COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Jiaojiao Cao,Chengbin Guo,Zhenyu Chen
A series of MOF-5 @BTA-X (X = -CH 3 /-NH 2 /-CO(CH 2 ) 6 CH 3 ) anticorrosion composites was fabricated through loading benzotriazole derivatives in a metal–organic framework (i.e., MOF-5). Their crystal structures and morphologies were characterized by single-crystal X-ray diffraction analysis, Fourier transform infrared spectroscopy , and transmission electron microscopy . The loading–releasing mechanisms between MOF-5 and BTA derivatives were revealed by experiments and theoretical calculations. Their anticorrosion performance for copper was also evaluated by electrochemical impedance spectroscopy and potentiodynamic polarization in 0.5 M NaCl. The corrosion product was analyzed via scanning electron microscopy and X-ray photoelectron spectroscopy. The results indicated that the loading capacities followed the order of MOF-5 @BTA-NH 2 > MOF-5 @BTA-CH 3 > MOF-5 @BTA-CO(CH 2 ) 6 CH 3 . The release rates followed the order of MOF-5 @BTA-NH 2 < MOF-5 @BTA-CH 3 < MOF-5 @BTA-CO(CH 2 ) 6 CH 3 . Furthermore, the results of theoretical calculations indicated that the differences in loading capacities depended on the polarity of the functional group. Meanwhile, the strong binding force decreased the release rate.
研究领域:
材料科学
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腐蚀防护
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纳米复合材料
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理论化学
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电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Sijia Liu,Xifei Zhou,Changqing Yang,Chaohai Wei,Yun Hu
The extensive use of sacrificial agents and the low carrier separation and utilization efficiency remain important factors limiting the development of photocatalytic hydrogen production . We report a three-layered, dual-functional photocatalysts of Cu atomics@UiO-66-NH 2 (U6N)/ZnIn 2 S 4 nanosheets (ZIS), for the simultaneous production of photocatalytic hydrogen and degradation of organic pollutants . When common and highly toxic organic pollutants (phenolic compounds and antibiotics) were substituted for the sacrificial agents, Cu@U6N/ZIS exhibited superior sustained hydrogen production, approximately 28 times greater than that of pure ZIS. The experimental results suggested that the window size of U6N (< organic pollutants molecular size) separates the reaction sites of organic pollutants oxidation and reduction of hydrogen ions (H + ), thereby achieving spatial separation of redox sites. Besides, the structure of Cu@U6N/ZIS, which was anchored Cu within U6N and encapsulated by ZIS nanosheets, forming Z-type heterojunctions, achieved the control of the directional transfer of photogenerated electrons. And the coupled system can effectively enhance water quality by reducing the biological toxicity of the wastewater. This study suggests new avenues for environmental restoration and non-fossil fuel production.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Shusu Shen,Honglin Li,Yang Shen,Renbi Bai,Ganwei Zhang
Metal organic frameworks (MOFs) possess excellent post-modification characteristics, high specific surface area, diversity of skeleton composition and pore tunability, have been increasingly applied in membrane modifications. In this work, NH 2 -MIL-88B(Fe) (NM88B) was first fixed onto polyvinylidene fluoride (PVDF) membrane by polyethyleneimine (PEI) through a vacuum-assisted self-assembly process, and the deposited NM88B was subsequently grafted with perfluoroalkyl polyethoxyacetic acid (FPEOAA) via a condensation reaction to realize the surface modifications. The modified membranes (named as N1F x ) showed improved hydrophilicity and underwater-oleophobicity. In addition, very high pure water flux (up to 9403 L‧m −2 ‧h −1 ) was obtained for the N1F x membranes due to the high porosity of introduced NM88B. In the dead-end filtration experiments of n -hexadecane-water emulsion, the optimum membrane N1F20 showed a good oil rejection rate (98.3%) and high permeation flux (667 L‧m −2 ‧h −1 ) which is approximately seven times of the pure PVDF membrane, indicating that the surface-modified membranes had excellent permeability and good separation performance. Even after four filtration cycles of oil-water emulsion, the rejection rate maintained higher than 97%, showing good reusability. Furthermore, the study found that N1F20 had certain acid and alkaline resistance and great potential for engineering applications.
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BIOCHEMICAL ENGINEERING JOURNAL
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2023
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IF 3.9
Chang Liu,Xiaoyue Zhang,Yu Zhou,Lin Zhu,Chengyu Zhang,Xiaohui Yan,Shengping You,Wei Qi,Rongxin Su
The enzyme leakage in physical adsorption dramatically limits the application of immobilized laccase (Lac) in environmental treatment. Therefore, a leakage-proof Zr-based metal-organic framework (MOF) carrier, UiO-66-NH 2 (30), was constructed for the stable loading of Lac and efficient antibiotic biodegradation, which could fix the Lac inside the carrier rather than only adsorbed on the surface. Based on the aperture modulation strategy, the pore size distribution of MOFs at about 10 nm was significantly increased to match the diameter of Lac (7.6 nm), by which Lac@UiO-66-NH 2 (30) was successfully prepared with a high enzyme loading amount (275.96 mg/g) and high enzyme recovery (618 %). The immobilized Lac@UiO-66-NH 2 (30) could nearly 100 % biodegrade rifampicin and lincomycin in 6 min and 6 h, respectively, and after 8 times reuse, the degradation rates of antibiotics remained at 81.46 % and 76.12 %, which showed excellent reusability and stability. Overall, Lac@UiO-66-NH 2 (30) is expected to be an ideal candidate for pollution control.
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NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 29
·13855-13865
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IF 3.3
Yong Cheng,Lin Deng,Dan Wang,Changchun Ji,Ying-Hua Zhou
The development of advanced catalysts is essential for efficient elimination of the emerging organic pollutants in water. Herein, Cu9S5 and Cu9S5@UiO-66-NH2 were prepared and both exhibited high Fenton-like photocatalytic activities for the degradation of organic contaminants. Removal efficiencies of 85% and 92% were achieved for Congo red (CR) and Rhodamine B (Rh B), respectively. It is found from active species trapping experiments and electron spin resonance (ESR) analysis that ˙O2−/h+ and ˙O2−/˙OH played key roles in the oxidation reaction of these two pollutants, respectively. The mechanisms were discussed on the basis of the cycles of Cu+/Cu2+.
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International Journal of Nanomedicine
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2023
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IF 8
Yongai Xiong,Tingting Chen,Lei Chen,Rongshan Cai
Introduction Radiotherapy and chemotherapy are the fundamental causes of myelosuppression in cancer patients, which usually induce a serious hematopoietic system toxicity, causing the hemocytes and immunity decline of patients. Ziyuglycoside I (ZgI), an active ingredient isolated from traditional Chinese medicine Sanguisorba officinalis L, has been demonstrated to increase the leucocytes and protect hematopoietic stem cells, which is related to its promotion of autophagy in hematopoietic stem cells.Methods In the present study, we formulated the SH-PEG-NH2-coated gold nanoparticles loading ZgI (ZgI-AuNPs) with a enhanced autophagy promotion in hematopoietic stem cells. ZgI-AuNPs were prepared by HAuCl4-sodium citrate reduction method, and the synthesis of ZgI-AuNPs was validated by XRD, FT-IR, DSC, and TEM findings. Furthermore, the drug loading rate and the release of ZgI were evaluated, and the ZgI-AuNPs’ effects on autophagy and immunofluorescence staining for LC3B were tested. Finally, the effect of ZgI-AuNPs on the autophagy and hematopoietic ability of HSCs in vivo was also carried out.Results The prepared ZgI-AuNPs have an irregular cubic crystal structure by TEM observation, and the average particle size was 340 ± 16.5 nm determined by DLS. The XRD, FT-IR and DSC detection showed that the ZgI had been well loaded in AuNPs, and the AuNPs can load the ZgI at a content of 160.63 ± 1.35 μg·mg−1. Meanwhile, the AuNPs can reduce the drug release rate of ZgI. Importantly, the ZgI-AuNPs enhanced autophagy of HSCs both in vitro and in vivo. At the same time, the gold nanoparticles enhance the hematopoietic effect of ZgI on mice HSCs.Conclusion Our research suggests that SH-PEG-NH2-coated gold nanoparticles loading ZgI has potential application in myelosuppression therapy.
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PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Shuting Tian,Yang Bai,Shuangshuang Li,Zuoming Chen,Liyun Zhang,Hongjie Li,Peng Zhou,Yi He
Microsphere layers/nanofibrous membranes decorated with UiO-66-NH 2 as a metal-organic framework (MOF) were successfully obtained by one-step coaxial electrospinning. The coaxially spun dense microsphere/wire-like structure and UiO-66-NH 2 hydrophilic components with excellent hydration ability enabled the prepared membrane to have excellent static and dynamic adsorption capacity for dyes and oil-in-water emulsion separation performance (adsorption capacity >247 mg/g; separation efficiency >99%). What's more, the membrane can purify complex wastewater dynamically and efficiently (separation efficiency >99%). After the membrane was desorbed in ethanol and methanol, the reversible recovery rate was as high as 98%, indicating its excellent recyclability. In a word, the as-prepared membrane has broad prospects in the remediation of complex polluted water bodies containing dyes-oil.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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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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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Wenqing Hou,Chen Chen,Diya Xie,Yiming Xu
Metal–organic frameworks (MOFs) as photocatalysts have received increasing attention. In this work, a dual metal-substituted UiO-66-NH2 (Ti/Ce-MOF) containing different Ti/Ce mole ratios (x = 0–2.46) has been prepared via post-synthetic exchange between Ce-UiO-66 and TiCl4, followed by amination. The solid had a high surface area (828–937 m2/g) and a large pore volume (0.451–0.507 m3/g). Under visible light, Ti/Ce-MOF showed x-dependent activity for H2O reduction and oxidation on a film electrode, respectively. However, such a change for H2 evolution in a Na2S/Na2SO3 aqueous solution was observed only after CdS loading. In combination with the photoluminescence and band parameters, we propose that the photoactivity of Ti/Ce-MOF for redox reaction is determined by its ability for electron transfer. Furthermore, there is an interfacial electron transfer from Ti/Ce-MOF to CdS and a hole transfer from CdS to Ti/Ce-MOF, respectively, significantly improving the efficiency of charge separation for redox reactions. This work offers a new insight that Ti substitution benefits the performance of Ce-based MOF.
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2022
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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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APPLIED CATALYSIS A-GENERAL
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2023
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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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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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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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