Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Liwei Sun,Meilin Yin,Shaokun Tang
In this work, short-chain bi-functionalized ionic liquid (IL) was grafted onto mesoporous alumina (MA) for ideal CO 2 /N 2 selectivity . First, bi-functionalized IL 1-(2-carboxymethyl)-3-methoxyethyl-imidazolium bromide ([CmMOEim][Br]) with ether and carboxyl group was successfully synthesized and the initial decomposition temperature is 165 °C. Then low-cost hydroxyl-MA (MA-OH) was obtained from ordered MA (OMA) with the assist of 30 wt% H 2 O 2 solution to prepare [CmMOEim][Br]-grafted MA with different molar ratios of [CmMOEim][Br] and MA-OH via facile chemical reaction without the introduction of alkoxysilanes . MA-OH material presents slit-like structure and more hydroxyl groups compared to OMA sample before hydroxylation. Crystal structure and morphology of grafted material remains unchanged after grafting process. [CmMOEim][Br] is successfully grafted onto MA-OH via the chemical link of carboxyl group on IL and hydroxyl group on MA-OH. Finally, CO 2 and N 2 capture capacities of different materials were separately evaluated at 0.1 MPa and 25 °C. With the increase of IL dosage, CO 2 capture capacity of the grafting material first enhances and then decreases while N 2 capture capacity gradually falls owing to the high CO 2 affinity of [CmMOEim][Br]. Wherein, [CmMOEim][Br]-grafted MA-0.15 exhibits the optimum CO 2 capture capacity of 45.3 cm 3 /g at 25 °C and ambient pressure. The ideal CO 2 /N 2 selectivity of [CmMOEim][Br]-grafted MA can reach up to 30 based on single-component adsorption isotherms , which is higher than that of [CmMOEim][Br] and MA-OH. Furthermore, CO 2 capture capacity, morphology and structure of [CmMOEim][Br]-grafted MA maintain well even after ten cycles.
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ACS Applied Materials & Interfaces
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2020
·
IF 8.758
Yunlei Shi,Dazhen Xiong,Zhiyong Li,Huiyong Wang,Jikuan Qiu,Hucheng Zhang,Jianji Wang
In recent years, metal–organic frameworks (MOFs) have been explored as emulsifiers for the fabrication of Pickering emulsions and then used for hybrid material synthesis and interface catalysis. Nevertheless, stimuli-responsive Pickering emulsions stabilized by MOFs have been rarely reported so far, although they are of great importance for fundamental research studies and practical applications. Herein, for the first time, triethylenetetramine (TETA)-functionalized MOFs (ZIF-90/TETA) have been designed, synthesized, and used for fabricating CO2-/N2-response Pickering emulsions. It is shown that even at the ZIF-90/TETA content of 0.25 wt %, the functional MOF can still efficiently emulsify n-hexane and water to form a high internal phase Pickering emulsion. Importantly, the Pickering emulsion can be easily and reversibly switched between emulsification and demulsification by bubbling of CO2 and N2 alternatively at atmospheric pressure. The possible mechanism of the CO2/N2 switchable emulsion is investigated by zeta potential, water contact angle, interfacial tension, 13C NMR spectroscopy, and an optical microscope. It is found that the acid–base reaction of CO2 with TETA anchored on the surface of ZIF-90 leads to the production of hydrophilic ammonium bicarbonate and carbamate, which results in the emulsification of the Pickering emulsion. However, when N2 is bubbled to remove CO2, the reverse reaction takes place to cause the demulsification of the Pickering emulsion. Moreover, the CO2/N2 switchable Pickering emulsion has been successfully used as a microreactor for Knoevenagel reactions to demonstrate a highly efficient integration of chemical reaction, product separation, and ZIF-90/TETA recycling for a sustainable chemical process.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Li Peng,Li Zhao,Guang Pan,Xuehong Gu
The separation of CO 2 from N 2 using MFI-type zeolite membranes relies on a mechanism dominated by adsorption and diffusion processes. In this investigation, we employed a tungsten (W) doping approach to elevate the CO 2 separation selectivity of MFI zeolite membranes. Isothermal adsorption assessments demonstrated an elevated heat of adsorption (Q st ) for CO 2 and a reduced pore sizes after W doping, corroborating the enhanced CO 2 /N 2 separation efficiency observed. Specifically, the W-doped MFI membrane exhibited a selectivity of 38.8 under dry conditions, a substantial improvement over the 8.7 selectivity achieved by the undoped Si-MFI membrane, while the CO 2 permeance remained comparable (3.9 × 10 -7 vs 4.5 × 10 -7 mol·m -2 ·s -1 ·Pa -1 ). Furthermore, the incorporation of tungsten curtails the formation of silanol groups by stabilizing the zeolite framework via energetically favorable W-O-Si linkages. These linkages diminish silanol-related defects, typically prone to water adsorption, thereby enhancing the membrane’s hydrophobicity. Consequently, the W-doped MFI membrane maintains a CO 2 /N 2 selectivity of 29.5 and a CO 2 permeance of 1.8 × 10 -7 mol·m -2 ·s -1 ·Pa -1 in the humid environments, outperforming most reported zeolite membranes and showing potential ability for practical post-combustion carbon capture applications.
研究领域:
材料科学
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环境工程
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化学工程
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhaohao Li,Tianjing An,Jiaxi Yang,Dan Gao,Hongyuan Zhang,Heng Zhang
Capturing CO 2 from the flue gas in the power plant is an important measure to realize the low-carbon combustion of the fossil energy. This paper presents a novel technique which combines traditional methods of the chemical absorption, the physical adsorption and the membrane absorption. The ionic liquid ([TEPA][MIm]) is utilized to improve the CO 2 absorption performance and reduce the energy consumption. While the porous skeleton (ZIF-8) is added to the ionic liquid to reduce the viscosity while introducing the physical adsorption. Moreover, the hydrophobic ceramic membrane is utilized as the separation interface between the gas phase and the liquid phase, which can avoid the entrainment and overflow of the liquid phase while increasing the specific surface area. In terms of the material preparation and the characterization, the addition of ZIF-8 does not destroy the original chemical composition of [TEPA][MIm]. The average contact angle of the hydrophobic ceramic membrane is 140.55°, and the failure temperature is greater than 400 K, which conforms to the application situation of the power plant. In terms of the CO 2 capture and the desorption performance, the maximum CO 2 capture amount reaches 2.03 mol/mol. The temperature of complete desorption is 70 °C. Furthermore, the capture performance after five cycles can reach 80 % of the initial performance. The performance is better than that of the CO 2 capture technology utilizing the traditional monoethanolamine solution.
研究领域:
能源与环境工程
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材料科学
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2012
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IF 3.85
Juan Zhao,Zhi Wang,Jixiao Wang,Shichang Wang
Polyaniline nanofibers, netlike polyaniline nanofibers and polyaniline nanosheets were prepared by chemical oxidative polymerization. Scanning electron microscopy (SEM) was employed to characterize morphology of the polyaniline (PANI) nanoparticles . The nanocomposite membranes were prepared by blending PANI nanoparticles with polyvinylamine (PVAm) as the active layer and polysulfone (PS) as the support layer. The surface and cross-section morphology and crystallization of nanocomposite membranes were measured by SEM and XRD. The permselectivity of nanocomposite membranes was investigated by the pure CO 2 and N 2 gases and gas mixture containing 20 vol.% CO 2 and 80 vol.% N 2 . The results demonstrate that the inclusion of the PANI nanoparticles to PVAm increases the gas permeance and selectivity of the membranes due to chain packing disruption of PVAm and N 2 barrier property of PANI nanoparticles. The influences of PANI nanoparticles, PVAm and the interaction between PANI and PVAm on gas transport properties of nanocomposite membranes have been discussed. At CO 2 partial pressure of 0.02 MPa, the nanocomposite membrane containing 17 wt.% PANI nanosheets displayed a CO 2 permeance of 1200 GPU and a CO 2 /N 2 selectivity of 120. The permeance increased about 852% and the selectivity increased about 137% compared with the PVAm/PS membrane. The separation performance stability of the PVAm/PS membrane and PANI–PVAm/PS membrane was investigated and no deterioration in membrane permselectivity was observed.
研究领域:
材料科学
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膜技术
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气体分离
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聚合物纳米复合材料
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环境工程
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DOI
高影响因子
AICHE JOURNAL
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2023
·Vol. 69
·期 5
·e18025
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IF 3.7
Chenxu Geng,Yuxiu Sun,Zhengqing Zhang,Zhihua Qiao,Chongli Zhong
Mixed matrix metal–organic framework (MOF) membranes show excellent application prospects in gas separation. However, their stability in various practical application scenarios is poor, especially under humid conditions. Herein, we encapsulated a hydrophobic ionic liquid (IL) into the cavity of MOFs, which effectively mitigated the competition between H 2 O and CO 2 in humid gas mixtures, leading to stable and high-performance gas separation. For this reason, the resulting membranes using polymer of intrinsic miroporosity-1 (PIM-1) as a polymer matrix show good CO 2 /N 2 separation performance and long-term test stability under humid environment. In particular, the 20 wt% IL-UiO/PIM-1 shows a high permeability of 13,778 Barrer and competitive CO 2 /N 2 separation factor of ~35.2, transcending the latest upper bound. Besides, the according membrane module exhibits slightly decreased CO 2 permeability and selectivity, promoting the application of self-supporting membranes. This work provides a reliable strategy for the rational design of MOF-based hybrid membranes under extreme conditions.
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Chemistry-An Asian Journal
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2021
·Vol. 16
·期 20
·3141-3150
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IF 4.568
Haoyu Wang,Jing Zheng,Jing Zhao,Wanqin Jin
Graphical Metal ions are successfully incorporated into GO channels , which contribute to facilitating CO 2 transport, decreasing N 2 solubility, hindering N 2 diffusion, and form multiple interactions with GO nanosheets, thus achieving the remarkably improved CO 2 /N 2 separation performance (with separation factor increasing 12.2 times) and excellent long-term stability. Graphene oxide (GO) membranes holds great potential for high-performance CO 2 capture. Aiming at enhancing the CO 2 separation performance and structural stability of GO membranes, functionalizing GO channels with metal ions confers a promising strategy. In this study, we reported the fabrication of metal ion-incorporated GO membranes with remarkably improved CO 2 /N 2 separation performance. The metal ions within GO channels contribute to facilitating CO 2 transport, decreasing N 2 solubility, hindering N 2 diffusion, and form multiple interactions with GO nanosheets. After introducing Mg 2+ ions, the CO 2 /N 2 separation factor of GO membrane is remarkably increased from 4 to 48.8 with the CO 2 permeance increases 1.5 times. Moreover, the separation performance of the GO-Mg 2+ membranes shows an excellent long-term stability owing to the structural robustness. This study could provide insights into the regulation of the microstructure of metal ion-functionalized GO membranes for highly selective transport of specific molecules.
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高影响因子
ACS Applied Polymer Materials
·
2025
·
IF 4.7
Yanling Liu,Xiao Peng,Yuan Li,Fei Wang,Xue Ai,Yuxi Huang,Xin Sun,Jie Zhao,Kai Li
Membrane separation technology has garnered significant attention for CO2 separation and purification, with mixed matrix membranes (MMMs) emerging as promising candidates due to their advantages of ease of processing, high mechanical strength, and thermal stability. The development of effective fillers for separation performance becomes one of the key foci in this area. In this work, CC3, a type of porous organic cages (POCs), was synthesized and functionalized with two amino-containing materials of different chain lengths. Polyethylenimine (PEI) and diethylenetriamine were used as modification agents to successfully graft amino groups onto the CC3 crystals to form defect-free Pebax mixed matrix membranes containing amino-functionalized CC3. The special porous structure of CC3 increases the gas permeability of the mixed matrix membrane by providing extra channels for the transportation of CO2. Besides, amino groups on functionalized CC3 interact with the chains of Pebax through hydrogen bonding, thus improving the compatibility between filler and matrix. The amino groups can further facilitate the transport of gases across the membrane through reversible reactions with CO2, which is further enhanced under humid conditions. Under optimal conditions, at 1 bar and 30 °C, the CO2 permeability of Pebax/PEI@CC3-MMMs was 342.33 Barrer with a selectivity of 33.38, while Pebax/DETA@CC3-MMMs exhibited a CO2 permeability of 273.34 Barrer and a selectivity of 35.77. This work demonstrates that amino-functionalized POCs (CC3) can effectively enhance the CO2 permeability and the CO2/N2 selectivity, which may provide a way to develop high-performance mixed matrix membranes with superior separation properties.
研究领域:
材料科学
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环境科学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Kaifang Wang,Danlin Chen,Jiali Tang,Zihao Hong,Zhongtai Zhu,Ziyi Yuan,Zhihong Lin,Yuqi Liu,Raphael Semiat,Xuezhong He
Membrane gas separation technologies have emerged as highly prospective avenues for the selective separation of CO 2 . In this research, a novel array of mixed-matrix membranes (MMMs) was engineered, integrating two-dimensional nanosheets of MXene, specifically Ti 3 C 2 T x , into polymers of intrinsic microporosity (PIMs) to selectively separate CO 2 from N 2 . The inclusion of Ti 3 C 2 T x nanosheets, rich in polar functional groups, significantly increases the affinity between CO 2 molecules and the fabricated MMMs. Additionally, the precise modulation of the molecular diffusion channels for CO 2 and N 2 is achievable due to the interlayer spacing between MXene layers (∼0.35 nm) within the PIM-1 matrix. This innovation is predicated on the synergistic effect of solution-diffusion and molecular sieving mechanisms that underpin the gas separation process, leading to a marked improvement in both selectivity for CO 2 over N 2 and the permeability of CO 2 . Among the series, the MMMs with a 0.5 wt% MXene display exceptional separation efficiency, achieving a CO 2 permeability of 12475.3 barrer and a CO 2 /N 2 selectivity of 32.7. Notably, all the PIM-1/MXene membranes prepared with different compositions in this study exceed the Robeson upper bound defined in 2019, indicating their substantial promise for CO 2 separation and capture in industrial applications.
研究领域:
材料科学
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环境工程
·
化学工程
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高影响因子
LANGMUIR
·
2024
·
IF 3.7
Zhenghao Zhang,Bo Peng,Yupeng Zhang,Jiaxin Xiong,Jingwei Li,Jianwei Liu
A CO2/N2-responsive emulsion provides milder reaction conditions, nontoxicity, and economic feasibility compared to other switchable surfactants. In this study, CO2/N2-responsive pickering emulsions were fabricated by using a compounded dispersion containing SiO2 nanoparticles (NPs) and superamphiphiles as the emulsifying agents. The synergistic effects of the SiO2 NPs and superamphiphiles significantly stabilized the emulsion at all of the tested concentrations and prevented complete phase separation of oil and water. The electrostatic interaction between the SiO2 NPs and superamphiphiles was disrupted after bubbling with CO2 for 30 s, resulting in the breaking of the emulsion. However, the dispersion recovered its interfacial activity after the introduction of N2 and again emulsified the emulsion. This reversible switching behavior was validated through three consecutive cycles of bubbling CO2/N2. The protonation and deprotonation of the SiO2 NPs and superamphiphiles in response to CO2/N2 facilitated reversible assembly and disassembly, which enabled the switching of the emulsions between inactive and active forms. The novel highly stable Pickering emulsions demonstrated rapid demulsification and emulsification in response to CO2/N2 and are promising for a wide range of applications.
研究领域:
材料科学
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化学工程
·
胶体与界面科学
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yang Hong,Yan Zhou,Jiaqi Chen,linqian Qin,Yongqi Li,Yang Li,Hongyan Jiang,Huiyang Zhao,Jinzhu Wu,Xiaohong Wu
Advances in carbon capture and storage (CCS) technologies are critical for mitigating global climate change due to their low cost and operational simplicity. Although zeolites hold promise for carbon capture, the development of advanced zeolite materials with optimized CO 2 separation efficiency and diffusivity remains challenging. In this study, we present a quantum dot-regulated growth strategy, in which silicon quantum dots (SiQDs) act as heterogeneous seeds to not only initiate the growth of nanoscale zeolite units but also guide their assembly. The resulting 13X-SiQDs exhibit a distinct micrometer-scale hollow sphere structure composed of nanoscale zeolite units, which provide additional adsorption sites and mesopores, significantly enhancing adsorption and diffusion. The amino groups on the surface of the SiQDs further enable chemical adsorption with CO 2 , strengthening the binding force. The synergistic combination of thermodynamic and kinetic advantages enables 13X-SiQDs to achieve substantial improvements in CO 2 adsorption capacity (132.20 cm 3 ·g −1 ), CO 2 /N 2 selectivity (561), and diffusion rate. This quantum dot-regulated synthesis strategy offers a promising approach for designing advanced adsorption materials with high performance, extending their potential applications beyond carbon capture.
研究领域:
材料科学
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环境科学
·
化学工程
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2019
·
IF 3.372
Shuangqing Sun,Xiqiang Zhang,Shengxiang Feng,Hongbing Wang,Yan Wang,Jianhui Luo,Chunling Li,Songqing Hu
A novel CO 2 /N 2 switchable aqueous foam was developed using a CO 2 -responsive surfactant N,N-dimethyl-N-dodecyl amine (C 12 A) and a conventional surfactant sodium dodecyl sulfate (SDS). The performance and mechanism of this switchable foam were studied by both experiment and molecular simulation methods. Experimental results demonstrate that the foam stabilized by SDS/C 12 A surfactants has better stability and water carrying capacity than single C12A foam. The foam could be rapidly switched between stable and unstable states at ambient temperature with CO 2 or N 2 as the triggers. Simulation results shows that when CO 2 was introduced, most of SDS and C 12 A molecules aggregated in the water phase, instead of adsorbing at the air-water interface to stabilize the foam films. The strong electrostatic attraction between protonated C 12 A and SDS molecules could account for the aggregation. Due to the presence of limited surfactants located at the air-water interface after introducing CO 2 , the foam bursts quickly.
研究领域:
化学
·
材料科学
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胶体与表面化学
·
分子模拟
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高影响因子
危险品化学品经营许可证（带存储）