CHEMICAL ENGINEERING JOURNAL
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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.
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JOURNAL OF MOLECULAR STRUCTURE
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2024
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IF 4
Mengjiao Yu,Xiong-Fei Zhang,Siting Yang,Yunhua Bai,Zhongguo Wang,Jianfeng Yao
Developing functional catalysts with both Lewis and Brønsted acid sites is an essential task for achieving the direct conversion of glucose to 5-hydroxymethylfurfural (5-HMF), a process that is crucial for the sustainable production of renewable fuels and chemicals. In this work, a mixed-linker strategy is proposed to prepare defective MIL-53(Al)-NH 2 by introducing trifluoroacetic acid into the MIL-53(Al)-NH 2 synthesis process. The creation of defects facilitates the exposure and accessibility of Al 3+ centers, as well as changes the coordination environment within the MIL-53(Al)-NH 2 skeleton. Both the number of Lewis and Brønsted acid sites are boosted, which is beneficial for glucose activation and 5-HMF generation. Through optimizing the reaction conditions, a glucose conversion of 98.3 % with a 5-HMF yield of 59.3 % was achieved by using defective 6d-MIL-53(Al)-NH 2 in a biphasic tetrahydrofuran/H 2 O NaCl system. Moreover, the 6d-MIL-53(Al)-NH 2 catalyst showed excellent recyclability and reusability, with its catalytic efficiency maintained almost unchanged for consecutive 10 cycles. The catalytic mechanism was elucidated and the acidity of the Lewis and Brønsted acid was modulated by defect engineering to achieve exceptional performance.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
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IF 3.9
Bolun Yu,Jun Chen,Quanzhang Liu,Shuoyang Li,Xiaohang Zhang,Bowen Liang,Zuhong Lin,Haipu Li,Jingjing Yao
The use of metal–organic framework-derived materials for removing micropollutants from water is increasing, but precise composition control remains a challenge. In this study, 14 MIL-100(Fe)-derived materials were synthesized to adsorb and remove antipyrine (ANT) from water by optimizing the heating rate, pyrolysis temperature, and activation methods. The adsorbents demonstrated excellent ANT removal performance across a pH range of 3 to 11, as well as in complex water bodies. They also exhibited easy recovery and outstanding regeneration capabilities. Under the optimized conditions (i.e., ANT content: 10 mg/L, M-600–2 dosage: 0.1 g/L, and pH: 7), M-600-10 displayed the highest adsorption capacity (23.10 mg/g for ANT) while MIL-100(Fe) had limited adsorption capability (2.56 mg/g for ANT). The adsorption process was exothermic and spontaneous, influenced by both membrane diffusion and intraparticle diffusion, and followed the Freundlich and pseudo-second-order models. Despite variations in surface areas (75.70–261.91 m2/g), total pore volumes (0.2019–0.5984 cm3/g), and average pore sizes (7.47–13.99 nm), there was no strong linear relationship with adsorption capacity (7.47–15.99 mg/g). The major components, including Fe/pyrrolic N-doped graphene (PING), Fe3C/PING, Fe3O4/PING, and PING, had calculated adsorption energies of −0.94, −2.16, −0.79, and −2.24 eV, respectively, which correlated positively with Bader charge transfer numbers. The adsorbents relied on van der Waals forces for ANT adsorption, with PING exhibiting the strongest interactions and Fe3O4/PING exhibiting the weakest. These findings enhance the theoretical understanding of derived materials and expand their application in water purification.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Hongbing Mao,Huijun Wang,Yanyan Xing,Deyong Wang,Xiujun Cao,Jie Yu,Junya Yan
In this work, a boronic acid decorated mesoporous iron-based metal-organic framework (MIL-100(Fe)-B) nanozyme as an efficient immobilization matrix for glucose oxidase (GOx) was designed and prepared through a facile microwave-assisted metal-ligand-fragment co-assembly strategy. Compared with the unboric acid-modified MIL-100(Fe), boron-doped MIL-100(Fe) exhibited enhanced peroxidase-like activity, which was mainly due to the introduced B causing MIL-100(Fe) defects, accelerating mass transfer, facilitating more active sites for H2O2 decomposition. Besides, the MIL-100(Fe)-B nanozyme possessed sufficient recognition sites for immobilizing glucose oxidase with little enzyme leakage to form a cascade nanozyme with both peroxidase-like and cascade catalytic activities. A colormetric biosensor based on the integrated nanozyme reactor (GOx@MIL-100(Fe)-B) was developed for glucose detection. The proposed cascade biosensor had a linear range of 5-150 μM and a limit of detection (LOD) of 0.97 μM (3.3 δ/S). Interestingly, a portable microfluidic paper-based analytic device (μPAD) biosensor based on the cascade nanoplatform was further fabricated for visualized detection of glucose combined with a ColorPicker App on smartphone. It indicated that the integrated nanozyme GOx@MIL-100(Fe)-B was a promising candidate for glucose detection and provided a potentially analytical avenue for biosensing and other applications.
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COMPOSITES COMMUNICATIONS
·
2024
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IF 6.5
Xinyue Yang,Yong Li,Deyun Yue,Rui Li,Haojie Song
The construction of ternary heterojunction photocatalysts can achieve multi-gradient transfer of charges and accurate control the position of photogenerated electrons which has received increasing attention. In this paper, NH 2 -MIL-53(Al)@BiOBr@CQDs-10 % (ABCQDs-10 %) was prepared via a facile hydrothermal and chemical synthesis processes. Three-dimensional serration of NH 2 -MIL-53(Al) as a platform for irregular BiOBr nanosheets, CQDs promote interfacial contact and act as electron transport channels between BiOBr and NH 2 -MIL-53(Al) and constitute Z-type heterojunctions with high redox properties. ABCQDs-10 % shows the best photocatalytic removal efficiency (94.24 %) of CIP, the reaction rate constants (0.045 min −1 ) were 1.2 and 64 times higher than BiOBr and NH 2 -MIL-53(Al), respectively. The excellent degradation performance is attributed to the construction of Z-type heterojunction of NH 2 -MIL-53(Al)@BiOBr@CQDs which improve electron-hole separation and transfer efficiency. The main active species was •O 2 - . The photocatalytic activity of ABCQDs-10 % had not obvious loss after cycle experiments and the crystal structure had no significant changes, means high stable photocatalytic activity.
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LANGMUIR
·
2024
·
IF 3.7
Yinyin Peng,Ting Pan,Chuang Chen,Yuchen Zhang,Guoyuan Yuan,Derong Liu,Xiaoqin Pu,Wei Xiong
In this study, researchers developed a novel composite material called NH2-MIL-53-Al/PAN, which consists of metal–organic frameworks (MOFs) grown on electrospun PAN nanofibers (NFs). The successful formation of the composite was confirmed by X-ray diffraction (XRD) and Fourier transform infrared (FTIR), and the hydrophilicity of NH2-MIL-53-Al/PAN was demonstrated by the water contact angle (WCA). Batch experiments were conducted to investigate the adsorption performance of Co(II) under different conditions. The maximum adsorption capacity reached 58.72 mg/g, and almost 95% of the adsorption was achieved within the first 6 h. The adsorption process was found to be spontaneous and endothermic and followed the pseudo-second-order kinetics and Langmuir models. Chemisorption and molecular layer adsorption are the main mechanisms of adsorption, and X-ray photoelectron spectroscopy (XPS) analysis further reveals that the interaction between the adsorbent and cobalt is a coordination interaction. In this study, NH2-MIL-53-Al was grown in situ on PAN to ensure effective loading of MOFs and prevent agglomeration during the NF mixing process. This approach successfully addressed the challenge of exposing active sites within the embedded MOF crystals. Additionally, it overcame the difficulty of recycling traditional MOF adsorbents. As a result, the exceptional performance of MOF NFs offers a promising solution for the efficient removal of cobalt-containing wastewater.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yanping Dong,Xiqiang Tian,Shoulei Huang,Abdullah N. Alodhayb,Muhammad Zahid
The interfacial characteristics of platinum (Pt) metal catalysts can be systematically regulated by interacting them with electropositive metals, leading to synergistic interactions for extensive catalytic applications. In this study, an evenly dispersed polyol-synthesized iron (Fe)-promoted Pt bimetallic nanoparticle (BNPs) system was embedded in MIL-101(Cr). The PtFe 2 @MIL-101(Cr) catalyst unveiled remarkable activity (86%) and selectivity (89%) for the superior hydrogenation of the targeted C O bond of cinnamaldehyde (CAL). The exceptional hydrogenation performance can be credited to the interplay of the geometric and electronic properties arising from charge shuttling between Fe and Pt within the homogenously distributed Pt–Fe bimetallic nanoparticle system. The experimental results indicate enhanced valence electrons in the Pt d-band through the mutual synergetic interface between the Pt and Fe BNPs. Consequently, these Fe–Pt sites functioned as interfacial electrophilic and nucleophilic (Lewis acid-base) sites, enhancing H 2 activation and facilitating C O bond conversion to yield unsaturated cinnamal alcohols (COL). Additionally, the narrow pores of MIL-101(Cr) encapsulating the Pt–Fe BNPs induced steric hindrance, allowing only C O bond hydrogenation. Furthermore, the PtFe 2 @MIL-101(Cr) catalyst maintained its optimal hydrogenation performance over five cycles, demonstrating no substantial loss in either CAL conversion or COL yield, thus endorsing the universal practical applicability of the catalyst.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Hui Li,Weiguo Liu,Zhihao Han,Ndzondelelo Bingwa,Tianyu Wang,Hengdi Li,Yunpu Wang,Feiqiang Guo,Xiaoling Ma,Chenggong Sun
Microwave heating (MW) is known for its efficacy in promoting transesterification for biodiesel production. However, the microwave-induced catalysis, linked to catalyst absorbing capability, remains poorly understood. Herein, a class of alkaline catalysts with strong microwave absorption were synthesized, validating their positive impact on transesterification. Various methods were used to reveal the relationship between microwave absorbing capacity and physicochemical properties of the synthesized catalyst (KF/Mg-MIL). Results indicated the previously recognized basicity’s role for KF/Mg-MIL was surpassed by microwave absorbing capability (permittivity and permeability) in MW (2.45 GHz). KF/Mg-MIL, with ε r = 4.94′- j 1.09″ and μ r = 1.03′- j 0.024″, efficiently transformed microwave into thermal energy via the dielectric loss and magnetic loss, saving 50 % energy consumption and reducing 1051.61 kg CO 2 for per ton biodiesel compared to water bath heating (WB). Notably, “non-thermal” effect was observed with KF/Mg-MIL in MW, which reduced activation energy by 2.49 kJ/mol and increased the frequency factor by 793.32 min −1 in comparison to WB.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2024
·
IF 5.9
Fuhao Gan,Chunmei Gao,Shifeng Ji,Yunqing Xing,Tianming Gong,Lihui Tian,Yiming Bai,Zhuolong Wu
In this study, the iron-based metal–organic framework MIL-53(Fe) was successfully prepared by a solvent method and used as a photocatalyst for the efficient degradation of DDBAC under visible light. The morphology, structure and photocatalytic properties of MIL-53(Fe) were investigated by SEM, XRD, XPS and UV–vis DRS characterization methods. The optimum conditions for the degradation of DD pathways of DDBAC were analyzed in combination with DFT calculations. Based on molecular orbital theory and free radical quenching experiments, it was demonstrated that hydroxyl radicals were the main contributors in the oxidative degradation of DDBAC. The toxicity of DDBAC and its intermediates was evaluated by culturing Chlorella vulgaris, and the results showed that the Vis/MIL-53(Fe)/H 2 O 2 system was capable of solution detoxification.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Tianmin Gong,Chunmei Gao,Shifeng Ji,Yunqing Xing
2-Methyl-4-chlorophenoxyacetic acid (MCPA) is a herbicide that poses a threat to the environment. In this study, MIL-88A was utilized as a photocatalyst to degrade MCPA. Results demonstrated that the Light/MIL-88A/H 2 O 2 system exhibited remarkable photo-Fenton catalytic activity . Under optimal conditions of pH = 3.8, H 2 O 2 concentration of 1.2 mL/L, MIL-88A dosage of 0.2 g/L and an initial MCPA solution concentration of 50 mg/L, the degradation efficiency reached its peak, achieving a 99.9 % degradation rate of MCPA within 60 min. The morphology, structure, and photocatalytic performance of MIL-88A were investigated using characterization techniques such as SEM, XRD , XPS , and UV–vis DRS . Free radical quenching experiments and ESR characterization demonstrated that the main active material in the degradation of MCPA was •OH. The possible degradation pathways of MCPA were hypothesized by combining the results of Gaussian software and LC-MS analysis. Furthermore, the toxicity of MCPA was evaluated using T.E.S.T. software and mung bean germination experiments. The results revealed that the degradation of MCPA by Light/MIL-88A/H 2 O 2 system could achieve solution detoxification .
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
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IF 8.2
Guohui Wang,Qixin Zhang,Lailai Qin,Kaixuan Tan,Chunguang Li,Lianshun Li,Tinggui Yang,Xiaojuan Liu
A novel metal-organic framework (MOF) material, MIL-100(Fe)-DMA, was synthesized using the solvothermal method. The structure of the MOF was characterized using scanning electron microscopy-energy dispersive X-ray spectroscopy, N 2 adsorption–desorption isotherms, X-ray diffraction analysis, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, and Mössbauer spectroscopy. Batch adsorption experiments were performed to investigate the effects of initial Sr 2+ and Cs + concentrations, adsorption time, pH, and coexisting cations on the adsorption performance of the material. The adsorption mechanism was further elucidated using adsorption kinetics and isotherm models. The results indicated that the adsorption of Sr 2+ and Cs + does not significantly affect the MOF material structure. As reaction time and initial ion concentration increased, the adsorption capacity of MIL-100(Fe)-DMA for Sr 2+ and Cs + increased rapidly and then gradually reached equilibrium. Optimal adsorption occurred under alkaline conditions, with maximum adsorption capacity observed at pH = 8. The adsorption process for Sr 2+ and Cs + was well described by the pseudo-second-order kinetic model, the Weber–Morris model, and the Langmuir adsorption isothermal model. The adsorption process was mainly identified as monolayer chemical adsorption, influenced by multiple factors. Characterization combined with density functional theory calculations revealed that the unsaturated carboxylic acid groups on the surface of the MOFs play a crucial role in the interaction with Sr 2+ and Cs + .
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Processes
·
2024
·Vol. 12
·期 9
·1879
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IF 2.8
Huiying Yang,Xiangchao Meng
The conversion of nitrogen (N2) and water (H2O) into NH3by photocatalysis under ambient conditions has been considered an environmentally friendly strategy. However, developing effective catalysts for N2fixation is still challenging. Herein, we report a bimetallic JH Fe, Co/TiO2derived from NH2-MIL-125(Ti) by the fast Joule heating (FJH) method for visible–light–driven catalytic N2fixation. It was found that the photocatalytic N2reduction efficiency of bimetallic FC@TiO2-JH was improved, enabling an NH3yield rate of 110.14 µmol g−1h−1without any sacrificial agents. Furthermore, the rate was higher than those of Fe@TiO2-JH and Co@TiO2-JH, suggesting that the synergistic effect between Fe and Co broke the electronic equilibrium and increased the center of its d-band, enhancing electronic feedback to the antibonding π* orbitals of N2while weakening the bonding energy of N≡N. Meanwhile, the rate was about 2.75 times higher than that of FC@TiO2-TF, which was calcined in a tube furnace. It is assumed that FJH might lead to the formation of lattice defects, leading to localized charge deficiency, enhanced carrier separation, and transport. Thus, doping of Fe and Co synergistically interacted with the defects produced from FJH, facilitating the photocatalytic reduction process. As detected, it had a greater ability to separate hole–electron pairs and transferred electrons to adsorbed N2at faster rates. Our work demonstrates a prospective strategy for designing bimetallic catalysts derived from NH2-MIL-125(Ti) for N2fixation.
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