JOURNAL OF MEMBRANE SCIENCE
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2023
·
IF 9.5
Shiwei Tian,Yaqi Zhang,Qiankun Sha,Tian Yang,Yan Huang,Xingxiang Zhang,Wei Wang,Na Han
Highly efficient treatment of oil-water emulsions in severe environments (organic solvents, strong acids) is recognized as a challenging subject. Polyphenylene sulfide (PPS) is an ideal membrane material with superior thermal stability as well as chemical resistance that is expected to settle this challenge. However, the hydrophobicity of PPS (h-PPS) membrane inherently prevents its efficient treatment of oil-in-water (O/W) emulsions. In this study, superhydrophilic modification of PPS substrates was achieved by in situ electrostatic self-assembly of hydrophilic Zr-MOFs to obtain UiO-66-NH 2 @h-PPS membranes. The introduction of UiO-66-NH 2 crystals constructed the micro/nanoscale hierarchical structure for the substrate, which transforms the PPS substrate from a hydrophobic to a superhydrophilic state (water droplets require only 0.6 s to be completely immersed in the membrane). Meanwhile, the UiO-66-NH 2 @h-PPS membranes gain under-water superhydrophobicity (the under-water oil contact angle exceeds 150° for toluene, hexane , dichloromethane , and carbon tetrachloride , of which toluene reaches 163.1°), thereby improving wettability selectivity and decreasing oil adhesion, permitting the fabricated UiO-66-NH 2 @h-PPS membranes to effectively separate different types of O/W emulsions. The UiO-66-NH 2 @h-PPS membranes acquire excellent permeate fluxes (for the surfactant-free toluene-in-water emulsion, it reaches up to 7638.1 L m −2 h −1 ) and separation accuracy (99.1% oil rejection). Moreover, the UiO-66-NH 2 @h-PPS membrane exhibited outstanding harsh environment resistance. Interestingly, the combination of UiO-66-NH 2 and h-PPS substrate was applicable to degrade the organic compound in water, and the degradation efficiency of the methylene blue achieved 85.7% under visible light within 120 min. In summary, loading Zr-MOFs onto h-PPS substrates provides a novel strategy for the efficient treatment of wastewater under complex conditions with great potential for practical applications.
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Catalysts
·
2023
·Vol. 13
·期 5
·817
·
IF 3.9
Haoyu Yuan,Chao Zhang,Wenjing Chen,Yuzhou Xia,Lu Chen,Renkun Huang,Ruiru Si,Ruowen Liang
Metal–organic frameworks (MOFs) are new porous materials composed of metal centers and organic ligand bridges, which received great attention in the field of photocatalysis. In this work, Ag2CrO4@MIL–125(Ti)–NH2(denoted as AgCr@M125) Z–scheme heterojunctions were synthesized via a simple microemulsion method, by which highly dispersed nano–sized Ag2CrO4can be anchored uniformly on the surfaces of porous MIL–125(Ti)–NH2(denoted as M125). Compared with pure M125 and Ag2CrO4, the as–prepared AgCr@M125 hybrids show significant photocatalytic efficiency against inactivatedStaphylococcus aureus(S. aureus), reaching over 97% inactivation of the bacteria after 15 min of visible light irradiation. Notably, the photocatalytic activity of the obtained 20%AgCr@M125 is about 1.75 times higher than that of AgCr–M125, which was prepared via a traditional precipitation method. The enhanced photocatalytic antibacterial activity of the AgCr@M125 photocatalytic system is strongly ascribed to a direct Z–scheme mechanism, which can be carefully discussed based on energy band positions and time–dependent electron spin response (ESR) experiments. Our work highlights a simple way to enhance the antibacterial effect by coupling with Ag2CrO4and M125 via a microemulsion–assisted strategy and affords an ideal example for developing MOFs–based Z–scheme photocatalysts with excellent photoactivity.Keywords:MIL–125(Ti)–NH2;Ag2CrO4;S. aureus;Z–scheme;microemulsion method
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 29
·13855-13865
·
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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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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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
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
·
2023
·
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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International Journal of Nanomedicine
·
2023
·
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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高影响因子
BIOCHEMICAL ENGINEERING JOURNAL
·
2023
·
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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ACS Applied Materials & Interfaces
·
2023
·
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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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2018
·Vol. 33
·期 2
·e4708
·
IF 3.581
Mingliang Ma,Yuying Yang,Dili Liao,Ping Lyu,Jinwei Zhang,Jianli Liang,Lizhi Zhang
A strategy has been developed for the synthesis, characterization and catalysis of magnetic Fe 3 O 4 /P(GMA-EGDMA)-NH 2 /HPG-COOH-Pd core-shell structure supported catalyst. The P(GMA-EGDMA) polymer layer was coated on the surface of hollow magnetic Fe 3 O 4 microspheres through the effect of KH570. The core-shell magnetic Fe 3 O 4 /P(GMA-EGDMA) modified by -NH 2 could be grafted with HPG. Then, the hyperbranched glycidyl (HPG) with terminal -OH were modified by -COOH and adsorbed Pd nanoparticles. The hyperbranched polymer layer not only protected the Fe 3 O 4 magnetic core from acid–base substrate corrosion, but also provided a number of functional groups as binding sites for Pd nanoparticles. The prepared catalyst was characterized by UV–vis, TEM, SEM, FTIR, TGA, ICP-OES, BET, XRD, DLS and VSM. The catalytic tests showed that the magnetic Fe 3 O 4 /P(GMA-EGDMA)-NH 2 /HPG-COOH-Pd catalyst had excellent catalytic performance and retained 86% catalytic efficiency after 8 consecutive cycles.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Dawei Gao,Zhili Wang,Cong Wang,Liying Wang,Yue Chi,Minggang Wang,Jingjing Zhang,Chen Wu,Yan Gu,Hongli Wang,Zhankui Zhao
Ultrafine and well dispersed CrPd nanoparticles are successfully immobilized on NH 2 -functionalized porous metal-organic framework MIL-101 by a facile sequential impregnation-reduction approach. By virtue of the bimetallic synergistic effect between Cr and Pd and the strong metal-support interaction between CrPd nanoparticles and MIL-101-NH 2 support, the resulting Cr 0.4 Pd 0.6 /MIL-101-NH 2 catalyst exhibits excellent catalytic activity for the generation of hydrogen from formic acid, affording an excellent initial turn over frequency value as high as 2009 mol H 2 mol Pd −1 h −1 at 323 K, which is much higher than most of the reported noble metal heterogeneous catalysts for this catalytic reaction under similar conditions.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 2
·1-11
·
IF 5.3
Sun Xueqin,Fan Yan,Zhang Wenyuan,Yang Xiaogang,Liu Jiacheng
A pentafluoropropionic acid–functionalized fluorescent metal–organic framework material (UiO-66-NH 2 -PFPA) is prepared by a simple post-synthetic modification (PSM) strategy for the sensitive and selective detection of dichloran (DCN). The results of fluorescence experiments demonstrate that the sensitivity of UiO-66-NH 2 -PFPA (limit of detection, LOD = 0.478 μM) to DCN is nearly 10.93 times higher than that of UiO-66-NH 2 (LOD = 5.225 μM) and the material has good selectivity and anti-interference ability. After the addition of DCN, the blue fluorescence of UiO-66-NH 2 -PFPA is obviously quenched. Therefore, the possible quenching mechanism is further discussed in combination with relevant experiments and density functional theory calculations. Moreover, the sensor is applied to the detection of DCN in fruit samples with a satisfactory recovery of 101.1—107.9%, which implies that UiO-66-NH 2 -PFPA is expected to be a candidate material for the detection of DCN in food. Graphical abstract
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高影响因子
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