Catalysis Science & Technology
·
2022
·Vol. 13
·期 3
·705-713
·
IF 6.177
Xu Zhang,Xiaoman Li,Senda Su,Mengyao Tan,Guodong Liu,Yingying Wang,Min Luo
The active sites of the catalyst and the charge transfer during the reaction are crucial for the photocatalytic nitrogen reduction reaction (PNRR). Here, ultrafine Ag Nanoparticles (Ag NPs) as the active sites and the electron transporters are successfully fixed in the cavities of the metal–organic frame MIL-101(Cr) by the “double solvent-photoreduction” method. The hydrophilic cages of MIL-101(Cr) could restrict and disperse the growth of Ag NPs, and the windows of the cages prevent them from being detached from the MOF carriers. The Schottky junction between Ag NPs and the MIL-101(Cr) leads to ligand–metal charge transfer (LMCT), while the localized surface plasmon resonance effect (LSPR) possessed by Ag NPs themselves generates hot electrons. Thus, N2 was converted to NH3 by the synergistic effect of the two mechanisms, which was 12 times higher than that of pure MIL-101(Cr) and reached 138.81 μmol g−1 h−1. Furthermore, the mechanism of nitrogen fixation and the reason for the stabilization of this catalyst were investigated, and the results were verified by density functional theory calculations.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Wei Zhao,Mengru Yan,Xinran Yang,Xiaojun Zeng,Yantong Chen,Benlin Dai,Xiaozhong Chu,Xuekun Hong,Feihu Mu,Shijie Li,Dennis Y.C. Leung
Environmental pollution caused by the overusage and uncontrolled discharge of antibiotics such as amoxicillin will endanger public health and ecosystems. Herein, a novel Ag/MIL-68(In)-NH 2 /Bi 4 O 7 plasmonic heterojunction has been successfully prepared through a two-step route followed by photoreduction for environmentally friendly photocatalytic amoxicillin degradation. Ag/MIL-68(In)-NH 2 /Bi 4 O 7 displayed the most efficient photocatalytic performance, which was 3.7 and 3.2 times that of Bi 4 O 7 and MIL-68(In)-NH 2 , respectively. The superior photocatalytic activity was directly linked to its large surface area and localized surface plasmon resonance (LSPR) effect, which provides more active sites and effectively promotes visible light absorption. Moreover, the degradation path of amoxicillin was explored in detail by combining Gaussian software calculation with liquid chromatography-mass spectrometry (LC-MS) analysis. Finally, a series of characterizations and simulations were carried out to demonstrate the S-scheme photocatalytic mechanism.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 17
·49301-49313
·
IF 5.8
Abd El-Monaem Eman M.,Eltaweil Abdelazeem S.,El-Subruiti Gehan M.,Mohy-Eldin Mohamed S.,Omer Ahmed M.
Water pollution is a dreadful affair that has incessantly aggravated, exposing our planet to danger. In particular, the persistent nitro aromatic compound like nitrophenols causes anxiety to the researchers due to their hazardous impacts, excessive usage, and removal difficulty. For this purpose, a novel multi-featured composite was constructed based on κ-Carrageenan (κ-Carr), MOF (MIL-125(Ti)), and magnetic Fe 3 O 4 for efficient adsorptive removal of o-nitrophenol (o-NP). Interestingly, BET measurements revealed the high surface area of Fe 3 O 4 -κ-Carr/MIL-125(Ti) of about 163.27 m 2 /g, while VSM showed its excellent magnetic property (20.34 emu/g). The comparison study pointed out the synergistic effect between Fe 3 O 4 , κ-Carr, and MIL-125(Ti), forming a composite with an excellent adsorption performance toward o-NP. The adsorption data obeyed pseudo-second-order kinetic model, and Freundlich isotherm model was better fitted than Langmuir and Temkin. Furthermore, Langmuir verified the supreme adsorption capacity of o-NP onto Fe 3 O 4 -κ-Carr/MIL-125(Ti) since the computed q max reached 320.26 mg/g at pH 6 and 25 °C. Furthermore, the XPS results postulated that the adsorption mechanism pf o-NP proceeded via H-bonding, π - π interaction, and electron donor–acceptor interactions. Interestingly, Fe 3 O 4 -κ-Carr/MIL-125(Ti) composite retained good adsorption characteristics after reusing for five cycles, suggesting its viable applicability as an efficient, renewable, and easy-separable adsorbent for removing nitro aromatic pollutants.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2022
·
IF 8.025
Shichen Wang,Yixuan Liu,Yue Hu,Weibo Shen
Metal-organic frameworks (MOFs) are gradually used since of their huge specific surface area and superior pore structure. However, there are problems such as easy aggregation and difficult separation in water treatment. In this study, we prepared composite microspheres (FMCS-1) by modifying MIL-125-NH 2 with Fe 3 O 4 and chitosan. The structural characterization and performance analysis of the materials showed that the introduction of chitosan effectively prevents the stacking of MOFs. The magnetic test manifested that Fe 3 O 4 solved the problem of the difficult separation of MOFs from water. The removal potential of toxic Cr(VI) was tested by adsorption experiments. The isotherm model indicated that FMCS-1 is a single molecular layer adsorbent with a maximum adsorption capacity of 109.46 mg/g at pH = 2. The adsorption kinetics showed that the adsorption of Cr(VI) by FMCS-1 was chemical adsorption. The acid resistance test demonstrated that FMCS-1 can exist stably in acid solutions. The recycling experiments proved that the adsorbent can be reused and the removal percentage still reaches 50 % after 5 cycles. This work expands the application of MOFs in water treatment and also provides an effective adsorbent for Cr(VI) removal.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Qun Ding,Xuejun Zou,Jun Ke,Yuying Dong,Yubo Cui,Hongchao Ma
Herein, a ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 heterojunction is successfully constructed through a facile hydrothermal strategy for enhancing solar energy harvesting and efficiency of catalytic nitrogen reduction induced by enlarged light absorption range, increasing interfacial charge transfer ability and desirable stability. Under the simulated sunlight irradiation, the N 2 fixation experiment shows that the yield of NH 3 reaches 1084.31 μmol/(g·h) over the TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalyst, and the yield is significantly enhanced, which is 33.68 and 13.94 times that is higher than the pure TiO 2 and g-C 3 N 4 , respectively. In a mean time, the excellent performance of the photocatalytic N 2 fixation over the ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is verified based on density function theory calculation and the decisive step over the composite is investigated by calculating Gibbs free energies of nitrogen reduction paths. The performance enhancement mechanism of TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is speculated, which indicates that the hybridized three-component system presents a desirable Z-scheme band alignment, resulting in the improvement of separation and transfer efficiency of photoinduced charge carriers. The article shows a new and high-efficiency TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalysis for excellent nitrogen reduction ability.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Hongai Zheng,Mengyao Li,Shuangyan Jiang,Cunzheng Xiao,Meilin Zhu,Yao Zhou,Derui Wang,Xin Sun,Daquan Zhang,Lizhi Zhang
Herein, the MIL-88A/Carbon quantum dots (CQDs) was synthesized by a hydrothermal method , and the polyvinylidene fluoride (PVDF) membrane modified by the MIL-88A/CQDs was fabricated by vacuum-assisted suction filtration. Compared with the pristine membrane, MIL-88A/CQDs modified membrane based on collaborative photo-Fenton/filtration process shows better removal efficiency for methylene blue (MB), rifampicin (RIF), methyl orange (MO), and Rhodamine B (RhB). In addition, the anti-fouling properties of the modified membrane are significantly improved, and the flux recovery of the MIL-88A/CQDs modified membrane increased from 56% to 89%, and the irreversible fouling ratio (R ir ) decreased from 44% to 11%. Significantly, the modified membrane contaminated by MB within 20 min can achieve self-cleaning through the photo-Fenton process. Finally, a possible membrane antifouling mechanism is proposed: superoxide radicals (•O 2 - ) and hydroxy radicals (•OH) are the main active substances. CQDs accelerates the e − and h + separation of MIL-88A and promotes the circulation of Fe substances. The fundamental research will present a promising strategy for improving antifouling properties of membrane.
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Huifang Feng,Yitong Sun,Qiaozhen Xu,Hong Liu
Developing efficient photocatalyst to promote the conversion of CO 2 into value-added chemicals remains challenging. Here, novel NH 2 -MIL-101(Fe)@Bi 2 MoO 6 S-scheme heterojunctions were fabricated via a solvothermal method, in which Bi 2 MoO 6 (BMO) nanoparticles uniformly growing on the NH 2 -MIL-101(Fe) (NM101) octahedrons with intimate contact interface. The resultant heterojunctions revealed significantly enhanced activity for CO 2 photoreduction. The optimal performance was achieved when the content of BMO was 10 wt%, and the formation rate of CO reached 67.0 μmol·g −1 ·h −1 under visible light illumination (with apparent quantum efficiency of 0.09 % at 450 nm), which was 3.2-fold of individual NM101. The boosting activity benefited from the formation of S-scheme heterojunction at the NM101 @BMO interfaces, which facilitated the separation of photoinduced electron-hole pairs with strong redox ability at the interface. This S-scheme charge transfer mechanism was further validated by the in-situ XPS and fluorescence probe molecular experiment. Besides, the intermediates and preliminary mechanism of photoreaction were unraveled based on in-situ DRIFTS analysis. This work provides some novel insights for designing efficient S-scheme photocatalysts for CO 2 photoreduction.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 30
·10472-10480
·
IF 4
Pingping Teng,Ying Liu,Zhongqiao Sun,Hao Meng,Yide Han,Xia Zhang
Development of binary MOF-on-MOF heterostructures is a research hotspot in MOFs chemistry due to the advantages elicited by a closely connected interface, which may endow more abundant functionality and even broader applications in interface chemistry. A MOF-on-MOF heterostructure was constructed by in situ growth of MIL-88B on the outer surface of UiO-66. The resultant MIL-88B@UiO-66 produced had an interesting flower-like morphology composed of MIL-88B (petal) on tetrahedral UiO-66 (core). The MIL-88B@UiO-66 heterostructure showed adsorption and Fenton-like oxidation abilities, with distinctly improved structural stability in aqueous solution compared with that of single MIL-88B. Methylene blue (MB) was selected as the target molecule to evaluate the adsorption and Fenton-like oxidation activities. The efficiency of total removal of MB was studied systematically under various operating conditions and the influencing factors were optimized. The kinetics of adsorption and catalytic oxidation were simulated to explore the interactions between MB and MIL-88B@UiO-66. The mechanisms of enhanced adsorption and Fenton-like oxidation were suggested. The cyclic removal performance and structural stability of MIL-88B@UiO-66 were also determined.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Jiangtao Dong,Aohui Han,Yanli Zhao,Haoming Li,Yue Yang,Bowen Yuan,Yishan Wang,Runqiang Liu,Xinming Yin,Xuezhong Du
Nanopesticides have been selected as one of the top 10 chemical innovations for enhancing the efficacy and safety of agrochemicals . Herein, smart, degradable, and eco-friendly metal−organic framework MIL-101(Fe III ) nanoherbicides coated with carboxymethyl cellulose-Ca II (CMC-Ca II ) cross-linking hydrogel-like networks are synthesized via a simple strategy. The coating of the CMC-Ca II hydrogel-like gatekeepers is oriented by the coordination unsaturated Fe III clusters on the surfaces of the MIL-101(Fe III ) nanocarriers to form a dense film network to prevent paraquat (PQ) leakage. Based on the stimuli factors (acid/basic pH, GSH, phosphates, and EDTA) of physiological and natural environments of target plants, the nanoherbicides are combined with five stimuli-responsive properties to attain the various controlled release of packaged PQ by the disassembly of the gatekeepers and/or the degradation of the MOF skeleton structure. More importantly, based on the stimuli-responsive controlled release mechanisms, the eco-friendly nanocarriers are ultimately degraded against bioaccumulation in plants or soil. The coating of natural CMC could promote the spreading of PQ owing to improvement of wettability for aqueous droplets of nanoherbicides on hydrophobic foliage. The PQ trapped in nanocarriers can effectively prevent PQ degradation, which showed that cumulative degradation rate is ca. 2.6 times lower than that of technical PQ under UV irradiation. The prepared nanoherbicides loaded with PQ show good control efficacy against weeds by controlling the release of PQ; good safety on seed germination (germination rate 97.32–99.67 %), seedling emergence (emergence rate 95.53–99.67 %), and are beneficial for the growth of wheat seedling (increase rate of plant height 1.89–6.97 % and 0.54–5.67 % after 7 and 15 days of seedling emergence, respectively) in the greenhouse; good biosafety for honeybees ( Apis mellifera L. ), which shows that lethal rates were 2.04 and 2.55 times lower than technical PQ for incubation 24 and 48 h, respectively. The nanoherbicides have potential applications in the field for PQ green agriculture.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Zhenbo Wu,Jinjuan Xue,Jiaqian Zhang,Mingxin Wang,Zhaoxia Chen,Yiting Lv,Shuaishuai Ma
Emulsified oils and microbial contaminations in water environments have posed huge risks to human health and ecological balance. In this work, we fabricated a polyaniline/NH 2 -MIL-125 (PANI/MIL) heterojunction decorated hydrolyzed polyacrylonitrile (HPAN) membrane with photocatalytic self-cleaning property for oil–water separation and bacterial inactivation. In which, PAN membrane was prepared by electrospinning and then HPAN membrane was obtained by alkaline hydrolysis. The photo-responsive PANI/MIL heterojunction was immobilized on HPAN membrane by vacuum-assisted assembly using protocatechuic acid (PCA) as the binder. The resultant PANI/MIL@HPAN composite membrane has a wettability of in-air superamphilicity and underwater superoleophobicity as well as surface nano-micro heterostructure. The composite membrane showed good separation efficiency (above 99.4%) and high flux (1446–3744 L m −2 h −1 ) in a series of oil-in-water/seawater emulsions separation. In particular, the membrane can effectively deal with viscous oil fouling under visible light to achieve a desired flux recovery ratio (FRR) after separating crude oil from water, which was ascribed to the self-cleaning capacity originating from the surface coating photocatalyst. Meanwhile, the multifunctional composite membrane showed 100% photocatalytic inactivation efficiency against pathogenic Gram-negative bacteria E. coli and Gram-positive bacteria S. aureus (6 log units) in water under visible light with low power intensity. The oil–water separation performance as well as photocatalytic inactivation efficiency of PANI/MIL@HPAN are superior to MIL@HPAN. The studies on the wettability, photothermal properties and photoelectric properties suggested that the coupling of conductive polymer PANI can simultaneously enhance the underwater superoleophobicity of the composite membrane, as well as improve the photocatalytic activity by creating a type II heterojunction to promote the separation of charge carriers and amplifying the photothermal effect, making the PANI/MIL@HPAN multifunctional membrane achieve the improved oil/water separation performance and antibacterial activity synergistically. This work provides a new strategy for developing effective self-cleaning membranes both toward oil/water separation and bacterial inactivation applications based on MIL metal–organic framework coupling with conductive polymers.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Jiabi Xu,Jiayi Peng,Xiangting Wang,Xiaohong Hou
Nanozymes have gradually become a research hotspot in the field of enzymology, benefiting from their low cost, high stability, and availability. To break through the limitation that conventional nanozymes exert peroxidase-like (POD-like) activity under only acidic conditions, we rationally designed Fe3O4@MIL-100(Fe) with excellent superparamagnetism and catalytic activity. An optimization of the microwave-assisted in situ synthesis conditions was carried out to obtain the highest POD-like activity of the nanozyme under nearly neutral conditions. Adenosine triphosphate (ATP) was appointed as an auxiliary regulator to further amplify the activity of the nanozyme Fe3O4@MIL-100(Fe). A series of behaviors related to enzymology and the mechanism of ATP-assisted enhancement were further explored. Consequently, a colorimetric sensing strategy was proposed for the one-step detection of cholesterol with a linear range of 0.05–0.4 mM and a limit of detection (LOD) of 1.3 μM (3.3 δ/S). The result of the present work implied that the established one-step platform could be successfully applied to the detection of cholesterol in actual samples. From the nanozyme synthesis to the colorimetric sensing process, the concepts of time savings and straightforwardness were always upheld and satisfactorily implemented. Most importantly, Fe3O4@MIL-100(Fe) could be a great potential biocatalyst candidate for the development of the corresponding commercial kits.
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 9
·1-13
·
IF 6.408
Chen Jing,Li Shuying,Chen Ying,Yang Jiao,Dong Jianbin
Adenine (A) and guanine (G) are mainly found in deoxyribonucleic acid (DNA) and ribonucleic acid (RNA) and play a crucial role in genetic information transfer and protein synthesis. In this study, NH 2 -MIL-53(Fe)/CS/MXene nanocomposites were prepared for detecting guanine and adenine. With high specific surface area, excellent water dispersion, and numerous active sites, MXene (transition metal carbides, nitrides, and carbonitrides) provides a good platform for loading primitive metal-organic frameworks (MOFs). At the same time, the problem of poor conductivity and dispersion of MOFs is solved. The electrochemical catalytic oxidation of adenine and guanine of NH 2 -MIL-53 (Fe)/CS/MXene nanocomposites was carried out by differential pulse voltammetry (DPV). Operating voltage of DPV: 0.7–0.9 V (vs. Ag/AgCl) for G, 1.0–1.2 V (vs. Ag/AgCl) for A, 0.8 V (vs. Ag/AgCl), and 1.1 V (vs. Ag/AgCl) for G and A. The concentration ranges for detecting A and G were 3–118 μM and 2–120 μM with detection limits of 0.57 μM and 0.17 μM (S/N = 3), respectively. The nanocomposite was used for detecting G and A in herring sperm DNA, and the content of G and A was found to be about 9 and 11 μM; the RSD values were 3.4 and 1.3%, respectively. Graphical abstract
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危险品化学品经营许可证（带存储）