DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 6
·2567-2576
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IF 4.569
Aijia Gao,Fangfang Li,Zhi Xu,Changchun Ji,Jing Gu,Ying-Hua Zhou
The development of heterogeneous catalysts for promoting epoxide cycloaddition with carbon dioxide is highly desirable for recycling CO2 and achieving the goal of carbon neutrality. Herein, we designed and synthesized Zr-based metal organic frameworks (MOFs) by implanting functional guanidyl into the framework via mixing different molar ratios of 4-guanidinobenzoic acid (Gua) with 1,4-benzenedicarboxylic acid (BDC). Consequently, a small sized Zr-MOF (∼350 nm) can be prepared by implanting Gua with 20% molar ligands, denoted as UiO-66-Gua0.2(s). Compared to large sized and different guanidyl Zr-MOFs, UiO-66-Gua0.2(s) exhibited an optimal activity on catalyzing epoxide cycloaddition with CO2 in the presence of the Bu4NBr cocatalyst. A yield of 97% for the product of chloropropene carbonate was achieved at 90 °C under 1 atm CO2. The great performance of UiO-66-Gua0.2(s) might be attributed to the synergistic effect of guanidyl groups as hydrogen-bond donors and Zr centers acting as Lewis-acidic sites. In addition, the heterogeneous catalyst of UiO-66-Gua0.2(s) exhibited a great versatility towards converting other epoxides and a satisfactory recyclability for five consecutive runs. Moreover, a plausible reaction mechanism has been proposed for UiO-66-Gua0.2(s) in promoting CO2 epoxide cycloaddition reactions.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Lili Ma,Xueting Feng,Fanghui Cai,Chunyu Sun,Hanming Ding
Metal-organic frame materials are intensively investigated in catalysis due to their outstanding thermal stability, large specific surface area, and ultra-high porosity. In this work, a cobalt-doped zirconium-based metal-organic framework, Co-UiO-66, was synthesized by the hydrothermal approach. Co-UiO-66 could successfully activate peroxymonosulfate (PMS) ions to produce reactive oxygen species for the degradation of rhodamine B (RhB) when it was used as a Fenton-like catalyst. The catalyst with 4% Co in mass in UiO-66 (4% Co-UiO-66) showed the highest degradation efficiency. About 97.3% of RhB (50 ml of 30 mg L −1 ) was degraded in 45 min under simulated sunlight when 10 mg of 4% Co-UiO-66 was used. The degradation efficiency was much higher than that when pure UiO-66 was used. Furthermore, it was even slightly higher than when cobalt ions were used as the activator. The single-atomic dispersion and confinement effect in Co-UiO-66, as well as the strong absorption in the visible light region are responsible for the high catalytic efficiency.
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LANGMUIR
·
2022
·
IF 4.331
Fa-Ting Xie,Yu-Long Li,Tong Yang,Yun-Hui Yang,Rong Hu
Electrochemical nanotags with strong signal input are necessary for a ratiometric electrochemical sensor to overcome the drawbacks of inaccurate detection results. In this paper, the metal–organic framework (MOF) UiO-66 was utilized as an electrochemical signal tag. A stable and strong current response at +0.9 V can be detected in neutral conditions. MicroRNA (miRNA) was employed as the model analyte. Herein, an enzyme-free DNA-walker-based ultrasensitive ratiometric electrochemical biosensor in combination with Zr MOF (UiO-66) signal tags to detect miRNA was demonstrated. In the presence of miRNA, the autonomous walker movement can be initiated by miRNA, leading to the release of biotin-modified fragments. Thus, streptavidin-labeled UiO-66 nanomaterials were not bound to the electrode, generating a low signal response of UiO-66 at +0.9 V. However, the current signal of electrolyte solution as reference at +0.2 V was increased due to the enhancement of electrode conductivity. This ratiometic sensor demonstrated high sensitivity, selectivity, and reproducibility. It can eliminate the disturbance of environmental factors and basic electrode characteristics, providing more accurate signals. A limit of detection (LOD) of 0.17 fM was achieved. Moreover, the method was also used to detect miRNA-21 spiked in real serum samples.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Ruyi Geng,Huanhuan Jia,Youwei Xie,Dahai Pan,Feng Yu,Binbin Fan
UiO-66 supported metal catalysts have shown high catalytic activity and selectivity to cinnamyl alcohol (COL) in the selective hydrogenation (SHYD) of cinnamaldehyde (CAL), but the roles of missing-linker defects (MLDs) in UiO-66 on the catalytic performance of the UiO-66 supported metal catalysts have less been reported. Here, UiO-66 supports with the different amount of MLDs were used as the supports, and three series of UiO-66 supported Pt (Pt/U) catalysts were prepared by sol-impregnation, wet-impregnation as well as in-situ encapsulation methods, respectively. The influences of the MLDs in UiO-66 on the catalytic properties of the prepared Pt/U catalysts in the SHYD of CAL were investigated. The series of Pt/U-720 catalysts with the more MLDs showed higher CAL conversion and selectivity to COL than the corresponding Pt/U-F catalysts with fewer MLDs. The different preparing methods affect the location and dispersion of Pt species on UiO-66 supports and the metal-support interaction, but the location of the supported Pt species on UiO-66 is the critical factor affecting the catalytic properties of Pt/U catalysts. The presence of the MLDs in UiO-66 is the key to preparing UiO-66 supported Pt catalysts with high SHYD performance.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2022
·Vol. 139
·期 31
·e52724
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IF 3.057
Chunhui Du,Jintai Hu,Fen Chen
Polypropylene (PP) porous flat membrane is ultrathin and has high porosity, which is suitable for the support of forward osmosis (FO) membrane. However, its high hydrophobicity is its Achilles heel. In this study, dopamine and UiO-66-NH 2 were co-deposited onto the surface of PP support, and then interfacial polymerization was performed to fabricate a thin-film nanocomposite (TFN) FO membrane. The reaction-generated polydopamine improved the hydrophilicity of PP membrane, and at the same time enhanced the adhering of UiO-66-NH 2 to the support. The experimental results indicated that the UiO-66-NH 2 nanoparticles were anchored evenly on the surface of the support, which improved the water flux of FO membrane from 11.1 LMH (TFC, TFN-0 without UiO-66-NH 2 ) to 20.7 LMH (TFN-0.1, with 0.1 wt% UiO-66-NH 2 ) using 1 mol/L NaCl as the draw solution in FO mode. Compared with TFC membrane, TFN-0.1 membrane also exhibited relative lower specific salt flux (~0.252) and structural parameter (~379 μm). When separating sodium alginate foulant, the normalized water flux recovery ratio of TFN-0.1 was remained 0.89, and most of the fouling was reversible, as for TFC membrane the data decreased to 0.76 after 2 cycles of operation. These results suggested that UiO-66-NH 2 modified FO membrane exhibited good permeation and antifouling property.
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Journal of Cleaner Production
·
2021
·
IF 9.297
Zijie Wang,Yannan Jia,Weikun Song,Xiaoqin Li,Kai Xu,Zheng Wang
The removal of boron in desalinated seawater has always been one of the keys to restrict the use of desalinated seawater. For this reason, a composite adsorbent named UiO-66-NH 2 /GO was successfully prepared by a simple solvothermal method through this research. It is composed of graphene oxide and water-stable metal organic framework UiO-66-NH 2 , and for the first time as a boron adsorbent for the treatment of desalinated seawater. Various technologies were applied to systematically analyze the stability, structure, topography and chemical characteristics of the composite adsorbent. The relationship between the influencing factors and the adsorption effect was investigated, including the amount of adsorbent, contact time, initial concentration of boron, and pH of the boron solution. It is proved that the boron adsorption complies the pseudo-second-order kinetic model , the intra-particle diffusion model and the Langmuir isotherm model through the fitting of experimental results. The adsorption of boron by UiO-66-NH 2 /GO has both physical and chemical adsorption , including electrostatic attraction , covalent bond or electron transfer . The results of thermodynamic study pointed out the adsorption of boron is spontaneous and feasible. The response surface method was designed to improve the adsorption conditions of boron. The optimized adsorption conditions to reach 26.45 mg/g of boron adsorption were found to be at dosage of 75.03 mg/g with pH of 5 and temperature of 321.19 k. UiO-66-NH 2 /GO showed good removal ability for low concentration boron and good reusability . The above suggest that UiO-66-NH 2 /GO has the potential to be applied to desalinated seawater treatment.
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RSC Advances
·
2020
·Vol. 10
·期 68
·41283-41295
·
IF 3.119
Ahmed S. Abou-Elyazed,Yinyong Sun,Ahmed M. El-Nahas,Ahmed M. Yousif
Recently, the incorporation of hydrophobicity on the surface of UiO-66(Zr) has received much attention due to the deactivation of hydrophilic active sites of UiO-66(Zr) upon water adsorption. In this work, we report UiO-66(Zr) catalysts with an assortment of surface hydrophobicities fabricated by the solvent-free method to elucidate the impact of the environment framing Lewis acid sites on their catalytic activity in the production of fatty acid methyl ester (biodiesel) via the esterification of fatty acids at room temperature with high selectivity (100%) and good recyclability. A detailed structural analysis of the materials by N2 sorption, FT-IR, SEM, XRD, water contact angle measurement, dynamic liquid scattering (DLS), NMR and TGA revealed the fabrication of stearic acid-grafted UiO-66(Zr) catalysts (10SA/UiO-66) with fine particle size and a highly hydrophobic network. 10SA/UiO-66(Zr) with enhanced hydrophobicity exhibited superior catalytic performance in the esterification of a fatty acid with a long alkyl chain compared with conventional solid acid catalysts and even liquid acid catalysts. Detailed kinetic studies corroborated that the adsorption of lipophilic acids at the Lewis acid sites besides the enhancement of wettability between the reactants was facilitated by the hydrophobic environment, thus significantly motivating the esterification reaction at room temperature. Furthermore, 10SA/UiO-66(Zr) showed good catalytic activity in the esterification of oleic acid in the presence of water (∼10% in the light of acid weight).
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Xiaoxue Zhao,Linlin Sun,Xian Jin,Mengyang Xu,Shikang Yin,Jinze Li,Xin Li,Dong Shen,Yan Yan,Pengwei Huo
Z-scheme heterojunction can effectively separate photo-generated carriers and enhance photocatalytic activity of CO 2 reduction. In this work, we report indirect Z-scheme heterojunction of UiO-66-NH 2 /Cu 2 O/Cu, which achieves highly CO 2 photocatalytic conversion to CO. Among these, UiO-66-NH 2 /Cu 2 O/Cu-0.39 (U/C/Cu-0.39) displays the best activity with a CO yield of 4.54 μmol·g −1 ·h −1 , which is 37.8 times higher than that for UiO-66-NH 2 and 50.4 times higher than that for Cu 2 O. Cu not only acts as the electron conductor of the indirect Z-scheme heterojunction to promote the charge carrier transmission, but also acts as the active site of CO 2 reduction. The increase of active sites and the CO 2 adsorption capacity results in the superior photocatalytic performances.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Jiali Tang,Yingbi Chen,Minghu Zhao,Shixing Wang,Libo Zhang
A novel metal-organic framework (UiO-66-PTC) for efficient removal of Pb 2+ ions from wastewater has been prepared by using 4-phenyl-3-thiosemicarbazide as the modifier. Various characterizations showed that UiO-66-PTC was successfully synthesized. The absorption results showed that the maximum adsorption capacity of Pb(II) is 200.17 mg/g at 303 K and optimal pH 5. The adsorption kinetic follows the pseudo-second-order model and the adsorption isotherms fit the Langmuir model. This shows that Pb(II) is a single-layer adsorption on the surface of the adsorbent and the rate-controlling step is chemical adsorption . The thermodynamic results show that the adsorption process can proceed spontaneously, belong to the exothermic reaction . The adsorbent can selectively uptake lead ions from wastewater containing multiple interfering ions. After four adsorption and desorption cycles, the adsorption efficiency is still high. The adsorption mechanism of Pb(II) on the adsorbent is mainly through the chelation of Pb(II) with N and S atoms. These results indicate that UiO-66-PTC is an effective material for efficiently and selectivity removal of Pb(II) from solution, which is of practical significance.
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Biomaterials Science
·
2021
·Vol. 9
·期 7
·2647-2657
·
IF 6.843
Xiaojuan Wang,Xuejian Zhou,Kai Yang,Qiong Li,Rongxin Wan,Guoying Hu,Jin Ye,Yue Zhang,Jiahui He,Hanqing Gu,Yongfang Yang,Lei Zhu
In this study, UiO-66-NH2 metal–organic framework (MOF) nanoparticles with peroxidase and oxidase mimetic activities were incorporated into a chitosan (CS) matrix by a simple and environmentally friendly method. The UiO-66-NH2/CS composite membrane possesses the peroxidase mimicking activity in the presence of traces of H2O2, thus resulting in good antibacterial properties. Intriguingly, 30 min of UV pre-irradiation of the UiO-66-NH2/CS composite membrane, in the absence of H2O2, still leads to a good antibacterial activity. This was attributed to the oxidase mimetic activity and the peroxidase mimicking activity of UiO-66-NH2. In such a way, the side effects of direct exposure to UV irradiation and H2O2 can be avoided for wound-healing treatments. The antibacterial mechanism was further proved by antibacterial experiments, TMB·2HCl color development experiments, reactive oxygen species generation tests and electron spin resonance tests. As a potential medical antibacterial dressing, in vitro membranes were also investigated.
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CHEMICAL PHYSICS
·
2021
·
IF 2.348
Xingchang Tang,Yongwei Luo,Zhijian Zhang,Wanwu Ding,Dexue Liu,Jingchuan Wang,Li Guo,Ming Wen
The high surface areas and tunable properties of Zr-based MOFs make them as attractive materials for gas capture, storage, and separation. In this work, UiO-66, one kinds of Zr-based MOFs, functionalized by single or binary –NO 2 and –NH 2 groups are synthesized. Water adsorption ability and hydrophilicity of UiO-66 and functionalized UiO-66-X were investigated. It is found that surface area of UiO-66 is decreased after introducing functional groups, while hydrophilicity of UiO-66 increased after functionalized with –NO 2 and –NH 2 . Therefore, after balance the effects of surface area and hydrophilicity, UiO-66-NH 2 shows the best water adsorption propriety.
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2020
·Vol. 2020
·期 10
·833-840
·
IF 2.529
Ruiping Wei,Jingdeng Fan,Xumin Qu,Lijing Gao,Yuanfeng Wu,Zongqi Zhang,Feng Hu,Guomin Xiao
Graphical Esterification of levulinic acid with ethanol was catalyzed by the cooperative effects between the Lewis acid sites offered by unsaturated Zr 6 nodes and Brønsted acid sites supplied by OH in defective UiO-66 MOFs with high defect density, which was tuned by precursor ratios and modulators. Due to their high stabilities and tunable defects, zirconium terephthalate UiO-66 type metal organic frameworks (MOFs) have been promising catalysts in many catalytic reactions. The catalytic activity of UiO-66 MOFs is significantly affected by the density of defects and hydroxyl groups bonded to Zr 6 nodes, which can be tuned by modulators. In this work, a series of defective UiO-66 were synthesized via tuning the ratio of H 2 BDC/Zr and adding monocarboxylic acids with different chain length as modulators. The synthesized UiO-66 MOFs were characterized by powder X-ray diffraction, N 2 physisorption, IR and 1 H NMR spectroscopy, scanning and transmission electron microscopy. Esterification of levulinic acid with ethanol was selected to reveal the influence of modulators, defects and hydroxyl groups. The results showed that UiO-66 with 0.5 of H 2 BDC/Zr ratio and lauric acid as the modulator owned excellent catalytic activity. The cooperative effects, between the Lewis acid sites offered by unsaturated Zr 6 nodes and Brønsted acid sites supplied by OH, has been revealed to have a significant influence on the catalytic activity.
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