CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
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2023
·Vol. 39
·期 6
·1084-1091
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IF 3.1
Gao Zhuangzhuang,Li Baoju,Ou Shuxian,Li Dongsheng,Fang Qianrong,Qiu Shilun,Xue Ming
M etal-organic frameworks (MOFs) are attractive in membrane separation due to their special pore structure and suitable aperture size. The fabrication of defect-free and robust MOF membranes with excellent durability is highly demanded but remains challenging. In this work, we report a one-step active γ -alumina conversion strategy for the facile and reliable fabrication of an MIL-96 membrane. In this case, the γ -Al 2 O 3 sol was dip-coated and sintered on the α -Al 2 O 3 disc as the active aluminum source and substrate for the nucleation and growth of MOF. A continuous and well-intergrown MIL-96 membrane was generated with exceptional stability due to the strong adhesion to the substrate. The resultant MIL-96 membrane yielded a satisfactory H 2 /CO 2 permselectivity and high-temperature resistance, delivering a selectivity of 12.35 with H 2 permeance of 6.20×10 −7 mol·m −2 ·s −1 ·Pa −1 at 150 °C. Moreover, the probe membrane presented remarkable durability and recyclability under harsh hydrothermal conditions. This method paves the way for constructing highly stable and selective MOF membranes and could accelerate the development of advanced membrane separation technologies for gas purification and recycling in addressing the severe energy and environmental problems.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Dingliang Dai,Jianhao Qiu,Ming Li,Jie Xu,Lu Zhang,Jianfeng Yao
A series of BiOI/MIL-121(Al) hybrid photocatalysts has been prepared by a facile hydrothermal method. Two-dimensional BiOI sheets are intimately anchored on rod-like MIL-121 due to the electrostatic and coordination effects between Bi 3+ and carboxyl. The BiOI/MIL-121(Al) hybrid exhibits favorable performances for visible-light-driven degradation of tetracycline. The degradation performance of the optimal sample BM-20 is more than twice as that of pure BiOI. Apart from the close contacts between BiOI and MIL-121, the hydrogen bond induced by carboxyl in MIL-121 promotes the adsorption of tetracycline, which is also conducive to the photocatalytic degradation process. Moreover, results show that photo-induced holes and superoxide radicals are both the main active species for the photocatalytic degradation of tetracycline over BiOI/MIL-121 composites. This work would inspire the materials design with specific functional groups for efficient (photo)catalytic reaction.
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Polymers
·
2021
·Vol. 13
·期 20
·3498
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IF 4.329
Shengqi Liu,Ye Meng,Hu Li,Song Yang
Considering economic and environmental impacts, catalytic biomass conversion to valuable compounds has attracted more and more attention. Of particular interest is furfural, a versatile biorefinery platform molecule used as a feedstock for the production of fuels and fine chemicals. In this study, the Cr-based metal-organic frameworks (MOFs) MIL-101 were modified by chlorosulfonic acid, and MIL-101 was changed into a hierarchical MOF structure with smaller particles and lower particle crystallinity by CTAB, which significantly improved the acidic sites of the MOFs. The original and modified MIL-101(Cr) catalysts were characterized by XRD, N2adsorption-desorption, SEM, TEM, and FT-IR. The effects of different catalysts, reaction temperature, catalyst amount, and alcohol type on the reaction were studied. Under the action of the MOFs catalyst, a new mild route for the condensation of furfural with various alkyl alcohols to the biofuel molecules (acetals) was proposed. The conversion route includes the conversion of furfural up to 91% yield of acetal could be obtained within 1 h solvent-free and in room-temperature reaction conditions. The sulfonic acid-functionalized MIL-101(Cr) is easy to recover and reuse, and can still maintain good catalytic activity after ten runs.Keywords:biomass conversion;MIL-101(Cr);furfural;green chemistry;heterogeneous catalysis
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JOURNAL OF POROUS MATERIALS
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2021
·Vol. 29
·期 1
·181-192
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IF 2.496
Wang Li,Zhou Yu,Xu Qi,Wu Xian-Kun,Xu Guo-Dong,Guo Ji-Xiang,Fang Dong
The development of high efficient and cost-effective photocatalysts for organic matters degradation and hydrogen evolution is of great importance. In this study, heterojunction photocatalysts based In 2 S 3 and MIL-68(In) were synthesized by hydrothermal method. These composites exhibit excellent bi-functionality of photocatalytic Rhodamine B degradation and hydrogen evolution. And it was found that the photocatalytic performance of the composites was dependent on the ratio of In to S. The optimum catalyst In 2 S 3 /MIL-68(In)-1.5 exhibits much enhanced photocatalytic performance, offering a removal efficiency of 94.7% within 30 min for 20 ppm of Rhodamine B and a hydrogen evolution rate of 1618.8 µmol h −1 g −1 as a result of the synergist effect of heterojunction between the two components, promoting the charge separation. Besides, the mechanisms for photocatalytic degradation of Rhodamine B and photocatalytic hydrogen evolution were also proposed. This protocol could provide guiding information on the development of other functional photocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Huanan Zhao,Zipeng Xing,Siyi Su,Sijia Song,Zhenzi Li,Wei Zhou
NH 2 -MIL-53(Al)/CdS p-n heterojunctions are fabricated via facile two-step hydrothermal method. The formation of p-n heterojunctions could form built-in field, which favors spatial charge separation. The resultant NH 2 -MIL-53(Al)/CdS p-n heterojunctions with narrowed band gap extend the photoresponse, and have a high specific surface area of 417.7 m 2 g −1 , and a narrow pore size of 8.8 nm. Under visible light irradiation, the photocatalytic efficiency for reduction of Cr(VI) and removal of refractory pesticide trichlorophenol is up to 99.23 and 98.85 %, respectively. The photocatalytic oxygen evolution is also as high as 563.6 μmol g −1 h −1 . The excellent photocatalytic activity can be ascribed to the efficient p-n heterojunctions accelerating charge transfer and favoring spatial charge separation, and the special mesoporous structure supplying adequate surface-active sites and facilitating mass transfer. This facile strategy opens up new insights for fabricating other p-n heterojunctions photocatalysts with efficient solar energy conversion.
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APPLIED SURFACE SCIENCE
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2020
·
IF 6.182
Zhihui Lu,Xuefang Cao,Hong Wei,Wenting Huo,Qiquan Wang,Kebin Li
Metal organic frameworks (MOFs) have shown a great potential to act as heterogeneous Fenton-like catalysts. However, the lower catalytic efficiency and reaction rate are limiting their practical applications. Herein, a facile and efficient strategy was studied to boost the catalytic oxidation performance of MIL-68(Fe)-mediated Fenton-like process with the addition of a minor amount of bisulfite. The factors affecting the catalytic oxidation capacity of the MIL-68(Fe)/HSO 3 − /H 2 O 2 system were investigated using methyl orange (MO) as model pollutant. Under the optimal condition, the degradation rate of MO could be increased by 11.5 times compared to that in MIL-68(Fe)/H 2 O 2 system, and the total organic carbon (TOC) removal in 120 min reached 46.8%. The MIL-68(Fe)/HSO 3 − /H 2 O 2 system also displayed a wide applicable pH range. Besides MO, other organic contaminants such as acid red 18 (AR18), rhodamine B (RhB), methylene blue (MB), xylenol orange (XO) and tetracycline hydrochloride (TC) could be effectively degraded in the MIL-68(Fe)/HSO 3 − /H 2 O 2 system as well. The quenching tests and electron paramagnetic resonance (EPR) spectrometry confirmed that OH, SO 4 − , HO 2 , and 1 O 2 were the main reactive species for MO degradation in the MIL-68(Fe)/HSO 3 − /H 2 O 2 system. The coumarin fluorometry further disclosed that much more hydroxyl radicals were generated in the MIL-68(Fe)/HSO 3 − /H 2 O 2 system than in MIL-68(Fe)/H 2 O 2 system. Cyclic voltammetry analysis, on the other hand, indicated that the presence of HSO 3 − facilitated the Fe(III)/Fe(II) cycle in the MIL-68(Fe)/HSO 3 − /H 2 O 2 system. Based on these results, the enhancement mechanism of the Fenton-like MIL-68(Fe)/HSO 3 − /H 2 O 2 system was proposed. Finally, the cyclic experiments manifested the MIL-68(Fe)/HSO 3 − /H 2 O 2 system had good stability and reusability. This study suggests that the addition of bisulfite being an excellent approach to construct the Fe-MOFs mediated Fenton systems for eliminating organic contaminants in water with high efficiency.
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Nanomaterials
·
2020
·Vol. 10
·期 10
·2000
·
IF 4.324
Yongpan Shan,Chunli Xu,Hongjun Zhang,Huiping Chen,Muhammad Bilal,Shujun Niu,Lidong Cao,Qiliang Huang
Recently, metal–organic frameworks (MOFs) have become a dazzling star among porous materials used in many fields. Considering their intriguing features, MOFs have great prospects for application in the field of sustainable agriculture, especially as versatile pesticide-delivery vehicles. However, the study of MOF-based platforms for controlled pesticide release has just begun. Controlled pesticide release responsive to environmental stimuli is highly desirable for decreased agrochemical input, improved control efficacy and diminished adverse effects. In this work, simple, octahedral, iron-based MOFs (NH2-Fe-MIL-101) were synthesized through a microwave-assisted solvothermal method using Fe3+as the node and 2-aminoterephthalic acid as the organic ligand. Diniconazole (Dini), as a model fungicide, was loaded into NH2-Fe-MIL-101 to afford Dini@NH2-Fe-MIL-101 with a satisfactory loading content of 28.1%. The subsequent polydopamine (PDA) modification could endow Dini with pH-sensitive release patterns. The release of Dini from PDA@Dini@NH2-Fe-MIL-101 was much faster in an acidic medium compared to that in neutral and basic media. Moreover, Dini@NH2-Fe-MIL-101 and PDA@Dini@NH2-Fe-MIL-101 displayed good bioactivities against the pathogenic fungus causing wheat head scab (Fusarium graminearum). This research sought to reveal the feasibility of versatile MOFs as a pesticide-delivery platform in sustainable crop protection.Keywords:metal–organic framework;polydopamine;pesticide;pH-sensitive release;fungicidal activity
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CHEMICAL PHYSICS LETTERS
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2020
·
IF 2.029
Wenbo Liu,Jiabin Zhou,Lidan Ding,Yuling Yang,Tianlei Zhang
The MIL-88/PVB nanofibers were prepared by hydrothermal synthesis and subsequent electrostatic spinning. The composite was used as a high efficiency heterogeneous catalyst for photocatalysis coupling of Fenton process to remove tetracycline hydrochloride (TC-HCl) under visible light irradiation. The results indicated that 99% of TC-HCl (500 mg·L −1 ) was degraded in 90 min. The MIL-88/PVB nanofibers were easy to separate from solution. The results of scavenging experiments and ESR analysis demonstrated that OH and O 2− were the predominant radicals for the TC-HCl degradation. Moreover, the possible mechanism for enhanced degradation performance of TC-HCl in the heterogeneous catalytic oxidation system was proposed.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2020
·Vol. 31
·期 6
·4822-4835
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IF 2.22
Zhou Nan,Tan Junjie,Li Xi,Wang Lu,Jin Chenglong,Chen Ming,Yu Zhengsong,Liang Yani,Qiu Zhidong,Li Wenlong,Dong Yulin,Xie Zhizhong,Lin Yawei,Qu Deyu,Zhang Chaocan
A series of Bi 5 O 7 I/MIL-53(Fe) (BOI/MIL- w ) composites were successfully prepared by a facile in-situ solvothermal approach. The matched energy bands enabled Bi 5 O 7 I and MIL-53(Fe) to form a Z-scheme heterojunction which resulted in an efficient separation of the photo-induced electron–hole pairs. The photocatalytic activity of BOI/MIL- w was evaluated by the degradation of Rhodamine B (RhB) in water under the visible light irradiation. Compared with Bi 5 O 7 I, photocatalytic performances of BOI/MIL- w notably boosted. When the content of added MIL-53(Fe) was 3 wt%, BOI/MIL-3 presented the highest activity with a degradation efficiency of 99.7% only after 60 min of irradiation. The reaction rate constant k could reach 0.0992 min −1 which was nearly 12.6 times as high as that of Bi 5 O 7 I. Moreover, BOI/MIL- w had a good stability and reusability, which could ensure its practical application. Trapping experiments confirmed that h + and ·O 2 − were the dominant active species during the photocatalytic process, and further demonstrated the formation of the Z-scheme heterojunction facilitated the photocatalytic performance of BOI/MIL- w .
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Qiong Wu,Yining Liu,Haochuan Jing,Hongbin Yu,Ying Lu,Mingxin Huo,Hongliang Huo
Special enhanced synergistic effect of ultra-small γ-Fe 2 O 3 and graphene oxide (GO) on MIL-53 (Fe) was achieved for boosting photocatalysis. Compared to traditional methods of surface coverage, the incorporation of γ-Fe 2 O 3 (average size 2–3 nm) inside MOFs particles not only increased the light absorption of catalyst, but also formed numerous micro-heterojunctions with MOFs units and thus effectively facilitated the separation of photogenerated carriers. By supplying attachment sites for MOFs crystal, the functionalized GO reduced the size of MOFs particles to 100–200 nm, meanwhile improved their dispersibility. The active sites and quantum yield of photocatalytic reaction were also intensified benefiting from the large surface area and high electronic conductivity of GO. Therefore, the novel γ-Fe 2 O 3 -MIL-53(Fe)-GO composite exhibited the highest photocatalytic activity towards norfloxacin, with a removal rate of 92.8% in 90 min. The kinetic constant was 4.49-fold higher than that using pure MIL-53 (Fe), and 1.43-time greater than that in the system of MIL-53 (Fe) and hydrogen peroxide, which usually acted as efficient electron acceptors to increase the quantum yield and final photocatalytic performance of MOFs. Based on the identified intermediates, three NOR degradation pathways including the cleavage of piperazine ring, defluorination and decarboxylation, as well as the conversion of quinolones group were proposed. Photocatalytic mechanism investigation revealed the holes and hydroxyl radicals came from the reaction of electrons with oxygen played the important role in γ-Fe 2 O 3 -MIL-53(Fe)-GO photocatalysis. Moreover, the utilization of magnetic nanoparticles improved the recovery and recyclability of ternary catalyst.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2020
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IF 4.551
Yanshu Luo,Bingqiong Tan,Xianghui Liang,Shuangfeng Wang,Xuenong Gao,Zhengguo Zhang,Yutang Fang
Metal organic frameworks (MOFs) MIL-100(Fe) is considered to be a promising porous adsorbent for dehumidification due to its good hydrophilicity and hydrothermal stability. However, the powdery MIL-100(Fe) prepared by the conventional hydrothermal method is not suitable for industrial rotary desiccant dehumidifier. In order to produce a high-performance rotor core component, a new dry gel conversion in situ synthesis strategy for glass-fiber MIL-100(Fe) monolithic adsorbent was proposed in this paper. The effects of the reaction sol concentration on the crystalline phase, morphology, pore structure , adsorption/desorption performance and the cycling stability of the monolith were discussed in detail. The results showed that MIL-100(Fe) crystals which evenly dispersed in the surface and voids of glass fiber, could be conveniently synthesized in the reaction sols with molar ratios of 1Fe (III)/0.67BTC/xH 2 O (x = 93–185). Among them, the MIL-100(Fe) monolith obtained at x = 93 exhibited a high loading (85.7%), large BET specific surface area (1441 m 2 /g), S-shaped water vapor adsorption isotherm and high saturated adsorption ratio (0.496 g/g) at 298 K and 60% RH , low desorption activation energy (48.28 kJ/mol) as well as a reliable cycling stability. Favorable adsorption/desorption performance of MIL-100(Fe) monolith and convenient dry gel preparation process provide a guidance for the manufacture of high-performance dehumidification rotary wheel.
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LANGMUIR
·
2020
·
IF 3.557
Xiaoxu Dong,Mei Cui,Renliang Huang,Rongxin Su,Wei Qi,Zhimin He
A superhydrophobic and superoleophilic porous composite was successfully prepared via a polydopamine-assisted surface coating of MIL-53(Fe) and 1-dodecanethiol (DDT) on a melamine formaldehyde (MF) sponge. The as-prepared sponge composite (MIL-DDT@MF) has a high water contact angle (WCA) of 151.8°, which is probably attributed to both the rough surface derived from in situ growth of MIL-53 nanocrystals and the low surface energy due to grafting of hydrophobic 1-dodecanethiol. The MIL-DDT@MF sponge can effectively absorb oil or organic solvent with an absorption capacity of up to 54.1 (for petroleum) to 120.2 (for chloroform) times its own weight. In addition, the MIL-DDT@MF sponge retained a high absorption capacity and maintained approximately 78% of its original value after 50 cycles of reuse. Moreover, the MIL-DDT@MF sponge can selectively absorb the oil/organic solvent from water and achieve continuous oil–water separation. The separation efficiency of n-hexane, dichloromethane, and crude oil from water or seawater can reach above 95%. The superhydrophobic and superoleophilic MIL-DDT@MF sponge has potential as a promising absorbent for treatment of oily wastewater.
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