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.
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产品关联
DOI
高影响因子
APPLIED ENERGY
·
2020
·
IF 8.848
Wenlong Xiang,Jie Ren,Si Chen,Chenyang Shen,Yifei Chen,Minhua Zhang,Chang-jun Liu
Metal-organic frameworks (MOFs) have been confirmed to be a promising material for carbon dioxide capture, while the simultaneous capture and conversion of carbon dioxide over the MOF-based catalysts is furthermore being a hot topic. In this work, we demonstrate that the zirconium-based MOF UiO-66 (UiO for University of Oslo) with missing-linker defects is a highly active catalyst for carbon dioxide cycloaddition with an epoxide, which is a reaction with 100% atom economy and broad industrial uses. A facile, rapid, energy-saving and environmentally friendly argon plasma treatment was employed to create the missing-linker defects in UiO-66 without using hazardous chemicals at atmospheric pressure and temperature below 398 K, whereas the bulk structure of UiO-66 remained stable. The energetic argon plasma species decomposed part of the linkers within UiO-66 structure, leaving unsaturated metal sites. The defect concentration in UiO-66 was tuned by changing the plasma bombardment time. After an argon plasma treatment for 30 min, the number of linker deficiencies per Zr 6 cluster can reach up to 2.3. The product yield of the UiO-66 with abundant missing-linker defects increased of ca. 43% over the defect-free UiO-66. The crucial role of the missing-linker defects of UiO-66 in the enhancement of the catalytic activity was confirmed. The present study will be helpful for the future preparation of defective MOFs with potential applications not only for carbon dioxide conversion but also for energy storage and conversion.
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Danhua Guo,Huijun Li,Jiwei Wang,Zhouqing Xu
Leaching of fluoride in drinking water can lead to fluorosis. It is a good method to reduce the concentration of fluoride ion in drinking water by selecting the adsorption material with large adsorption capacity and good selectivity. Herein, the NH 2 -UiO-66 based loofah sponge modified porous composite was prepared. The composite material took loofah sponge (LS) as the carrier, and loaded NH 2 -UiO-66 on the surface of LS by in-situ growth method. The structure of the prepared NH 2 -UiO-66 @LS was investigated by PXRD , FTIR, SEM, and XPS. The influencing factors of different materials, contact time, adsorbent dosage, preliminary fluoride concentration, and co-existing anions were optimized. Compared with LS, the adsorption efficiency of NH 2 -UiO-66 @LS was greatly improved, and the adsorption capacity was 65.08 mg/g for fluoride ion. Moreover, the maximum removal efficiency of NH 2 -UiO-66 @LS was the initial fluoride concentration of 100 mg/L. Under the condition of the coexistence of other anions, the composite material has a specific adsorption performance for fluoride within 40 min. Furthermore, the data of fluoride adsorption was best fitted with pseudo-second-order kinetic model. The thermodynamic studies showed that the fluoride adsorption process on NH 2 -UiO-66 @LS was feasible, spontaneous and endothermic. In addition, synthesized NH 2 -UiO-66 @LS can be reused upto eight cycles. The plausible fluoride adsorption mechanism of NH 2 -UiO-66 @LS was majorly ruled by electrostatic attraction and complexation. Furthermore, the raw material is easy to obtain and the preparation process of NH 2 -UiO-66 @LS is simple. Hence, the large adsorption capacity of NH 2 -UiO-66 @LS compared with reported adsorbents for fluoride makes it have potential application prospect from wastewater on industrial scale.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ruimeng Wang,Long Liu,Sidra Subhan,Yaseen Muhammad,Yang Hu,Meiyun Huang,Yi Peng,Zhongxing Zhao,Zhenxia Zhao
The pH-switchable UiO-66 were engineered via in-situ amino acids (AA) doping for the highly selective adsorption of anionic dyes (i.e. sunset yellow FCF (SY)). Three AA doped samples, i.e. UiO-66-V (valine), UiO-66-T (threonine), and UiO-66-Y (tyrosine), have fabricated hierarchical structure and endowed –NH 2 surface in framework structure concurrently. These AA doped UiO-66s awarded highly selective adsorption and fast diffusivity towards the mentioned anionic dyes. More interestingly, enriched –NH 2 groups endowed AA doped UiO-66s a significant pH-responsive character for selectivity of anionic/cationic dyes. Textural characterization and adsorption measurement confirmed that high surface areas (>1070 m 2 /g) with defected pores and –NH 2 surface significantly enhanced adsorption uptake (352.8 mg/g) and diffusion rate (168 × 10 −3 min −1 ) for SY on AA doped UiO-66s, about 1.9 and 5.9 times respectively as that on pristine UiO-66. The AA doped UiO-66s exhibited one order of magnitude higher selectivity (>390) for SY against MB than that of original UiO-66. More importantly, the alteration in surface charge (–NH 2 H + ⇌ O H - -NH 3 + ) endorsed a great variation in the selectivity of AA doped UiO-66s to dyes when adjusting pH from 4 to 8, showing an excellent pH on-off switchable property. Also, it realized a stable self-adsorption/desorption recycling process via pH-switching for 6 consecutive cycles. With these features, the pH-switchable defected UiO-66 realized highly efficiency adsorption and non-thermal separation/regeneration process for anionic dyes.
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Huazhen Sun,Beibei Tang,Peiyi Wu
Metal–organic frameworks (MOFs) are being intensively explored as filler materials for polymeric proton exchange membranes (PEMs) due to their potentials for the systematic design and modification of proton-conducting properties. S-UiO-66, a stable MOF with functional groups of −SO3H in its ligands, was selected here to prepare S-UiO-66@graphene oxide (GO) hybrid nanosheets via a facile in situ growth procedure, and then a series of composite PEMs were prepared by hybridizing S-UiO-66@GO and sulfonated poly(ether ether ketone) (SPEEK). The resultant hybrid nanosheets not only possessed abundant −SO3H groups derived from the ligands of S-UiO-66 but also yielded a uniform dispersion of S-UiO-66 onto GO nanosheets, thus effectively eliminating the agglomeration of S-UiO-66 in the membrane matrix. Thanks to the well-tailored chemical composition and nanostructure of S-UiO-66@GO, the as-prepared SPEEK/S-UiO-66@GO composite PEMs present a significant increase in their proton conductivity under various conditions. In particular, the proton conductivity of the SPEEK/S-UiO-66@GO-10 membrane was up to 0.268 S·cm–1 and 16.57 mS·cm–1 at 70 °C-95% RH and 100 °C-40% RH (2.6 and 6.0 times that of recast SPEEK under the same condition), respectively. Moreover, the mechanical property of composite membranes was substantially strengthened and the methanol penetration was well-suppressed. Our investigation indicates the great potential of S-UiO-66@GO in fabricating composite PEMs and also reveals that the high proton conductivity of MOFs can be fully utilized by means of MOF/polymer composite membranes.
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DOI
PubMed
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Dongxue Liu,Ye Li,Chang Liu,Yuzhi Zhou
A nanocomposite of a zirconium-based metal-organic framework (UiO-66) @ polypyrrole (PPy) (UiO-66@PPy) was successfully synthesized to eliminate F − from groundwater. The optimum initial pH and adsorbent dose for maximum uptake of F − from aqueous solution were found to be 3.0 and 0.1 g/L, respectively. The fluoride removal performance of UiO-66 was greatly enhanced through the introduction of polypyrrole guests, and the maximum adsorption capacity of UiO-66@PPy, namely, 290.7 mg/g, was reached, which is far superior to those of other previously reported adsorbents. The fluoride adsorption by UiO-66@PPy agreed well with the pseudo-second-order equation model and Langmuir isotherm model. The coexisting PO 4 3− and CO 3 2− substantially influence fluoride removal. The synthesized UiO-66@PPy could be reused five times in adsorption-desorption cycles. The incorporation of conducting polymers opened additional paths for the development of adsorbent materials; thus, UiO-66@PPy could be a viable adsorbent material and contribute to fluoride removal from groundwater.
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Fukun Bi,Xiaodong Zhang,Jinfeng Chen,Yang Yang,Yuxin Wang
The highly dispersed Pd nanoparticles supported UiO-66 catalysts were successfully prepared via ethylene glycol reduction method (Pd-U-EG). And their catalytic performances were evaluated by toluene degradation. A series of characterization methods were carried out to characterize the physicochemical properties of the samples. During the effect of high weight hourly space velocity, stability and reusability test, the catalytic activity of Pd-U-EG remains unchanged, which also indicated good catalytic performance. More importantly, water resistance test (10-20 vol.% water) indicated that Pd-U-EG had a great water resistance. The study of toluene-TPD, toluene-TPSR and in-situ DRIFTS at different temperatures under different conditions over Pd-U-EG indicated the role of H 2 O. The introduction of H 2 O at low temperature was conducive to the adsorption of toluene, but inhibited the degradation of toluene. Differently, the H 2 O presence at high temperature was favorable to toluene degradation. In addition, toluene degradation mechanism was also revealed.
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DOI
高影响因子
JOURNAL OF NANOPARTICLE RESEARCH
·
2020
·Vol. 22
·期 3
·1-12
·
IF 2.132
Ma Wenzhong,Li Taiyu,Zhang Qi,Zhong Jing,Matsuyama Hideto
Hydrophilic UiO-66 crystals with superior water adsorption ability were synthesized and incorporated into the polyimide (PI) membrane for efficient aprotic solvent separation via pervaporation. The effect of the different UiO-66 addition in the pyromellitic dianhydride (PMDA)-2, 2-bis[4-(4-amlnophenoxy)phenyl]propane (BAPP)-based PI membrane on the membrane structure, thermal stability, surface hydrophilicity, solvent-resistant, and pervaporation performance was systematically studied. The UiO-66/PI hybrid membranes with small amount content (2 wt%) exhibited high hydrophilicity and excellent swelling resistance due to the superb dispersion benefiting from the excellent complexation of UiO-66 and PI chain. The effects of operational variables such as operating temperature and concentration of feed solution on the pervaporation separation performance of the hybrid membranes with different UiO-66 loadings were investigated. When the mass fraction of UiO-66 was 2 wt%, the hybrid membranes show the permeation flux of 109.7 and 57.1 g/(m 2 h) and separation factor of 34.1 and 133.9, respectively, for DMF/H 2 O and DMAc/H 2 O systems.
Graphical abstract
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DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Hao Guo,Jiaqin Liu,Yanhong Li,Jürgen Caro,Aisheng Huang
Due to their rationally controlled pore size and easy functionalization, metal-organic frameworks (MOFs) are a promising candidate for membrane separation . As one of the most stable MOFs, UiO-66 has attracted intense attention for the preparation of molecular sieving membranes. A new post-synthesis modification (PSM) strategy was developed to enhance the separation selectivity of supported UiO-66-NH 2 membranes on porous ceramic tubes called UiO-66-NH 2 @SA by using salicylaldehyde (SA) modification. The mixed gas separation factors of H 2 /CO 2 and H 2 /CH 4 can be improved due to constrictions of the pore size through reaction of –NH 2 with SA giving iminophenol moieties. Notably, SA-modified UiO-66-NH 2 membranes are rather stable, at a high operation temperature of 200 °C and 1 bar, mixture separation factors of 11.3 for H 2 /CO 2 and 22 for H 2 /CH 4 can be obtained. Further, no obvious performance degradation has been observed after 3 months storing in air. This high stability of UiO-66-NH 2 @SA membrane could provide possibility for the industrial applications of hydrogen separation and purification.
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DOI
高影响因子
LANGMUIR
·
2020
·
IF 3.557
Huihui Lv,Yunting Zhang,Pan Chen,Jinping Xue,Xiao Jia,Juanjuan Chen
Harmful bacteria have seriously threatened human health and wealth for a long time. Herein, a multifunctional drug delivery system based on UiO-66 was fabricated, and it showed potent synergistic antibacterial effects when used in conjunction with photodynamic therapy and chemotherapy. First, UiO-66-NH2 was prepared via a facile solvothermal method. Then, carboxylic zinc phthalocyanine, a broad-spectrum photosensitizer, was connected to UiO-66-NH2 by amidation. Next, synergistic chemical antibiotic linezolid was loaded in the pores, and lysozyme was coated on the surface by electrostatic interactions. In vitro antibacterial experiments were then carried out to evaluate the antibacterial effects of this system against three kinds of bacteria, Staphylococcus aureus, Escherichia coli, and methicillin-resistant S. aureus (MRSA). The combination of lysozyme, linezolid, and singlet oxygen generated by irradiation of the photosensitizers resulted in a potent antibacterial effect against S. aureus, E. coli, and even MRSA, which demonstrates the synergistic antibacterial efficacy of photodynamic therapy and chemotherapy.
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DOI
PubMed
高影响因子
Environmental Science-Nano
·
2018
·Vol. 5
·期 6
·1441-1453
·
IF 6.087
Jingmiao Wei,Wei Zhang,Weiyi Pan,Chaoran Li,Weiling Sun
Adsorption behaviors and mechanisms of selenite [Se(IV)] and selenate [Se(VI)] on two types of zirconium metal–organic frameworks (MOFs, UiO-66 and UiO-66-NH2) were investigated using batch experiments, spectroscopic analyses, and theoretical calculations. Se(IV) adsorption was substantially greater than Se(VI) adsorption. Intriguingly, with increasing solution pH, Se(IV) adsorption increased to a maximum at pH 7, whereas Se(VI) adsorption monotonically decreased. Se(IV) adsorption was not influenced by coexisting ions except for PO43−, whereas Se(VI) adsorption was in general decreased with increasing coexisting ion concentrations. The underlying molecular binding mechanisms were elucidated via zeta potential, XPS, and FTIR analyses as well as density functional theory calculations. Se(IV) formed a strong inner-sphere complex with the MOFs via Lewis acid/base complexation between the Zr coordinatively unsaturated sites and HSeO3− or SeO32− (−59.4 to −142 kJ mol−1) and hydrogen bonding between Zr–O–C and H2SeO3 (−24.4 to −29.8 kJ mol−1). Se(VI) formed outer-sphere complexes with the MOFs through electrostatic interactions (−50.6 to −62.1 kJ mol−1). Thus, the BET surface area was the predominant factor determining the Se(IV) adsorption, whereas both the surface charge and BET surface area controlled the Se(VI) adsorption. This study provided new insights on the molecular interactions between Se(IV) and the MOFs, and revealed the distinct differences between the Se(IV) and Se(VI) adsorptions.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Chaohui He,Yong Wang,Yang Chen,Xiaoqing Wang,Jiangfeng Yang,Libo Li,Jinping Li
The separation of propane (C 3 H 8 ) from propylene (C 3 H 6 ) to obtain high purity C 3 H 6 as a petrochemical raw material is an important, but challenging process. In the traditional industrial process, the separation mainly relies on energy-intensive cryogenic distillation. One alternative process that is currently becoming more attractive in the separation of C 3 H 6 is adsorptive separation technology. Using porous materials, especially C 3 H 8 selective adsorbents, high purity C 3 H 6 can be directly obtained and thus, significantly simplifies the process. Herein, a series of functionalized ligands were introduced into UiO-type materials to finely regulate the C 3 H 8 separation performance. Single-component adsorption isotherms reveal that BUT-10 has a distinct binding affinity for C 3 H 8 over C 3 H 6 over a wide range of temperature from 298 to 338 K and thus, achieved by far the highest C 3 H 8 capture capacity (105 cm 3 g −1 at 0.1 bar and 298 K) reported among the C 3 H 8 -selective materials reported to date. A combination of Grand Canonical Monte Carlo and density-function theory simulations demonstrate that the favorable pore environment provided by the multiple host-guest interactions toward C 3 H 8 result in the higher C 3 H 8 binding affinity observed in the separation process. Breakthrough experiments indicate that BUT-10 can selectively separate C 3 H 8 from C 3 H 8 /C 3 H 6 (1/1 and 1/15, v/v) mixtures and thus, directly produces high purity C 3 H 6 (>99.99%) under ambient conditions.
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DOI
高影响因子
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