Polymers
·
2021
·Vol. 13
·期 20
·3498
·
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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ChemElectroChem
·
2018
·Vol. 5
·期 19
·2893-2901
·
IF 4.446
Jianxia Gu,Xiangdang Yin,Xiangjie Bo,Liping Guo
Graphical With a sense of selectivity : the metal-organic framework/reduced graphene oxide composite MIL-101(Cr)/rGO is prepared via a simple hydrothermal method. The electrochemical sensor based on the composite shows low detection limits and wide linearity ranges for the determination of metronidazole, Cd 2+ and Pb 2+ , and shows excellent selectivity, reproducibility and stability. In this work, a Cr-based MOF (MIL-101(Cr))/reduced grapheme oxide(rGO) electrocatalyst was prepared through a one-pot hydrothermal method. The obtained composite was characterized via scanning electron microscopy, transmission electron microscopy, X-ray diffraction and other standard techniques. Electrochemical methods were adopted to study the electrocatalytic ability of the composite. The results imply that, compared to the single components, it exhibits higher electrocatalytic activity for the reduction of metronidazole and stripping of Cd 2+ and Pb 2+ . Optimizing the ratio of MIL-101(Cr) and rGO, an electrochemical sensor was prepared using MIL-101(Cr)/rGO-20 and used for detection of metronidazole, Cd 2+ and Pb 2+ , respectively. The linear range for metronidazole can be divided in two parts, i. e. from 0.5 to 200 μM and from 200 to 900 μM. The limit of detection is 0.24 μM (S/N=3, n=10). Likewise, it also exhibits a wide linear range from 0.05 to 6.0 μM for the detection of Cd 2+ and Pb 2+ . The corresponding detection limits are found to be 5.2 nM and 3.0 nM (S/N=3, n=10), respectively. The proposed sensor also possesses superb selectivity, reproducibility, stability and can be applied to detect real samples with desired recovery rates. In addition, the possible reduction mechanism of metronidazole and adsorption mechanism of Cd 2+ and Pb 2+ were further discussed simply in this work.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Tien Tran Nguyen,Minh Kim Nguyen,Vipin Kumar,Ha Huu Do,Anh Thi Kim Le,Anh Van Nguyen,Jin Seog Gwag,Pham Cam Nam,Le Gia Trung
The widespread use and subsequent release of antibiotics by humans and animals pose health and environmental risks, compelling their removal from aquatic ecosystems. MIL-101(Cr), a metal-organic framework (MOF), exhibits versatile applications in antibiotic adsorption owing to its exceptional structural characteristics. In this context, MIL-101(Cr) nanoparticles are successfully prepared via the hydrothermal method to remove pefloxacin (PEF) from aqueous solutions. The resulting MIL-101(Cr) adsorbents showcase high crystallinity (97.6%), a large surface area (3166 m 2 /g), broad nanopore sizes, good thermal stability, and efficient reusability. Factors including initial PEF concentration, pH, dosage of adsorbent, and temperature are thoroughly investigated. The findings reveal a good adsorption capacity (254.3 mg/g) with an optimal removal efficiency (99.7%) at 308 K in a neutral pH of 7.0 when the adsorbent dosage is 250 mg/L and the initial PEF concentration is 200 mg/L within 80 min of contact. Among the three adsorption isotherms (Langmuir, Freundlich, Temkin models), the Langmuir equation best fits the studies, indicating a maximum adsorption capacity of 253.8 mg/g at 25°C, while the experimental equilibrium adsorption capacity is 229.2 mg/g at the same temperature. Adsorption kinetics aligns with the pseudo-second-order model. Thermodynamic parameters and activation energy affirm the endothermic and spontaneous behavior of the adsorption process, attributed to both physisorption and chemisorption. This study highlights the promising potential of synthesized MOF nanocrystals as an effective adsorbent for antibiotics in wastewater treatment and environmental remediation.
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TALANTA
·
2015
·
IF 3.545
Fang Yang,Cheng-Xiong Yang,Xiu-Ping Yan
Effective separation of tocopherols is challenging and significant due to their structural similarity and important biological role. Here we report the post-synthetic modification of metal–organic framework (MOF) MIL-101(Cr) with pyridine for high-performance liquid chromatographic (HPLC) separation of tocopherols. Baseline separation of four tocopherols was achieved on a pyridine-grafted MIL-101(Cr) packed column within 10 min using hexane/isopropanol (96:4, v/v) as the mobile phase at a flow rate of 0.5 mL min −1 . The pyridine-grafted MIL-101(Cr) packed column gave high column efficiency (85,000 plates m −1 for δ-tocopherol) and good precision (0.2–0.3% for retention time, 1.8–3.4% for peak area, 2.6–2.7% for peak height), and also offered much better performance than unmodified MIL-101(Cr) and commercial amino-bonded silica packed column for HPLC separation of tocopherols. The results not only show the promising application of pyridine-grafted MIL-101(Cr) as a novel stationary phase for HPLC separation of tocopherols, but also reveal a facile post-modification of MOFs to expand the application of MOFs in separation sciences.
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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2020
·Vol. 20
·期 3
·1807-1813
·
IF 1.134
Wang Yulin,Qiu Xiuzhen,Li Yangyang,Guo Huishi,Lu Wenguan,Nie Libo
A novel molecularly imprinted polymer material based on the metal-organic framework NH2-MIL-101(Cr) (MOF-MIP) was prepared. The synthesized MOF-MIP was characterized by IR, XRD, SEM and N2 absorption. The characterization results displayed that the MOF-MIP which exhibited
an octahedral shape had good dispersibility, good thermal stability and a high surface area. Subsequently, the adsorption behavior of MOF-MIP to diclofenac sodium (DS) in aqueous solution was examined. A series of adsorption experiments demonstrated that the MOF-MIP had high transfer mass
rates and high sensitivity and selectivity for DS. Then the MOF-MIP was used as the adsorbent of dispersive micro-solid phase extraction (DMSPE) for the detection of DS in urine. Under optimum conditions, the average recovery of DS ranged from 88.3 to 101.6% with RSD of 5.6%. The described
method provides a rapid route for determination of DS in human urine.
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高影响因子
ACS Omega
·
2019
·
IF 2.584
Xiaofang Liu,Hu Pan,Heng Zhang,Hu Li,Song Yang
Enlarging the dispersed micropores of metal-organic frameworks to the well-ordered mesostructure can enhance the accessibility of acidic sites for reactants resulting in the improvement of selectivity. With the regulation of cetyltrimethylammonium bromide/Cr3+ and ClSO3H sulfonation, a series of mesoporous MIL-101(Cr)-SO3H (MMSs) with multiple pore sizes and acidic properties were synthesized and explored to further facilitate the furfuryl alcohol (FA) ethanolization to ethyl levulinate (EL) for the first time. The optimal catalytic activity of 83.8% EL yield at full FA conversion demonstrated that the appropriate mesopore size, acidic density, and accessible −SO3H sites contributed to the superior performance of the MMS(0.3)-0.15. The turnover frequency value (14.8 h–1) obtained with MMS(0.3)-0.15 was comparable to the commercial Nafion NR50 (18.3 h–1) and much higher than the classical Amberlyst-15 (1.9 h–1), confirming the predominant catalytic performance. Furthermore, two coexistent reaction paths with 2-ethoxymethylfuran and 4,5,5-triethoxy-pentan-2-one as intermediates indicated the possibility of producing EL from FA.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Ziyang Xu,Zicheng Yang,Jiale Ni,Yi Feng,Jianfeng Yao
Defective metal organic frameworks have emerged as promising catalysts for CO2 conversion owing to their tunable active sites and exceptional catalytic activities. Despite their potential, achieving high defect densities through simple and scalable methods remains a major challenge. To address this, we developed an innovative low-temperature calcination strategy (300 °C, 10 min) to introduce abundant ligand defects into MIL-101(Cr) while maintaining crystallinity, thereby exposing additional Cr3+ Lewis acid sites to participate in epoxide activation. The resulting defective MIL-101 demonstrates remarkable catalytic efficiency in CO2 cycloaddition, achieving a >99% yield under mild conditions (80 °C, 0.1 MPa) within 6 h, significantly surpassing that of pristine MIL-101 (52%). Furthermore, the catalyst exhibited outstanding recyclability, retaining full activity over multiple reaction cycles. In addition to synthetic simplicity, this work provides fundamental insights into the critical role of defects in promoting epoxide activation and ring opening, establishing a sustainable pathway for CO2 utilization under mild conditions and the energy-efficient production of cyclic carbonates.
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npj Clean Water
·
2025
·Vol. 8
·期 1
·1-16
·
IF 11.4
Keshta Basem E.,Yu Haojie,Wang Li,Yi Hong,Jian Shan,Uddin MD Alim,Ouyang Chenguang,Wang Yu,Yuan Xunchun,Zhang Yanhui,Jin Yang,Basit Abdul,Owais Malik Muhammad,Awan Khan Manqoosh
Anionic dyes contaminate water and severely disrupt aquatic ecosystems, urgently demanding effective treatment solutions for safety. This study explores the synthesis of unsaturated MIL-101(Cr) and its exceptional performance in removing anionic dyes from polluted water systems. The synthesized MIL-101(Cr) exhibits medium Lewis’s acid and strong Brønsted acid sites, a high specific surface area (>3000 m 2 /g), and a Zeta potential of 30 mV, contributing to its strong adsorption capability. Adsorption studies reveal Langmuir isotherm model fitting, with maximum adsorption capacities of 4231, 1266, and 568 mg/g for Acid Blue 92, Congo Red, and Acid Blue 90, respectively. The chemisorption process follows pseudo-second-order kinetics and is spontaneous and exothermic. MIL-101(Cr) demonstrates chemical and water stability, maintaining over 80% removal efficiency after five recycling cycles. This research provides valuable insights into treating anionic dye-contaminated wastewater using MIL-101(Cr) as an efficient adsorbent.
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KEY ENGINEERING MATERIALS
·
2015
·
IF 0
Xin Liu,Yan Ying Zhao
An N, N-dimethylformamide (DMF)-functionalized metal–organic framework, namely, DMF-MIL-101(Cr), was prepared and then used for the adsorptive removal of methylene blue (MB), a cationic dye, from aqueous solutions. MIL-101(Cr) was synthesized by the hydrothermal method. Next, by dipping the MIL-101(Cr) sample in DMF, DMF-MIL-101(Cr) was synthesized. The results of X-ray diffraction analysis, Fourier transform infrared spectroscopy, and thermogravimetric analysis confirmed that DMF and MIL-101 could be combined successfully. More importantly, the MB uptake capacity of DMF-MIL-101(Cr) was significantly higher than that of MIL-101(Cr). Unlike MIL-101(Cr), DMF-MIL-101(Cr) could adsorb the entire MB in a solution with a concentration of 10.92 mg/L, owing to the electrostatic interactions between DMF and the MB molecules. In 100 mL of a 10.92-mg/L MB solution, DMF-MIL-101(Cr) can reach a state of absorbance equilibrium within10 min. After that, the adsorption process exhibited the characteristics of a zero-order reaction. This result indicates that it may be possible to exploit different functionalization methods and improve the rate of adsorption of dyes onto metal–organic frameworks.
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CATALYSIS LETTERS
·
2026
·Vol. 156
·期 9
·245
·
IF 2.5
Xia Ruixin,Song Jiahe,Guo Bao,Sun Daolai,Lv Jianhua
An ionic liquid-grafted catalyst, denoted as IL@MIL-101-NH 2 , was synthesized by introducing a novel functionalized bis-imidazolium ionic liquid containing carboxyl groups into the MIL-101-NH 2 (Cr) using a simple one-step method. The structural features of the catalyst were characterized by FT-IR, XRD, XPS, BET, SEM and so on, and its catalytic performance in the cycloaddition reaction of carbon dioxide (CO 2 ) with propylene oxide (PO) to propylene carbonate (PC) was investigated. The results demonstrated that IL@MIL-101-NH 2 exhibited excellent catalytic activity. Under the conditions of 110 °C, 2 MPa, 3 h, and a catalyst loading of 3.0 wt%, a PO conversion of 95.1% and a PC selectivity of 98.7% were achieved. The superior catalytic performance of IL@MIL-101-NH 2 was attributed to the synergistic effect among the Cr 3+ metal active centers, nucleophilic Br − species and hydrogen-bond-donating –COOH groups. In addition, the catalyst maintains good catalytic performance after four consecutive cycles, indicating its favorable stability and promising application potential. Graphical
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122400
·
IF 7.5
Longjie Lai,Jie Tao,Yutao Xue,Xusheng Suo,Juan Liu,Qi Liu,Aihua Yuan
Interfacial engineering in heterostructure photocatalysts is crucial for efficient charge migration, yet achieving rational and controllable interface design remains a major challenge. In this work, SnIn 4 S 8 nanosheets were in situ grown on the octahedral surface of MIL-101(Cr) to leverage the Lewis acid-base properties of Cr and S, thereby enabling the controlled construction of an ion-coordinated interface. The resulting MIL-101(Cr)@SnIn 4 S 8 heterojunction enabled efficient capture and conversion of CO 2 and H 2 O. Furthermore, the Lewis acid-base coordination induces interfacial electron density redistribution, generating a built-in electric field that drives the formation of an S-scheme heterojunction between MIL-101(Cr) and SnIn 4 S 8 , while simultaneously preserving high‑energy photogenerated electron-hole pairs. Consequently, MIL-101(Cr)@SnIn 4 S 8 exhibited superior CO 2 photoreduction performance with H 2 O in the gas-solid phase, delivering a CO evolution rate of 26.9 μmol·g −1 ·h −1 . This work provides a viable strategy for interfacial engineering and demonstrates the application potential of S-scheme heterojunctions in photocatalytic reactions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Yi Hao,Kaili Wang,Cheng Chen,Xingyu Chen,Rongrong Jia,Ping Cheng,Liyi Shi,Lei Huang
Waste PET-derived MIL-101(Cr) enables polyethylene oxidation. • Photogenerated holes directly participate in PE C–H activation. • A thermally assisted photoinduced oxidation pathway is established. • Polyethylene is converted into recoverable dicarboxylic acids. • Cross-polymer valorization integrates PET and PE waste streams. Heterogeneous catalytic oxidation of polyethylene (PE) into dicarboxylic acids remains challenging because of the difficulty in activating chemically inert C–H bonds. Here, we report a waste polyethylene terephthalate (PET)-derived MIL-101(Cr) photothermal catalyst that enables photogenerated hole ( h + )-driven activation of PE during oxidation. Under 130 °C, 1.0 MPa O 2 , and 370 mW cm −2 light irradiation, complete conversion of PE is achieved, affording aliphatic dicarboxylic acids (C4-C22) with a carbon yield of up to 63.7 wt%. Experimental and theoretical investigations reveal that photogenerated h + directly activate C–H bonds of surface-adsorbed PE through hydrogen abstraction, thereby initiating the oxidation process. The carboxylate ligands on the MIL-101(Cr) surface promote favorable interfacial interactions with PE chains, facilitating effective catalyst-polymer contact for interfacial C–H bond activation. This work provides new mechanistic insights into heterogeneous photothermal PE oxidation and offers new guidance for catalyst design based on photogenerated h + oxidation. Download: Download high-res image (246KB) Download: Download full-size image
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