ACS Applied Materials & Interfaces
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2022
·
IF 10.383
Si-Yuan Fang,Ji-Lai Gong,Lin Tang,Wei-Cheng Cao,Juan Li,Zi-Kang Tan,Yu-Wen Wang,Wen-Bo Wang
Thin-film nanocomposite (TFN) membranes with efficient molecular separation and organic solvent resistance are active in demand in wastewater treatment and resource reclamation, meeting the goal of emission peaks and carbon neutrality. In this work, a simple and rational design strategy has been employed to construct a sandwich-structured membrane for removing fluoroquinolone antibiotics and recycling organic solvents. The sandwich-structured membrane is composed of a porous substrate, a hydrophilic tannic acid–polyethyleneimine (TA–PEI) interlayer, and a polyamide (PA) selective layer decorated with metal–organic framework (PA-MOF). Results manifest that the hydrophilic TA–PEI interlayer played a bridging and gutter effect to achieve effective control in amide storage, amine diffusion, and nanomaterial downward leakage at the immiscible interface. The PA-MOF selective layer has been changed to a loosely crumpled surface, endowing functionalities on the sandwich-structured membrane that included limited pores, strengthened electronegativity, and stronger hydrophilicity. Thus, an enhanced water flux of 87.23 ± 7.43 LMH was achieved by the TFN-2 membrane (0.04 mg·mL–1 UiO-66-NH2), which is more than five times that of the thin-film composite membrane (17.46 ± 3.88 LMH). The rejection against norfloxacin, ciprofloxacin, and levofloxacin is 92.94 ± 1.60%, 94.62 ± 1.29%, and 96.92 ± 1.05%, respectively, effectively breaking through the “trade-off” effect between membrane permeability and rejection efficiency. Further antifouling results showed that the sandwich-structured membrane had lower flux decay ratios (3.36∼7.07%) and higher flux recovery ratios (93.40∼98.40%), as well as superior long-term stability after 30 days of filtration. Moreover, organic solvent resistance testing confirms that the sandwich-structured membrane maintained stable solvent flux and better recovery rates in ethanol, acetone, isopropanol, and N,N-dimethylformamide. Detailed nanofiltration mechanism studies revealed that these outstanding performances are based on the joint effect of the TA–PEI interlayer and PA-MOF selective layer, proposing a new perspective to break through the bottleneck of nanofiltration application in a complex environment.
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ANALYTICAL CHEMISTRY
·
2022
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IF 8.008
Liuying He,Xiao Wang,Junyu Chen,Yuze Li,Liping Wang,Caiqiao Xiong,Zongxiu Nie
Liver cancer (LC) is the third frequent cause of death worldwide, so early diagnosis of liver cancer patients is crucial for disease management. Herein, we applied NH2-coated polystyrene@Fe3O4 magnetic beads (PS@Fe3O4–NH2 MBs) as a matrix material in laser desorption/ionization mass spectrometry (LDI-MS). Rapid, sensitive, and selective metabolic profiling of the native biofluids was achieved without any inconvenient enrichment or purification. Then, based on the selected m/z features, LC patients were discriminated from healthy controls (HCs) by machine learning, with the high area under the curve (AUC) values for urine and serum assessments (0.962 and 0.935). Moreover, initial-diagnosed and subsequent-visited LC patients were also differentiated, which indicates potential applications of this method in early diagnosis. Furthermore, among these identified compounds by FT-ICR MS, the expression level of some metabolites changed from HCs to LCs, including 29 and 12 characteristic metabolites in human urine and serum samples, respectively. These results suggest that PS@Fe3O4–NH2 MBs-assisted LDI-MS coupled with machine learning is feasible for LC clinical diagnosis.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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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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REACTIVE & FUNCTIONAL POLYMERS
·
2022
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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
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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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JOURNAL OF APPLIED POLYMER SCIENCE
·
2022
·Vol. 139
·期 24
·52332
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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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Polymers
·
2022
·Vol. 14
·期 2
·283
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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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OPTICAL MATERIALS
·
2023
·
IF 3.9
Siyue Wang,Xiaoman Teng,Chao Liu,Hanfei Zhu,Hongbu Cheng,Jing Yan,Li Wang,Zhenyan Liang,Jun Ouyang
Due to a synergistic effect of piezo-catalysis and photocatalysis , piezo-photocatalysis is gaining popularity as an effective approach to remove organic pollutants. In this work, single-component piezo-photocatalytic nanoparticles of UiO-66-NH 2 (Hf) metal-organic frameworks were prepared by a hydrothermal process with an average diameter of ∼52.6 nm. An ultrafast piezo-photocatalysis degradation of RhB solution was achieved by using the UiO-66-NH 2 (Hf) nanoparticles . Under UV light and ultrasound irradiation, the percentage of dye degradation for an initial RhB concentration of 5 mg/L reached 91 % in 60 s. The removal mechanism of RhB was investigated via capture experiments of active species, which revealed that the hydroxyl radicals and hole play a key role in the degradation of RhB. This work provides a reference for the piezo-photocatalytic capability and the underlying mechanism of single-component metal-organic framework based nanomaterials , promoting their further development in technological applications involving highly efficient catalysts.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 46
·21505-21512
·
IF 3.3
Yuhao Lu,Tao Wang,Chengshun Tang,Qijian Niu,Tianyan You
Oxytetracycline (OTC) residues in the environment seriously endanger ecosystems and human health. Hence, it is critical to develop a selective and sensitive sensor for trace OTC detection. In this work, a facile and highly selective colorimetric aptasensor was constructed for OTC detection by the surface electrostatic assembly between aptamers and Fe-MOFs. Due to the steric effects and the decrease in the electron transfer rate, the peroxidase-like activity of NH2-MIL-88B was significantly inhibited after the adsorption of aptamers. Furthermore, the selective binding between aptamers and OTC triggered the release of aptamers from the surface of NH2-MIL-88B, which led to the reactivation of peroxidase-like activity. The colorimetric aptasensor exhibited a satisfactory detection range (1.0 × 10−10 M to 3.0 × 10−7 M) and the limit of detection (LOD) was as low as 1.9 × 10−11 M. Additionally, the colorimetric aptasensor was successfully used to detect OTC in real samples. The developed colorimetric aptasensor provided an important reference value for the sensitive detection of other antibiotics in the environment.
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RSC Advances
·
2023
·Vol. 13
·期 50
·35078-35087
·
IF 3.9
Yi Liu,Zhipeng Yuan,Yanrong Chen
Excessive accumulation of bilirubin in patients with hyperbilirubinemia can lead to tissue and organ damage and neurological diseases, and is even life-threatening in severe cases. Hemoperfusion is an effective method for removing bilirubin, but clinically used hemoperfusion adsorbents have unsatisfactory adsorption capacity and kinetics. In order to obtain a safe and efficient bilirubin adsorbent, Zr-based Metal–Organic Framework (MOF) material UiO-66 with high specific surface area and aqueous medium stability was prepared and modified with varying degrees of amination to improve its adsorption capacity. According to adsorption experiments in aqueous solution and simulated plasma, it was confirmed that the unsaturated coordinated zirconium in UiO-66 can effectively induce the aggregation and precipitation of free bilirubin unbound to albumin and the amino group on UiO-66-NH2 has a strong affinity for albumin bound bilirubin. The adsorption effect of UiO-66-NH2 with a high degree of amino modification is significantly stronger than that of UiO-66-NH2 with a low degree of modification. In simulated plasma with a bilirubin concentration of 40 mg dL−1, the adsorption capacities of UiO-66 and UiO-66-NH2-1.9 can reach 69.08 mg g−1 and 81.13 mg g−1. The adsorption isotherm fitting and adsorption kinetics fitting results also show that UiO-66 and UiO-66-NH2 are good adsorbents for bilirubin. In dynamic adsorption, the adsorbents also showed good performance and did not affect the protein in the plasma. The hemolysis test, coagulation time test, and cytotoxicity test confirmed that the bilirubin adsorbents based on UiO-66 and UiO-66-NH2 have good blood compatibility and biocompatibility. This study provides new ideas for the development of a novel bilirubin adsorbent and a theoretical basis for the study of bilirubin adsorption mechanisms.
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International Journal of Low-Carbon Technologies
·
2023
·
IF 2.3
Wang Tingting,Yue Xiaoju,Han Lin,Wang Jinnong,Zhang Yuzhen,Tang Xiaofeng,Wang Shifeng
We reported anchoring mesoporous silica onto the microporous metal–organic frameworks (MOF) (UiO-66-NH2) to obtain a hierarchical porous framework (UiO-66-NH2@SiO2). This strategy maintains the high specific surface area (SA) of the MOF and addresses the mass transfer issue frequently encountered in microporous materials, providing more possibilities for subsequent modified structural frameworks. The structural characteristics of UiO-66-NH2@SiO2 were evaluated by Fourier transform infrared spectroscopy, X-ray diffraction, thermogravimetric analysis, scanning electron microscopy, surface analysis and X-ray photoelectron spectroscopy. In this work, the specific SA of the composite material was 196.667 m2/g, which decreased due to the occupation of some pores by anchored silica. Adsorption experiments showed that the composite material had a better adsorption effect (Congo red, 393.83 mg/g; bromophenol blue, 446.46 mg/g) than UiO-66-NH2, with electrostatic interaction and hydrogen bonding being the main driving forces. Therefore, this is a material that has a positive impact on dye adsorption. The strategy proposed in this work has potential applications not only in the construction of new materials but also in the exploration of dye adsorbents.
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Journal of Physical Chemistry C
·
2023
·
IF 3.7
Huan-Yu Chen,Xing-Biao Liu,Qi-Xin Guan,Can-Jun Zou,Ping-Ping Fang
The detection of antibiotics has attracted great attention among scientists and health researchers in the past decades. However, it is still difficult to realize the sensitive and selective detection of antibiotics with similar structures. Herein, the antibiotic molecules of oxytetracycline (OTC) can be sensitively and selectively detected by surface-enhanced Raman spectroscopy (SERS) on NH2–UiO-66(Zr)@Au nanoparticles (NPs). The SERS substrate of NH2–UiO-66(Zr)@Au NPs realizes a detection sensitivity of 1 × 10–12 g·L–1 for 4-mercaptobenzoic acid, indicating its high SERS activity. A high detection sensitivity of 10–11 g·L–1 is obtained for OTC on such a SERS substrate. Besides the high sensitivity, NH2–UiO-66(Zr)@Au NPs can also selectively detect OTC from streptomycin sulfate, salicylic acid, and ofloxacin by SERS on NH2–UiO-66(Zr)@Au NPs, with a selective detection limit of 10–10 g·L–1. Furthermore, OTC can be selectively detected in a real sample of river water with a detection limit of 1.0 × 10–10 g·L–1. Therefore, this study provides an effective way to enrich and detect antibiotics in real samples in the environment.
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