SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Hesong Wang,Jinlong Wang,Jing Zhao,Han Zhang,Luming Liu,Xueying Sun,Guibai Li,Heng Liang
As an emerging metal organic framework (MOF) material, MIL-101(Cr) has a large specific surface area and good hydraulic stability, making it ideal in applications before ultrafiltration (UF). However, the unclear interaction between MIL-101(Cr) and natural organic matter (NOM) was identified as the main limitation to understand membrane fouling. To reveal the working mechanisms of NOM removal using MIL-101(Cr), an integrated system of MOF and UF was constructed and operated in separation mode (SM) and coating mode (CM). Based on the results, MIL-101(Cr) had a high NOM adsorption capacity of 68.454 mg/g for HA and 174.725 mg/g for BSA at saturation. Permeate quality improvement occurred in both modes over a 37.7% UV 254 removal rate and a 15% fluorescence intensity decrease, and permeation performance of the hybrid system was simultaneously enhanced. We found that MIL-101(Cr) influenced membrane fouling behaviors and models because of the foulant transformation in SM and dispersed NOM in the MIL-101(Cr) layer in CM. Furthermore, MIL-101(Cr) played a dual role in the integrated system. It could remove NOM by adsorption, leading to membrane fouling reduction, but also caused additional filtration resistance. Notably, MIL-101(Cr) showed the overall positive effects due to its open hollow structure and good hydrophilicity. The π-π interactions and salt-bridges between MIL-101(Cr) and NOM played a dominant role in adsorption. Whilst SM was more efficient in membrane fouling mitigation due to reduced membrane fouling resistance and a normalized flux increase above 15%, CM could achieve the same permeate quality with less MIL-101(Cr) usage and reaction time. This study reveals the interaction between MIL-101(Cr) and NOM and their effects on UF, providing a scientific basis for the widespread application of MOFs.
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Materials
·
2022
·Vol. 15
·期 10
·3645
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IF 3.748
Minmin Zou,Ming Dong,Mingliang Luo,Hexin Zhu,Tian Zhao
Hierarchically porous MIL-101(Cr) (H-MIL-101(Cr)) with meso/macro-pores was directly prepared via nanofusion progress by using butyric acid as a modulating agent. In the methyl orange (MO) adsorption experiments, H-MIL-101(Cr) showed a high adsorption capability of 369.8 mg g−1, which was 1.52-fold greater than that of pristine MIL-101(Cr) (P-MIL-101(Cr)). While in the oxidation reaction of indene and 1-dodecene tests, H-MIL-101(Cr) presented much higher catalytic efficiency, with turnover frequency (TOF) values of 0.7242 mmol g−1min−1and 0.1492 mmol g−1min−1, respectively, which were 28% and 34% greater than that in the case of P-MIL-101(Cr). Thus, compared with P-MIL-101(Cr), H-MIL-101(Cr) exhibited better removal efficiency and higher levels of activity in the oxidation reactions of indene and 1-dodecene. The unique structure of H-MIL-101(Cr) also contributed to its superior performance in these processes.Keywords:hierarchically porous;MIL-101(Cr);butyric acid;MO adsorption;catalysis
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Ye Zhaochun,Yao JiaCheng,Zheng Wen,Yuan Wenhui,Guan Jianyu,Li Li,Xiao Hong
Octafluoropropane (C 3 F 8 ) is a kind of super greenhouse gas, and the low concentration of octafluoropropane makes it difficult to be adsorbed and removed. In this study, a series of Co-doped MOFs (Co x Cr-MIL-101) have been successfully synthesized using a hydrothermal method without the addition of strong acids such as HF. The structural properties of the prepared Co x Cr-MIL-101 are characterized using SEM, XRD, nitrogen adsorption desorption test, etc. The adsorption properties of C 3 F 8 are measured by single-component isothermal adsorption experiments and fixed bed adsorption breakthrough experiments. The adsorption mechanism was investigated via the adsorption theory models. The results show that the introduction of cobalt ions can effectively improve the adsorption capacity of MIL-101, among which the Co 0.2 Cr-MIL-101 exhibits the best adsorption performance. The C 3 F 8 equilibrium adsorption capacity reaches 0.077 mmol/g at 298 K and 180 Pa, which is 3.03 times that of the pristine MIL-101 and the dynamic adsorption capacity is 20.710 mmol/g (298 K, 1.2 L/min), which is 9.37 times that of the pristine MIL-101. Inspiringly, the IAST separation selectivity of C 3 F 8 /N 2 at 100 kPa is up to 146.7, which is 14.3 times that of the pristine MIL-101. More importantly, the co-modified adsorbent showed better thermal stability and cyclic stability. In addition, Co 0.2 Cr-MIL-101 fits the Freundlich isothermal adsorption model, and the adsorption mechanism analysis shows that the high adsorption capacity of Co 0.2 Cr-MIL-101 benefits from the unique pore structure and abundant active sites of the modified MOFs.
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JOURNAL OF THE INDIAN CHEMICAL SOCIETY
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2021
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IF 0.284
Jiacheng Li,Xiaoqin Li,Zichuang Wang,Yannan Jia,Kai Xu,Zijie Wang,Zheng Wang
Amino-functionalized magnetic MIL-101(Cr) was prepared via a one-step solvothermal method, characterized, and applied in adsorptive Sb(III) removal. The effects of solution pH, adsorbent dosage, and coexisting substances on the adsorption of Sb(III) by MIL-101(Cr)–NH 2 /MnFe 2 O 4 were studied. The adsorption kinetics were analyzed using pseudo-first order, pseudo-second order, intraparticle diffusion, and Elovich models, while Freundlich and Langmuir isotherm models were used to fit the experimental data. The pseudo-second-order kinetic model provided the best fit for the kinetic data. The maximum adsorption capacity of MIL-101(Cr)–NH 2 /MnFe 2 O 4 for Sb(III) was 91.07 mg/g, as calculated using the Langmuir adsorption isotherm model. Thermodynamic analysis revealed that the adsorption of antimony onto MIL-101(Cr)–NH 2 /MnFe 2 O 4 is spontaneous and endothermic, while response surface optimization revealed that the optimal conditions for Sb(III) adsorption by MIL-101(Cr)–NH 2 /MnFe 2 O 4 are an adsorbent loading of 222.55 mg/L, a pH of 4.5, and a temperature of 294.59 K. The predicted adsorption capacity of MIL-101(Cr)–NH 2 /MnFe 2 O 4 for Sb(III) is only a 1.8% deviation from the actual value. Furthermore, MIL-101(Cr)–NH 2 /MnFe 2 O 4 exhibits strong magnetism, allowing it to be separated from wastewater using a magnet. Finally, a preliminary economic analysis showed that the cost of treating a ton wastewater containing 25 mg/L antimony using this composite would be 26.24 USD. Thus, MIL-101(Cr)–NH 2 /MnFe 2 O 4 is promising for treatment of Sb(III)-containing wastewater.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
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IF 4.084
Guoru Li,Xiaobo He,Fengxiang Yin,Biaohua Chen,Huaqiang Yin
The development of highly efficient electrocatalysts with low cost for oxygen reduction reaction (ORR) is urgently required for metal-air batteries and fuel cells. In this work, Fe Co/MIL-101(Cr) with various molar ratios of Fe/Co as hybrid catalysts was prepared by a facile and mild impregnation method. MIL-101(Cr) increased the specific surface areas of the hybrid catalysts, thus improving the dispersion of Fe and Co species at their surfaces. The effects of Fe and Co species on ORR activity of the hybrid catalysts were investigated. It is found that the synergistic effects between the well-dispersed Fe and Co species contribute mainly to ORR activity. More specifically, Fe species exert a partial-charge-transfer-activation effect on Co ones, which reduces the charge transfer resistance and thus improves the catalytic activity . As a result, Fe Co/MIL-101(Cr) showed the excellent ORR activity, in which Co 50 Fe 50 /MIL-101(Cr) exhibited the superior ORR activity to the other prepared hybrid catalysts.
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JOURNAL OF POROUS MATERIALS
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2019
·Vol. 26
·期 6
·1607-1618
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IF 1.947
Hou Pengchao,Xing Guangjian,Han Dan,Zhao Yan,Zhang Gang,Wang Hao,Zhao Chang,Yu Chunna
MIL-101(Cr)/graphene aerogel (MIL-101(Cr)/GA) was synthesized using a two-step synthesis and used as a high efficient adsorbent for wastewater purification. The as-prepared MIL-101(Cr)/GA was characterized using XRD, FTIR and Raman spectroscopy, XPS and FESEM to investigate its structure, composition and morphology. MIL-101(Cr)/GA exhibited a 3D interconnected macroporous framework comprised of graphene sheets, on which MIL-101(Cr) particles were dispersed uniformly. Dyes, organic solvents and oils were used to evaluate the adsorption performance of MIL-101(Cr)/GA, which exhibited an excellent adsorption capacity for both anionic methyl orange (331.5 mg g −1 ) and cationic rhodamine B (345.7 mg g −1 ) as well as 51–101 times its own weight of various solvents/oils. In addition, the MIL-101(Cr)/GA showed superior recycling stability for dyes and a rapid adsorption rate for solvents/oils. The excellent adsorption performance was attributed to a synergistic effect between MIL-101 and the graphene aerogel. The kinetic behavior for adsorption observed for MIL-101(Cr)/GA was well-fitted by a pseudo-second-order kinetic model. It is envisaged that MIL-101(Cr)/GA will be a promising adsorbent for the removal of pollutants and wastewater purification.
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NANO
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2018
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IF 1.1
Shipeng Yang,Siwei Peng,Chunhui Zhang,Xuwen He,Yaqi Cai
Nanoparticles of the semiconductor catalyst Cd x Zn 1 − x S were embedded into the metal organic framework MIL-101(Cr) to obtain Cd x Zn 1 − x S@MIL-101(Cr) nanocomposites. These materials not only possess high surface areas and mesopores but also show good utilization of light energy. The ultraviolet-visible diffuse reflectance patterns of Cd x Zn 1 − x S@MIL-101(Cr) nanocomposites showed that Cd 0 . 8 Zn 0 . 2 S@MIL-101(Cr) possessed good visible light response ability among the synthesized nanocomposites. The photocatalytic performance of the Cd x Zn 1 − x S@MIL-101(Cr) nanocomposites were tested via degradation and mineralization of methylene blue in neutral water solution under light irradiation using a 300W xenon lamp. As a result, using Cd 0 . 8 Zn 0 . 2 S@MIL-101(Cr) as a catalyst, 99.2% of methylene blue was mineralized within 30 min. Due to the synergistic effect of adsorption by the MIL-101(Cr) component and photocatalytic degradation provided by the Cd 0 . 8 Zn 0 . 2 S component, the Cd 0 . 8 Zn 0 . 2 S@MIL-101(Cr) catalyst displayed superior photocatalytic performance relative to Cd 0 . 8 Zn 0 . 2 S and MIL-101(Cr). Furthermore, Cd 0 . 8 Zn 0 . 2 S@MIL-101(Cr) possessed excellent stability during photodegradation and exhibited good reusability. The remarkable photocatalytic performance of Cd 0 . 8 Zn 0 . 2 S@MIL-101(Cr) is likely due to the effective transfer of electrons and holes at the heterojunction interfaces.
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RSC Advances
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2018
·Vol. 8
·期 71
·41003-41011
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IF 2.936
Wen Bing Wu,Sun Xue,Jian Hua Chen,Xiao Li
Membrane separation technologies have great promising potential for applications in several industries. Metal–organic frameworks (MOFs), for their large surface areas, low framework densities, transition-metal ions in the skeleton and high pore volumes relative to other porous matrices, have great potential for the removal of sulfur from gasoline with high efficiency. In the present study, a novel porous membrane adsorbent MIL-101(Cr)/SA was prepared by immobilizing MIL-101(Cr) onto sodium alginate (SA) matrix, which can combine the size/shape selectivity of MIL-101(Cr) with the processability and mechanical stability of SA polymer. The physico-chemical properties of MIL-101(Cr)/SA were investigated by FT-IR, SEM, BET, XRD and EDX methods. To investigate the effects of some important factors on the adsorption behavior for thiophene, a batch of experiments were performed by changing the concentration of porogen polyethylene glycol in the MIL-101(Cr)/SA, solution temperature, initial thiophene concentration and contact time. Meanwhile, benzothiophene, thiophene and 3-methyl thiophene were used to test the selectivity of MIL-101(Cr)/SA. The MIL-101(Cr)/SA showed an excellent uptake capacity of 671 mg g−1 under the optimal adsorption conditions. Selectivity testing indicated that the uptake capacity of MIL-101(Cr)/SA follows the order of benzothiophene > thiophene > 3-methyl thiophene. Kinetics experiments indicated the pseudo-second-order model displayed good correlation with adsorption kinetics data. The Crank model showed that the intraparticle solute diffusion is the rate-controlling adsorption step. Regeneration experiment result shows that the prepared MIL-101(Cr)/SA has excellent adsorption and desorption efficiencies.
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RSC Advances
·
2016
·Vol. 6
·期 93
·90232-90238
·
IF 3.289
Xiao-Fang Liu,Hu Li,Heng Zhang,Hu Pan,Shan Huang,Kai-Li Yang,Song Yang
Catalytic ethanolysis of furfuryl alcohol (FA) to ethyl levulinate (EL) with MIL-101(Cr)–SO3H, prepared by simple one-pot hydrothermal treatment, is presented for the first time. The as-prepared catalyst with high surface area, hydrothermal and chemical stability, good dispersion, and feasible accessibility of –SO3H Brønsted acid sites was found to show superior performance to other sulfonic acid-functionalized solid catalysts. Besides the special textural properties, the obtained good catalytic activity of 79.2% EL yield and 100% FA conversion were also dependent on the density and strength of the Brønsted acid and the reaction parameters. A slight loss of catalytic activity after five consecutive recycles and the hot filtration experiment confirmed the good stability of MIL-101(Cr)–SO3H. Two coexisting reaction paths for the ethanolysis of FA to EL catalyzed by MIL-101(Cr)–SO3H were proposed, wherein 2-ethoxymethylfuran (2-EMF) was observed to be the dominant intermediate.
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Journal of Inorganic and Organometallic Polymers and Materials
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2024
·
IF 3.9
Li Mengke,Cao Panpan,Dong Wenwen,Zhao Jun,Li Dongsheng
Organic dyes pollution has caused significant threat to flora, fauna and humans because the toxic of dyes. In this work, with the help of acetic acid as a defect initiator, the hierarchical porous MIL-101(HP-MIL-101) has been synthesized and used for removing anionic dyes Eosin y (EY), Methyl orange (MO), Congo red (CR) and Acid fuchsin (AF) from water. Due to its positive surface charge, larger specific surface area, well-matched pore structure, and the charge, size, and diameter of dyes, HP-MIL-101 showed rapid adsorption and an excellent maximum adsorption capacity of 425 and 336 mg⋅g − 1 for CR and AF, respectively. A series of batch experiments were carried out to investigate the impact of various key factors, including adsorption duration, initial dye concentration, and temperature. In addition, the kinetics, isotherm, and thermodynamics about the adsorption properties were also discussed. In addition, HP-MIL-101 showed stable and high reusability for at least three cycles, with an efficiency of over 95% without significant structural changes. This study highlights the potential of hierarchical porous MOF for mitigating dye pollution and advancing sustainable water treatment methodologies.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
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IF 10.8
Yacong Liu,Yue Lin,Weichao Wang,Ke Min,Weibo Ling,Wende Ma,Weican Zhang,Xingwang Hou,Linfeng Wei,Qian Liu,Guibin Jiang
With the increasing use of metal–organic frameworks (MOFs), they will inevitably enter the environment intentionally or unintentionally. However, the effects of MOFs on plant growth are poorly understood. Here, we investigated the effects of exposure of the rhizosphere to MOFs on plant growth. MIL-101(Cr) was selected as a research model due to its commercial availability and wide use. Soybean plants at the two-leaf stage were subjected to various durations (1–7 days) and concentrations (0–1000 mg/L) of exposure in hydroculture with a control group treated with ultrapure water. We found that MIL-101(Cr) had a positive effect on soybean growth at a lower dose (i.e., 200 mg/L); however, at higher doses (i.e., 500 and 1000 mg/L), it exhibited significant toxicity to plant growth, which is evidenced by leaf damage. To investigate the mechanism of this effect, we used Cr as an indicator to quantify, track, and image MIL-101(Cr) in the plant with laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). Results indicated that MIL-101(Cr) primarily accumulated in the cortex of roots (up to 40 times higher than that in stems), with limited translocation to stems and negligible presence in leaves and cotyledons. In addition, metabolomic analysis of soybeans indicated that low-dose MIL-101(Cr) could increase the sucrose content of soybean roots to promote plant growth, while a high dose could induce lipid oxidation in roots. This study provides valuable insights into the ecological toxicology of MOFs and underscores the importance of assessing their environmental impact for sustainable agricultural practices.
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ANALYTICAL CHEMISTRY
·
2011
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IF 5.874
Cheng-Xiong Yang,Xiu-Ping Yan
The diverse structures and pore topologies, accessible cages and tunnels, and high surface areas make metal–organic frameworks attractive as novel media in separation sciences. Here we report the slurry-packed MIL-101(Cr) column for high-performance liquid chromatographic separation of substituted aromatics. The MIL-101(Cr) packed column (5 cm long × 4.6 mm i.d.) offered high-resolution separation of ethylbenzene (EB) and xylene, dichlorobenzene and chlorotoluene isomers, and EB and styrene. The typical impurities of toluene and o-xylene in EB and styrene mixtures were also efficiently separated on the MIL-101(Cr) packed column. The column efficiencies for EB, m-dichlorobenzene, and m-chlorotoluene are 20000, 13000, and 10000 plates m–1, respectively. The relative standard deviation for five replicate separations of the substituted aromatics was 0.2–0.7%, 0.9–2.9%, 0.5–2.1%, and 0.6–2.7% for the retention time, peak area, peak height, and half peak width, respectively. The MIL-101(Cr) offered high affinity for the ortho-isomer, allowing fast and selective separation of the ortho-isomer from the other isomers within 3 min using dichloromethane as the mobile phase. The effects of the mobile phase composition, injected sample mass, and temperature were investigated. The separation of xylene, dichlorobenzene, and chlorotoluene on MIL-101(Cr) was controlled by entropy change, while the separation of EB and styrene on MIL-101(Cr) was governed by enthalpy change.
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