INORGANIC CHEMISTRY COMMUNICATIONS
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2022
·
IF 3.428
Zihao Hu,Huiqi Wu,Fang Zhu,Sridhar Komarneni,Jianfeng Ma
MIL-101(Fe)/Co 3 O 4 composites were synthesized using a facile solvothermal method to establish the superiority of a heterogeneous photochemical catalysis system in the presence of Na 2 S 2 O 8 with visible light irradiation. In the present system, the MIL-101(Fe)/Co 3 O 4 catalyst showed better catalytic performance than the single photocatalytic or chemical catalytic system, implying that the MIL-101(Fe)/Co 3 O 4 catalyst can combine both photocatalysis and chemical catalysis well. When tetracycline (TC) is the target pollutant, the highest degradation efficiency can be achieved within 40 min, reaching to 86 %. Crystallinity, morphology, and elemental valence of the MIL-101(Fe)/Co 3 O 4 composite were explored by using X-ray diffraction (XRD), scanning electron microscopy (SEM) as well as X-ray photoelectron spectroscopy (XPS). From the quenching experiments, it was found that 1 O 2 , SO 4 ‾, OH, and O 2 ‾ make contributions to the effective removal of tetracycline. Apart from that, the recovery and reuse characteristics of MIL-101(Fe)/Co 3 O 4 may facilitate the sustainable wastewater treatment.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 42
·21029-21038
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IF 9.931
Liang Zhang,Jing Wang,Xinyi Ren,Wentao Zhang,Tianshu Zhang,Xinnan Liu,Ting Du,Tao Li,Jianlong Wang
The excessive accumulation of toxic copper species makes it imperative to develop smart dual-functional materials for the simultaneous removal and detection of Cu(II) in drinking water. In this work, novel core–shell NH2-MIL-101(Al)@ZIF-8 nanoflowers were successfully fabricated via an internal extended growth mode under the regulation of polyvinylpyrrolidone (PVP) to achieve this goal. Benefiting from the specific affinity of imidazole nitrogen in ZIF-8 toward Cu(II), the resultant NH2-MIL-101(Al)@ZIF-8 shows high adsorption capacity (526.74 mg g−1). Moreover, the fluorescence of NH2-MIL-101(Al) shows a Cu(II)-dependent change, causing this composite to possess superior selective/sensitive detection with a broad linear range (1.5–625 μM) and a low detection limit (0.17 μM) for Cu(II). Specifically, the hybrid MOF@MOF structure provides greater sensitivity as compared to the individual constituent (pristine NH2-MIL-101(Al)) and the mixed state, which is ascribed to the rational optimization of the smart adsorbent based on the following two aspects. (i) The synergistic effect of the core–shell nanostructure improves the preconcentration ability at the interface between single MOFs. (ii) The existence of the three-dimensional hierarchical nanoflower architecture (structure optimization) accelerates the mass transport and sculpts the final composite with enhanced adsorption and detection ability. These indicate that the smart NH2-MIL-101(Al)@ZIF-8 nanoflower could be an excellent candidate for the synchronous remediation and selective detection of Cu(II) in aqueous systems, which could be potentially useful in wastewater treatment and water quality monitoring.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 38
·18418-18425
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IF 3.925
Fangfang Li,Yan Chen,Aijia Gao,Wenjing Tong,Changchun Ji,Yong Cheng,Ying-Hua Zhou
It is highly desired yet an enormous challenge to exploit efficient catalysts for epoxide cycloaddition with carbon dioxide to achieve the goal of carbon neutrality. Herein, the novel heterogeneous catalysts of MIL-101-IL(RBr) (R = Et, Pr, Bu, and Pe) were synthesized by grafting polypyridyl-based ionic liquids (IL) into the nodes of MIL-101(Cr) through the post-synthetic modification of metal–organic frameworks (MOFs). The octahedral MIL-101-IL(BuBr) with an average size of ca. 800 nm exhibited superior activity for catalyzing epichlorohydrin–CO2 cycloaddition into chloropropene carbonate, with an yield of 92% at 110 °C under 1.0 MPa CO2 without any cocatalyst and solvent. The excellent performance could be attributed to the nucleophilic nature of grafted ionic liquids in the MOF along with the effectiveness of mass transfer afforded by the MOF porosity. Moreover, MIL-101-IL(BuBr) presented a favorable versatility toward other epoxides and a satisfactory recyclability. In addition, a possible mechanism has been proposed for the catalytic reaction of epichlorohydrin–CO2 cycloaddition over MIL-101-IL(BuBr).
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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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Lan Shi,Tianding Hu,Ruiyan Xie,Haibin Wang,Jiangqin Li,Shuangjiang Li,Yi Liu,Yunfei Zhi,Kaili Yao,Shaoyun Shan
The development of high carbon dioxide (CO 2 ) sorption capacity materials is necessary for the deployment of the CO 2 capture and storage strategy. Metal-organic frameworks (MOFs) have emerged as promising substitutes for traditional liquid and solid CO 2 capture sorbents due to their high surface area, tunable pore size, diverse composition, and various physical and chemical properties. However, MOFs feature the intrinsic limitations of powder agglomeration, weak binding affinity, and sluggish diffusion kinetics, thus hindering their industrial application in CO 2 capture. Herein, we design an amine-functionalized MIL-101@cellulose (NH 2 -MIL-101@BM) composite sorbent by anchoring NH 2 -MIL-101 nanoparticles onto the BM matrix through hydrogen bonding interaction. The dual synergistic effect, origin from the physical sorption synergistic effect and chemisorption synergistic effect proposed between NH 2 -MIL-101 and BM, not only facilitates the mass transfer of CO 2 by reducing the diffusion resistance through hierarchical-pore structure but also offers stronger sorption sites with CO 2 by increasing the adsorption energy of metal-CO 2 or amine-CO 2 , which are confirmed by series of characterizations and theory functional calculations. Benefiting from the above merits, the NH 2 -MIL-101@20 %BM sorbent delivers a superior initial CO 2 sorption capacity of 13.4 mmol/g when the BM doping amount is 20 wt% at 25 °C, and also shows good recycle stability even after 15 runs with maintainable structure. This work displays the in-depth mechanism understanding for enhanced CO 2 capture, providing value inspiration for future MOF-based composite sorbent construction for CO 2 capture at ambient temperatures.
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
WATER AIR AND SOIL POLLUTION
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2024
·Vol. 235
·期 5
·1-17
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IF 3.8
Zhou Zhuyou,Ji Yufeng,Wang Yong,Liu Menghe,Xu Ying,Liu Ruijie,Yang Mingjie,Zou Congyang
In this study, the carbon-doped bimetallic organic framework C 60 /MIL-101(Fe,Cu) catalyst was prepared for the first time via solvothermal synthesis method. The catalysts were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), and a series of other instruments. At the same time, methylene blue (MB) was used as the target degradation material to investigate the catalytic performance of H 2 O 2 for MB degradation under visible light. The degradation experiment showed that the removal rate of C 60 /MIL-101(Fe,Cu) to MB reached 99.2% within 80 min. Furthermore, cyclic experiments demonstrated good stability and reusability of the catalyst. Finally, the degradation mechanism of the reaction was deduced by quenching experiment, UV–vis diffuse reflection and mott-Schottky plots. The results show that hydroxyl radical (·OH) and superoxide radical (·O 2 − ) play a major role in the degradation of MB during photo-Fenton process.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2020
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IF 4.65
Hongtao Zou,Shiliang Zhang,Xiaoling Hong,Qilu Yao,Yan Luo,Zhang-Hui Lu
As an ideal hydrogen supplier in liquid phase, hydrous hydrazine has gained a lot of attention for safe and efficient storage as well as transportation of hydrogen. Herein, a low Pt-containing Ni–Pt bimetallic catalyst immobilized on novel MIL-101/rGO composite has been prepared by a facile impregnation-reduction approach. Unexpectedly, the resultant Ni 0.9 Pt 0.1 /MIL-101/rGO catalyst exhibits optimal catalytic performance and 100% H 2 selectivity for hydrogen evolution from hydrous hydrazine under alkaline conditions at 323 K, giving a turnover frequency (TOF) value of 960.0 h −1 , which is a relatively higher value ever reported heterogeneous catalysts. Even at room temperature, Ni 0.9 Pt 0.1 /MIL-101/rGO catalyst shows excellent catalytic activity for dehydrogenation of hydrazine as well as hydrazine borane. In addition, the Ni 0.9 Pt 0.1 /MIL-101/rGO catalyst also exhibits excellent durability. Even after eight recycles, the catalytic activity is no significant decrease, and the H 2 selectivity still remains 100%.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF SOILS AND SEDIMENTS
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2022
·Vol. 22
·期 7
·2009-2021
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IF 3.536
Liu Quanfeng,Yu Jiang,Jiang Yinying,Zhong Chengwei,Ding Senxu,Zhou Peng,Jin Yuanxiao
Purpose Soil organic matter pollution is a serious threat to the human living environment. The purpose of this paper is to investigate the effect of MIL-101(Fe)/g-C 3 N 4 catalyzed peroxynitrite degradation of 2-chlorophenol in soil and to analyze the reaction mechanism and further to explore the optimal parameters of this reaction system with utilizing the mathematical model. Methods MIL-101(Fe)/g-C 3 N 4 was successfully obtained by hydrothermal synthesis method by growing MIL-101(Fe) on the surface of g-C 3 N 4 to catalyze the degradation of 2-CP (2-chlorophenol) in soil by sodium persulfate. The influence factors on the removal rate of 2-CP were analyzed by the response surface methodology (RSM) and combined with theoretical calculations. RSM can be used to model continuous variable surfaces with less data and determine the optimal level range. Results MIL-101(Fe)/g-C 3 N 4 had a good catalytic performance due to its good catalytic properties and the adsorption of g-C 3 N 4 on 2-CP in the system and made the best removal rate of 2-CP increase to 91.2%. The correlation of model fitting results was significant, and the verification of its optimal parameters yielded results with an error of only 4.1%. Conclusion Further studies revealed that SO 4 •− and • OH were the reactive radicals, and SO 4 •− was the dominant, which impelled Fe 2+ and Fe 3+ to interconvert in the complex system. Possible degradation pathways were derived by analyzing the intermediates. Generally, this experiment provides some ideas for future research of MOFs in soil organic pollutant removal systems. Graphical abstract
研究领域:
环境科学
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催化化学
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DOI
高影响因子
JOURNAL OF CATALYSIS
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2018
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IF 6.759
Sen Xu,Meng Wang,Bo Feng,Xinchen Han,Zijie Lan,Huajun Gu,Hexing Li,Hui Li
Dynamic kinetic resolution (DKR) of amines is an important strategy for the synthesis of chiral drugs and their building blocks; however, improving the matchability of metal-catalyzed racemization and enzymatic resolution is still a task. In this paper, Pd nanoparticles (NPs) were encapsulated inside the cages of ethylenediamine-grafted MIL-101 (ED-MIL-101), giving highly efficient catalysts (Pd/ED-MIL-101) for the racemization of primary amines. The racemization can be combined with lipase-catalyzed resolution in a one-pot DKR of rac -1-phenylethylamine leading to optically pure product (>99% ee value) with an excellent conversion and selectivity up to 99% and 93%, respectively, superior to other catalysts, such as Pd/MIL-101, Pd/MCM-41 and commercially available Pd/C. Furthermore, the heterogeneous chemoenzymatic catalyst combination can be recovered and recycled 8 times without significant loss of efficiency. The enhance catalytic performances were found to depend on the amine modification of MIL-101 that not only endows the surface of its cages with basic property, but also enables efficiently confining Pd NPs in the cages. In addition, the matchability of such chemoenzymatic catalyst combination can be further enhanced by conducting the DKR process under microwave irradiation.
研究领域:
化学
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生物催化
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材料科学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 46
·期 5
·2309-2319
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IF 3.591
Yichen Jiang,Yifei Zhao,Lin Liang,Xiao Zhang,Jianmin Sun
Imidazolium-based ionic liquid 1,n-dialkyl-3,3′-bis-1-vinyl imidazolium dibromide (n = 2, 4 and 6) monomers were synthesized and further polymerized inside a MIL-101 framework to afford poly(ionic liquid)@MIL-101 composites (PIL-n@MIL-101, n = 2, 4 and 6). Furthermore, the ratio of poly(ionic liquid) to MIL-101 affected the structures of the composites. Different molar ratios of PIL-4/MIL-101 were prepared and characterized using elemental analysis, powder X-ray diffractometry, thermogravimetric measurements, N2 adsorption/desorption and CO2 adsorption measurements. Thanks to the high Brunauer–Emmett–Teller surface area and porous structure of MIL-101 together with the incorporated poly(ionic liquid), PIL-4@MIL-101-0.5 exhibited good CO2 uptake capacity (42.7 cm3 g−1 at 100 kPa, 273 K). Additionally, due to the synergistic effects of the unsaturated coordinated Lewis acidic Cr sites and nucleophilic Br− in the PIL-4@MIL-101 composites, the developed composites exhibited efficient catalytic performance in the CO2 and epichlorohydrin cycloaddition reaction, with 99.6% conversion obtained at 90 °C and 1.0 MPa for 2.5 h without an additional cocatalyst or solvent. The composites also showed easy separation and better recycling stability. Combining the advantages of facile synthesis, excellent performance for CO2 adsorption and conversion, good thermal stability and recycling stabilities, the poly(ionic liquid)@MIL-101 composites are appealing candidates for application in CO2 capture and utilization.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2016
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IF 5.31
Ting Wang,Pan Zhao,Nan Lu,Hongche Chen,Conglu Zhang,Xiaohong Hou
Attractive magnetic metal-organic framework (MOF) material Fe 3 O 4 /MIL-101(Cr) (Matérial Institute Lavoisier, MIL) was synthesized by a simple reduction–precipitation method, and applied as an effective sorbent to the removal of two acid dyes, acid red 1 (AR1) and orange G (OG), in water. The novel synthetic method avoided the oxidation of Fe 2+ and made the Fe 3 O 4 /MIL-101(Cr) composite have the advantages of strong magnetism, large surface areas and excellent dispersion effect. Parameters that influenced the adsorption process, such as solution pH, adsorbent dosage, ionic strength, and so on, were investigated. Under the optimum conditions, adsorption kinetics and isotherms were determined from the obtained experimental data. The adsorption kinetics suggested the adsorption process of Fe 3 O 4 /MIL-101(Cr) toward AR1 and OG met the pseudo-second-order kinetic model. The adsorption isotherms were fitted by Langmuir, Freundlich and Dubinin–Radushkevich (D–R) isotherm models. Compared with the Freundlich and D–R models, the Langmuir isotherm model was found to be suitable to describe the equilibrium data, suggesting that the uptake of AR1 and OG by the Fe 3 O 4 /MIL-101(Cr) would be through monolayer adsorption. The thermodynamic results demonstrated that the adsorption was a spontaneous, exothermic and entropy decreased process. In addition, the Zeta potential data with pH value of AR1 and OG indicated that the electrostatic interactions between the dyes and the adsorbent might be critical to the adsorption mechanism. The used Fe 3 O 4 /MIL-101(Cr) could be regenerated by washing with NaOH solution and reused at least six times. The maximum adsorption capacities of the magnetic composite toward AR1 and OG were up to 142.9 mg g −1 and 200.0 mg g −1 , respectively. These results demonstrated that the novel composite would be an effective and easily re-usable adsorbent for AR1 and OG.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120944
·
IF 7.2
Yong Xiang,Li Xu,Guoji Liu
Efficient recovery of Au(III) from electronic and industrial waste streams is of both economic and environmental importance. Herein, a pore-regulation strategy was developed to construct hierarchically porous NH 2 -MIL-101(Fe 1-x Cu x ). By employing 2-aminoterephthalic acid to coordinate simultaneously with Fe 3 + and Cu 2+ , the unstable Cu–O bonds were selectively removed through a mild acid-soaking treatment, thereby generating enlarged channels and hierarchical micro–mesoporous structures. The optimized framework achieved an Au(III) adsorption capacity of 944 mg g −1 , which was ∼30.7 % higher than that of unmodified NH 2 -MIL-101. Mechanistic studies demonstrated that the hierarchical pore architecture not only facilitated mass transfer but also enhanced accessibility of active sites, synergistically contributing to the superior adsorption performance. This work highlights that rational pore-channel engineering around adsorption sites can substantially boost the recovery efficiency of reducible precious metals, offering a novel design paradigm for advanced MOF-based adsorbents.
研究领域:
环境科学
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材料化学
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吸附分离
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资源回收
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配位化学
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Applied Ceramic Technology
·
2022
·Vol. 20
·期 1
·24-38
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IF 2.328
Cong Zhou,HaiPeng Feng,GuangAo Liu,Feng Tao,Qi Liu
SiFeCO ceramic nanocomposites with porous structure have been successfully prepared via pyrolysis of novel iron-containing precursors, which were synthesized by modification of polycarbosilane with different contents of MIL-101(Fe), a kind of metal-organic framework made by our laboratory. Iron-containing precursors were pyrolyzed at relatively low temperatures ranging from 500 to 900°C under nitrogen atmosphere, the polymer-to-ceramic conversion process were investigated by Fourier transform infrared spectroscopy, X-ray diffraction (XRD), and thermo gravimetric analysis (TGA) measurements. SiFeCO ceramics with different iron contents were intensively studied with respect to their crystallization behavior, microstructure evolution, and porous morphology influenced by additive amount of MIL-101(Fe). The results of XRD and Transmission electron microscopy revealed that MIL-101(Fe)-modified precursors converted into amorphous SiFeCO ceramics when pyrolyzed below 700°C under nitrogen, extremely small Fe 3 O 4 and α-Fe crystallites with grain size of only 2–5 nm were in situ generated and dispersed uniformly in the SiCO ceramic matrix. Simultaneously, interconnected porous structure was created in the matrix by the decomposition of MIL-101(Fe). The as-obtained SiFeCO ceramics could serve as heterogeneous Fenton-like catalysts for the degradation of xylene orange and exhibit outstanding catalytic properties.
研究领域:
材料科学
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催化化学
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）