SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Guangren Qu,Yawen Bo,Qihan Gong,Yanxi Li,Hua Xu,Jinbo Lai,Jiayu Ding,Sheng Liu,Kebin Chi,Dejun Shi,Rongguan Li,Chun Deng,Xili Cui,Huabin Xing
Metal-organic framework (MOF) ZnAtzPO 4 enables precise control of the pore size to achieve C 2 H 4 /C 2 H 6 adsorption separation. However, the industrial application of MOF powder faces problems such as pipe clogging and dust pollution, and the key to solving these problems lies in shaping. The shaped material should enhance mechanical stability while maintaining its physicochemical properties. This study aimed to explore the effects of shaping on the physicochemical properties of ZnAtzPO 4 using different binders. Hydroxypropyl cellulose (HPC), polyethylene glycol (PEG), sodium alginate (SA), and starch were used as binders, and the shaping body of ZnAtzPO 4 was prepared by extrusion shaping in different proportions. A series of characterization experiments such as XRD, BET, XPS, and mechanical strength testing, were carried out, then C 2 H 4 and C 2 H 6 adsorption isotherms were collected, and breakthrough experiments were performed on C 2 H 4 /C 2 H 6 (50:50 and 80:20 v/v) gas mixture. The selection of binders and the different proportions have significant impacts on the mechanical strength and adsorption properties of the shaped body, in which the shaped adsorbent with 5 % HPC shows a considerably high mechanical strength of 70.50N/cm, the ethylene adsorption capacity of that is up to 89 % of the powder, and the breakthrough experiments showed about 80 % adsorption separation time of ethylene/ethane compared to powder, exhibiting the best overall performance. Additionally, the 5 % HPC-shaped extrudate exhibits excellent cyclic stability and maintains crystalline integrity in both acidic and alkaline environments. The comprehensive investigation provides valuable insights into the shaping of MOF materials and helps to promote the practical application of MOFs in gas separation technology.
研究领域:
材料科学
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化学工程
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工业应用
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2017
·
IF 2.843
Yongli Sun,Hanrong Bi,Haozhen Dou,Huawei Yang,Zhaohe Huang,Baoyu Wang,Rong Deng,Luhong Zhang
For the separation of an ethylene/ethane mixture, a novel copper(I)-based supported ionic liquid membrane (SILM) with high permeability has been fabricated. This SILM was prepared from a polyvinylidene fluoride microporous membrane impregnating the copper(I) based IL which formed by the cuprous chloride (CuCl) and 1-butyl-3-methylimidazolium chloride ([Bmim][Cl]). Scanning electron microscopy, attenuated total reflection Fourier transform infrared spectroscopy, and time of flight mass spectroscopy were used to characterize the SILM. Pure and mixed gas permeation experiments were carried out to investigate the influences of ILs composition, trans-membrane pressure, temperature, and time upon the separation performance. This SILM showed comparable C2H4 permselectivity but outstanding permeability with a long-term stability beyond the reported polymeric membrane upper bound. At the CuCl/[Bmim][Cl] ratio of 2, the C2H4 permeability and permselectivity reached 2653 barrer and 11.8, respectively. Furthermore, the facilitated transport effect was studied by 1H NMR and quantum mechanical calculations. The anionic species formed by sp hybridization of Cu+ possesses unfilled attachment sites to selectively complex with C2H4 and weaken the interionic hydrogen bond of [Bmim][Cl], thus lowering the system’s viscosity.
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
JOURNAL OF MEMBRANE SCIENCE
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2020
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IF 7.183
Bin Jiang,Junhan Zhou,Mi Xu,Haozhen Dou,Haiming Zhang,Na Yang,Luhong Zhang
Membrane technology is a forward-looking approach for gas separation, while the implementation of membrane with high performance for ethylene/ethane separation still challenges the world. Herein, a multifunctional ternary deep eutectic solvent (DES)-based membrane was constructed for the cost-effective ethylene/ethane separation. The incorporation of a sweetener (Al(NO 3 ) 3 ) with the AgNO 3 /methylacetamide (NMA) mixture to form a ternary DES not only significantly promoted the ethylene/ethane selectivity but also enhanced the long-term stability of resultant membranes, which killed two birds with one stone. Various spectroscopic characterization and quantum mechanical calculations revealed that the complexing interaction between Ag + and NMA and the complexing interaction between Al 3+ and NO 3 − weakened the electrostatic interaction between Ag + and NO 3 − , and improved the interaction energy between ethylene molecule and Ag + carrier. By the synergy effects of two different complexing interactions, the ternary DES-based membranes exhibited high ethylene permeability, ethylene/ethane selectivity and stability, outperforming majority of the previously published data. Therefore, the membranes proved the grand potential for ethylene/ethane separation, and this work will shed light on the design of multifunctional liquid membranes for precise molecular separation.
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
JOURNAL OF MEMBRANE SCIENCE
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2018
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IF 6.578
Haozhen Dou,Bin Jiang,Luhong Zhang,Mi Xu,Yongli Sun
For ethylene/ethane separation, fabrication of facilitated transport membranes (FTMs) with properties of high ethylene permeability, selectivity, long-term stability and economic feasibility remains a great challenge. In this study, a series of deep eutectic solvents (DESs) containing NO 3 - as anion were designed, synthesized and characterized for the first time. Then, novel DES-FTMs were fabricated successfully through the incorporation of the transport carrier (AgNO 3 ) into as-synthesized DESs. The investigation of structure-performance relationships of FTMs suggested that the hydrogen bond acceptors (HBAs), hydrogen bond donors (HBDs) and their molar ratios greatly manipulated separation performance of FTM, which was also greatly affected by the carrier concentration. The right combinations of HBAs, HBDs and carrier concentration could significantly enhance the ethylene/ethane selectivity up to 125. The operating conditions of the separation process were optimized, confirming ethylene/ethane selectivity increased with the decrease of the transmembrane pressure and operating temperature. The synergetic regulation of hydrogen bond and coordination interactions between DES and carrier could tune the interactions between the silver cation and its counter anion, which efficiently promoted the disassociation of carrier and increased carrier activity, leading to high ethylene permeability and ethylene/ethane selectivity. The Brönsted acidic property of HBAs endowed the FTMs with good stability. The low cost and facile availability of the DESs and carrier rendered FTMs with good economic feasibility. This study may reveal the definite potentiality of DES-FTMs in ethylene/ethane separation.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 26
·12279-12286
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IF 3.3
Chaowen Liu,Mudi Xin,Xuejing Zhang,Chunlu Wang,Limei Qiu,Guangtong Xu
As an alternative to conventional cryogenic distillation, LTA zeolites act as cost-effective adsorbents for the adsorptive separation of ethylene and ethane. In this approach, the thermodynamic and kinetic separation of ethylene and ethane by LTA zeolites with regulated particle sizes and pore structures has been studied. Herein, LTA zeolites, with different particle sizes ranging from 0.82 μm to 4.96 μm and a pore diameter distribution concentrated around 4.16–5.07 Å, were prepared using the hydrothermal method followed by an ion-exchange procedure. The results indicated that variation of the zeolitic particle size and the Ca2+ exchange rate has a great influence on the separation process, including the selectivity of C2H4 and the breakthrough time intervals of C2H4 and C2H6. Several issues, including the intracrystalline diffusion, accessibility of active sites, reinforced interaction between adsorbents and adsorbates, and the confined space in the zeolitic channels, were investigated to explain the altered nature of the separation performance. The optimized separation performance was achieved using LTA zeolites with a particle size of 0.82 μm or with an ion-exchange rate of 69.13% and a pore diameter distribution of 4.94 Å.
研究领域:
化学工程
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材料科学
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吸附分离技术
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Mi Xu,Bin Jiang,Haozhen Dou,Na Yang,Xiaoming Xiao,Xiaowei Tantai,Yongli Sun,Luhong Zhang
Mixed strategy has been widely utilized to design novel membranes or tailor membrane structure, however the construction of facilitated transport membranes (FTMs) with mixed strategy has rarely been reported. In this work, eight kinds of mixed protic ionic liquid (MPIL) derived FTMs (MPIL-FTMs) were designed with mixed strategy for highly efficient ethylene/ethane separation by impregnating MPILs and ethylene transport carrier into porous support. The morphology of MPIL-FTMs were characterized by SEM and AFM, and their molecular interactions were investigated by 1 H NMR, FTIR and DSC. The MPIL-FTMs exhibited long-term stability and various ethylene permeability-ethylene/ethane selectivity combinations, which indicated mixed strategy could easily customize the separation performances of MPIL-FTMs. Moreover, a fundamental law for mixed strategy was obtained that the two parent PILs with similar chemical structure and molecular interactions favored the synchronous improvement of C 2 H 4 permeability and C 2 H 4 /C 2 H 6 selectivity. For example, the C 2 H 4 permeability of the [BA][Pyr][NO 3 ] derived MPIL-FTM reached up to 561.0 Barrer with improved C 2 H 4 /C 2 H 6 selectivity of 26.7, which were superior to most of reported membranes, thus breaking through the ubiquitous trade-off effect. This study proves the mixed strategy is a promising platform for the design of high-performance FTMs as well as their structure modification, and the marriage of mixed strategy with diversity of ILs creates enormous opportunities to construct advanced membranes for energy-intensive gas separations.
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
ENERGY & FUELS
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2017
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IF 3.091
Rong Deng,Yongli Sun,Hanrong Bi,Haozhen Dou,Huawei Yang,Baoyu Wang,Wenjun Tao,Bin Jiang
In the petrochemical industry, it is critical to separate the light olefins/paraffins mixtures via an efficient and economic method. In this work, a series of deep eutectic solvents (DESs) (choline chloride (ChCl)-glycerol (G), ChCl-ethylene glycol (EG), 1-butyl-3-methylimidazolium chloride ([Bmim][Cl])-G, and [Bmim][Cl]-EG) dissolving CuCl were used as novel membrane liquids to fabricate supported liquid membranes (SLMs) for the C2H4/C2H6 mixture separation. Interactions based on a hydrogen bond network in different DESs were characterized by time-of-flight mass spectroscopy (TOF-MS), nuclear magnetic resonance (1H NMR), and Fourier transform infrared (FT-IR) spectroscopy. Moreover, by absorption experiments, the Cu+ activity was quantitatively described based on a first-order equilibrium model. The effects of DESs species, CuCl concentration, transmembrane pressure, temperature, and time on separation performances were investigated by C2H4/C2H6 mixture permeation experiments. CuCl/ChCl-EG-based SLMs possessed good permeability and comparable permslectivity, as well as good long-term stability, surpassing the reported polymeric membrane upper bound. Systemic study demonstrated that the strength of the hydrogen bond networks in DESs could be tailored by optimizing the combinations of the HBAs and HBDs, and eventually improved the separation performances of the CuCl/DES-based SLMs.
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
Science Advances
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2022
·Vol. 8
·期 7
·
IF 14.957
Ruicong Wei,Xiaowei Liu,Zongyao Zhou,Cailing Chen,Youyou Yuan,Zhen Li,Xiang Li,Xinglong Dong,Dongwei Lu,Yu Han,Zhiping Lai
Zeolitic imidazolate framework 8 (ZIF-8) is effective for C3H6/C3H8 separation because of the “sieving effect” of a six-membered (6-M) window. Here, we demonstrate that ZIF-8 is a versatile material that could effectively separate C2H4 from C2H6 via its 4-M window along the <100> direction. We established a facile and environmentally friendly carbon nanotube (CNT)–induced oriented membrane (CNT-OM) approach to fabricate a {100}-oriented ZIF-8 membrane (100-M). In this approach, 2-methyimidazole was anchored onto the CNT surface followed by 3-hour in situ growth in aqueous solution at room temperature. The obtained 100-M, whose 4-M window is aligned along the transport pathway, showed ~3 times higher C2H4/C2H6 selectivity than a randomly oriented membrane. Thus, this work demonstrates that the membrane orientation plays an important role in tuning selectivity toward different gas pairs. Furthermore, 100-M exhibited excellent mechanical stability that could sustain the separation performance after bending at a curvature of ~109 m−1.
研究领域:
材料科学
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化学工程
✓ 已验证
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Yanyan Cheng,Fujian Li,Qingrong Wu,Kuilin Peng,Bangyu Fan,Yinge Bai,Zhongzhi Wang,Nian Zhang,Xiangping Zhang
Metal-containing ionic liquids (MILs) have been considered as promising solvents for ethylene/ethane (C 2 H 4 /C 2 H 6 ) separation. With multiple 4f and 5d empty electronic orbitals, special electronic configuration and abundant electron energy levels, rare earth elements have potential to be great electron acceptor of C 2 H 4 . Herein, a new strategy of rare earth metal ionic liquids (REMILs), 1-butyl-3-methylimidazolium trifluoromethanesulfonate containing erbium ([Bmim][TFO]/Er(TFO) 3 ) in N, N-dimethylformamide (DMF) was exploited to separate C 2 H 4 /C 2 H 6 for the first time. The complexation between Er 3+ and C 2 H 4 and interactions in absorbents were adopted to achieve fast and selective C 2 H 4 absorption. The physical properties of the absorbents were measured and studied firstly. The addition of 20 wt% DMF in REMILs was optimized with a decrease in viscosity of 6–7 times at 293 K. The absorption parameters, such as Er 3+ concentration, temperature and regeneration of absorbents were also investigated systematically. The results showed that the selectivity of C 2 H 4 /C 2 H 6 was enhanced with increasing Er 3+ concentration. The solubility of C 2 H 4 in [Bmim][TFO]/Er(TFO) 3 + 20 wt% DMF was 0.95 mg/g with C 2 H 4 /C 2 H 6 selectivity of 10 (at 303 K, 0.1 MPa), much higher than that of conventional ILs. The interaction energy (ΔE) of Er 3+ -C 2 H 4 was more negative than Er 3+ -C 2 H 6 through density functional theory (DFT). Furthermore, the rare earth absorbents exhibited excellent reversibility after five cycles. In summary, this work provides a potential method for efficient separating C 2 H 4 /C 2 H 6 via REMILs in DMF solution.
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
JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Lu Bai,Yongchao Sun,Tianyou Li,Jianyu Guan,Yijun Liu,Gaohong He,Canghai Ma
Carbon molecular sieve (CMS) membranes have garnered substantial attention for their ability to separate similarly sized gas mixtures. Despite their high gas permeability, CMS membranes exhibit moderate selectivity for the C 2 H 4 /C 2 H 6 gas pair. To address these issues, this study explores two types of polyimide precursors made from 2-(4-aminophenyl)benzo[d]oxazol-5-amine (APBO) and p-diaminobiphenyl (DABP) with 6FDA monomer to prepare CMS membranes. The integration of the flat, rigid polybenzoxazole (PBO) structure with the bulky, twisted 6FDA structure facilitates the formation of ultramicropores and micropores in the CMS membrane. The 6FDA-APBO-based CMS membrane, pyrolyzed at 700 °C, exhibits superior C2H4 permeability and C 2 H 4 /C 2 H 6 selectivity compared to the 6FDA-DABP-derived CMS membrane. Moreover, 6FDA-APBO-based CMS achieves an exceptional C 2 H 4 permeability of 160.8 Barrer with a C 2 H 4 /C 2 H 6 selectivity as high as 13.7, significantly surpassing the C 2 H 4 /C 2 H 6 upper bounds for both the polymeric and CMS membranes. The design principle provides an effective approach to enhance the C 2 H 4 /C 2 H 6 separation performance of membranes, paving the way for the development of energy-efficient C 2 H 4 /C 2 H 6 separation processes.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2017
·
IF 2.843
Bin Jiang,Wenjun Tao,Haozhen Dou,Yongli Sun,Xiaoming Xiao,Luhong Zhang,Na Yang
Binary metal chloride deep eutectic solvents (DESs) were first prepared by adding different metal chlorides into 1-butyl-3-methylimidazolium chloride ([BMIM]Cl)/CuCl DESs to improve the activity of the Cu+ carrier for ethylene/ethane separation. The binary metal chloride DESs were impregnated in the polyvinylidene fluoride microporous membrane to prepare the supported liquid membranes (SLMs). The performance of the SLMs based on binary metal chloride DESs was evaluated by ethylene/ethane separation experiments. For the SLM based on 0.5[BMIM]Cl-CuCl-1/15ZnCl2 DES, the selectivity of ethylene/ethane mixture increased from 10.7 to 17.8, and the ethylene permeability decreased slightly from 28.6 barrer to 25.8 barrer, compared to 0.5[BMIM][Cl] SLM without ZnCl2. Furthermore, it exhibited long-term stability for more than 150 h. The beneficial role of ZnCl2 for Cu+ carrier was analyzed by electrospray ionization mass spectrometry, Raman spectroscopy, and quantum mechanical calculation. The Raman spectrum showed that the Cu–Cl bond was weakened with the addition of ZnCl2. Quantum mechanical calculation revealed that the electron transferred from a Cl– ion of CuCl2– to the Zn2+ ion, which led to the weakening of the Cu–Cl bond and the activation of the Cu+ carrier.
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
JOURNAL OF MEMBRANE SCIENCE
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2022
·
IF 10.53
Ruisong Xu,Xiaofeng Xu,Yue Wang,Mengjie Hou,Lin Li,Zonglin Pan,Chengwen Song,Tonghua Wang
Fine tailoring the pore structure and sorption capability of carbon molecular sieve (CMS) membrane is highly desirable for efficient separation of C 2 H 4 /C 2 H 6 gas pair. In this work, a facile approach was proposed to enrich the ultramicroporosity of CMS membrane and enhance the affinity adsorption capacity for C 2 H 4 , in which ZIF-8 nanoparticles were incorporated into a novel precursor polymer of phenolphthalein-based poly (arylene ether ketone) (PEK-C) followed by carbonization to prepare mixed matrix CMS membranes to achieve simultaneously high C 2 H 4 permeability and high C 2 H 4 /C 2 H 6 selectivity. The ZIF-8-derived nanocomposites partially maintain the pore structure of ZIF-8 precursor, and have good compatibility with the carbon matrix. The BET surface areas, micropore volume and the number of ultramicropore with molecular sieving ability of CMS membrane are greatly improved due to the introduction of ZIF-8-derived microporous carbons, resulting in a significant increase in the C 2 H 4 permeability and C 2 H 4 /C 2 H 6 diffusion selectivity. The C 2 H 4 /C 2 H 6 sorption selectivity of CMS membrane is also enhanced owing to the selective adsorption affinity of the ZIF-8-derived Zn 2+ metal oxides for C 2 H 4 . The C 2 H 4 permeability of mixed matrix CMS membrane with 10 wt% ZIF-8 loading is increased by 42% compared to that of neat CMS membrane, and the C 2 H 4 /C 2 H 6 selectivity is increased by 102%.
研究领域:
材料科学
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化学工程
✓ 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）