Energies
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2018
·Vol. 11
·期 2
·399
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IF 2.676
Rong Li,Xiao-Sen Li,Zhao-Yang Chen,Yu Zhang,Chun-Gang Xu,Zhi-Ming Xia
Tetra-n-butyl ammonium bromide (TBAB) was widely used in the research fields of cold storage and CO2hydrate separation due to its high phase change latent heat and thermodynamic promotion for hydrate formation. Agglomeration always occurred in the process of TBAB hydrate generation, which led to the blockage in the pipeline and the separation apparatus. In this work, we screened out a kind of anti-agglomerant that can effectively solve the problem of TBAB hydrate agglomeration. The anti-agglomerant (AA) is composed of 90% cocamidopropyl dimethylamine and 10% glycerol, which can keep TBAB hydrate of 19.3–29.0 wt. % in a stable state of slurry over 72 h. The microscopic observation of the morphology of the TBAB hydrate particles showed that the addition of AA can greatly reduce the size of the TBAB hydrate particles. CO2gas separation experiments found that the addition of AA led to great improvement on gas storage capacity, CO2split fraction and separation factor, due to the increasing of contact area between gas phase and hydrate particles. The CO2split fraction and separation factor with AA addition reached up to 70.3% and 42.8%, respectively.Keywords:CO2separation;TBAB;IGCC;anti-agglomerant;micromorphology;hydrate
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Yan-Mei Zhang,Li-Hao Xu,Xiao-Xue Hu,Bing-Hong Chen,Xin-Ru Chen,Qian-Qian Li,Heng Mao,Zhi-Ping Zhao
Metal-organic framework (MOF) membranes, by virtue of their high selectivity and low diffusion resistance, make a significant contribution to energy conservation and CO 2 emission reduction via separation technology. Despite possessing substantial potential for propelling the production of high-performance membranes, hurdles persist in the process of constructing MOF membranes that are both highly integrated and structurally sound on flexible polymer substrates. We propose a strategy for constructing highly stable cobalt zeolitic imidazolate framework (ZIF-67) composite membranes on seeded polyacrylonitrile (PAN) substrate. Through a timed-interrupted in-situ growth process, the amino-modified polycrystalline ZIF-67 as a CO 2 affinity layer is precisely and completely confined within the “top sites” and partial “face sites” of the vertical layered double hydroxide (LDH) precursor layer, creating a barrier-low passage for CO 2 as a fast diffusion layer. The substrate and the hybrid ZIF-67@LDH layer were robustly anchored together by the pre-embedded LDH seeds, thereby producing an appealing membrane-multilayer interlocked-support (MMIS) composite architecture. This fast diffusion-CO 2 affinity Pebax/ZIF-67@LDH/PAN membranes with MMIS architecture show average CO 2 permeability of 1487 Barrer and CO 2 /N 2 selectivity of above 55.1 after the surface repair coating of polyether-block-amide (Pebax), maintaining stable performance over 150 h, surpassing the Robeson upper bound. The Pebax/ZIF-67@LDH/PAN membranes also exhibit the durability and mechanical robustness, because of the highly inducible activity of LDH precursor layer serving as a linker between the membrane and substrate. These results promote the development of MOF-based membranes in practical separation applications.
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
SEPARATION SCIENCE AND TECHNOLOGY
·
2024
·
IF 2.3
Chengpeng Zhang,Hongjing Liu,Hanyu Qiu,Wei Zhao,Xu Zhao,Xiaochun Jing,Hui Yao
Nano-organic hybrid materials (Al2O3-NOHMs) were synthesized with nano-alumina as the core, γ-(2,3-epoxypropyl) propyl trimethoxysiane (KH560) as the corona, and three of polyetheramine M2070, D2000, M1000 as the canopy, respectively. Al2O3-NOHMs were used as fillers to prepare MMMs with Pebax as substrate to improve the CO2 separation performance. The Al2O3-NOHMs were characterized by TEM and rheological properties. The results showed that the synthesized Al2O3-NOHMs were liquid-like and had a core-shell structure, which can effectively reduce Al2O3 agglomeration in the membrane. FT-IR analysis of MMMs showed that Al2O3-NOHMs and Pebax were physically blended, TGA indicated that Al2O3-NOHMs do not affect the thermal stability of the membrane, and XRD indicated that the addition of Al2O3-NOHMs destroyed the interchain hydrogen bond of Pebax and reduced the crystallinity of MMMs. The gas permeability of the membrane was tested under ideal gas conditions, compared with pure membrane, the CO2 permeability of Al2O3-NOHM(M2070)/Pebax MMMs and Al2O3-NOHM(D2000)/Pebax MMMs reached 137.15 Barrer (24.68%) and 147.52 Barrer (34.11%), and the selectivity of CO2/N2 reached 77.82 (58.84%) and 72.31 (47.59%) at 30°C and 0.3 MPa, respectively, surpassing 2008 Robeson upper bound.
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
INORGANIC CHEMISTRY
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2022
·
IF 5.436
Yingwu Zhou,Yujie Ban,Weishen Yang
Reversible phase transformations (RPTs) of metal–organic frameworks not only create material diversity but also promise a self-restoration of crystals in a controllable manner. However, there are only limited examples because seeking for a convenient and effective trigger for RPTs, especially for RPTs with respect to spatiotemporal harmony in cleavage and reconstruction of metal–linker chemical bonds, is challenging. In this work, we found that zeolitic imidazolate framework (ZIF)-108 with Zn–N coordination bonds showing moderate strength was an ideal platform. We reported three crystal phases of ZIF-108, namely, sodalite (SOD), diamondoid (DIA), and large pore_sodalite (lp_SOD) topologies, and identified RPTs between phases: (1) when exposed to water or water vapor, the SOD structure could transform to a compact DIA version as a result of the decomposition of four-membered rings and synchronous reorganization of six-membered rings. Then, the DIA structure could also return back to SOD when soaked in dimethylformamide (DMF) or DMF vapor. (2) High-temperature treatment of SOD gives rise to lp_SOD, which then reverts to SOD by DMF. (3) lp_SOD could also be compressed into the DIA phase by water or water vapor and can then be restored via a two-step treatment, namely, soaking in DMF (DIA → SOD) right before a high-temperature therapy (SOD → lp_SOD). From the perspective of the separation utility, we found that the lp_SOD version of ZIF-108, relative to SOD-structured ZIF-108, can produce mixed matrix membranes having an interesting interfacial structure with the polymer chains, though both share the same chemical composition. We verified that the large pore of lp_SOD can allow being penetrated by polymer chains, which contributed to not only reinforcing the bi-phase interface but also sharpening the molecule sieve properties of fillers toward CO2 and CH4.
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
Journal of CO2 Utilization
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2024
·
IF 7.2
Heming Deng,Haoshuang Gu
Two-dimensional membranes are considered the next generation separation membrane with great application potential due to their excellent separation performance, good mechanical strength and thermal stability compared with traditional membrane materials. In this work, the flexible NH 2 -UIO-66@MXene membrane was successfully prepared for gas separation by loading NH 2 -UIO-66 particles onto Ti 3 C 2 nanosheets based on an in-situ growth strategy. A LiF-HCl mixed solution was used as the etchant to obtain the Ti 3 C 2 nanosheets. The loading of NH 2 -UIO-66 particles can regulate the interlayer spacing of Ti 3 C 2 nanosheets, improving the specific surface area of Ti 3 C 2 and the adsorption capacity for specific gases. The -NH 2 group in NH 2 -UIO-66 enabled preferential adsorption of CO 2 over H 2 , and the CO 2 molecules adsorbed in the channel can even block the molecules passing through, increasing the resistance of CO 2 diffusion. As a result, the NH 2 -UIO-66@Ti 3 C 2 hybrid membrane realizes the selective separation of H 2 /CO 2 mixed gas, and the separation selectivity is as high as 155. The gas separation selectivity and permeation of the final prepared NH 2 -UIO-66@MXene were enhanced and exceeded the upper limit of Robeson upper bound (2017).
研究领域:
材料科学
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化学工程
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Yueyangchao Yu,Yanting Tang,Longjie Liu,Qingnan Wang,Chongshan Yin,Keming Zhang,Chenlu Liu,Yi Ye,Xinglei Zhao,Tianhe Gu,Shaofei Wang
Covalent organic frameworks (COFs) show exceptional promise for CO2-selective mixed matrix membranes (MMMs) due to their tunable porosity and structural robustness. To mitigate COF aggregation in MMMs, we present an in situ growth strategy by directly integrating COF precursors into a polymer matrix. By optimizing reaction conditions, we achieve uniform dispersion and successful in situ formation of TpPa (derived from 1,3,5-triformylphloroglucinol and p-phenylenediamine) within the Pebax matrix. The optimized membrane exhibits a high CO2 permeability of 313.4 Barrer (45.8% higher than pure Pebax) and CO2/N2 selectivity of 22.6, along with long-term stability. Positron annihilation lifetime spectroscopy further reveals how the integration of COFs modulates the membrane’s free-volume properties. This study not only addresses filler dispersion challenges but also provides a viable approach for fabricating high-performance, stable CO2 separation membranes.
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Peng Li,Yuxiu Sun,Zhengqing Zhang,Zhenjie Gu,Zhihua Qiao,Chongli Zhong
Metal-organic frameworks (MOFs) have driven the development of polycrystalline membranes in the field of gas separation owing to the strong adsorption-desorption behavior and stable framework structure. However, the poor heterogeneous bonding ability between crystals and the substrate leads to the unsatisfactory gas separation as well as low stability of MOF membranes, especially in the humid environment . Herein, we prepared a thin and defect-free UiO-66 membrane by a crystal heterogeneous nucleation assisted growth strategy for efficient CO 2 /N 2 separation. The addition of small amount of water in the precursor solution promoted the crystal nucleation process on the substrate surface. Meanwhile, the smooth PDMS interlayer guaranteed the heterogeneous well-intergrown of crystals into thin UiO-66 membranes, and provided a hydrophobic environment. Therefore, the dense UiO-66 membrane with a small thickness exhibited a high CO 2 permeance (177.4 × 10 −9 mol·m −2 ·s −1 ·Pa −1 ) with moderate CO 2 /N 2 selectivity (24.3) under humid conditions. Furthermore, the prepared membrane demonstrated excellent renewable performance after dehumidification at high temperature, and maintained good hydrothermal stability during long-term operation under the humid environment. This work provides a new insight for the design of high-quality MOF membranes and promotes the development of MOF membranes in practical gas separation process.
研究领域:
材料科学
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化学工程
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气体分离技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Polymer Materials
·
2024
·
IF 4.4
Ziru Yu,Zhenghua Guo,Liang Yu,Xiao Feng,Bo Wang
Various metal–organic framework (MOF)-based porous nanomaterials have been adopted to fabricate mixed matrix membranes (MMMs) aiming at breaking through the Robeson upper bound of individual polymer membranes for gas separation. However, the insufficient compatibility between the polymeric matrix and MOF nanofillers limits the further improvement of their gas separation performance. To overcome this challenge, we constructed relatively ideal Pebax/PEG/NH2–UiO-66 mixed matrix membranes inspired by θ solvent theory of polymer solutions. Polyethylene glycol (PEG) molecules were introduced to selectively swell the polar poly(tetramethylene oxide) (PTMO) domains of the Pebax matrix via hydrophobic–hydrophilic interactions and in turn furnished dispersed “nests” for NH2–UiO-66 nanofillers with polar nature to reduce the interparticle agglomeration (PEG nesting effect). MOF nanofillers tended to be relatively undisturbed, in which either the rigidity of polymer chains or the pore blocking of MOFs seen in unideal MMMs was restricted. The PEG “nesting effect” proposed herein could bring benefits to further improve the allowed maximum loading capacity of MOF nanofillers as well as adjust the interactions therein and therefore maximize the CO2 separation performance of Pebax/PEG/NH2–UiO-66 MMMs. Compared with individual Pebax membranes, Pebax/PEG/NH2–UiO-66 with a 15 wt % loading of NH2–UiO-66 showed a 73% higher CO2 permeability (210 barrer) and a 220% higher CO2/N2 selectivity (130), which demonstrated the most dramatical increases among Pebax-based MMMs until now and as well significantly exceeded the Robeson upper bound. Therefore, the proposed PEG “nesting effect” for the preparation of θ-type MMMs holds promising potential for membrane-based carbon capture and is possibly extended to the preparation of other MMMs.
研究领域:
材料科学
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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
JOURNAL OF APPLIED POLYMER SCIENCE
·
2020
·Vol. 138
·期 20
·50424
·
IF 2.52
Junfeng Qian,Tingting Wu,Jianqun Shi,Hao Chang,Donghui Liu,Yichang Pan
Membrane-based technology is an attractive alternative in terms of CO 2 separation. Pebax-based membranes are regarded as potential candidates for CO 2 separation due to the favorable interaction between its poly (ethylene oxide) chains with CO 2 molecules and inorganic fillers. However, the separation performance for CO 2 /CH 4 mixture is still suffered from the moderate gas permeability and selectivity. To overcome this problem, in this work, amino-functionalized zeolite imidazolate framework (ZIF-7-NH 2 ) nanocrystals were used as fillers to blend with Pebax 1657 for fabricating mixed-matrix membranes (MMMs). XRD, Brunauer–Emmett–Teller (BET), scanning electron microscope, and 1 H nuclear magnetic resonance characterization indicated that ZIF-7-NH 2 with the highest crystallinity was synthesized. Fourier transform infrared spectroscopy, thermogravimetric analysis, differential scanning calorimetry (DSC), and Young's modulus showed that it has good interfacial interaction. Gas separation test results showed that both the CO 2 permeability and CO 2 /CH 4 selectivity of the 31 wt% ZIF-7-NH 2 /Pebax MMMs increased by 80 and 170%, respectively. The improved performance is attributed to the addition of ZIF-7-NH 2 nanocrystals and the favorable interfacial interactions between the polymer and ZIF-7-NH 2 nanocrystals. Furthermore, the polyvinylidene fluoride supported hollow fiber composite membranes also exhibit the long-term stability for CO 2 /CH 4 separation.
研究领域:
材料科学
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化学工程
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Lei Hou,Zhe Wang,Zhaoyu Chen,Wenbo Chen,Cancan Yang
PIM-1 and poly(arylene fluorene ether ketone) (Am-PAFEK) were synthesized by polycondensation . Their structures were characterized by 1 H NMR and FT-IR spectral analyses. A series of flexible and transparent blend membranes were prepared by solution blending with different ratios of PIM-1 and Am-PAFEK. DSC and SEM analyses showed good compatibility between them. PIM-1 and Am-PAFEK in the blend membrane perform their respective functions. The former provides excellent permeability; the latter provides high selectivity for CO 2 . Addition of 20% Am-PAFEK into the blend membrane increased the gas separation selectivity of CO 2 /CH 4 and CO 2 /N 2 by 75% and 65%, respectively. The optimum separation performance was achieved with blend membrane with a CO 2 permeability of 752.4 Barrer and a CO 2 /N 2 selectivity ratio of 26.7, extremely close to the Robeson upper bound (2008). After 140-days aging test, the blend membranes still maintained above 70% CO 2 permeability, indicating that it has good antiaging properties. Consequently, the new type of membranes have great potential in industrial 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
DALTON TRANSACTIONS
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2025
·
IF 3.3
Zhaojie Wang,Xinle Sun,Qinglong Liu,Caifeng Xia,Qikang Yin,Siyuan Liu,Xiaoqing Lu,Hongyu Chen
Mixed matrix membranes (MMMs), which incorporate metal-organic frameworks (MOFs) nanofillers within a polymer matrix, offer a highly promising solution for CO2 capture and separation. However, poor interfacial compatibility and filler aggregation in MMMs pose significant challenges to enhancing CO2/N2 separation performance. Here, we present a novel approach using amino ionic liquid modification to optimize MMMs, where the modified AFIL promotes the formation of ZIF-8 with well-defined facets and sharp edges, and enhances the compatibility between ZIF-8 particles and PIM-1 polymer matrix for favorable CO2 affinity and selective CO2 transport. The resulting 10 wt.% AFIL@ZIF-8/PIM-1 exhibits exceptional gas separation performance with a CO2 permeability of 7864262.2 Barrer and a CO2/N2 selectivity of 29.661.96. More importantly, the incorporation of AFIL into the ZIF-8 pores significantly enhances the thermal stability and aging resistance of AFIL@ZIF-8/PIM-1 MMMs via structural support and hydrogen bonding interactions. This work provides a practical approach to developing hybrid membranes for CO2/N2 separation, showcasing improved overall performance and strong interfacial compatibility.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Li Peng,Zhaofeng Duan,Shumin Cen,Xuehong Gu
High-silica CHA (SSZ-13) zeolites membranes, with pore size between the molecular size of CO 2 and N 2 or CH 4 , are promising for some industrial CO 2 separation process. Considering water is typically present in these industrial gas feed and the negative impact of moisture on the membranes’ gas permeation, it is highly desirable to increase the surface hydrophobicity of membranes to reduce the adsorption of water. In this paper, a W-doping strategy was proposed to increase the hydrophobicity of SSZ-13 membranes by eliminating the silanols on the surface, and the W-doped high-silica CHA (W-SSZ-13) zeolite membranes were prepared for the first time. Characterizations such as SEM, XRD, and XPS confirmed the successful incorporation of W into CHA membrane. The incorporation of W reduced the pore mouth size, and the W-SSZ-13 zeolite membranes showed improved CO 2 /N 2 and CO 2 /CH 4 separation performance. After W-doping, the maximum separation factors ( α max ) for the CO 2 /N 2 mixture with equimolar composition under dry conditions increased from 8.8 to 16.9, and for the equimolar CO 2 /CH 4 mixture, the value increased from 105.9 to 176. The W-SSZ-13 membranes also showed better separation performance under wet conditions. For both systems, the W-SSZ-13 membrane showed higher α max and less CO 2 permeance reductions, indicating a more resistance in wet conditions.
研究领域:
材料科学
·
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）