RSC Advances
·
2021
·Vol. 11
·期 46
·28863-28875
·
IF 3.361
Yu Qin,Li Xu,Liying Liu,Xiaoyu Deng,Yucheng Gao,Zhongwei Ding
A novel gas separation approach is proposed in this work by combining an amine-based solid adsorbent with a zeolitic imidazolate framework-8 (ZIF-8) membrane. This was achieved by incorporating the amine-based solid adsorbent during the fabrication of the ZIF-8 membrane on a macroporous substrate. An amine-based solid adsorbent was prepared using porous ZIF-8-3-isocyanatopropyltrimethoxysilane (IPTMS) and N-[(3-trimethoxysilyl)propyl]diethylenetriamine (3N-APS) amine compounds. The as-prepared porous amine-based solid adsorbent (denoted as ZIF-8-IPTMS-3N-APS) possessed excellent adsorptive CO2/N2 and CO2/CH4 separation performances. As the adsorbent needs to be regenerated, this could indicate that the CO2 adsorption separation process cannot be continuously operated. In this work, an amine-based solid adsorbent was applied during the preparation of the ZIF-8 membranes owing to the following reasons: (i) gas separation by the membrane can be operated continuously; (ii) the amino group provides a heterogeneous nucleation site for ZIF-8 to grow; and (iii) the reparation of surface defects on the macroporous substrate can be performed prior to the growth of the ZIF-8 membrane. Herein, the ZIF-8 membrane was successfully fabricated, and it possessed excellent CO2/CH4, CO2/N2, and H2/CH4 separation performances. The 0.6 μm ultrathin ZIF-8 membrane demonstrated a high CO2 permeance of 4.75 × 10−6 mol m−2 s−1 Pa−1 at 35 °C and 0.1 MPa, and ideal CO2/N2 and CO2/CH4 selectivities of 4.67 and 6.02, respectively. Furthermore, at 35 °C and 0.1 MPa, the ideal H2/CH4 selectivity of the ZIF-8 membrane reached 31.2, and a significantly high H2 permeance of 2.45 × 10−5 mol m−2 s−1 Pa−1.
研究领域:
材料科学
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化学工程
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DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Xi Chen,Nana Wang,Guining Chen,Zhenggang Wang,Gongping Liu,Rongfei Zhou,Wanqin Jin
Mixed-matrix formulation is a promising method to overcome permeability-selectivity trade-off of polymers with incorporation of fillers with well-defined nanopores . The filler properties play a key role in determining the performance of mixed-matrix membrane (MMM). In this work, for the first time, we explored the critical effect of filler structural integrity on separation performance of MMM. Typically, micron as-synthesized, submicron as-synthesized and submicron ground SAPO-34 zeolites were incorporated into 6FDA-DAM polyimide , respectively. The interface compatibility between two phases was ensured by (3-aminopropyl) trimethoxysilane (APTMS) modification on SAPO-34 fillers. It was found that the directly synthesized micron and submicron fillers contributed to enhance the CO 2 /CH 4 separation performance whereas the submicron ground filler lowered the CO 2 permeability. Notably, incorporating 30 wt% micron as-synthesized SAPO-34 into 6FDA-DAM enhanced the CO 2 permeability by 68% and CO 2 /CH 4 by 37%, surpassing the performance upper-bound. Moreover, the hydrogen bonding between the filler and polymer matrix endowed the membrane with outstanding plasticization resistance with CO 2 partial pressure up to 20 bar. Adsorption isotherms and Maxwell model prediction revealed that the filler transport properties could be significantly affected by commonly-used methods of reducing the filler size. A decreased structural integrity was identified in the sequence of micron as-synthesized, submicron as-synthesized and submicron ground fillers. This work highlights the importance of a careful balance between structural integrity and crystal size of filler, and reliable routes to obtain nanofillers with desirable structural integrity as pursuing high-performing MMM toward practical application.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2017
·
IF 6.035
Xingyu Wu,Wei Liu,Hong Wu,Xue Zong,Leixin Yang,Yingzhen Wu,Yanxiong Ren,Chengyou Shi,Shaofei Wang,Zhongyi Jiang
In this study, novel kinds of MMMs were fabricated by incorporating ZIF-67 nanoparticles into polymers of intrinsic microporosity (PIM-1). ZIF-67 (Co substituted ZIF-8) displays stiffer Co-N bond as compared with the Zn-N bond in ZIF-8, which might led to the slightly smaller effective pore aperture of ZIF-67. Good compatibility between ZIF-67 nanoparticles and PIM-1 matrix rendered ideal interfacial morphology. The intrinsic separation performance of ZIF-67 was estimated from our experimental separation results based on the Maxwell model. The calculation demonstrated its superior CO 2 /CH 4 selectivity of 45, which is twice compared with that of ZIF-8, supporting the high molecular sieving efficiency of PIM-1/ZIF-67 MMMs. Particularly, the CO 2 and H 2 permeability increased by 15.1% and 59.6% for PIM-1 membrane with 20 wt% ZIF-67 loading, meanwhile CO 2 /CH 4 and H 2 /CH 4 selectivity increased by 34.4% and 86.96%, respectively. The strategy of incorporating highly selective ZIFs into polymers of intrinsic microporosity may have promising potential in fabricating high performance membranes for efficient gas separation.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Xi Chen,Zhenggang Wang,Zhuo Yang,Guozhen Liu,Guining Chen,Gongping Liu,Xiuxia Meng,Naitao Yang,Wanqin Jin
Towards natural gas purification , polymeric membranes generally face challenges of trade-off between permeability and selectivity , as well as CO 2 -induced plasticization effect. Previous works demonstrated that incorporating high-performing nanofillers and crosslinking the polymers are effective methods to overcome these two issues, respectively. In this work, we aimed to simultaneously improve permeability, selectivity and plasticization resistance of polymeric membranes by incorporating surface-engineered nanoporous fillers for CO 2 /CH 4 separation. DD3R zeolite nanoparticles with high purity were synthesized and then surface-functionalized by 3-aminopropyl trimethoxysilane (APTMS) to serve as the filler. Mixed-gas permeation measurements showed that DD3R zeolites offered CO 2 -selective channels in 6FDA-DAM polyimide based on molecular sieving effect of zeolitic aperture. 30 wt% DD3R-APTMS zeolite imparted the membrane with CO 2 permeability of 1661 Barrer (increased by 71.7%) and CO 2 /CH 4 selectivity of 28.0 (increased by 44.5%), which was beyond the upper-bound of polymeric membranes. Meanwhile, the hydrogen bond interaction between amino groups on APTMS and carboxyl groups on 6FDA-DAM rendered the resulting DD3R-APTMS MMMs highly enhanced plasticization resistance over 40 bar when equimolar CO 2 /CH 4 mixture as the feed. This work demonstrates a facile approach to simultaneously enhance separation performance and mitigate the plasticization effect.
研究领域:
材料科学
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化学工程
·
膜技术
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2018
·
IF 6.578
Leixin Yang,Shengbo Zhang,Hong Wu,Chumei Ye,Xu Liang,Shaofei Wang,Xingyu Wu,Yingzhen Wu,Yanxiong Ren,Yutao Liu,Nayab Nasir,Zhongyi Jiang
For high-performance mixed-matrix membranes (MMMs), it is crucial to design gas transport channels in fillers to rationally manipulate the structure-property relationship. In this study, the novel porous organosilicon nanotubes (PSiNTs) were incorporated into Pebax to prepare MMMs for biogas purification (CO 2 /CH 4 separation). After comparing the separation performance of MMMs containing PSiNTs and MMMs containing non-porous organosilicon nanotubes (SiNTs)，it can be found that the porous structure on wall of organosilicon nanotubes had a significant effect on the improvement of the gas permeability . In addition, the amino-modified PSiNTs (N-PSiNTs) were prepared and introduced into membranes to significantly enhance the CO 2 permeability and CO 2 /CH 4 selectivity. Firstly, the porosity of N-PSiNTs afforded rapid gas transport channels in MMMs and intensified the diffusion mechanism, increasing the CO 2 permeability. Secondly, the reversible reaction between amino groups and CO 2 in MMMs intensified the facilitated transport mechanism, increasing the CO 2 /CH 4 selectivity. In particular, the Pebax-N-PSiNTs with 0.5 wt% and 1 wt% N-PSiNTs exhibited the optimal separation performance, which surpassed 2008 upper bound and were superior to the MMMs incorporated with other kinds of nanotubes.
研究领域:
材料科学
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环境工程
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DOI
高影响因子
HIGH PERFORMANCE POLYMERS
·
2021
·
IF 2.161
Tao Yang,Hongchang Pang,Zan Chen,Cuijia Duan,Biao Yuan,Shuo Yan
A series of hyperbranched copolyimides (co-HBPIs), as the completely symmetrical tetraamine monomer successfully incorporated into the linear polyimide 6FDA-ODA, were synthesized under the chemical imidization after the gel formation was avoided, as to more effectively separate CO2/CH4. CO2/CH4 selectivity (74%) was observed to be improved significantly under 7‰ tetraamine contents at 2 bar and 35°C; thus, the acceptable CO2 permeability was maintained compared with the pure membrane, exceeding the 1991 upper bound. Moreover, the as-prepared membrane with 6FDA-ODA-7‰ was reported to exhibit higher CO2/CH4 selectivity (109.14) at 10 bar and 35°C. Accordingly, the hyperbranched copolyimides will be promising candidates as membrane materials for the further separation of CO2/CH4 gas pair.
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DOI
高影响因子
FUEL
·
2020
·
IF 5.578
Jing Bai,Xiang Zhen,Kele Yan,Pan Li,Shuqi Fang,Chun Chang
Lots of thermodynamics and kinetics accelerators have been used in the process of mixture gas separation by hydrate method, but there is still lack of valid screening method for seeking reliable and effective hydrate promoters. In this work, the effects of additive molecular diameter on the hydrate phase equilibrium condition and the quantity of hydrogen bond donor and accepter of additive on the separation efficiency during CO 2 (40.0 mol%)/CH 4 hydrate formation process were investigated. The results demonstrated that the larger molecular diameter of additive in cyclopentane (CP), tetrahydrofuran (THF) and tetrahydrothiophene (THT) systems, the phase equilibrium promotion effect of additive is more significant. And the empirical equations were proposed for predicting the phase equilibrium condition of CO 2 /CH 4 hydrate under the impact of additive with different molecular diameters. Moreover, on account of the quantity of hydrogen bond donor and acceptor of additive were different, the degree of mutual dissolution between additive molecule and aqueous solution was different, so that the number of additive molecules that could participate in the formation of hydrate was different, which had a certain impact on the separation efficiency.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2019
·
IF 3.372
Zihan Qu,Hong Wu,Yue Zhou,Leixin Yang,Xingyu Wu,Yingzhen Wu,Yanxiong Ren,Ning Zhang,Yutao Liu,Zhongyi Jiang
Membranes with fast CO 2 transport pathways have attracted intense attention due to their outstanding CO 2 permeability, showing potential for industrial application. Regulating the spatial distribution of CO 2 -philic groups in polymer-based membranes is expected to be a promising strategy to achieve the fast CO 2 transport pathways. In membrane matrix, the interconnected network of concentrated domains of CO 2 facilitated transport groups provides membranes with specific CO 2 transport pathways and finally leads to their high separation performance. In this study, a novel kind of polyelectrolyte membrane, quaternary ammonium polysulfone with interconnected ionic clusters, is prepared to enhance the CO 2 permeability. The hydrophilic quaternary ammonium groups tend to aggregate spontaneously to create ionic clusters. Furthermore, under humidified conditions, these ionic clusters are connected by water to form an ionic cluster network in the membrane matrix. The ionic cluster network plays the crucial role in accelerating the selective transport for CO 2 molecules over CH 4 by the reversible interaction between CO 2 and ion pairs. By tuning the quaternization degree of polysulfone, a series of polyelectrolyte membranes with different size of ionic clusters were developed. Membranes with hydrated ionic clusters (5–9 nm) show dramatic enhancement in CO 2 separation performance, especially in CO 2 permeability. The as-prepared quaternary ammonium polysulfone membrane with 8.98 nm ionic clusters exhibited the high CO 2 permeability of 1109.44 Barrer and a high CO 2 /CH 4 selectivity of 29.70, which exceeds 2008 Robeson upper bound limit. The optimized separation performance of QA-PSf membranes is attractive for potential application such as CO 2 capture from flue gas and natural gas.
研究领域:
材料科学
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化学工程
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环境科学
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产品关联
DOI
高影响因子
Polymers
·
2024
·Vol. 16
·期 3
·393
·
IF 4.7
Xiaoyu Du,Shijun Zhao,Yanqing Qu,Hongge Jia,Shuangping Xu,Mingyu Zhang,Guoliang Geng
Imidazole ionic liquids (ILs) have good affinity and good solubility for carbon dioxide (CO2). Such ionic liquids, combined with polyimide membrane materials, can solve the problem that, today, CO2is difficult to separate and recover. In this study, the ionic liquid (IL) of 1-ethyl-3-methylimidazolium tetrafluoroborate (IL1), 1-pentyl-3-methylimidazolium tetrafluoroborate (IL2), 1-octyl-3-methylimidazolium tetrafluoroborate (IL3), and 1-dodecylimidazolium tetrafluoroborate (IL4) with different contents were added to a polyimide matrix, and a series of polyimide membranes blended with ionic liquid were prepared using a high-speed mixer. The mechanical properties and gas separation permeability of the membranes were investigated. Among them, the selectivity of the PI/IL3membrane for CO2/CH4was 180.55, which was 2.5 times higher than the PI membrane, and its CO2permeability was 16.25 Barrer, which exceeded the Robeson curve in 2008; the separation performance of the membrane was the best in this work.
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2016
·
IF 1.207
Xiaoqing Wang,Libo Li,Jiangfeng Yang,Jinping Li
Two isomeric metal–organic frameworks (MOFs) with 2-dimensional (2D) and 3-dimensional (3D) topologies both comprised of Cu(II) and OTf (OTf = trifluoromethanesulfonate) ions were synthesized and characterized. The CO 2 , CH 4 and N 2 adsorption properties of the two isomeric MOFs were investigated from 263 K to 298 K at 0.1 MPa. The results showed that the 2D MOF exhibited a higher selectivity for CO 2 from CO 2 /CH 4 and CH 4 from CH 4 /N 2 compared to the 3D MOF, even though it possessed a lower surface area and pore volume. The higher adsorption heats of gases on the 2D MOF inferred the strong adsorption potential energy in the layered MOFs. Dynamic separation experiments using CO 2 /CH 4 and CH 4 /N 2 mixtures on the two MOFs proved that the 2D MOF had a longer elution time than the 3D MOF as well as better separation abilities.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Juanjuan Dai,Danyan Xie,Ying Liu,Zhiguo Zhang,Yiwen Yang,Qiwei Yang,Qilong Ren,Zongbi Bao
Supramolecular metal–organic frameworks (SMOFs) are emerging as a new family of porous materials. In this work, a SMOF, [Cu2(ade)4(H2O)2](SiF6)2 (SMOF-SIFSIX-1, ade = adenine) was successfully synthesized from the cationic complex of copper and adenine and hexafluorosilicate anions by a slow diffusion method and was demonstrated for trapping carbon dioxide in preference to methane and nitrogen. With one-dimensional pores of about 3.6 × 3.6 Å to induce their distinguishing interactions with the three components, SMOF-SIFSIX-1 exhibited excellent selective gas sorption behaviors for CO2/CH4 (50:50) and CO2/N2 (15:85) gas mixtures with ideal adsorbed solution theory selectivities of 21.1 and 131.7 at 273 K and 100 kPa pressure, respectively, outperforming most of reported hydrogen-bonded organic frameworks so far. Neutron powder diffraction and DFT-D calculations were also carried out to investigate the CO2 adsorption configuration on SMOF-SIFSIX-1a, which suggested that this framework catch CO2 due to “C···F” and “O···H” supramolecular interactions between CO2 molecules and SMOF-SIFSIX-1a. This study demonstrates that the rarely studied SMOF material shows promising potential in gas adsorption separation.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Tong Huang,Qiuyu Wu,Dong Qi,Feifan Yang,Yaqiong Xie,Guangru Zhang,Xin Liu,Gongping Liu,Haipeng Zhu
Natural gas upgrading demands advanced CO 2 /CH 4 separation membranes for CO 2 removal. Polymer of intrinsic microporosity (PIM-1) represents a novel polymeric molecular sieve featuring exceptional permeability and processability, but its moderate CO 2 /CH 4 selectivity remains challenging. Plasma treatment, a well-applied technique for surface modification of dense polymers, has been adopted to PIM with abundant interchain micropores for the first time. The physical alteration of plasma treatment in He gas atmosphere, primarily the chain scission, has significant impacts on CO 2 /CH 4 separation performance of PIM-1 membrane, by means of regulating its hierarchical microporous structure. Wide angle X ray scattering (WAXS) results suggest that the relatively large micropores are more prone to shrinkage and collapse than relatively small ones, which effectively enhances the selectivity. Moreover, owing to near-surface localization effect, the plasma modification is constrained within a skin layer onto a bulk intact layer. This asymmetric membrane structure allows the balance of enhancing CO 2 /CH 4 selectivity and sustaining high CO 2 permeability. By optimizing plasma input power and duration, the selectivity of plasma-treated PIM-1 membrane increased by 1.65 times, with a high permeability of over 4000 Barrer. After 2-month aging, the permeability was still maintained 60 % of its initial value. This suggests plasma treatment as a promising post-modification method for PIM CO 2 /CH 4 separation membranes.
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高影响因子
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