SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xiaoming Xu,Guoyan Hua,Yuxuan Chen,Yanhong Zhang,Zepeng Zhang,Weiben Yang,Fuqiang Liu,Aimin Li
Traditional polyamide nanofiltration membranes suffer from permeability-selectivity trade-off limitation and unsatisfactory rejection for divalent cations. Herein, a novel dually charged membrane was constructed by incorporating positively charged UiO-66-(NH 2 ) 2 into the negatively charged polyamide layer. Thanks to the customizable nanochannels of metal-organic frameworks, the amino-rich nanochannels of UiO-66-(NH 2 ) 2 could be fabricated through a ligand replacement strategy. UiO-66-(NH 2 ) 2 played a crucial role in the enhanced rejection of divalent cations, meanwhile negatively charged polyamide surface guaranteed the efficient Na 2 SO 4 rejection. Satisfactory rejections of CaCl 2 (96.07 %) and Na 2 SO 4 (90.62 %) were achieved simultaneously by optimal TFN-D5. Meanwhile, TFN-D5 owned the greatly-improved water permeance of 19.44 LMH/bar, which was about 1.5 times better than that of the TFC-control. Calculations based on density functional theory further confirmed UiO-66-(NH 2 ) 2 rejected Ca 2+ efficiently since the migration energy barrier across UiO-66-(NH 2 ) 2 was an order of magnitude higher than that of UiO-66-NH 2 and UiO-66. Moreover, the desirable rejections were beyond 94 % towards many divalent cation salts including MgCl 2 , NiCl 2 , PbCl 2 , MnCl 2 , CdCl 2 and ZnCl 2 . Thus, this work provided an efficient way to realize the synergistic removal of both divalent cations and anions.
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Polymers
·
2022
·Vol. 14
·期 2
·283
·
IF 4.967
Wei Chen,Ping Zhu,Yating Chen,Yage Liu,Liping Du,Chunsheng Wu
Iodine has been widely used as an effective disinfectant with broad-spectrum antimicrobial potency. However, the application of iodine in an antibacterial polymer remains challenging due to its volatile nature and poor solubility. Herein, iodine immobilized UiO-66-NH2metal-organic framework (MOF) (UiO66@I2) with a high loading capacity was synthesized and used as an effective antibacterial additive for poly(ε-caprolactone) (PCL). An orthogonal design approach was used to achieve the optimal experiments’ conditions in iodine adsorption. UiO66@I2nanoparticles were added to the PCL matrix under ultrasonic vibration and evaporated the solvent to get a polymer membrane. The composites were characterized by SEM, XRD, FTIR, and static contact angle analysis. UiO-66-NH2nanoparticles have a high iodine loading capacity, up to 18 wt.%. The concentration of iodine is the most important factor in iodine adsorption. Adding 0.5 wt.% or 1.0 wt.% (equivalent iodine content) of UiO66@I2to the PCL matrix had no influence on the structure of PCL but reduces the static water angle. The PCL composites showed strong antibacterial activities againstStaphylococcus aureusandEscherichia coli. In contrast, the same content of free iodine/PCL composites had no antibacterial activity. The difference in the antibacterial performance was due to the different iodine contents in the polymer composites. It was found that MOF nanoparticles could retain most of the iodine during the sample preparation and storage, while there was few iodine left in the free iodine/PCL composites. This study offers a common and simple way to immobilize iodine and prepare antibacterial polymers with low antiseptic content that would reduce the influence of an additive on polymers’ physical properties.Keywords:UiO-66-NH2metal-organic framework;iodine;poly(ε-caprolactone);antibacterial
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高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2022
·Vol. 139
·期 24
·52332
·
IF 3.057
Xibin Wu,Zhimei Wei,Jie Yang,Gang Zhang,Shengru Long,Xiaojun Wang
The purification of dye wastewater plays a critical role in water pollution treatment. Adsorption is a cheap and effective separation technology but is limited by the reuse of adsorption materials. Ultrafiltration membranes have a relatively high flux but their pores are too large to reject small dye molecules. In this study, negatively charged oxidized poly (arylene sulfide sulfone) (O-PASS) membrane, NMP pretreatment oxidized O-PASS (N-O-PASS) membrane, and O-PASS@UiO-66-NH 2 /O-PASS composite membranes were fabricated to retain cationic methylene blue (MB) from wastewater by combining ultrafiltration and adsorption techniques. The increased porosity of the N-O-PASS membrane provides more available adsorption sites for an equilibrium MB adsorption amount of 22.5 (mg g −1 ) and 100% rejection in the first 10 min during ultrafiltration with a pure water flux of 162.32 (L m −2 h −1 bar −1 ). Due to the enhanced hydrophilicity and separating property by deposited UiO-66-NH 2 particles and PASS resin, O-PASS@UiO-66-NH 2 /O-PASS composite membrane shows a flux of 170.32 (L m −2 h −1 bar −1 ) and a 100% MB rejection in 60 min with great reusability. The O-PASS@UiO-66-NH 2 /O-PASS composite membrane is a new promising membrane for the removal of dyes from wastewater. Meanwhile, the superior solvent resistance endows it great adaptability in wide applications, especially in harsh conditions.
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REACTIVE & FUNCTIONAL POLYMERS
·
2022
·
IF 4.966
Xiaoling Fan,Fei Xin,Wenchao Zhang,Haoyu Liu
A novel phosphorus-containing flame retardant PZN@UiO-66-NH 2 was synthesized by covalent bonding between HCCP and UiO-66-NH 2 , and applied in unsaturated polyester (UPR). The Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron energy spectra (XPS), scanning electron microscopy (SEM) was used to confirm the chemical structure of PZN@UiO-66-NH 2 . The appearance of new P-N-C bond indicated that HCCP was successfully reacted with UiO-66-NH 2 . The thermal stability and the flame-retardant properties of the UPR composites were characterized by thermogravimetric analysis (TGA), limiting oxygen index (LOI) and cone calorimeter test. The limiting oxygen index (LOI) of UPR composite with 4 wt% PZN@UiO-66-NH 2 can reach 23.9%. Compared with pure UPR, the peak heat release rate (PHRR) value, total heat release (THR) value and average effective heat of combustion (av-EHC) value of UPR composite with 4 wt% PZN@UiO-66-NH 2 dropped by 36.53%, 28.70%, 23.50%, respectively. The addition of PZN@UiO-66-NH 2 slightly improved the impact performance of UPR composite. PZN@UiO-66-NH 2 can solve UiO-66-NH 2 's agglomeration dilemma in UPR to some extent.
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Journal of Water Process Engineering
·
2022
·
IF 7.34
JongNam Choe,JongMin Ji,MyongBok Kim,JuHyon Yu,JongYol Ri,KyongSu Ri,HyonIl Kim
In this paper, a novel hydrophilic composite polyethersulfone (PES) ultrafiltration membrane was prepared by blending sunlight response photocatalyst NH 2 -MIL-125 via the phase inversion method. The physical-chemistry performance of membrane was carried out by XRD, FTIR, UV-VIS/DRS, contact angle, and cross-section SEM images. The separation ability, anti-fouling ability, and self-cleaning efficiency of ultrafiltration membrane were analyzed by ultrafiltration experiment using the congo red solution. The results indicate that fouling resistance and the flux recovery ratio of ultrafiltration membrane is significantly improved, and it has higher solar response energy. There was no significant change in the rejection ratio of pollutants before and after illumination. For the pristine PES membrane and the 0.5% NH 2 -MIL-125/PES nanocomposite membrane, the water flux recovery ratio (FRR) could increase from 37.84% to 77.09%, and the R r could increase from 22.22% to 44.09%, and the R ir could decrease from 67.11% to 47.09%. In a conclusion, the addition of NH 2 -MIL-125 at a low concentration could result in membranes with more pure water flux, better rejection, and good fouling resistance compared to the unfilled PES membrane.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
·
IF 4.831
Yuzhu Zhai,Yijing Li,Xiaoke Huang,Juying Hou,Houshen Li,Shiyun Ai
A colorimetric and ratiometric fluorescent dual-mode assay is constructed for sensitive and specific Hg 2+ sensing based on UiO-66-NH 2 and Au composite (UiO-66-NH 2 @Au). The addition of Hg 2+ stimulates the peroxidase-like activity of UiO-66-NH 2 @Au by the formation of Au-Hg amalgam, promoting the oxidizing of chromogenic substrate OPD to DAP with the aid of H 2 O 2 , which lead to the change of colorimetric and fluorescent signals. The absorbance of the sensing system at 450 nm is linear positive correlation with Hg 2+ concentration of 30–1400 nM and the color of the solution under visible light shaded from light yellow to dark yellow. With the increase of Hg 2+ concentration, the fluorescence signal at 570 nm (DAP) increased whereas that at 455 nm (intrinsic fluorescence of UiO-66-NH 2 ) decreased due to inner filter effect (IFE), the fluorescence intensity ratio (F 455 /F 570 ) decreasing linearly with Log [Hg 2+ ] over the range 60–1700 nM; the fluorescence emission of sensing system under UV excitation changed from blue to yellow, which can easily be discerned visually. This assay was successfully applied to the determination of Hg 2+ in tap water and river water. The results indicate that the colorimetric and ratiometric fluorescent dual-mode assay based on UiO-66-NH 2 @Au realized visual determination of Hg 2+ rapidly and reliably, revealed application prospect in Hg 2+ monitoring.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yicheng Ye,Qiaohong Zhang,Guoying Weng,Zhuwei Zhu,Zhenguo Lyu,Chen Chen
The species and amount of the surface groups are closely related with the catalytic performance for a heterogeneous catalyst. High content of alkylamino (50 mol%) and n -propyl (15 mol%) were simultaneously introduced onto the surface of SiO 2 nanospheres with a one step reverse-phase microemulsion method. Accompanying the formation of plenty of surface nano-bulges, a high ratio (86.5 %) of the silicon species were exposed on the surface of this novel material. Abundant of surface groups including Si-NH 2 (5.5 mmol g −1 ), Si-C 3 H 7 (1.7 mmol g −1 ), and Si-OH (6.1 mmol g −1 ) coexisted on the surface enabled this novel material to be a very efficient catalyst for the Aldol condensation reaction between benzaldehyde and n -heptanal. Higher content of alkylamino supplied more catalytic sites. Proper ratio of silanol-to-alkylamino (a little higher than 1) facilitated the adsorption of the substrate molecules and strengthened the cooperation between alkylamino and silanol. Surface hydrophobic modification with n -propyl further facilitated the adsorption of the substrate molecules at the presence of the byproduct of water. Conversion of 99 % was successfully obtained at a lower temperature (90 °C) and in a very short time of 25 min with the present material being used as the catalyst. In some other Aldol condensation reactions, the present catalyst NH 2 -SiO 2 -C 3 H 7 also showed excellent catalytic performance.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 1
·2283-2297
·
IF 5.19
Hu Yuting,Wang Shixing,Zhang Libo,Yang Fan
In wastewater, heavy metal Hg causes serious harm to ecology, so it needs to be removed. In this paper, a novel MOF adsorbent (UiO-66-QU) was prepared by modifying UiO-66-NH 2 with 4-quinolinecarboxaldehyde, which was used to selectively remove Hg(II) from water. The adsorbent was characterized using Fourier transform infrared spectroscopy (FT-IR), field emission scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET), zeta potentiometer, and X-ray photoelectron spectroscopy (XPS). In order to investigate the Hg(II) adsorption performance of UiO-66-QU, the effect of time, initial concentration, pH, and temperature were carried out. Langmuir model fitting shows that the maximum adsorption capacity of UiO-66-QU for Hg(II) is 556 mg/g at 298 K. The experimental results show that UiO-66-QU has better Hg(II) adsorption capacity than UiO-66-NH 2 . The isotherm is in accordance with pseudo-second-order models. It is indicated that the adsorption process is mainly monolayer chemical adsorption. The thermodynamic parameters also indicate that the adsorption process is spontaneous and endothermic. It has excellent reusability and selectivity. XPS and the zeta potential showed that the adsorption mechanism was the complex reaction of Hg(II) with nitrogenous group. Therefore, the adsorbent has potential application prospects in removal of Hg(II) from wastewater.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Jiayou Liu,Xiaoxiang Huang,Linfeng Liu,Qianqian Nie,Zhongchao Tan,Hesheng Yu
UiO-66 variants are widely used for photocatalysis and adsorption, but few studies reported their combined effects in one process. This paper reports that the mechanism behind NO removal using UiO-66-NH 2 includes photocatalytic oxidation and subsequent adsorption. First, the UiO-66-NH 2 was selected out of UiO-66-X variants (X = H, NH 2 , NO 2 , OH, Br, Br 2 ) because of its high NO removal efficiency ( i.e ., 80.54%), which is 8.55–64.95 times higher than those of other UiO-66 variants. Then, the NO reaction pathway and degradation mechanisms are proposed based on the experimental results and theoretical calculations. In an anhydrous environment, the NO removal efficiency increases from 80.54% at 40–60% of humidity to 96.23%. Moreover, NO 2 emissions and catalyst deactivate are not observed. These findings indicate that the photocatalytic NO degradation includes the photocatalytic oxidation of NO into NO 2 on the surface of UiO-66-NH 2 and subsequent NO 2 adsorption in micropores. The reason is that the formation of NO x - ions without H 2 O is theoretically impossible according to the principle of electroneutrality. In-situ DRIFTS also confirms the mechanism. Furthermore, density functional theory (DFT) and grand canonical Monte Carlo (GCMC) simulations were carried out to understand the improved NO removal caused by synergistic photocatalysis and adsorption. In summary, this work proposes a new mechanism for NO removal that combines the photocatalytic oxidation and adsorption capability of UiO-66-NH 2 , the new mechanism provides a new strategy to further improve the NO removal efficiency of UiO-66-NH 2 and a new way of inhibiting the deactivation.
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Journal of CO2 Utilization
·
2022
·
IF 8.321
Nicui Yuan,Yuxin Mei,Yuwei Liu,Yating Xie,Baining Lin,Yonghua Zhou
The development of efficient and highly selective photocatalysts is a key point for the photocatalytic conversion of CO 2 . In this paper, a composite catalyst UiO-66-NH 2 /Ce(HCOO) 3 (simplified to UNH/Ce(HCOO) 3 ) was fabricated by one pot method with CeCO 3 OH as the precursor. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) characterizations results confirmed that UNH was dispersed on the surface of Ce(HCOO) 3 and strongly interacted with it via Ce-N bond. The yield of CH 4 on the optimal UNH/Ce(HCOO) 3 catalyst reached 3 times of that on pristine UNH, up to 128.81 μmol g −1 , with the CH 4 selectivity of 71.9 %, and the R electron reached 286.46 μmol g −1 h −1 . The UV–vis diffuse reflection spectra and photoelectrochemical tests results confirmed that the improved photocatalytic CO 2 reduction performance and high CH 4 selectivity could be attributed to the formation of the type-Ⅱheterojunction of UNH/Ce(HCOO) 3 with abundant Ce 3+ , which expanded the visible light absorption range, accelerated the separation and transfer rates of photogenerated charges, and thus efficiently promoted the multi-electron reduction reaction of CO 2 to CH 4 . In addition, the reaction temperature affected profoundly the cycle performance of the catalyst. The results presented here illustrated the possibility for improving the stability of UNH/Ce(HCOO) 3 -1.80 by decreasing reaction temperature.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Shao-zhong Hu,Ting Huang,Nan Zhang,Yan-zhou Lei,Yong Wang
The discharge of wastewater rich in heavy metals and organic substances has led to the deterioration of the ecosystem, resulting in serious environmental and food pollution, and there is an urgent need to treat the pollutants in the wastewater. Metal organic frameworks (MOFs) have the advantages of large specific surface area and pore volume, as well as the designability of their structures, and are extremely promising materials for wastewater treatment. In this work, a novel adsorbent was synthesized by grafting polyethyleneimine (PEI) onto the UiO-66-NH 2 metal framework (PEI@UiO-66-NH 2 ) via glutaraldehyde-assisted reaction. This new type of adsorbent not only exhibits improved chemical stability in water but also shows greatly increased adsorption sites in comparison with the common UiO-66-NH 2 . The various factors that possibly affect the adsorption behaviors of the PEI@UiO-66-NH 2 were systematically studied. The results show that the PEI@UiO-66-NH 2 can nearly reach the adsorption equilibrium of Pb(II) and methyl orange (MO) within 5 min. The theoretical adsorption capacities toward Pb(II) and MO achieve 692.80 mg/g and 497.51 mg/g, respectively. Specifically, the dynamic theoretical adsorption models were established through the study of the dynamic adsorption of pollutants, providing the theoretical guidance for the scale-up experiments of wastewater treatment with this adsorbent. PEI@UiO-66-NH 2 also shows excellent recycling performance for removing Pb(II) and MO. All these results suggest that PEI@UiO-66-NH 2 has a good application prospect for the removal of wastewater containing Pb(II) and MO.
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Food Analytical Methods
·
2022
·Vol. 15
·期 10
·2830-2839
·
IF 3.498
Tang Jing,Li Jie,Liu Tianna,Tang Wenjing,Li Nali,Zheng Shengbiao,Guo Jiahao,Song Changchun
Electrochemical determination of tert-butylhydroquinone (TBHQ) is vital to food safety due to negative health effects; however, bare electrode of traditional electrochemical sensors generally has a narrow linear range and low sensitivity, limiting their practical application. Accordingly, the nano-architecture fabricated with N-doped TiO 2 –carbon nano-composites (TiO 2 /NC) is prepared by the thermolysis of NH 2 functionalized MIL-125(Ti) metal–organic frameworks (NH 2 -MIL-125(Ti)). TiO 2 /NC composites are firstly developed as the electrochemical material for electrochemical determination of TBHQ. The TiO 2 /NC composites with a highly porous structure, excellent conductivity and electron transportation, and large surface area show remarkable electrochemical oxidation ability for TBHQ. Under optimal conditions, TiO 2 /NC composite-modified electrode presents a broader linear response to TBHQ concentration of 0.05–100 μM with the detection limit as low as 4 nM (S/N = 3). Finally, the sensor platform is implemented directly to determine TBHQ in edible oil for evaluation of its practical application. TiO 2 /NC composites sensor fabricated perform larger linear range with high sensitivity and anti-interference properties, which can be used as a potential for electrochemical determination of TBHQ.
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