LANGMUIR
·
2014
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IF 4.384
Pingwei Liu,Weiqiang Lu,Wen-Jun Wang,Bo-Geng Li,Shiping Zhu
Cross-linked polymer particles were prepared via surfactant-free emulsion copolymerization of 2-(diethylamino)ethyl methacrylate (DEAEMA) and sodium methacrylate (SMA) using N,N′-methylenebis(acrylamide) (MBA) as a cross-linker. Generated particles are zwitterionic, possessing unique isoelectric points in the pH range of 7.5–8.0, which is readily tunable through CO2/N2 bubbling. The particles were found to be highly responsive to CO2/N2 switching, dissolving in water with CO2 bubbling and precipitating with N2 bubbling at room temperature. Pickering emulsions of n-dodecane were prepared using these particles as the sole emulsifier. These emulsions can be rapidly demulsified with CO2 bubbling, resulting in complete oil/water phase separations. Nitrogen bubbling efficiently re-emulsifies the oil with the aid of homogenization. The rapid emulsification/demulsification using CO2/N2 bubbling at room temperature provides these cross-linked zwitterionic particles with distinct advantages as functional Pickering surfactants.
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
REACTIVE & FUNCTIONAL POLYMERS
·
2021
·
IF 3.975
Hui Wang,Yunxia Ni,Zhiyue Dong,Qiang Zhao
Interface compatibility is crucial to performance and robustness of nanocomposite membranes for molecular separation. In this work, a covalent crosslinking method was exploited to fabricate polydimethylsiloxane/metal-organic-frameworks (PDMS/MOFs) mixed matrix membranes with improved interfacial compatibility. Zirconium MOF particles (UiO-66-NH 2 ) were grafted with methoxysilane groups, which further formed covalent crosslinks with silanol terminated PDMS matrix. The strengthened interfacial compatibility prevented sedimentation and aggregation of MOF particles in PDMS precursor solution during the solvent evaporation process, thus the composites showed good membrane formation ability at high MOFs loading (60 wt%). Tensile strength of the hybrid membrane is 2.8 times improved while retaining good flexibility. Moreover, the CO 2 /N 2 selectivity and CO 2 permeability of the PDMS composite membrane incorporated with 40 wt% UiO-66-MS particles are improved by 1.3 times and 0.7 times, respectively.
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
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IF 9.136
Yonghong Wang,Zhuo Jin,Xinru Zhang,Jinping Li
The incorporation of lamellar materials into polymer matrix can improve the gas separation performance of mixed matrix membranes (MMMs), which have great potential in chemical separation process. However, few intrinsic selectivity sites on MoS 2 sheets suppress further employment in the membrane separation. In this work, the vacancies and defects-containing MoS 2 sheets were prepared by high temperature oxidation and hydrothermal reaction in NaOH solution, and then L-cysteine-functionalized MoS 2 (Cys-MoS 2 ) was synthesized by a thiol-click chemistry reaction between S vacancies and thiol groups as confirmed by transmission electron microscope (TEM), Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and N 2 absorption. After blending with polyether-block-amide (Pebax), the as-prepared MMMs showed outstanding mechanical properties as a result of the homogeneous dispersion of Cys-MoS 2 and hydrogen bonding between two phases as evidenced by attenuated total reflectance-FTIR, scanning electron microscope (SEM), thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). The highest permeability of 297 Barrer accompanied with a CO 2 /N 2 selectivity of 120 was obtained for MMMs loaded with 1.5 wt% Cys-MoS 2 , which were enhanced by 206.2 % and 124.7 % over the pristine Pebax membrane, respectively. Meanwhile, this value was superior to that of the previously reported Pebax-based MMMs, transcending 2019 upper bound. The enhanced gas separation performance is due to the improved CO 2 adsorption selectivity by the vacancies and defects of Cys-MoS 2 , while the amine groups carrier enhanced CO 2 reactivity selectivity.
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
ACS Applied Polymer Materials
·
2025
·
IF 4.7
Jinpeng Liu,Chengcheng Hao,Huili Zhang,Hongyu Chen,Ling Zhang,Xiaodong Chen,Jianye Wang,Maohuai Wang,Shuxian Wei,Xiaoqing Lu,Zhaojie Wang,Siyuan Liu
Covalent organic frameworks (COFs) have become potential candidates for gas purification technology, especially in carbon capture and storage applications. By utilizing strategies such as pore structure design and functional modification, COFs have been developed to exhibit high selectivity and superior adsorption capacity for the effective capture and separation of CO2 from industrial waste gases. Notably, alkali metals exhibit strong interactions with the backbone of the COFs, which can enhance the CO2/N2 adsorption separation performance of these porous materials. This study details the synthesis of two-dimensional COF materials modified with acidic groups (TpPa-COOH and TpPa-SO3H) via mechanical grinding. Alkali metals such as Na, Li, and K were introduced into these groups through simple ion exchange reactions, thereby creating metal-modified COF materials. The impact of various alkali metals on the CO2/N2 adsorption separation performance of COF materials was investigated. Among the resulting products, lithiated TpPa-COOH showed the highest CO2 capture capacity of 2.65 mmol/g at 273 K and 1 bar. This may be due to the smaller atomic size of Li that offers larger adsorption space. Under the same conditions, the K-modified TpPa-SO3H exhibited the highest selectivity of 548, which surpasses most COFs reported in the literature. The superior performance was caused by the high polarization of the COF backbone triggered by the alkali metals. The inference was further confirmed by computational simulations. This work provides a facile method for the modification of porous materials with alkali metals to achieve superior gas separation performance.
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
JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Shichen Zeng,Xu Liang,Mingang Zhao,Yanxiong Ren,Hanze Ma,Ziting Zhu,Yuhan Wang,Shaoyu Wang,Junyi Zhao,Guangzhaoyao Yang,Xuerui Wang,Fusheng Pan,Guangwei He,Zhongyi Jiang
Covalent organic frameworks (COF) are deemed as disruptive membrane materials owing to their versatile functionalities, high stability and ordered nanochannels. However, the size mismatch between the COF intrinsic pore and gas molecules becomes a grand challenge when using COF membrane for carbon capture. Herein, we propose a new type of polymer-functionalized COF laminar membranes through grafting CO 2 -phlic polyethyleneimine (PEI) polymer onto carboxylic acid COF (cCOF) laminar membranes. The cCOF nanosheets with high density of carboxyl groups are prepared via modified single phase solution method and then assembled to fabricate membranes. Further, the cCOF membranes are functionalized with PEI using 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide/N-Hydroxysuccinimide (EDC/NHS) coupling chemistry. The introduction of abundant amino groups from PEI afford the affinity of membranes toward CO 2 . Meanwhile, the graft of the PEI polymers reduces the defects or pinholes on the membrane surface. As a result, the PEI functionalized cCOF membranes exhibit a high CO 2 permeance of 1004 GPU and a CO 2 /N 2 selectivity of 33.7, which reach the carbon capture target performance and show great prospect for treating real flue gas. Our approach of functionalizing cCOF membranes with tailored functionalities may inspire the design of molecule-selective COF membranes.
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
JOURNAL OF MATERIALS SCIENCE
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2025
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IF 3.9
Zhang Lei,Cao Xueting,Xin Qingping,Ding Xiaoli,Jin Huimin,Chen Hao,Chu Qingquan,Du Yifei,Huang Wei,Zhang Ruihua,Bao Shiya,Zhang Yuzhong
In this study, a top-down etching method is used to obtain MXene nanosheets with an accordion-like structure, and the surface of the MXene nanosheets is functionalized with 3-aminopropyltriethoxysilane to obtain functionalized MXene nanosheets (f-MXene), which is combined into polyethylene oxide (PEO) copolymer matrix for fabricating mixed matrix membranes (MMMs). The f-MXene nanosheets enhance the CO 2 /N 2 separation performance of membranes in multiple ways. Firstly, the accordion-like structure of f-MXene increases the channel for rapid gas transport. Secondly, the two-dimensional sheet-shaped material has a high aspect ratio, which effectively weakens the interaction between polymer chains and inhibit crystallization. This increases free volume for molecular transport and helps improve gas permeability. Thirdly, the amino group can react reversibly with CO 2 , improving reaction selectivity, and facilitates CO 2 transport. Therefore, the PEO/f-MXene membrane exhibits excellent CO 2 permeability and CO 2 /N 2 selectivity. To explore more efficient separation technology, the membrane separation performance at low-temperature is investigated. At − 20 °C, the PEO/f-MXene-3% membrane has a CO 2 permeability of 47.8 Barrer and a CO 2 /N 2 selectivity of 280.9, which is 576.9% higher than that at 35 °C, exceeding the latest upper bound. Graphical
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高影响因子
Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Xingqian Wang,Yifei Wang,Yongjiang Shan,Xuerong Wang,Yingdong Yang,Fei Zhang,Xiangshu Chen
In recent years, membrane separation technology has received extensive attention in CO 2 /N 2 separation. Carbon nanotubes (CNTs) were regarded as ideal fillers for constructing high permeability mixed matrix membranes (MMMs) due to their special tubular structure. However, the interfacial compatibility between CNTs and organic polymer phases is a large challenge, seriously hindering the development of carbon-based mixed matrix membranes. In this work, we proposed a novel polyethyleneimine (PEI) surface functionalization strategy to effectively improve the compatibility between multi-walled carbon nanotubes (MWCNTs) and Pebax-1657. The as-prepared PEI@MWCNTs/Pebax-1657 MMMs were analyzed by XRD, EDS, FTIR, TG, etc. The PEI can improve the compatibility of MWCNTs with the polymer matrix. In addition, the abundant amino groups in the PEI structure can provide ample active sites for CO 2 , which can improve CO 2 permeability and CO 2 /N 2 selectivity simultaneously. Combining the low resistance of MWCNTs to gas transport, the membrane showed 178.08% enhancement in selectivity (82.06) of CO 2 /N 2 compared to the pristine membrane with 152.49% increment in the permeability (150.51 Barrer) of CO 2 . This work provides a novel strategy for preparing carbon-based mixed matrix membranes with high gas separation performance.
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DOI
高影响因子
ADSORPTION SCIENCE & TECHNOLOGY
·
2022
·
IF 4.373
Zhijuan Zhang,Pengwei Li,Ting Zhao,Yuanhan Xia
The ZIF-8 crystals were successfully postsynthetically modified using methylamine (MA), ethylenediamine (ED), and N, N-dimethylethylenediamine (MMEN) to improve their adsorption performance toward CO2. Results showed that, compared with the original ZIF-8, the BET specific surface area of MA-ZIF-8, MMEN-ZIF-8, and ED-ZIF-8 has increased by 118.2%, 92.0%, and 29.8%, respectively. In addition, their total pore volume increased separately by 130.8%, 100%, and 48.7%. The adsorption capacities of CO2 on the amine-modified ZIF-8 samples followed the order . The CO2 adsorption capacities at 298 K on MA-ZIF-8, MMEN-ZIF-8, and ED-ZIF-8 were increased by 118.2%, 90.2%, and 29.8%, respectively. What is more, the CO2/N2 selectivities calculated using an IAST model of the amine@ZIF-8 samples at 0.01 bar and 298 K were also significantly improved and followed the order , which increased by 173.0%, 121.4%, and 22.6%, respectively. The isosteric heat of CO2 adsorption () on the MA-ZIF-8, MMEN-ZIF-8, and ED-ZIF-8 all becomes higher, while of N2 on these samples was slightly lower in comparison with that on the ZIF-8. Furthermore, after six recycle runs of gravimetric CO2 adsorption-desorption on MA-ZIF-8, the adsorption performance of CO2 is still very good, indicating that the MA-ZIF-8 sample has good regeneration performance and can be applied into industrial CO2 adsorption and separation.
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高影响因子
Journal of Environmental Chemical Engineering
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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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高影响因子
ACS Applied Materials & Interfaces
·
2020
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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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产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Jie Gao,Haizhuo Mao,Hua Jin,Chen Chen,Armin Feldhoff,Yanshuo Li
Membrane-based separation technology has evolved as a competitive approach for CO 2 capture from flue gas (mainly N 2 ). To achieve high separation performance, three partially NH 2 -, OH- and CH 3 OH- functionalized mixed-linker-ZIF-7 were successfully synthesized, and incorporated into polyether-block-amide (Pebax® 2533) polymer to form mixed-matrix membranes (MMMs). As evidenced by the CO 2 adsorption isotherms , introducing functional groups in the ZIF-7 framework was indeed beneficial for CO 2 adsorption. All MMMs composed of ZIF-7-NH 2 , ZIF-7-OH and ZIF-7-CH 3 OH offered better CO 2 /N 2 separation performance than the parent ZIF-7-Pebax® 2533 membrane, suggesting the positive effect of functionalized ZIF-7 fillers on the gas separation performance. Among the three functionalized ZIF-7 based MMMs, the ZIF-7-OH-Pebax MMMs exhibited the best performance for CO 2 /N 2 separation, which might be ascribed to the highest adsorption selectivity of CO 2 over N 2 predicted by ideal adsorbed solution theory (IAST) for ZIF-7-OH fillers. The 14% ZIF-7-OH-Pebax MMM showed high CO 2 permeability of 273 Barrer and CO 2 /N 2 separation factor of 38, which increased by 60% and 145% as compared with the neat Pebax membrane. The strategy of preparing functionalized MOFs with strong affinity for CO 2 provides an effective method to develop MMMs for highly efficient CO 2 separation.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2018
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IF 6.578
Xiong-Fei Zhang,Yi Feng,Zhongguo Wang,Mingmin Jia,Jianfeng Yao
Incorporating metal-organic frameworks into cellulose matrix to prepare composite membranes is promising in gas-separation applications. In this study, UiO-66-NH 2 (Zr-based MOF) nanoparticles are wrapped into the densely packed cellulose nanofibrils (CNF-COOH) via a facile vacuum filtration process. The existence of acid-base interactions and electrostatic forces between UiO-66-NH 2 and CNF-COOH renders ideal interfacial morphology. Results show that UiO-66-NH 2 is cross-linked by -COOH groups and well-dispersed in the CNF matrix. The porous UiO-66-NH 2 strengthens the diffusion process of CO 2 molecules, thus elevating the permeation flux and separation factor simultaneously. The optimum separation performance is achieved over CM-1 membrane with a CO 2 permeability of 139 Barrer and a CO 2 /N 2 selectivity ratio of 46.
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高影响因子
危险品化学品经营许可证（带存储）