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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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 1
·2283-2297
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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
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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
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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
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2022
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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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ACS Applied Materials & Interfaces
·
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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JOURNAL OF HAZARDOUS MATERIALS
·
2021
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IF 10.588
Muhammad Zahid,Dongxiang Zhang,Xiyan Xu,Meng Pan,Muhammad Hammad ul haq,Alemtsehay Tesfay Reda,Wenguo Xu
Efficient iodine gas capture is necessitated in many industries like spent nuclear fuel off-gas treatment in view of environmental protection and resource recycling. However, the adsorption efficiency and stability of the current adsorbents are limited. In the present work, efficient and stable barbituric and thiobarbituric acid-based UiO-66-NH 2 adsorbents (i.e., UiO-66-NH-B.D and UiO-66-NH-T.D, respectively) have been synthesized by post-synthetic covalent modification. Characterization approaches, including SEM-EDS, TEM , XRD, FTIR, XPS, 1 H NMR, TGA and BET, are used to obtain information on the properties and adsorption mechanisms of these metal-organic framework (MOF) adsorbents. The kinetics and mechanisms involved are studied in detail. The treatment efficiency and recyclability of the adsorbents are checked and compared with the adsorbents reported in previous works. The results show that the current adsorbents are potentially suitable for efficient iodine gas capture. High maximum iodine adsorption amount by UiO-66-NH-B.D and UiO-66-NH-T.D (1.17 and 1.33 g/g) was achieved under 75 °C. These new adsorbents are thermally stable for iodine adsorption and regenerated and reused with good performance. The adsorption mechanisms were revealed based on experimental results, indicating that iodine is adsorbed by both physisorption and chemisorption .
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ANALYTICAL CHEMISTRY
·
2020
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IF 6.785
Yuqiang Xiang,Huaduo Yan,Bingjie Zheng,Aroosha Faheem,Yonggang Hu
High-throughput analyses of multitarget markers can facilitate rapid and accurate clinical diagnosis. Suspension array assays, a flow cytometry-based analysis technology, are among some of the most promising multicomponent analysis methods for clinical diagnostics and research purposes. These assays are appropriate for examining low-volume, complex samples having trace amounts of analytes due to superior elimination of background. Physical shape is an important and promising code system, which uses a set of visually distinct patterns to identify different assay particles. Here, we presented a morphology recognizable suspension arrays based on the microorganisms with different morphologies. In this study, UiO-66-NH2 (UiO stands for University of Oslo) metal–organic frameworks (MOFs), was wrapped on the microorganism surface to form an innovative class of microorganism@UiO-66-NH2 composites for suspension array assays. The use of microorganisms endowed composites barcoding ability with their different morphology and size. Meanwhile, the UiO-66-NH2 provided a stable rigid shell, large specific surface area, and metal(IV) ions with multiple binding sites, which could simplify the protein immobilization procedure and enhance detection sensitivity. With this method, simultaneous detection of three colorectal cancer-related microRNA (miRNA), including miRNA-21, miRNA-17, and miRNA-182, could be easily achieved with femtomolar sensitivity by using a commercial flow cytometer. The synergy between microorganisms and MOFs make the composites a prospective barcoding candidate with excellent characteristics for multicomponent analysis, offering great potential for the development of high throughput and accurate diagnostics.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2019
·
IF 1.795
Jiajia Sun,Sheng Feng,Shanshan Feng
A novel ternary heterojunction MWCNT/N-TiO 2 /UiO-66-NH 2 was synthesized by in-situ solvothermal-hydrothermal approach, showing superior photocatalytic degradation of KET under visible-light irradiation. The optimal MWCNT/N-TiO 2 /UiO-66-NH 2 (3:7) composite exhibits the highest degradation efficiency of KET (96%) in 120 min in comparison with pristine TiO 2 , N-TiO 2 , MWCNT , UiO-66-NH 2 and MWCNT/N-TiO 2 . The improved photocatalytic activity of MWCNT/N-TiO 2 /UiO-66-NH 2 can be ascribed to its improved visible-light absorption range, the large specific surface area based on UiO-66-NH 2 as well as the formation of an effective heterojunction. The formed ternary composite facilitates the separation and transfer of photoexcited charge carrier, which is confirmed from the results of PL. The photocatalytic mechanism is further proposed based on the trapping experiment, and the transfer process of photoinduced electron-hole pairs is discussed. This work provides an effective strategy for designing a new ternary photocatalytic system toward degradation of organic pollutants.
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RSC Advances
·
2023
·Vol. 13
·期 50
·35078-35087
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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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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 40
·18865-18871
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IF 3.3
Chao Liu,Gang-Gang Chang,Ting-Ting Luo,Yi-Tian Wang,Shi-Tian Xiao,Yao Yao,Hong-Jian Xu,Ge Tian,Christoph Janiak,Hai-Hu Yu,Xiao-Yu Yang
Metal–organic frameworks (MOFs) have great potential for producing photoelectrocatalyzed hydrogen and degrading pollutants, owing to several factors such as high porosity and tunable semiconductor-like properties. Wide band gaps, which restrict their use to only UV light induced reactions, and low efficiencies for the separation of photogenerated charge carriers (electrons and holes) pose significant challenges to the widespread applications of MOFs. In this study, a hierarchical hollow Pt@H-UiO-66-NH2/CdS ternary catalyst was designed and synthesized. The immobilized CdS nanoparticles (NPs) in this catalyst endow the MOF H-UiO-66-NH2 with high visible light absorption ability and the Pt NPs serve as electron sinks to improve charge carrier separation. Furthermore, the hierarchical hollow structure of H-UiO-66-NH2 in the composite contributes to boosting light absorption and shortening the distance for charge transfer. As a proof of principle, Pt@H-UiO-66-NH2/CdS catalyzes methylene blue (MB) degradation with a high rate constant of 1.025 × 10−2 and hydrogen production with a rate of 12 810 μmol g−1 h−1, the latter of which is about 2.3, 11.7 and 173 times higher than those of Pt@UiO-66-NH2/CdS, H-UiO-66-NH2/CdS and Pt@H-UiO-66-NH2, respectively.
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