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Small · 2024 ·Vol. 20 ·期 29 ·2310092 · IF 13

Supported Ionic Liquid Membrane with Highly-permeable Polyamide Armor by In Situ Interfacial Polymerization for Durable CO2 Separation

Yu-Ren Xue,Chang Liu,Hao-Cheng Yang,Hong-Qing Liang,Chao Zhang,Zhi-Kang Xu

Supported ionic liquid membranes (SILMs), owing to their capacities in harnessing physicochemical properties of ionic liquid for exceptional CO 2 solubility, have emerged as a promising platform for CO 2 extraction. Despite great achievements, existing SILMs suffer from poor structural and performance stability under high-pressure or long-term operations, significantly limiting their applications. Herein, a one-step and in situ interfacial polymerization strategy is proposed to elaborate a thin, mechanically-robust, and highly-permeable polyamide armor on the SILMs to effectively protect ionic liquid within porous supports, allowing for intensifying the overall stability of SILMs without compromising CO 2 separation performance. The armored SILMs have a profound increase of breakthrough pressure by 105% compared to conventional counterparts without armor, and display high and stable operating pressure exceeding that of most SILMs previously reported. It is further demonstrated that the armored SILMs exhibit ultrahigh ideal CO 2 /N 2 selectivity of about 200 and excellent CO 2 permeation of 78 barrers upon over 150 h operation, as opposed to the full failure of CO 2 separation performance within 36 h using conventional SILMs. The design concept of armor provides a flexible and additional dimension in developing high-performance and durable SILMs, pushing the practical application of ionic liquids in separation processes.

研究领域: 膜科学与技术 · 气体分离 · 环境化学 · 材料化学 · 化学工程 · 可持续能源技术
✓ 已验证 DOI 高影响因子
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JOURNAL OF APPLIED POLYMER SCIENCE · 2023 ·Vol. 141 ·期 10 ·e55068 · IF 3

Process parameter optimization for ionic liquids as gas separation membranes based on a GWO–BPNN model

Zhu Mian,Wang Bin,Lv Chao,Yu Zhenhui,Jingxian Liu

Gas separation membranes offer a cost-effective solution for capturing greenhouse gases, mitigating the global greenhouse effect. Ionic liquids (ILs) have emerged as one of the promising materials for greenhouse gas separation due to their strong affinity for CO 2 . In this study, we propose a laboratory-scale method for preparing IL–PVDF blend membranes with high CO 2 /N 2 selectivity. The separation performance of the membranes was evaluated using a custom gas permeation measurement system. The effects of casting solution composition, solidification method, and film-forming processes on separation performance were experimental investigated, and the obtained experimental data were used to train a back propagation neural network (BPNN) optimized by the Gray Wolf Optimizer (GWO) algorithm. This hybrid GWO–BPNN model was utilized to predict separation membrane efficiency, optimize the film-forming process, and identify the optimal range of process parameters. Notably, the GWO–BPNN model demonstrated a 2.76% higher prediction accuracy compared to a standalone BPNN. The results indicated that the GWO–BPNN algorithm has a great potential to accurately predict membrane separation efficiency and apply in optimal membrane process design (OMPD), and this method can significantly reduce the number of experimental trials required to achieve OMPD.

研究领域: 材料科学 · 化学工程 · 环境科学 · 膜分离技术 · 计算材料学
✓ 已验证 DOI 高影响因子
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JOURNAL OF MEMBRANE SCIENCE · 2020 · IF 7.183

Microstructural optimization of NH2-MIL-125 membranes with superior H2/CO2 separation performance by innovating metal sources and heating modes

Yanwei Sun,Chunshan Song,Xinwen Guo,Sungwon Hong,Jungkyu Choi,Yi Liu

Metal-organic framework (MOF) membranes have received increasing attention due to their unprecedented potential for energy-efficient gas separation. Compared with other MOF materials (like ZIF), fabrication and microstructural manipulation of high-performance Ti-MOF-based membranes, although being very attractive due to their excellent chemical and thermal stability, remained relatively less investigated due to the limitations of available titanium sources and heating modes. In this study, different Ti sources (TPOT, TiS 2 , and MXene) and heating modes (conventional heating, multi-mode microwave heating, and single-mode microwave heating) were examined for the preparation of NH 2 -MIL-125 membranes showing diverse microstructures and gas separation performances. The present work revealed that for the first time, MXene , the new two-dimensional Ti carbide , could be used as Ti source for synthesizing MOF membranes. The best performing NH 2 -MIL-125 membranes, which were obtained with TiS 2 as the metal source under single-mode microwave heating, exhibited the highest H 2 /CO 2 selectivity (ca. 17.2) as well as considerable H 2 permeance (1.7 × 10 −7  mol m −2  s −1  Pa −1 ), owing to an enhanced non-thermal effect of single-mode microwave heating and balanced dissolution rate of TiS 2 .

研究领域: 材料科学 · 膜分离技术 · 化学工程 · 纳米材料 · 气体分离 · 可持续能源
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

The absorption behavior of SO2 by amine alkyl organosilicon: Experimental analysis and numerical simulation

Bo Wang,Jinyu Wang,Yuan Chen,Zhiyong Xu,Wenbo Zhao

N-Benzyl-N-methyl-1-(methyl diphenyl silyl) methanamine (MPSA) with high thermal stability was synthesized for the absorption of SO 2 in the present work. The absorption capacity was measured at low partial pressures ranging from 0.002 to 0.016 bar and thermodynamic parameters, including enthalpy change (Δ H ) and entropy change (Δ S ) were calculated to analyze the absorption behavior. The desulphurization rates and absorption capacities at different temperatures and partial pressures were simulated based on thermodynamic parameters. An optimal absorption temperature T 1 that maximizes the absorption capacity, and an optimal desorption temperature T 2 that minimizes the desorption residual capacity and thermal desorption energy consumption were defined, and a function was proposed to calculate them. The kinetic behavior of the absorption was described using a pseudo-first-order model, and kinetic data at different temperatures and partial pressures were simulated based on a combination of kinetic and thermodynamic parameters. Ultimately, selectivity and cycles experiment showing MPSA has excellent CO 2 selectivity and thermal regeneration performance.

研究领域: 环境化学 · 气体分离 · 热力学 · 化学工程 · 功能材料 · 大气污染控制
✓ 已验证 DOI 高影响因子
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MICROPOROUS AND MESOPOROUS MATERIALS · 2020 · IF 4.551

Synthesis of well-shaped and high-crystalline Ce-based metal organic framework for CO2/CH4 separation

Junjie Zhou,Hao Liu,Yichao Lin,Chen Zhou,Aisheng Huang

A well-shaped Ce (IV)-based metal organic framework (Ce-BDC) is prepared under solvothermal method. The influence of synthesis time, temperature and the amount of acetic acid (HAc) as a modulator is studied to develop a new strategy for the synthesis of well-shaped Ce-based MOF. The relationship between the synthesis parameters and morphology as well as crystallinity of Ce-BDC is investigated by XRD and SEM. Furthermore, the obtained well-shaped Ce-BDC shows a CO 2 uptake capacity of 2.28 mmol g −1 at 0 °C and 1.0 bar. Meanwhile, the breakthrough curve behaviors of Ce-BDC are investigated for a CO 2 /CH 4 and CO 2 /N 2 mixture gas . It is found that the Ce-based MOF adsorbs CO 2 under ambient temperature and pressure, but completely excludes CH 4 and N 2 , suggesting that it is a promising adsorbent for efficient separation of CO 2 from natural gas.

研究领域: 材料科学 · 无机化学 · 多孔材料 · 气体分离 · 环境催化
✓ 已验证 DOI 高影响因子
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JOURNAL OF APPLIED POLYMER SCIENCE · 2019 ·Vol. 136 ·期 27 ·47723 · IF 2.188

Synthesis and CO2 separation of novel polyurethane membranes containing urea linkages

Yayun Zheng,Yaofang Hu,Xing Yang,Meng Yuan,Jie Zhang,Yaodong Zhang,Jujie Luo

We synthesized novel polyurethane (PU) membranes from isophorone diisocyanate (IPDI), poly(ethylene glycol) (PEG) with a molecular weight of 2000, aminopropyl-terminated poly(dimethyl siloxane) (PDMS) with a molecular weight of 2000, and 1,4-butanediol (BDO) via a two-step polymerization. The structure of each synthesized membrane was studied through Fourier transform infrared spectroscopy and gel permeation chromatography. The effect of the thermal behavior was determined by differential scanning calorimetry and thermogravimetric analysis. The gas-permeability characteristics of the PU membranes were then tested for a single gas. The results show that the permeability of CO 2 ( P CO2 ) gradually increased with PDMS content. Among these PU membranes, PU-d (PEG/PDMS = 1:1, PEG/PDMS/IPDI/BDO = 1:3:2) showed the best P CO2 (132.6 Barrer) at 25°C and 1 bar pressure. The gas-permeability coefficients of each PU membrane at different operating temperatures were investigated, and the results show that P CO2 reached 302.6 Barrer at 65°C and 1 bar. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136 , 47723.

研究领域: 高分子材料科学 · 膜分离技术 · 气体分离 · 功能高分子 · 环境化工
✓ 已验证 DOI 高影响因子
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JOURNAL OF MEMBRANE SCIENCE · 2016 · IF 5.557

Adjusting carrier microenvironment in CO2 separation fixed carrier membrane

Jiayou Liao,Zhi Wang,Ming Wang,Chengyun Gao,Song Zhao,Jixiao Wang,Shichang Wang

An ion-exchange material – Poly(diallyldimethylammonium carbonate) (PDDACA) containing mobile carbonate has been prepared and it has been blended in a fixed carrier membrane material – polyvinylamine (PVAm) containing abundant amine-group to adjust the carrier microenvironment of the fixed carrier membrane. It makes the mobile carrier cruise around the fixed carrier. On one hand, the CO 2 can be transported continuously in the swing area of fixed carrier through the mobile carriers, the passivity of fixed carrier can be overcome and the utilization efficiency of fixed carrier can be enhanced. On the other hand, a loose and low crystalline system will be obtained by blending two polymers, the number of effective mobile carrier will be increased with mobile carriers unlocking from the crystalline area, and the loose and low crystalline system will provide a good environment for the movement of mobile carriers. These are conducive to enhance the performance of blend membrane in comparision with single polymer membrane. The CO 2 permeance and CO 2 /N 2 selectivity of PVAm-PDDACA membrane, which concurrently contains fixed amine carriers and movable carbonate carriers, can reach 909   GPU and 102 at 0.11   MPa, respectively. The performance of PVAm-PDDACA membrane is enhanced obviously in comparision with PVAm membrane and PDDACA membrane.

研究领域: 膜科学与技术 · 气体分离 · 高分子材料 · 化学工程 · 环境化工 · 能源材料 · 功能材料
✓ 已验证 DOI 高影响因子
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JOURNAL OF MEMBRANE SCIENCE · 2022 · IF 10.53

Build up ‘highway’ in membrane via solvothermal annealing for high-efficient CO2 capture

Shuo Li,Shu-Mei Chang,Ming-Jie Yin,Wen-Hai Zhang,Wei-Shi Sun,Angus Shiue,Quan-Fu An

Poly (ethylene oxide) (PEO) membranes are attractive for CO 2 capture due to the particular dipolar–quadrupolar interaction between EO units and CO 2 molecules, which offer high CO 2 /N 2 selectivity. However, the low CO 2 permeability of PEO membranes hampers their practical applications. Herein, a simple solvothermal annealing approach was proposed to enhance the flexibility of PEO chains via ‘activating’ the disengagement and rearrangement of side chains, which is essential for boosting the gas permeability . The effects of solvothermal annealing temperature, time, and solvent on the CO 2 /N 2 separation performance were comprehensively investigated. The mechanism for the performance enhancement was proposed: a “highway” for gas transportation was built up by the released flexible side chains, which were confirmed by the mechanical and Li ion conductivity characterizations. The optimized PEO membrane offers a superior CO 2 permeability of 1294 Barrer, a high CO 2 /N 2 selectivity of 50, and 110-h long-term running stability, being beyond the 2008 Robeson’s upper bound line and promoting the practical application of PEO membranes in CO 2 capture by reducing the cost.

研究领域: 高分子科学 · 膜分离技术 · 气体分离 · 环境工程 · 材料化学
✓ 已验证 DOI 高影响因子
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DALTON TRANSACTIONS · 2012 ·Vol. 41 ·期 41 ·12915-12919 · IF 3.838

Ionothermal synthesis of two open-framework zirconium phosphates and their gas adsorption properties

Wei Wang,Lei Liu,Jiangfeng Yang,Sanying Li,Jinping Li,Jinxiang Dong

From a deep eutectic mixture consisting of trimethylammonium chloride (TMACl) and oxalic acid, two templated zirconium phosphates, ZrPOF-TMA1 with 8- and 10-ring pore channels as well as ZrPOF-TMA2 with 7- and 8-ring pore channels, have been synthesized. A low P/Zr ratio is necessary for ZrPOF-TMA1, and higher P/Zr ratios tend to form ZrPOF-TMA2, but the former cannot be obtained by templating TMACl under hydrothermal conditions. This is the first example in which a trimethylammonium cation, a protonated tertiary amine, has been used as a template to successfully synthesize two microporous zirconium phosphate materials, showing the potential for novel chemistry in ionothermal reactions. Both materials have a relatively high thermal stability and are stable up to 410 °C. Of the two microporous materials, ZrPOF-TMA2 with small pore openings exhibits a highly effective pore-selective behaviour that can discriminate between CO2 and CH4, with a CO2/CH4 adsorption ratio of 12.7 at 1 bar.

研究领域: 材料化学 · 无机化学 · 气体分离 · 多孔材料 · 可持续化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF CHEMICAL AND ENGINEERING DATA · 2012 · IF 1.693

Solubility of Hydrogen Chloride in Three 1-Alkyl-3-methylimidazolium Chloride Ionic Liquids in the Pressure Range (0 to 100) kPa and Temperature Range (298.15 to 363.15) K

Ru-Hao He,Bing-Wen Long,Ying-Zhou Lu,Hong Meng,Chun-Xi Li

To study the possibility of using ionic liquids (ILs) as a novel solvent for the absorption of hydrogen chloride (HCl) from the industrial tail gases, the solubility of HCl gas in three ILs has been measured at four temperatures, (298.15, 323.15, 348.15, and 363.15) K, in the pressure range of (0 to 100) kPa. The ILs used are 1-butyl-3-methylimidazolium chloride ([Bmim]Cl), 1-hexyl-3-methylimidazolium chloride ([Hmim]Cl), and 1-octyl-3-methylimidazolium chloride ([Omim]Cl). The results indicate that these ILs show high solubility for HCl gas, and the solubility decreases with the increasing length of the alkyl substitutes of the ILs, following the order [Bmim]Cl > [Hmim]Cl > [Omim]Cl. The solubility of HCl in [Bmim]Cl at 298.15 K is about 0.68 mole fraction at ca. 100 kPa partial pressure of HCl, which is much higher than that of 36.5 % HCl aqueous solution. The solubility of different ILs is discussed in detail, and the experimental data (P–T–x) are correlated successfully by an empirical relation.

研究领域: 化学工程 · 绿色化学 · 气体分离 · 离子液体 · 环境工程
✓ 已验证 DOI 高影响因子
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2014 · IF 2.235

Highly Efficient and Reversible Absorption of SO2 by Aqueous Triethylenetetramine Tetralactate Solutions

Jianguo Qian,Shuhang Ren,Shidong Tian,Yucui Hou,Chenxing Wang,Weize Wu

The capture of SO2 by ionic liquids (ILs) has drawn much attention. In this work, a series of triethylenetetramine (lactate)n ([TETA]Ln) was synthesized and triethylenetetramine tetralactate ([TETA]L4) was selected to prepare aqueous IL solutions to absorb SO2. It has been found that the aqueous IL solutions can absorb large amounts of SO2; the saturated mole ratio of SO2 to IL in the aqueous IL solution decreases with increasing temperature, and increases with increasing water content of the aqueous IL solution; the density and viscosity of the aqueous IL solution decreases with increasing temperature and water content, and the density and viscosity of aqueous IL solution after SO2 absorption is higher than that before SO2 absorption. The absorption of SO2 by the aqueous IL solution is reversible. Compared with other ILs, [TETA]L4 has many advantages in application, including inexpensive synthetic materials, uncomplicated synthetic procedures, high SO2 capacity, and excellent reversibility.

研究领域: 环境化学 · 绿色化学 · 气体分离 · 材料科学
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