CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Min Zhang,Jieshu Zhou,Xiulan Guo,Xiangke Zeng,Lan Shi,Tingting Zhang,Yunfei He,Xintao Zhou,Shaoyun Shan,Kaili Yao
Mitigating the rise of atmospheric carbon dioxide (CO 2 ) levels presents one of humanity’s significant challenges. Metal-organic frameworks (MOFs) have emerged as promising materials for CO 2 capture, owing to their unique chemical structure and operability. Many researchers have demonstrated that amination treatment can further enhance CO 2 adsorption performance. However, the relatively low capture efficiency and limited cycling stability of these materials continue to impede their development. Alkali metal cations exhibit high CO 2 adsorption capacities and can be incorporated into the MOF structure to significantly enhance CO 2 capture capacity and cycling stability. Therefore, we synthesized novel alkali metal ion-doped M−NH 2 −MIL−101 (M = Li, Na, K) adsorbents using a post-modification method, successfully anchoring alkali metal cations to carboxylate group sites within the MOFs framework. The integration of microscopy, spectroscopy, and density functional theory (DFT) calculations has confirmed that the introduction of alkali-metal cations enhances the adsorption between MOFs and CO 2 , thereby providing stronger adsorption sites. Experimental studies have demonstrated that doping with 0.1 M K + (denoted as 0.1 K-NH 2 -MIL-101) exhibits a higher CO 2 adsorption capacity (8.2mmol g −1 ) at 298 K, approximately 3.2 times greater than that of NH 2 -MIL-101. Furthermore, it maintains an adsorption capacity of 7.4mmol g −1 after the sixth adsorption–desorption test, indicating excellent cyclic stability. Additionally, 0.1 K-NH 2 -MIL-101 was employed for in situ capture and electrocatalytic CO 2 reduction. By integrating 0.1 K-NH 2 -MIL-101 with a Bi-based catalyst to enhance the local CO 2 concentration, the Faraday efficiency for the formic acid product was effectively increased from 67 % to 85 %.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Chiyu Wen,Chao Wang,Defang Liu,Zhuo Cheng,Jing Zhao,Hongli Zhang,Jun Wang,Guoxiang Zhu,Yongfa Zhu
Nitro-aromatic compounds constitute predominant explosive materials extensively utilized in military applications and industrial blasting operations. However, the manufacturing, consumption, and decommissioning of these explosives generate significant quantities of wastewater exhibiting both ecotoxicological hazards and explosive potential. Herein, an amino-functionalized MIL-100(Fe) (AFM) catalyst demonstrating simultaneously enhanced explosive capture and degradation is developed. The synergistic interplay of electrostatic attraction and hydrogen bonding between the amino groups of AFM and nitro groups of nitro-aromatic explosive confer exceptional binding affinity. The optimized AFM exhibits a remarkable 2,4,6-trinitrotoluene (TNT) adsorption of 14.93 mg/g, which is 3.6 times of unmodified MIL-100(Fe). In photo-Fenton reactions, the optimized AFM completely degrades TNT within 30 min, and achieves a mineralization efficiency as high as 96.7 %. Moreover, the AFM exhibits excellent stability, retaining a high TNT degradation efficiency of 97.7 % after five consecutive cycles. The currently designed AFM catalyst possessing fascinating explosive affinity and high explosive mineralization efficiency is expected to advance sustainable remediation of high-risk explosive wastewater.
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Bioresources and Bioprocessing
·
2025
·Vol. 12
·期 1
·1-16
·
IF 5.1
Li Yuhan,Wu Guowei,Liu Zeqing,Dai Lingmei,Liu Dehua,Du Wei
Mesoporous MIL-88A (Meso-MIL-88A) shows significant potential as an effective carrier for immobilizing large molecules such as lipases. This study investigates Meso-MIL-88A immobilized lipase for the catalysis of eicosapentaenoic acid (EPA) and docosahexaenoic acid (DHA) incorporation into soybean phosphatidylcholine. Phosphatidyl-EPA and phosphatidyl-DHA are known for their superior health benefits and have garnered significant global attention. Firstly, we developed a novel and green water-washing strategy to synthesize Meso-MIL-88A, demonstrating its significant potential as an effective carrier for immobilizing large molecules such as lipases. Nitrogen adsorption/desorption and XPS analyses revealed that water as the eluent yielded larger average pore diameters and lower sulfur residue content compared to ethanol. This optimized Meso-MIL-88A carrier was used to immobilize Candida antarctica lipase B (CalB@Meso-MIL-88A), which was applied to the production of phosphatidyl-EPA and phosphatidyl-DHA. The immobilized CalB@Meso-MIL-88A exhibited exceptional catalytic efficiency, achieving an unprecedented sn -1 positional incorporation rate of 86.8% (44.2% EPA, 42.7% DHA) with 90% EPA/DHA-ethyl ester (EE) donors, while 97% DHA-EE resulted in a record-high 90.1% DHA incorporation at the sn -1 position. Kinetic studies and molecular docking simulations indicated a higher substrate affinity for DHA-EE, attributed to enhanced transfer efficiency of EPA/DHA-EE in organic solvent system. This study presents the first demonstration of the potential of Meso-MIL-88A for industrial lipase immobilization via this optimized route, offering an eco-friendly and highly efficient catalytic application for nutraceutical synthesis. Graphical abstract
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TALANTA
·
2015
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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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TALANTA
·
2025
·
IF 6.1
Qiaoli Yang,Xiao Yang,Ke Guo,Guangrui Pan,Qiuzheng Du,Liang Ming,Wanhai Wang
Pseudomonas aeruginosa (PA) infection poses a significant threat to human health and the economy, with the issue of drug resistance becoming increasingly severe. How to quickly, accurately, and inexpensively detect PA and differentiate live bacteria from dead ones is crucial for clinical follow-up treatment. To this end, we have developed a biosensor based on fluorescent metal-organic frameworks (MOFs) (Eu 3+ @MIL-53(Al)) and specific-phages for PA detection, where the Eu 3+ @MIL-53(Al) prepared by one-pot method exhibits excellent fluorescence properties. By covalently binding specific phages isolated from hospital wastewater to the EuMOF surface, we constructed a fluorescent biosensor capable of detecting PA within 15 min, with a sensitivity threshold of 2 CFU/mL. Notably, this biosensor demonstrates high specificity, accurately quantifying live PA in complex bacterial mixtures and distinguishing live from dead bacteria. Its practical application has been validated in clinical blood and stool samples. As a novel platform for clinical microbial monitoring, the Eu 3+ @MIL-53(Al)-phage biosensor not only holds substantial economic potential but also carries significant public health implications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Huijing Ma,Bing Yu,Qingping Wang,Gary Owens,Zuliang Chen
While Fe-based metal-organic frameworks (MOFs) can be used to remove antibiotics by adsorption, knowledge of how antibiotics are degraded by MOFs is still limited. In this study, one Fe-based MOF, NH 2 -MIL-88B was used to remove pefloxacin from aqueous solution via a combination of adsorption and Fenton-like oxidation. NH 2 -MIL-88B exhibited a high adsorption capacity for pefloxacin (41.37 mg·g −1 ), with >99% removal efficiency within 120 min based on Fenton-like oxidation. To better understand the mechanisms involved in integrated adsorption and Fenton-like oxidation, various advanced characterization techniques were used to monitor the changes in morphology and composition of NH 2- MIL-88B before and after removal of pefloxacin. Scanning electron microscopy/energy dispersive X-ray spectroscopy (SEM/EDS), Fourier transform infrared spectroscopy (FTIR) and X-ray diffraction (XRD) all supported adsorption and Fenton oxidation of pefloxacin. In addition, the pefloxacin degradation products identified by LC-UV and LC-MS provided information on the potential adsorption-Fenton oxidation mechanism. These results suggested that NH 2 -MIL-88B has remarkably potential to be used in an integrated adsorption and Fenton-like process for the removal of antibiotics from aqueous solution.
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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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TALANTA
·
2025
·
IF 6.1
Luyang Zhao,Yang Song,Guoyang Xie,Hengyi Xu
A colorimetric assay based on the Fe/Al bimetallic organic framework NH 2 -MIL-53(Fe, Al) was developed for the sensitive detection of Escherichia coli O157:H7 ( E. coli O157:H7), a critical pathogen threatening food safety. The framework’s high specific surface area facilitated efficient antibody immobilization, whereas the incorporation of Al 3+ enhanced electron transfer between Fe 2+ /Fe 3+ , thereby significantly boosting peroxidase activity. The optimized NH 2 -MIL-53(Fe, Al) exhibited 1.4-fold and 4.9-fold higher relative absorbance than NH 2 -MIL-53(Fe) and NH 2 -MIL-53(Al), respectively. And it demonstrated 40-fold and 2-fold greater affinity for TMB and H 2 O 2 , respectively, compared to the natural enzyme. By integrating a dual-recognition system based on antibody and aptamer, the method enabled rapid detection with a limit of detection of 10 1 CFU/mL in colorimetric mode. Its successful application in complex matrices, including lettuce, juice, pool water, and chocolate milk, had yielded satisfactory recovery and precision, confirming its promising potential for food safety monitoring.
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Journal of Cleaner Production
·
2024
·
IF 9.7
Song Xiao,Menglei Jin,Junyi Chen,Peng Wu,Ju Tang,Yi Luo,Yi Li
Perfluoroisobutyronitrile (C 4 F 7 N) mixed with CO 2 has emerged as a promising eco-friendly alternative to sulfur hexafluoride (SF 6 ) in gas-insulated equipment (GIE). However, thermal or discharge faults in GIE inevitably lead to the generation of harmful decomposition by-products, necessitating their prompt removal to safeguard equipment operation and personnel safety. In this study, we propose a nanofiber composite material comprising polyacrylonitrile (PAN) as the base and multi-metal organic frameworks (MOFs) as the primary adsorbent material for removing typical decomposition components of C 4 F 7 N/CO 2 gas mixture. Utilizing grand canonical Monte Carlo (GCMC) and molecular dynamics (MD) simulations, we elucidate the selective adsorption mechanisms. Experimental results show that PAN@HKUST-1(Cu) exhibits superior adsorption efficiency for fluorocarbon gases compared to PAN@MIL-101(Cr), while the latter demonstrates better performance for nitrile gases. The PAN@HKUST-1(Cu)/MIL-101(Cr) composite adsorbent effectively removes eight typical harmful decomposition products while minimally affecting C 4 F 7 N. Our findings suggest that PAN@HKUST-1(Cu)/MIL-101(Cr) nanofiber film holds promise as an adsorbent for C 4 F 7 N/CO 2 based GIE.
研究领域:
材料科学
·
环境工程
·
化学工程
·
纳米技术
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 3
·1-10
·
IF 5.3
Miao Pandeng,Chen Jiaquan,Xu Guangfu,Yu Tao,Du Yingxiang
Chiral phenyl aromatic compounds (CPACs) are widely used in drug development, food/cosmetic production, and other organic synthesis processes, and their different enantiomers have distinct physiological activities and application differences. A double-layer metal–organic framework composite (MOF-on-MOF) was obtained by in situ synthesis of chiral metal–organic framework (CMOM-3S) on the surface of an iron-based metal–organic framework (NH 2 -MIL-101(Fe)). According to our investigation, MOF-on-MOF composite was for the first time applied to the stationary phase of capillary electrochromatography (CEC), and enantioseparations of eight CPACs were accomplished. Compared with single CMOM-3S, the enantioseparation performance of the coated capillary columns based on NH 2 -MIL-101(Fe)@CMOM-3S was improved by 34.07 ~ 720.0%. The R-/S-mandelic acid in actual sample (apricot leaves) was detected by the newly CEC system to be 0.0118 mg mL −1 and 0.0523 mg mL −1 , respectively. The spike recoveries were 96.60 ~ 104.7%, indicating its good stability and accuracy. In addition, the selective adsorption capacity of MOF-on-MOF composites was verified by adsorption experiments. Graphical Abstract
研究领域:
分析化学
·
材料科学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 10
·106518
·
IF 4.386
Qingxiao Zhang,Pei Han,Hui Zhang,Jixin Yao,Xinyu Wang,Dongmeng Chen,Xueqin Zuo,Qun Yang,Shaowei Jin,Guang Li
The oxygen evolution reaction (OER) is a critical process in the operation of electrochemical water splitting. Metal-organic frameworks (MOFs) are applied in the field of OER electrocatalysis because of their unique structure, but the high impedance and unstable framework during pyrolysis remain unresolved. Here, MIL-88A (iron-based MOF) was modified by hydrolysis and loading Co(OH)2 to improve the catalytic activity. The electrochemical results showed that the Co(OH)2/MIL-88A achieved the optimized performance with the current density of 10 mA cm−2 at 278 mV (vs RHE). Density functional calculations (DFT) combined with characterization tests suggest that electrons transfer from Co(OH)2 to MIL-88A at the interface of the heterostructure, leading to a larger hole electron pair density. D-band theory calculations demonstrated that the synergistic effect of MIL-88A and Co(OH)2 in heterostructure strengthens the adsorption between active sites and adsorbate. The above proofs are the source of the excellent OER performance of the Co(OH)2/MIL-88A. The finding has certain reference significance for the heterogeneous treatment of iron-based MOF catalysts.
研究领域:
材料科学
·
电化学
·
催化科学
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APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Wentao Zhang,Kunrui Wei,Wenguang Huang,Jianghua Yang,Yonghai Gan,Shujuan Zhang
Post-synthetic modification with β -diketone has been proven as an effective strategy to improve the visible light response activities of metal-organic frameworks (MOFs). Nevertheless, the effects of the anchored-diketones on the excitonic behaviors and photocatalytic mechanisms of MOFs are still unclear. Herein, two MOFs (MIL-101 with Cr III and MIL-101 with Al III ) were employed as prototypical materials to further understand this post-synthetic modification strategy. Diketone anchoring could enhance the photocatalytic generation of singlet oxygen ( 1 O 2 ) by the two MOFs in a joint mechanism: exciton-mediated energy transfer and photosensitization. Diketone anchoring induced triplet exciton was found playing an important role in the photocatalytic generation of 1 O 2 . The photosensitization of the anchored-diketone also played a key role in the photocatalytic generation of 1 O 2 . The results here provide a useful guidance for the development of MOFs-based photocatalysts and are helpful to realize the regulation of excitonic behaviors and photocatalytic mechanisms of MOFs.
研究领域:
材料科学
·
光化学
·
环境科学
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