JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Run Li,Ying Yang,Zezhou Zhang,Shaohan Lian,Quan Zhao,Chunfeng Song
As a promising strategy to reduce greenhouse gas emissions, carbon dioxide capture from industrial and power plants has been proposed. Due to its advantages of low consumption and a modest environmental impact, membrane technology has been widely used in the gas separation process. Advanced porous fillers can be successfully added into the polymer matrix to create mixed matrix membranes (MMMs) with simple processing and applicable gas separation performance. The high porosity and stability of microporous carbon materials make them desirable for use in the gas separation process. Herein, N-doped microporous carbon microparticles (NMCP) were successfully synthesized and incorporated into UV crosslinked polyethylene oxide (XLPEO) matrix membranes. Fast CO 2 transport channels are created in MMMs by rationally constructing NMCP fillers with ultra-micropores (∼0.53 nm), high-content heteroatoms (N, 13.94%), and two-dimensional morphology. The relationship between the structure of the NMCP samples and the gas separation performance of MMMs was discussed. Additionally, tests were conducted on the effects of NMCP loading, operating conditions, and long-term stability of NMCP/XLPEO membranes. NMCP/XLPEO membranes with a 2.5 wt% NMCP loading displayed a CO 2 permeability of 606 Barrer and a CO 2 /N 2 selectivity of 56.4, approaching the 2019 upper bound. This work offers a novel perspective to build fast gas transport channels in porous carbon-based MMMs for carbon capture.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Rui Ding,Ziheng Li,Yan Dai,Xiangcun Li,Xuehua Ruan,Jiaming Gao,Wenji Zheng,Gaohong He
The amino functionalization of MOFs has been verified to be effective in improving the selective permeation of CO 2 . However, the introduction of amino groups into ZIF-8 by mixed ligands strategy is hard to achieve due to the high steric hindrance of benzene ring in 2-aminobenzimidazole ligand, resulting in insufficient content of amino groups. Therefore, in this work, polystyrene-acrylate (PSA) template is proposed to provide abundant adsorption and reaction sites for the rapid synthesis of NH 2 -ZIF-8 with high content of 2-aminobenzimidazole. Furthermore, the incomplete etching strategy is used to construct PSA modified hollow NH 2 -ZIF-8 nanospheres (PHNZ). Importantly, the thickness of PSA layer and the hollow size are adjusted by the etching time, as revealed by the SEM and TEM images. In this PHNZ, the modified PSA can provide good interface compatibility between PHNZ and Pebax matrix to enhance the CO 2 selectivity, while the hollow structure can reduce the mass transfer resistance and improve the gas permeability. Moreover, the introduced amino groups can enhance the CO 2 affinity of PHNZ and further improve the CO 2 /N 2 selectivity of the PHNZ-based mixed matrix membranes (MMMs). Benefiting from the synergy of good interface compatibility and enhanced CO 2 affinity from the amino groups, the PHNZ/Pebax MMMs present greatly improved CO 2 /N 2 selectivity in contrast with pure Pebax and NH 2 -ZIF-8 based membranes. Besides, as the etching time increases, the PHNZ-2 and PHNZ-3 based MMMs present a higher CO 2 permeability than that of NH 2 -ZIF-8 based MMM, revealing the significance of the hollow structure. The PHNZ-2/Pebax MMM with filler loading of 10 wt% expresses the best gas separation performance with the CO 2 permeability of 121.9 Barrer and CO 2 /N 2 selectivity of 96.6, respectively, showing an increase of 54.7 % and 98.0 % in contrast with pure Pebax membrane. Meanwhile, this CO 2 separation performance is far beyond the Robeson upper bound in 2008 and close to the McKeown upper bound in 2019, demonstrating that the proposed PHNZ displays a promising and competitive potential in MMM based CO 2 capture.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Wenbo Chen,Zhenguo Zhang,Lei Hou,Cancan Yang,Hongcheng Shen,Kai Yang,Zhe Wang
This work mainly studies the CO 2 separation performance of a new type mixed-matrix membranes (MMMs) based on MOF-801 as the microporous filler and PIM-1 as the polymer matrix. MMMs was successfully formed via simple casting/solvent evaporation approach at room temperature. The samples were systematically characterized by SEM, XRD, TGA and FTIR, the permeability-selectivity of MMMs to CO 2 , O 2 and N 2 was studied by gas permeability test. The experimental results show that the uniform dispersion of the CO 2 -philic MOF-801 filler provides a channel for the rapid and selective transport of CO 2 , so the MOF-801/PIM-1 MMMs revealed much higher CO 2 permeability and CO 2 /N 2 ideal selectivity (CO 2 = 9686 Barrer, CO 2 /N 2 = 27, all selectivity in the paper is ideal) than pure polymer membrane. After 90-days aging test, the CO 2 permeability of MMMs remains above 70%, which reflects its good anti-aging performance. After 120 h continuous gas permeability test, it also shows good long-term working stability. The experimental results show that the good gas separation performance of MMMs exceeds the Robeson upper bound (2008), showing good application prospect for practical greenhouse gas CO 2 separation.
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Membranes
·
2021
·Vol. 11
·期 9
·693
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IF 4.106
Fei Guo,Bingzhang Li,Rui Ding,Dongsheng Li,Xiaobin Jiang,Gaohong He,Wu Xiao
Mixing a polymer matrix and nanofiller to prepare a mixed matrix membrane (MMM) is an effective method for enhancing gas separation performance. In this work, a unique UiO-66-decorated halloysite nanotubes composite material (UiO-66@HNT) was successfully synthesized via a solvothermal method and dispersed into the Pebax-1657 matrix to prepare MMMs for CO2/N2separation. A remarkable characteristic of this MMM was that the HNT lumen provided the highway for CO2diffusion due to the unique affinity of UiO-66 for CO2. Simultaneously, the close connection of the UiO-66 layer on the external surface of HNTs created relatively continuous pathways for gas permeation. A suite of microscopy, diffraction, and thermal techniques was used to characterize the morphology and structure of UiO-66@HNT and the membranes. As expected, the embedding UiO-66@HNT composite materials significantly improved the separation performances of the membranes. Impressively, the as-obtained membrane acquired a high CO2permeability of 119.08 Barrer and CO2/N2selectivity of 76.26. Additionally, the presence of UiO-66@HNT conferred good long-term stability and excellent interfacial compatibility on the MMMs. The results demonstrated that the composite filler with fast transport pathways designed in this study was an effective strategy to enhance gas separation performance of MMMs, verifying its application potential in the gas purification industry.Keywords:composite material;UiO-66;HNT;mixed matrix membrane;CO2/N2separation
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NEW JOURNAL OF CHEMISTRY
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2019
·Vol. 43
·期 24
·9725-9731
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IF 3.069
Suresh Mutyala,Sobhy M. Yakout,Shebl S. Ibrahim,Madhavi Jonnalagadda,Harisekhar Mitta
Iron metal–organic framework, MIL-100(Fe) was prepared by a hydrothermal method and used as a support to incorporate diethylenetriamine (DETA) for the study of CO2 adsorption and separation of CO2/N2. All synthesized adsorbents were characterized by PXRD, N2 adsorption–desorption isotherms, FT-IR, TGA, SEM, and elemental analysis. Structural characterization results have revealed that the structure of MIL-100(Fe) was not changed by the incorporation of diethylenetriamine. The CO2 adsorption capacities were 29 cm3 g−1 and 41 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. Adsorption of CO2 on DETA–MIL-100(Fe) was higher than that on MIL-100(Fe). The enhancement was due to the presence of amine groups which could form ammonium carbamate by interaction with CO2. Similarly, the N2 adsorption capacities were 3 cm3 g−1 and 0.9 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. The decrease in N2 adsorption capacity was due to the decrease in surface area. The selectivity of CO2/N2 on DETA–MIL-100(Fe) was four times higher than that on MIL-100(Fe). The heat of CO2 adsorption was 74.2 kJ mol−1 at low coverage of CO2 on DETA–MIL-100(Fe) and the CO2 adsorption capacity was constant in each adsorption cycle over the same adsorbent.
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CHINESE CHEMICAL LETTERS
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2014
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IF 1.178
Wei Wang,Ye Yuan,Fu-Xing Sun,Guang-Shan Zhu
Novel porous aromatic frameworks (PAF-53 and PAF-54) have been obtained by the polymerization of amino compound ( p -phenylenediamine and melamine) and cyanuric chloride. They display a certain amount of CO 2 adsorption capacity and highly selective separation of CO 2 /CH 4 and CO 2 /N 2 as 18.1 and 83 by Henry Law respectively. They may be applied as ideal adsorbents to separate and capture CO 2 .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2015
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IF 2.587
Song Zhao,Xiaochang Cao,Zijian Ma,Zhi Wang,Zhihua Qiao,Jixiao Wang,Shichang Wang
In this work, imidazolate framework ZIF-8 nanoparticles were synthesized and incorporated into a poly(vinylamine) (PVAm) coating solution. The chemical structure of a PVAm/ZIF-8 film was characterized by X-ray diffraction and attenuated total reflectance Fourier transform infrared spectroscopy techniques. Mixed-matrix membranes (MMMs) were developed by coating the PVAm/ZIF-8 mixed dispersion on a polysulfone (PSf) support membrane. Surface and cross-sectional scanning electron microscopy images of the MMMs were employed to observe the dispersion of nanoparticles in the polymer matrix. The CO2 permeance and CO2/N2 selectivity of the MMMs were evaluated by using a CO2/N2 mixture gas. Optimal preparation parameters for the MMMs were achieved by varying the incorporated ZIF-8 contents in the coating solution and the wet coating thickness. The effect of incorporated ZIF-8 on improving the gas permselectivity was revealed, and the mechanism of CO2-facilitated transport in the PVAm/ZIF-8/PSf membrane was analyzed. The CO2/N2 separation performance of PVAm/ZIF-8/PSf membranes with different wet coating thicknesses was also evaluated at 22–60 °C to analyze the changes of the gas permselectivity with increasing temperature.
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 7
·2957-2963
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IF 3.5
Peng Zhang,Sai Ma,Yujuan Zhang,Chaohui He,Tuoping Hu
The energy-saving separation of CO2/N2 and CH4/N2 in the energy industry facilitates the reduction of greenhouse gas emissions and replenishes energy resources, but is a challenging separation process. The trade-off between adsorption capacity and selectivity of the adsorbents is one of the key bottlenecks in adsorption separation technologies’ large-scale application in the above separation task. Herein, we introduced a series of fluoroborate or fluorosilicate salts (Cu(BF4)2, Zn(BF4)2 and ZnSiF6) into the open coordination nitrogen sites of aluminum-based metal–organic frameworks (MOF-253) to create multiple binding sites to simultaneously enhance the adsorption capacity and selectivity for the target gas. By the synergistic adsorption effect of metal ions (Cu2+ or Zn2+) and fluorinated anions (BF4− or (SiF6)2−), the single-component adsorption capacity and selectivity of salt-modified MOF-253 (MOF-253@Cu(BF4)2, MOF-253@Zn(BF4)2 and MOF-253@ZnSiF6) for CO2 and CH4 were effectively improved when compared to pristine MOF-253 at 298 K and 1 bar. In addition, the salt-modified MOF-253 has a moderate adsorption heat (<30 kJ mol−1) which could be rapidly regenerated at low energy by evacuation desorption. As confirmed by the ambient breakthrough experiments of MOF-253 and MOF-253@ZnSiF6, the real separation performance for both CO2/N2 (1/4) and CH4/N2 (1/4) was obviously improved. This work provides a feasible post-modification strategy on uncoordinated sites of the framework to improve adsorption separation performance and promote the development of ideal adsorbents with a view to realizing their application in the energy industry.
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INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
Wenjing Zhao,Shanjian Liu,Ning Li,Jiawen Zhang,Guanshuai Zhang,Shuntao Xu
The product distribution of cellulose pyrolysis at varying nitrogen carrier and temperature was studied in a tube furnace, elucidating the reaction mechanism of cellulose and urea (chitosan) in CO 2 pyrolysis. The nitrogen-rich pyrolysis in CO 2 atmosphere improves the nitrogen compound content in bio-oil. CO 2 , serving as a mild oxidizing agent, enhances the production and release of biochar volatiles and the creation of additional pores. This leads to an improved development of porosity across the micropore, mesopore, and macropore ranges. When the mixing ratio of urea is 60% at 550 ℃, the highest nitrogen compound content is 45.03%, which is 1.7 times higher than that in N 2 atmosphere. When the mass mixture ratio of chitosan is less than 60%, its content reaches its maximum at 500 ℃, reaching 13.32%, which is 1.2 times the content under N 2 atmosphere. The formation paths of oxygen compounds (aldehydes, ketones and alcohols) and main nitrogen compounds (pyridine, pyrrole, imidazole and pyrazine) in bio-oils under CO 2 atmosphere are discussed. The coupling relationship between biochar N functional groups and the generation of bio-oil N heterocyclic substances was proposed.
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DESIGNED MONOMERS AND POLYMERS
·
2018
·
IF 1.37
Liang Xu,Tianyang Lei,Boyu Jing,Yu Zang,Fengjuan Miao,Toshiki Aoki,Masahiro Teraguchi,Takashi Kaneko
Three soluble hyperbranched polyazomethines containing oligosiloxane end group HBP-PAZ-SiOn were successfully synthesized. HBP-PAZ-SiOns were used as modifiers of ethyl cellulose (EC) and polysulfone (PS) membranes. Blend membranes, HBP-PAZ-SiOn/EC and HBP-PAZ-SiOn/PS were prepared by blending the THF solution of HBP-PAZ-SiOn with ethanol solution of EC and dichloromethane solution of PS, respectively. Surprisingly, the permeabilities for CO2 of the blend membranes were more than 15–16 times higher than those of pure EC and PS membranes without any drop of pemselectivity to N2. This unusual improvement has been achieved by both enhancement of diffusivity for carbon dioxide and nitrogen by the oligosiloxane groups and enhancement of affinity of the amino groups with carbon dioxide at the end groups of HBP-PAZ-SiOn.
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JOURNAL OF POROUS MATERIALS
·
2025
·
IF 3.2
Shen Fumin,Yao Shunyang,Pei Yuanchao,Sun Rubin
The increasing levels of carbon dioxide (CO 2 ) emissions driven by industrial activities highlight the urgent need for the development of efficient and sustainable CO 2 capture technologies. Biomass-derived porous carbons have emerged as promising candidates for CO 2 adsorption due to their low cost, high surface area, and adjustable pore structure. In this study, hierarchically porous carbons (HPCs) were synthesized from waste acer truncatum wood through pre-carbonization and subsequent KOH activation. The synthesis conditions, including activation temperature and activating agent concentration, were optimized to precisely tailor the pore architecture. The resulting HPC exhibited excellent CO 2 adsorption capacities of 7.56 mmol·g⁻ 1 at 0 °C and 4.29 mmol·g⁻ 1 at 25 °C under ambient pressure. Notably, ultramicropores (< 0.7 nm) exhibited a dominant role in CO 2 capture at low pressures, while narrow micropores (< 1.0 nm) contributed significantly across a range of low-pressure conditions. The hierarchical pore structure enhanced CO 2 uptake at higher pressures. Furthermore, the material demonstrated exceptional CO 2 /N 2 selectivity, reaching up to 112 at 0.15 bar and 0 °C, along with good cyclic stability, highlighting its potential in post-combustion CO 2 capture. This work provides a sustainable strategy for converting waste biomass into high-value adsorbents, offering a solution that addresses both environmental concerns and economic feasibility.
研究领域:
环境科学
·
材料科学
·
碳材料
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气候变化缓解
·
吸附技术
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Jia Wang,Yizhen Situ,Wenyu Zheng,Weidong Zhang,Qingyuan Yang
Polymer transport resistance was tuned by controlling the solvent evaporation rate. • Reduced polymer transport resistance promoted a more effective contribution of ZIF-8 transport pathways to CO 2 /N 2 separation. • The 7.8 wt% in situ-grown MMM achieved a CO 2 permeability of 510 Barrer and a CO 2 /N 2 selectivity of 33.0. Beyond filler modification, regulating the polymer structure is also crucial for optimizing gas transport in mixed-matrix membranes (MMMs), yet this aspect remains insufficiently explored. Herein, the solvent evaporation rate was controlled to regulate the transport resistance of Pebax 2533 and elucidate its influence on the transport contribution of ZIF-8 in ZIF-8/Pebax MMMs for CO 2 /N 2 separation. For Pebax 2533 membranes, increasing the evaporation rate reduced both crystallinity and relative fractional free volume, resulting in a non-monotonic variation in CO 2 permeability and a decrease in CO 2 /N 2 selectivity. At a moderate evaporation rate of 2.5 × 10 −5 kg·m −2 ·s −1 , the balance between reduced crystallinity and preserved free volume resulted in lower polymer transport resistance, enabling the contribution of ZIF-8 to be more effectively translated into membrane separation performance. As a result, the in situ-grown MMM containing 7.8 wt% ZIF-8 achieved a CO 2 permeability of 510.0 Barrer and a CO 2 /N 2 selectivity of 33.0, with its CO 2 permeability exceeding that of most reported Pebax-based MMMs. This work demonstrates that controlling solvent evaporation is an effective strategy to regulate polymer transport resistance and enhance the contribution of ZIF-8 in MMMs. Download: Download high-res image (207KB) Download: Download full-size image
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