shuhang Ren,Chenxing Wang,Jianguo Qian
The capture of SO 2 by recyclable absorbents has drawn much attention all over the world. In this work, it was found that aqueous calcium lactate (CaL 2 ) solution can be used as a recyclable absorbent for the capture of SO 2 . The solution shows high SO 2 absorption capacities up to 24.8 g SO 2 /kg absorbent at 40 °C. The effects of temperature, excessive lactic acid and CaL 2 concentration on the absorption of SO 2 , the desorption of SO 2 , and the reuse of aqueous CaL 2 solution were systemically studied. Furthermore, the difference between CaL 2 method and traditional calcium method was discussed. Compared with traditional calcium method, there are some advantages, such as regeneration of absorbent, recovery of SO 2 and reduction of CaSO 4 . This work suggests that aqueous CaL 2 solution, which can be obtained at quite low cost, is a promising recyclable absorbent in the process of desulfurization of flue gas.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Huifang Guo,Jia Liu,Yunlong Shi,Xiaohong Xie
In this study, bio-based pyrrolidone (2-Pyr) and low-toxicity tetraethylammonium chloride (TEAC) were selected to prepare inexpensive, low-viscosity deep eutectic solvents (DESs), which is in line with the concept of green and sustainable chemistry and is suitable for industrial production. The highest absorption capacity of TEAC:2-Pyr (1:4) was determined to be 1.03 g SO2 /g DES at 20 °C. Eight absorption–desorption cycling tests were performed, and it was found that the absorption performance of DESs for SO 2 slightly varied. It was also proved that DESs have a certain degree of water resistance and high SO 2 selectivity. Fourier transform infrared spectroscopy and computational chemical analysis showed that the DESs composed of TEAC:2-Pyr formed intermolecular hydrogen bonds, the O atoms in Cl − and 2-Pyr played a role in the absorption of SO 2 , and hydrogen bonds were broken by the addition of SO 2 .
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION SCIENCE AND TECHNOLOGY
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2013
·
IF 1.164
Guangfei Qu,Jun Zhang,Junyan Li,Ping Ning
Two kinds of phosphate ionic liquids were synthesized and their SO2 absorption performance was investigated. It was found that both ionic liquids could readily absorb SO2, and the absorption capacity could reach 2.8 and 2.7 mol SO2 per mole ILs, respectively, at ambient temperature and under normal pressure. Moreover, the cycle of SO2 absorption and desorption from ionic liquids was repeated for four times and no change in the absorption capacity was observed. FT-IR spectrum and 1H NMR were used to characterize the microstructure of SO2-absorbed ILs and ILs, analysis showed that both ionic liquids absorbed SO2 purely by physical absorption. Comparing with the previous reported ionic liquids such as [Bmim][PF6] and [Emim][BF4], the synthesized ionic liquids showed higher absorption capacity, due to the anion based phosphate (O˭P‒O) with the free electrons on the oxygen interacting with the Lewis acidic sulfur of SO2, and then showing a great affinity for SO2.
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Bo Wang,Jing Chen,Jinyu Wang,Zhiyong Xu,Wenbo Zhao
The high viscosity of ionic liquids (ILs) and the poor thermal stability of deep eutectic solvents (DESs) limit their application in the real industry of SO 2 removal. Amine alkyl organosilicon can be considered as a potential candidate owing to its excellent physicochemical properties, desulfurization performance, and low regeneration sensible heat. In this work, an amine alkyl organosilicon, namely N-butyl-N-((methyldiphenylsilyl)methyl) butan-1-amine (BMMBA), characterized by low viscosity and high thermal stability, was innovatively synthesized. Dynamic absorption experiments show that BMMBA exhibits high SO 2 absorption capacity and excellent SO 2 /CO 2 selectivity. In addition, the absorption mechanism was revealed by quantum chemical (QC) calculation and molecular dynamics (MD) simulations. The consistency between experiments and theoretical calculation indicates that SO 2 interacts mainly with the N atom and benzene group of BMMBA. Further, thermodynamic analysis reveals that BMMBA displays exceptionally steep gradient of absorption capacity curves with temperature variations, which arise from an extremely negative absorption entropy change (Δ S ), favoring the reduction of regeneration sensible heat energy consumption. Ultimately, the optimization results suggest that the BMMBA system has a lower sensible heat of regeneration compared to conventional absorbents. The novel absorbent and investigate conclusions demonstrated herein could provide a theoretical basis for designing highly effective SO 2 absorbents.
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
CHEMICAL ENGINEERING JOURNAL
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2013
·
IF 3.473
Kuan Huang,Yong-Le Chen,Xiao-Min Zhang,Shuang Xia,You-Ting Wu,Xing-Bang Hu
Two new simple acid salt ionic liquids (ASILs), tetraethylammonium diglutarate ([N 2222 ][diglutarate]) and dimethylethanolammonium diglutarate ([DMEA][diglutarate]) were synthesized and the ASILs/sulfolane binary mixtures containing 40 wt% ASILs were prepared for SO 2 absorption in this work. The SO 2 absorption rate is found to be quite fast with an equilibrium time within 2 min, due to the low viscosity of the mixtures. The solubilities of SO 2 in the two binary mixtures were measured under the pressure range of 0–1 bar and the temperature range of 303.15–333.15 K and results demonstrate the binary mixtures could trap as much as 6.836–7.624 mol SO 2 /kg absorbents at 1 bar and 303.15 K. The solubilities are 0.826–0.954 mol SO 2 /kg absorbents at a pressure as low as 0.004 bar, which is important for capturing SO 2 from the flue gas with low content of SO 2 . Thermodynamic analysis based on a Reaction Equilibrium Thermodynamic Model (RETM) was used to calculate the Henry’s law constants, reaction equilibrium constants, chemical absorption capacity, physical absorption capacity and thermodynamic functions of SO 2 absorption in the mixtures. The calculated absorption enthalpy are −53.73 and −47.15 kJ/mol for the two binary mixtures, respectively. The ASILs/sulfolane binary mixtures are shown to be an attractive alternative to pure ILs to be applied in SO 2 absorption due to the large absorption capacity and low absorption enthalpy, as well as the fast absorption rate.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Green Chemical Engineering
·
2025
·
IF 7.6
Wei Hui,Xin Wang,Xiao-Ya Wang,Fei-Feng Mao,Tiao Zhang,Yan Zhou,Jia-Yin Zhang,Duan-Jian Tao
The mass transfer and diffusion limitations of ionic liquids (ILs) have hindered their application in SO 2 separation. In this work, five diethyl sulfate (DiEtSO 4 ) based ionic liquids (DiEtSO 4 -based ILs) with different viscosities ( μ , 3∼285 cP) were synthesized by tuning the cationic structures. The SO 2 absorption capacities and kinetics of DiEtSO 4 -based ILs were evaluated at 298-313 K. Meanwhile, liquid-side volumetric mass transfer coefficients ( k L a ) and liquid-side mass transfer coefficients ( k L ) were determined using the pressure drop method to assess SO 2 mass transfer in DiEtSO 4 -based ILs quantitatively. The results indicated a physical absorption mechanism for SO 2 , consistent with Henry's law (Δ H < ∼21 kJ/mol). Specifically, both 1-methylimidazole diethyl sulfate ([MIM][DiEtSO 4 ]) and 1,8-diazabicyclo[5.4.0]undec-7-ene diethyl sulfate ([DBU][DiEtSO 4 ] demonstrated high capacities (∼9.6 mmol/g), rapid kinetics (equilibrium within < 2.5 min), and excellent cyclic stability with minimal capacity loss (∼0.1%). Moreover, density functional theory (DFT), conductor-like screening model for real solvent thermodynamics (COSMOtherm), and independent gradient model (IGM) analyses confirmed that Van der Waals and weak electrostatic interactions predominate over chemical bonding in the absorption process. Mass transfer analysis confirmed an inverse relationship between μ and k L ( k L ∝ μ −0.5 ) in DiEtSO 4 -based ILs, which is consistent with Danckwerts' theory. Based on its superior overall performance in SO 2 absorption capacity, mass transfer rate, and cyclic stability, [MIM][DiEtSO 4 ] emerged as the most promising candidate for SO 2 separation and recovery.
研究领域:
化学工程
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环境科学
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分离科学
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物理化学
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绿色溶剂
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jihan Yang,Airong Li,Junping Guo,Zhihong Wang
The control of sulfur dioxide (SO 2 ) emissions from natural gas purification processes has become an urgent environmental priority due to increasing regulatory pressures and public concerns over air pollution. In this study, a series of 1-methylimidazolium-based ionic liquids ([MIM]-ILs) were synthesized and structurally characterized, followed by systematic evaluation of their SO 2 absorption capacities under simulated flue gas conditions (2000 ppm SO 2 ). Among them, [MIM]Lac showed the relatively better absorption performance, reaching a saturated capacity of 1.986 mol SO 2 per mol IL at a low concentration of 2000 ppm SO 2 . The regeneration experimental results demonstrated that [MIM]Lac achieved an optimal SO 2 removal efficiency of 99.71 % at 85 °C, indicating excellent thermal responsiveness. Even after 10 consecutive absorption-desorption cycles, [MIM]Lac retained 92.52 % of its initial absorption capacity, highlighting its outstanding cyclic stability and thermal durability. The insights based on FT-IR and 1 H NMR analyses revealed that SO 2 absorption by [MIM]Lac primarily involved the reversible chemical interactions between SO 2 and the lactate anion, particularly at the S O and S−O sites. This study provides a practical strategy for designing efficient SO 2 absorbents and the development of ionic liquid-based desulfurization systems.
研究领域:
环境化学
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大气污染控制
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绿色溶剂
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工业生态学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
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2025
·
IF 4
Bo Wang,Shuangjiang Li,Xiandong Hao,Wenbo Zhao,Zhiyong Xu,Yongming Luo
Traditional amine scrubbing for SO 2 capture typically dilutes alcohol amines with water to improve mass transfer, resulting in high volatility and desorption energy consumption. Inspired by the exceptional properties of ionic liquid (IL) 1-ethyl-3-methylimidazolium thiocyanate ([EMIM][SCN]), we herein propose substituting water with [EMIM][SCN] in a novel SO 2 absorbent system based on N -methyl ethanolamine (MDEA). MDEA acts as the primary SO 2 absorbent, while [EMIM][SCN] serves as an auxiliary absorption component and physical properties regulator. Performance evaluations reveal that MDEA-[EMIM][SCN] achieves high thermal stability (~483.15 K), low viscosity (~26 mPa s), excellent absorption capacity (~1.64 mol/kg at 298.15 K and 2000 ppm SO 2 ), high SO 2 /CO 2 selectivity (~101), and low desorption energy (approximately −95.6 kJ/mol). Thermodynamic modeling illustrates MDEA and [EMIM][SCN] contribute independently to absorption. Optimal energy consumption was determined by the proposed objective function. This work exemplifies the non-aqueous alkanolamine/IL system for SO 2 capture, offering a promising approach for developing efficient, low-energy SO 2 absorbents.
研究领域:
化学工程
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环境科学
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热力学
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Siheng Qian,Jing Hu,Rimin You,Xiaobing Wang,Lifeng Yang,Huabin Xing,Xili Cui
SO2 emission has become an important issue due to its harmful impact on human health and the ecological environment. Adsorption separation is an energy-efficient technology to capture SO2, but it suffers from competitive adsorption of CO2. Here, we present a strategy to improve the separation performance of porous adsorbents through the fabrication of mixed-matrix adsorbents. By the introduction of a perm-selective polymer (P(D[VImC6]Br)) as the matrix to enclose anion-pillared microporous materials (SIFSIX-3-Ni), CO2 molecules were selectively blocked, while the SO2 molecules could still permeate the polymer matrix and access the porous particles of SIFSIX-3-Ni. As a result, a high SO20.2%/CO210% uptake ratio of 32 at 298 K and 1 bar and a high SO2 uptake capacity of 0.67 mmol g–1 at 0.002 bar were achieved for the mixed-matrix adsorbents of SIFSIX-3-Ni@PIL-1/1. The strategy for fabricating a perm-selective matrix around the porous adsorbent particles to improve the adsorption performance is generally applicable to other porous adsorbents.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）