CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yue Xiao,Haodong Huang,Shangpu Zhuang,Dong Yang
Metal oxide cluster MOF nodes are a good platform to understand the reactivities and catalysis. MIL-96, MIL-100 and MIL-110 are drastically different in their node structures. Following our previous reported results for MIL-100, we report the modified synthesis and characterization of the node sites of MIL-110 and MIL-96 and their catalytic sites by using methanol dehydration as probe reaction. We show that these MOFs can be synthesized from the same solution by adding various amounts of formic acid as modulator. Herein, the chemistry of hydroxyl, formate and methoxy groups were used to probe the three MOFs’ node sites. IR data show the bonding structures of these ligands are highly diverse, with reactivities and flexibilities depending on node sites. We identified terminal OH group and various µ 2 -OH groups in single, paired or hydrogen bonded modes on the MOF nodes. Formate ligands were introduced to the node sites during the synthesis or by a post treatment in formic acid/DMF solution. Surprisingly, the bonding modes of formate ligands on Al 3 (OH) 3 node structure of MIL-96 can be reversibly switched between monodentate and bidentate through a process induced by water molecules. Further, methoxy ligands—likely to be the intermediate for catalytic reaction—were also observed on the node sites under methanol dehydration conditions at 250 ℃. The activities of MIL-100 and MIL-96 for methanol dehydration determined by TOF per node were similar, both approximately 3-fold higher than that of MIL-110. The data suggests that catalytic sites incorporate adjacent vacancy and defect node sites, which constitute a minority among all observed MOF node sites. We foresee the opportunities in expanding the chemistry and understanding into other MOFs with metal oxide cluster nodes.
研究领域:
材料科学
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催化
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化学工程
·
无机化学
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2018
·Vol. 48
·期 3
·989-996
·
IF 4.099
Ling Yang,Tian Zhao,Ishtvan Boldog,Christoph Janiak,Xiao-Yu Yang,Qiang Li,Yan-Jia Zhou,Yong Xia,Deng-Wang Lai,Yue-Jun Liu
The concentration of benzoic acid was found to exercise efficient control over the formation of either MIL-101(Cr) or MIL-88B(Cr) under otherwise similar hydrothermal synthetic conditions. Nanocrystals of MIL-101(Cr) with ∼100 nm average size and excellent SBET = 3467 m2 g−1 are obtained at lower concentrations of benzoic acid, while at higher concentrations the microparticulated MIL-88B(Cr) product is formed. Hereby a new efficient synthetic method towards the elusive MIL-88B(Cr), yet reported only once without synthetic details, is proposed. The obtained MIL-88B(Cr) has an interesting and potentially valuable property of retaining its high-volume form (Vcell ∼ 2000 Å3) after thermal activation. The degassing of MIL-88B(Cr) in a vacuum at 250 °C yields a porous material with a SBET area of 1136 m2 g−1, which is around the theoretical maximum. The transition to the denser ‘closed’ form (Vcell ∼ 1500 Å3) occurs only at 350 °C, when all of the benzoate/benzoic acid, hindering the process, is removed.
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
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Hailin Tian,Tirusew Araya,Ruiping Li,Yanfen Fang,Yingping Huang
Microcystin-LR (MC-LR), which is produced from cyanobacteria, is the common microcystin with a serious threat to aquatic life and human beings. And the efficient removal method of MC-LR is urgent needed. In this work, the MIL-100/MIL-53 (Fe) photocatalysts, which were successfully prepared by the electrostatic interaction with each other, were applied for the photocatalytic degradation of MC-LR. The structure and optical properties of the MIL-100/MIL-53 (Fe) photocatalysts were characterized by using SEM, XRD, XPS, FT-IR and UV–vis DRS. The very low dosage of the MIL-100/MIL-53 (Fe) photocatalysts achieved the degradation of MC-LR, and the optimized loading was the 50% MIL-100/MIL-53 (Fe) photocatalyst. Compared to MIL-100 (Fe) and MIL-53 (Fe), the MC-LR degradation was up to 96.5% after 3 h under visible light illumination with the 50% MIL-100/MIL-53 (Fe) photocatalyst due to the pore-effect adsorption and the effective separation of photogenerated carriers. The effect of coordinate immobilized layers between MIL-100 (Fe) and MIL-53 (Fe) contributed to the stable and efficient removal of MC-LR for the 50% MIL-100/MIL-53 (Fe) photocatalyst. The MC-LR photocatalytic mechanism and degradation pathway, which the photogenerated holes (h + ) were the main active species, were proposed by radical capture experiments and LC-MS analysis.
研究领域:
环境科学
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生物学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
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IF 2.7
Xia Zhang,Jialong Chu,Yifang Zhang,Fei Li,Chen Wang,Tiemei Li,Jing Fan
A novel microporous iron-based MIL-101@MIL-53 Z-scheme heterojunction photocatalyst was synthesized via a one-pot solvothermal strategy. Composition, structure, morphology and optical properties of the prepared photocatalyst were characterized using XRD, SEM, FT-IR, XPS and UV-vis DRS. The formation mechanism of the iron-based MIL-101@MIL-53 Z-scheme heterojunction was proposed to be attributed to the gradual transformation from MIL-101 to MIL-53. The in situ formation of an iron-based MIL-101@MIL-53 Z-scheme heterojunction facilitated the electron transfer from MIL-53 to MIL-101. Therefore, the separation of photogenerated charge carriers was enhanced. The removal efficiency of 300 mg L−1 tetracycline hydrochloride reached 99.6% in 90 min under simulated solar light irradiation. Radical capturing experiments showed that ˙O2− was the main active substance for the degradation of tetracycline hydrochloride. This work provided strategies for development and application of iron-based MIL-101@MIL-53 Z-scheme heterojunction and efficient treatment of wastewater with a high tetracycline hydrochloride concentration.
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
MATERIALS CHEMISTRY AND PHYSICS
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2020
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IF 3.408
Yanan Dong,Tianding Hu,Manoj Pudukudy,Hongying Su,Lihong Jiang,Shaoyun Shan,Qingming Jia
In this paper, the effect of conventional solvothermal and a microwave-assisted method for the synthesis of MIL-101(Fe) and NH 2 -MIL-101(Fe) as adsorbents for the removal of tetracycline in wastewater is reported for the first time. The results had shown that the microwave treatment led to a significant reduction in the material synthesis time, which greatly saved the energy. It was also found that the microwave-assisted synthesized material exhibited small particle size, high specific surface area and better adsorption capacity. The introduction of amino group further enhanced the adsorption capacity of MIL-101(Fe). The adsorption capacity of MIL-101(Fe) and NH 2 -MIL-101(Fe) samples for tetracycline adsorption by microwave assisted synthesis method reached up to 332 mg/g and 378 mg/g, respectively. Moreover, the adsorption isotherm was well-fit with Freundlich model, indicating a multilayer adsorption . The kinetic studies indicated that the reaction followed pseudo second-order reaction kinetics with a best fit to the theoretical value. Due to the higher adsorption efficiency and lower energy consumption of the synthesis, the as-prepared microwave assisted materials could be used as potential adsorbents for different pollutants in wastewater.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
MATERIALS LETTERS
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2017
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IF 2.572
Yana Liu,Lu Fan,Chen Xu,Keke Sun,Zhennan Shi,Ling Li
A composite MIL-101/CDs/MIL-101 comprising MIL-101 and carbon quantum dots (CDs) was prepared and characterized. The particles were uniform in size and found to be potentially used for fluorescence imaging. Cytotoxicity assays indicated the particles were biocompatible and suitable for carrying drugs. In the drug release experiments, the MIL-101/CDs/MIL-101 demonstrated an excellent pH-triggered drug release.
研究领域:
材料科学
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生物医学工程
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药学
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产品关联
DOI
高影响因子
Catalysis Science & Technology
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2023
·Vol. 13
·期 15
·4525-4533
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IF 5
Qiuyu Zhang,Yajie Chen,Xinyan Yu,Yuejia Yin,Yaxin Ru,Guohui Tian
Fabricating photocatalysts with customizable structure and composition using different metal–organic framework (MOF) building blocks has intriguing implications in chemistry and material science, but it is challenging to do so. Here, a two-step synthetic strategy was designed to prepare MIL-125(Ti)@TiO2 hollow nanodiscs decorated with Co3S4 nanoparticles for CO2 photoreduction. The Co-based zeolite imidazolium ester backbone (ZIF-67) nanolayer was first loaded on the prepared MIL-125(Ti) nanodiscs to form core@shell MIL-125(Ti)@ZIF-67 nanodiscs. The following sulfidation process under solvothermal condition led to the production of MIL-125(Ti)@TiO2 hollow nanodiscs decorated with Co3S4 nanoparticles (MIL-125(Ti)@TiO2\Co3S4). This ternary hybrid catalyst with hollow nanodisc structure possessed a significantly enhanced charge separation efficiency and visible light absorption, along with offering a huge number of active sites. Considering the above advantages, the CO2 photoreduction activity of the optimized MIL-125(Ti)@TiO2\Co3S4 catalyst was significantly increased when compared to single-component catalysts (MIL-125(Ti), TiO2, and Co3S4) and binary hybrid catalysts (MIL-125(Ti)@TiO2 and TiO2\Co3S4) under simulated sunlight irradiation. CO is the main product with a productivity of 587.50 μmol g−1 h−1, which is almost seven times higher than that of pure MIL-125(Ti). The potential photocatalytic mechanism of the hybrid photocatalyst has also been demonstrated. This study presents a simple and effective technique for fabricating MOF-based hybrid catalysts for photocatalytic applications.
研究领域:
材料科学
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化学
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产品关联
DOI
高影响因子
CATALYSIS COMMUNICATIONS
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2017
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IF 3.33
Zhiming Chen,Bo Xu,Xiaomei Wang,Li Zhang,Xiaoqing Yang,Cuncheng Li
Separation and recycling of noble metal nanoparticles after catalytic reaction is critical to promote its application efficiency and cut down the cost. This work presents a facile synthesis strategy for the fabrication of sandwich-like MIL-100(Fe)@Pt@MIL-100(Fe) (denoted as S-Pt) nanoparticles with high stability and improved catalytic activity for hydrogenation of nitrophenol. MIL-100(Fe) acts as both carrier to make the catalyst easily separated and shield to protect the tiny Pt nanoparticles from leaching or aggregation during reaction. Moreover, mass transfer effect of the porous MIL-100(Fe) with its pore structure serving as nano-reactor is also benefit for promoting the catalytic efficiency.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
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2021
·Vol. 11
·期 8
·2864-2872
·
IF 6.119
Xiaoli Li,Yuan Tang,Yue Jiang,Manman Mu,Xiaohong Yin
A series of composites composed of Bi4O5Br2 and Fe-MIL were successfully fabricated for mimicking sunlight-driven photocatalytic reduction of CO2. Herein, Bi4O5Br2, as a modulator of solid acids, could turn NH2-MIL-101(Fe) into NH2-MIL-88B(Fe) completely at 0.07 wt% catalytic loading, where further addition could construct the corresponding composites of Bi4O5Br2 and NH2-MIL-88B(Fe). The highest activity in the photocatalytic reduction of CO2 was achieved at 7.96 μmol g−1 h−1 of CH4 at 3.28 wt% of Bi4O5Br2. Besides, this catalyst possessed high photostability during the recycling experiments and the mechanism of this process was thoroughly explored. This study provides a novel strategy employing solid acid modulators for regulating the structure and morphology of MOFs showing high activity and stability in the photocatalytic reduction of CO2 to CH4.
研究领域:
材料科学
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环境科学
·
化学
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2015
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IF 2.037
Yu Zhang,Wei Su,Yan Sun,Jia Liu,Xiuwu Liu,Xiaojing Wang
MIL-101 is a promising adsorbent because of its large pore volume, high separation selectivity, easy regeneration, and good stability. MIL-101 was synthesized and characterized by X-ray diffraction, scanning electron microscopy, and nitrogen adsorption at 77 K. Adsorption isotherms of pure N2, CH4, and CO2 were measured on MIL-101 from 263 K to 313 K and at pressures up to 0.8 MPa. The Langmuir model was a good fit for the experimental isotherms and the isosteric heats of adsorption decreased in the order: CO2 > CH4 > N2. The CO2/CH4 separation selectivity was sensitive to the adsorption pressure and temperature and it varied from 3.2 to 6.3. In contrast, the CH4/N2 separation selectivity changed from 2.6 to 3.3 with temperature and pressure.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2025
·
IF 3.3
Yanjia Zhou,Xiao-Dong Tang,Jingjing Li,Da-Yong Qing,Hong Wang
MIL-101(Cr) and MIL-100(Fe) are both representative MIL-type Metal-Organic-Frameworks (MOFs) materials, renowned for their large specific surface areas and size-tunable characteristics, making them suitable candidates for Li+ extraction from lithium-containing solvent. By introducing -NH2 functional groups and using LiNO3 as both a template and mineralizer, the functionalized MOF materials Li/NH2/MIL-101(Cr) and Li/NH2/MIL-100(Fe) were synthesized. Following modification, their Li+ adsorption capacities were increased, reaching 43.58 and 38.22 mg/g, respectively. The dosage of mineralizer, initial Li+ concentration, adsorbent dosage, solution pH value, and temperature all have an impact on the adsorption capacity of adsorbents. In addition, through the establishment of the pseudo-first-order kinetic model, pseudo-second-order kinetic model, as well as Langmuir and Freundlich thermodynamic models, it can be known that the adsorption of the materials belonged to monolayer chemisorption, and the adsorption process was exothermic. Furthermore, both adsorbents showed good reusability, retaining over 85% of their initial adsorption capacity after four adsorption-desorption cycles, highlighting their practical applicability in lithium recovery processes. In Mg-Li mixed solution systems, both materials exhibited exceptional Li+ selectivity. At a low Mg2+/Li+ ratio of 3, the separation factor (α) exceeded 80; even at a high Mg2+/Li+ ratio of 10, α remained near 50. Additionally, in systems with coexistence of multiple interfering ions, the distribution coefficient (Kd) followed the order: Li+ ≫ Mg2+ > Ca2+ > Na+ > K+. In the mixed systems, Li/NH2/MIL-101(Cr) and Li/NH2/MIL-100(Fe) exhibited certain separation effect for Li+ against competing cations.
研究领域:
材料科学
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环境科学
·
化学工程
·
无机化学
·
分离技术
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Meng Zhang,Yu Zhang,Yucong Chen,Xiaoru Tian,Lingzhi Liu,Yizhong Wang,Ruijie Guo,Hong Yan
MIL-88(Fe) was used as an oxidant and a hard template for the synthesis of polypyrrole (PPy) on its surface, and the formation of PPy made the surface of MIL-88(Fe) rougher as well as more voids formed in the interior. The increased specific surface area allowed more benzotriazole (BTA) (17.8 wt%) loaded on PPy/MIL-88 particles. BTA/PPy/MIL-88(Fe) was employed as a novel corrosion inhibitor to enhance the corrosion resistance of epoxy coating for carbon steel. BTA/PPy/MIL-88(Fe) filler improved the corrosion resistance of EP coating without/with artificial scratch by delaying the cathodic and anodic reactions in corrosive media. Both BTA and MIL-88(Fe) played the role of corrosion inhibitors, making EP coating possess active corrosion protection and pH-sensitive performance. Besides, BTA/PPy/MIL-88(Fe) enhanced the adhesion of EP coating by filling the pores inside.
研究领域:
材料科学
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防腐蚀工程
·
化学工程
✓ 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）