CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Xiaoqian Li,Dechao Wang,Zhongjie He,Fangfang Su,Nan Zhang,Yangyang Xin,Hongni Wang,Xiaolu Tian,Yaping Zheng,Dongdong Yao,Mingtao Li
Porous liquids (PLs) as a novel class of materials combine the permanent porosity of microporous solids, the rapid mass transfer of liquids, and fluidity, thus exhibiting extraordinary promise for gas capture and separation. However, the practical application of PLs was severely restricted by their undesirable relative high viscosity and melting temperature. In this work, the symmetric dicationic ionic liquids [C 6 BIm 2 ][NTf 2 ] 2 was synthesized as a steric hindrance solvent to construct a type of low viscosity zeolitic imidazolate frameworks (ZIFs)-based PLs. Specifically, the ZIF-67-PLs-2 ( i.e. , ZIF-67 loading of 2.0% in PLs) presented a low viscosity with 543.4 mPa·S at 25 °C, which was about 20 times lower than that of type III PLs reported previously. Meanwhile, ZIF-67-PLs showed long-term stability even over 180 days and broke the fluidity limitation down to −64 °C, broadening the work conditions. Moreover, ZIF-67-PLs-10 ( i.e. , ZIF-67 loading of 10.0% in PLs) achieved 55 times CO 2 and 7 times toluene adsorption capacity more than those of the corresponding pure DILs, respectively. Remarkably, the fascinating features of ZIF-67-PLs including lower viscosity, wide liquid range and higher adsorption pave a new way for the optimal design of novel PLs towards gas uptake and 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
NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 46
·期 5
·2189-2197
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IF 3.591
Yangyang Xin,Dechao Wang,Dongdong Yao,Hailong Ning,Xiaoqian Li,Xiaoqian Ju,Yichi Zhang,Zhiyuan Yang,Yahong Xu,Yaping Zheng
Porous liquids (PLs), a new class of materials with permanent pores and macroscopic flowing behaviors, have attracted much attention for CO2 capture. However, the preparation of PLs is always complicated, which is not suitable for the scale-up. Herein, we propose a rather simple and feasible strategy based on post-synthetic modification of pore generators and the like-dissolves-like principle to synthesize UiO-66-PLs with low-viscosity. To be specific, the metal–organic framework (MOF) UiO-66 with hydroxyl groups (denoted UiO-66-OH) was modified by an organosilane (denoted KH550 or SID) via a post-synthetic modification method, obtaining the pore generator UiO-66-OS (denoted UiO-66-KH550 or UiO-66-SID). Then, the UiO-66-OS was dispersed into two different sterically hindered polydimethylsiloxane solvents (PDMS400 or PDMS6000). Thereby, a series of type 3 PLs (UiO-66-PLs) with superior fluidity at room temperature and accessible porosity were obtained. For instance, the viscosities of UiO-66-KH550-PDMS400 and UiO-66-SID-PDMS400 were 1.1 and 1.5 Pa S at 25 °C, respectively, which were far lower than those of values reported thus far. In addition, gas sorption–desorption measurements indicated that the UiO-66-PLs exhibit superior CO2 sorption performance and great potential for CO2/N2 separation. Moreover, molecular simulation was carried out to verify the retained accessible porosity. Notably, the strategy of constructing type 3 PLs based on the post-synthetic modification of MOFs with organosilane and the like-dissolves-like principle not only provides a new solution for the development of low-viscosity PLs, but also opens a new path for the construction of other types of advanced porous material (APM)-based (e.g., covalent organic frameworks (COFs), porous organic cages (POCs)) PLs, which have potential applications in the fields of gas trapping storage, and catalysis.
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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DOI
高影响因子
Journal of Cleaner Production
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2024
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IF 9.7
Shuai Han,Zhe Wang,Junjian Yu,Fei Wang,Xiangwei Li
Low-silica SOD zeolites are among the most promising inorganic materials for mixed matrix membranes (MMMs). However, the gas separation performance is severely hindered by the non-selective voids formed by both the zeolite and polymer membranes, as well as the rigid layer. In this work, SOD-liquid-M2070 PL type I porous liquid was synthesized and subsequently filled into an Amidoxime-functionalized polymer of intrinsic microporosity (AO-PIM) to prepare MMMs. The fillers and MMMs were characterized using FTIR, SEM, TGA, XRD, and gas permeation techniques. SOD-liquid-M2070 PL facilitates the rapid diffusion of CO 2 and H 2 gas molecules for efficient gas separation. The liquid-like fluidity of SOD-liquid-M2070 PL improves the formation of non-selective pores in the SOD and polymer matrix membranes to enhance gas permeability and selectivity. The CO 2 , H 2 permeability and CO 2 /N 2 , H 2 /N 2 selectivity of MMMs composed of 5 wt% SOD-liquid-M2070 PL with optimal filling ratio were increased by 248%, 246%, and 173%, 222%, respectively, compared with pure membranes. It exceeds the 2008 Robeson limit for H 2 /N 2 and approaches much closer to the 2019 Robeson limit for CO 2 /N 2 . The field of green environment presents a promising development prospect for low silica SOD zeolite, which exhibits high separation efficiency.
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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DOI
高影响因子
CHEMICAL ENGINEERING RESEARCH & DESIGN
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2024
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IF 3.7
Ayesha Komal,Amna Kasuri,Muhammad Yasin,Asim Laeeq Khan,Abdul Razzaq,Hamad Alhmohamadi,Faheem Hassan Akhtar,Arsalan Ahmad Raja,R. Nawaz,Emilia Abdulmalek,Mazhar Amjad Gilani
Separating butanol/water mixtures via distillation is notably energy-intensive and costly, highlighting the urgent need for more efficient alternatives. This study introduces a novel approach using mixed matrix membranes (MMMs) infused with Zeolitic Imidazolate Framework-8 (ZIF-8) transformed into its porous liquid (PL) form, aimed at enhancing the separation efficiency of butanol/water mixtures through pervaporation (PV). We selected ZIF-8 for its hydrophobic nature and high surface area, which are critical for improving both flux and selectivity in membrane-based separation processes. The study details the synthesis of ZIF-8-PL, its characterization through techniques such as Fourier Transform Infrared (FTIR) spectroscopy, X-ray diffraction (XRD), and scanning electron microscopy (SEM), and the fabrication of the MMMs. Our results demonstrate that ZIF-8-PL-based membranes at 55°C with a 30 wt% PL loading significantly enhance biobutanol-selective PV efficiency. Specifically, these membranes show an improvement in flux of approximately 102% and an increase in separation factor by 64% when compared to unmodified polydimethylsiloxane (PDMS) membranes. This significant enhancement highlights the effectiveness of PL-based fillers in advancing MMM performance for biofuel separation, providing a promising route to optimize energy efficiency and cost-effectiveness in industrial scale applications.
研究领域:
材料科学
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化学工程
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生物燃料技术
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DOI
高影响因子
Journal of Materials Chemistry A
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2024
·Vol. 12
·期 24
·14659-14668
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IF 10.7
Leqin Li,Miaojiang Wu,Sa Yao,Yinglai Hou,Ruizhe Yuan,Jianhe Liao,Xuetong Zhang
Porous liquids (PLs), porous materials with flowable states, show promising applications in some emerging fields. However, creating porous materials with on-demand flowability is still significantly challenging. Herein, aerogel-based stimulus-responsive porous liquids have been proposed and fabricated via dispersing superhydrophobic silica aerogel microparticles in a polymer aqueous solution with either lower or upper critical solution temperature (LCST or UCST), respectively. The resulting aerogel-based intelligent porous liquids possess quite low density (0.56 g cm−3), high porosity (up to 48.57%), low thermal conductivity (0.239 W m−1 K−1) and appropriate viscosity (4.1–220.6 Pa s). Most importantly, the resulting porous liquids show reversible thermal responsiveness. Thus, a new condensed state, i.e., solid–liquid–vapor triple-state gels, might be obtained via on-demand thermal triggering of these aerogel-based porous liquids. Cut triple-state gels show interesting self-healing behaviors via either thermal treatment or replenishment of a small extra amount of porous liquids. To our surprise, the reversible transition between aerogel-based flowable porous liquids and solid–liquid–vapor triple-state non-flowable gels has endowed these materials with plastic-like processing capability upon demand. These porous liquids, together with those triple-state gels, might find broad applications in some emerging fields, and the work reported here might inspire scientists to fabricate more aerogel-based porous liquids and triple-state gels.
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Xiaoqian Li,Dechao Wang,Hailong Ning,Yangyang Xin,Zhongjie He,Fangfang Su,Yudeng Wang,Jing Zhang,Hongni Wang,Liwei Qian,Yaping Zheng,Dongdong Yao,Mingtao Li
Porous liquids (PLs), as a novel liquid sorbent with permanent porosity, still present challenges such as high viscosity and melting temperatures. Herein, an efficient electrostatic repulsion strategy is proposed to engineer zeolitic imidazolate frameworks (ZIFs) type III PLs employing ZIF-8- g -BPEI nanoparticle stability dispersed into BPEI. The viscosity and melting temperatures of ZIF-8- g -BPEI PLs could be tailored via control particle size, grafting polymer, and concentration of porous nanoparticles . The existence of BPEI on the surface of ZIF-8- g -BPEI facilitates the stable dispersion of ZIFs nanoparticles in BPEI via the electrostatic repulsion as well as enhances CO 2 adsorption capacity of PLs. Moreover, the CO 2 adsorption amount of ZIF-8- g -BPEI-30 PLs is 6.5 times high than that of neat BPEI, suggesting the permanent free volume of ZIFs is retained in their corresponding PLs. Benefiting from the branched structure of BPEI grafted onto the outer surface of ZIFs , ZIF-8- g -BPEI-10 PLs remain liquified down to -71.1 °C, together with viscosity as 1.7 Pa·s −1 at 25 °C. Therefore, the electrostatic repulsion strategy opens an effective avenue to prepare novel liquid materials and shows numerous potential applications in gas adsorption and 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
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2021
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IF 7.312
Fangfang Su,Xiaoqian Li,Yudeng Wang,Zhongjie He,Ling Fan,Hongni Wang,Jinliang Xie,Yaping Zheng,Dongdong Yao
Porous liquids (PLs) are a type of porous materials that combine the porosity of solids and fluidity of liquids, which has attracted widespread attention. In this paper, we report a new TypeⅠhollow carbon sphere-based porous liquids, which are constituted of hollow carbon sphere (HCS) as the porous host, polymeric ionic liquid (PILs) as the corona and poly(ethylene glycol) 4-nonylphenyl 3-sulfopropyl ether potassium salt (PEGS) as the canopy. The viscosity of PLs is 8900 mPa·s at 50 ℃ (like syrup), which has good fluidity. Under 3 MPa pressure conditions, the best CO 2 adsorption capacity of 450-P[VHIm]Br-PEGS and 450-P[VBBI]Cl-PEGS are 2.06 and 1.90 mmol/g at 25 °C, respectively, higher than PILs-PEGS. Under the same conditions, the CO 2 adsorption capacity of PLs is 10.5 times higher than that of N 2 . Therefore, HCS-based PLs have the potential for CO 2 /N 2 selective gas separation. Not only PILs and the anionic alkyl chain of the outer layer widen the liquid range of PLs, but also is suitable for preparing PLs with other cavity units.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Zhiwei Dong,Yudong Ding,Hong Wang,Min Cheng,Xun Zhu,Qiang Liao
Combining the fluidity of ionic liquids (ILs) with the permanent porosity of metal-organic frameworks (MOFs), type III porous liquids (type III-PLs) demonstrate exceptional catalytic activity for CO 2 capture and cycloaddition reactions. The ZIF-8-based type III-PLs (ZIF-8/1-methyl-3-propylimidazolium bromide ([PMIm]Br)) catalysts achieved a 50.39 % increase in CO 2 conversion and a styrene carbonate yield of 93.08 % at 80 °C and 1.0 MPa. DFT calculations revealed a synergistic effect of ZIF-8/[PMIm]Br catalysts: The Zn active sites in ZIF-8 lowered the energy barriers for epoxide ring opening and CO 2 insertion, while [PMIm]Br provided nucleophilic sites to facilitate the reaction. Additionally, molecular dynamics simulations showed enhanced CO 2 diffusion at the gas-liquid interface in the ZIF-8/[PMIm]Br system, accelerating the reaction rate. This study offers theoretical insights for designing more efficient type III-PLs catalysts for the industrial utilization of CO 2 as a C1 resource.
研究领域:
化学
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催化材料
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环境科学
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2025
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IF 5.4
Xingxing Zhao,Yudong Ding,Lijiao Ma,Xun Zhu,Hong Wang,Min Cheng,Qiang Liao
Porous liquids are promising absorbents for CO 2 capture due to porosity and liquidity. In this paper, three amines, TEPA, PEI, and MEA, were used to reinforce CO 2 capture in type III porous liquids, and the influences of these amines on the CO 2 uptake of the porous liquids were discussed. First, determining the optimal TEPA, PEI, and MEA loadings were 30 wt%, 30 wt%, and 50 wt%, respectively. Then, the amine-modified type III porous liquids, TEPA@ZIF-8/[EMIm]/[NTf 2 ], PEI@ZIF-8/[EMIm]/[NTf 2 ], and MEA@ZIF-8/[EMIm]/[NTf 2 ] were prepared. The effects of different parameters on the CO 2 absorption characteristics were systematically investigated. It was found that amines-modification could significantly reinforce CO 2 absorption of type III porous liquids at low CO 2 partial pressures. The CO 2 uptake capacity of 5-30TEPA@ZIF-8/[EMIm][NTf 2 ], 5-30PEI@ZIF-8/[EMIm][NTf 2 ], 5-50MEA@ ZIF-8/[EMIm][NTf 2 ] was 4.43, 2.28, and 3.96 times higher and the corresponding absorption rates were 8.45, 2.25, and 26.3 times higher than that of 5-ZIF-8/[EMIm][NTf 2 ]. The CO 2 absorption kinetic properties were revealed, and the results showed the fractional-order kinetic model best fitted the CO 2 absorption process, suggesting the CO 2 absorption coupled with the CO 2 diffusion inside the main units and the chemical reaction at the active sites. Finally, the cyclic regeneration performance results displayed that TEPA@ZIF-8/[EMIm][NTf 2 ] exhibited a good cyclic regeneration performance and has the potential for CO 2 capture.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Yangyang Xin,Dechao Wang,Weirui Zhang,Fangfang Su,Yisong Liu,Yaru Lu,Wendi Fan,Dongdong Yao,Yaping Zheng
Porous liquids represent an innovative class of materials that combine the porosity of porous solids with the dynamic fluidity of liquids, garnering significant interest. However, the preparation of type II porous liquids is often hindered by complex methodologies and stringent requirements for both the porous host and the sterically hindered solvent. Herein, we present a simple and universal approach to prepare type II porous liquids, utilizing the metal organic cage ZrT-1-OH as the porous host and deep eutectic solvents (DES) as the sterically hindered solvent, respectively. Through hydrogen bonding interactions, ZrT-1-OH dissolves efficiently in DES, resulting in porous liquids with low viscosity. These porous liquids exhibit enhanced CO2 sorption performance and demonstrate potential for selective gas separations of CO2/N2 and CH4/N2. Given the diversity of available porous organic cages and the high tunability of DES compositions, this approach offers a promising and universal pathway for the design and preparation of type II porous liquids.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
POLYMER BULLETIN
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2025
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IF 4
Zhang Chengpeng,Bei Pengzhi,Liu Hongjing,Zhao Xu,Shi Meiling,Jing Xiaochun,Li Zhao,Yao Hui
A novel porous liquid, M2070-UiO-66-OH@[BMim][PF 6 ], has been synthesized using zirconium-based metal–organic framework (UiO-66-OH), 1-butyl-3-methylimidazolium hexafluorophosphate ([BMim][PF 6 ]) and polyetheramine M2070. To enhance the CO 2 separation performance, M2070-UiO-66-OH@[BMim][PF 6 ] was incorporated as a filler into a mixed matrix membrane (MMM) using polyether block amide (Pebax-1657) as the membrane matrix. The properties of the synthesized M2070-UiO-66-OH@[BMim][PF 6 ] and the resulting MMMs have been characterized through FTIR, TGA, DSC, and SEM analyses. The results of porous liquid stability revealed that grafting polyetheramine M2070 onto the surface of UiO-66-OH@[BMim][PF 6 ] significantly increased the steric hindrance, thereby preventing agglomeration within the membrane. Additionally, the functional groups (amino and ether) present in M2070-UiO-66-OH@[BMim][PF 6 ] contributed to an increased number of active sites for CO 2 adsorption, facilitating enhanced CO 2 transport through the membrane. Compared to the Pebax membrane, the MMM containing 3% M2070-UiO-66-OH@[BMim][PF 6 ] exhibited significantly improved CO 2 permeability of 104.07 Barrer (an increase of 73.22%) and CO 2 /N 2 selectivity of 92.37 (an increase of 148.95%) at 30 °C and 0.3 MPa, surpassing the 2008 Robeson upper bound. These findings suggest that M2070-UiO-66-OH@[BMim][PF 6 ] is a highly promising additive for the fabrication of mixed matrix membranes with superior CO 2 separation performance. Graphical abstract A porous liquid, (M2070-UiO-66-OH@[BMim][PF 6 ]) has been prepared using UiO-66-OH@[BMim][PF 6 ] as the core and polyetheramine M2070 as the canopy. Afterwards, M2070-UiO-66-OH@[BMim][PF 6 ] has been added to the Pebax matrix to prepare M2070-UiO-66-OH@[BMim][PF 6 ]/Pebax mixed matrix membranes, which have been subjected to gas separation studies.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Lisha Sheng,Jie Lei,Zhenqian Chen,Yi Wang
Type I porous liquids (PLs) containing porosity are promising candidates for gas sorption and separation, homogeneous catalysis , and so forth. In this research, large porous silica nanoparticles (PSNs) and hollow wormhole silica nanoparticles (HSNs) are reported to fabricate Type I PLs through a facile synthetic strategy, where polyether amine is linked to nanoparticles by the silane coupling agent for CO 2 capture. Experimental results showed that canopies endow PSNs and HSNs with excellent fluidity along with the thermal stability of PLs at high temperature. The CO 2 sorption capability and dispersion stability were profoundly influenced by the specific surface area and pore size of PLs cores. At 25 °C and 2 bar, the CO 2 sorption capacities of pure M2070, PL_1_M2070, PL_2_M2070, and PL_3_M2070 were 10.9317 cm 3 /g, 9.1295 cm 3 /g, 6.2504 cm 3 /g, and 5.3518 cm 3 /g, respectively. Results showed that CO 2 sorption capability of porous silica nanoparticle assisted PLs with a large specific surface area and small pore sizes was superior. If the pore size was large enough, canopy would enter and fill the pores of silica nanoparticles, preventing part pores and polyether amine from offering active CO 2 sorption sites, thereby minimizing the CO 2 sorption and affecting the stability of the PLs. Sorption kinetics fitting results showed that the CO 2 sorption of PLs was the combination of physical dissolution and chemisorption . Furthermore, the adsorption capacity of PL_1_M2070 was 90.5% of the original CO 2 adsorption capacity after 10 adsorption/desorption cycles, indicating excellent recyclability.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）