Journal of Cleaner Production
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2023
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IF 11.1
Di Zhang,Hao Tang,Bing Zhao,Lijie Liu,Hongwei Pang,Xiangxue Wang,Shujun Yu
Radioactive uranium removal plays a key role in energy development and environmental security. Sulfide nanoscale zero-valent iron (S-NZVI) has good antioxidant capacity, dispersibility and activity to eliminate U(VI) from wastewater, but the removal efficiency is limited. To improve the reduction and adsorption capacity of S-NZVI, through treating Fe 3+ solution by nitro-functionalized UiO-66 (UiO-66-NO 2 ) with high porosity, UiO-66-NO 2 enhanced S-NZVI adsorbent (S-NZVI/UiO-66) was prepared by liquid phase reduction method. The smaller size and larger specific surface area of S-NZVI/UiO-66 were confirmed by a variety of characterization techniques. Based on the excellent surface structure and reactivity, the U(VI) removal capacity of S-NZVI/UiO-66 (895 mg g −1 ) was much better than S-NZVI (434 mg g −1 ) and UiO-66-NO 2 (267 mg g −1 ). The impacts of pH, background ion strength, coexisting ions and different water environments on adsorption were studied via macroscopic batch experiments. The results showed that S-NZVI/UiO-66 could remove U(VI) adequately in a wide pH range. The removal rate was basically not affected by the concentration of NaNO 3 , demonstrating that the adsorption process of U(VI) on S-NZVI/UiO-66 tended to inner surface complexation. From XPS technique combined with the results of batch adsorption experiments, it was clear that the elimination mechanisms of U(VI) by S-NZVI/UiO-66 were mainly the physical adsorption, electrostatic attraction and complexation of UiO-66-NO 2 , and the reduction and complexation of S-NZVI. Therefore, it is believed that S-NZVI/UiO-66 has a great potential to be an excellent adsorbent in the field of the environment remediation. Moreover, S-NZVI/UiO-66 promises to be a novel nanomaterial for solving the problem of radionuclide contamination in practical environments.
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JOURNAL OF COORDINATION CHEMISTRY
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2023
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IF 1.9
Yanbing Yin,Yang Liu,Zhou Wang,Yongming Feng,Bei Jiang
A ternary composite α-DMACoPc/UiO-66-NH2/TiO2 was synthesized by solvothermal method and characterized by X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR), scanning electron microscopy (SEM) and other means. The composite catalyst was applied to decompose methylene blue dye in visible light, and the degradation rate reached 93.4%. Compared with the monomer, the composite significantly enhanced the efficiency of the catalytic degradation due to the synergistic effect between composites. The transport speed of charge is accelerated and the recombination of hole-electron pairs is inhibited due to the larger specific surface area. A feasible scheme was provided for preparation of composite catalyst and photocatalytic degradation of dye.
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CHEMOSPHERE
·
2023
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IF 8.8
Jun Wang,Junxian Qin,Changqing Yang,Yun Hu
A series of functionalized X-UiO-66 (X = NH 2 , H, Br and NO 2 ) materials were prepared using a hydrothermal method and modified with various ligands. Their photocatalytic activity was evaluated by the oxidation of acetaldehyde. Experimental results show that the introduction of different ligands significantly influences the physicochemical properties of UiO-66. Br-UiO-66 exhibited the highest photocatalytic activity and CO 2 selectivity of 85.6% and 85.7%, respectively. Photochemical properties reveal that -Br functional group facilitate the separation of photogenerated electrons and holes, significantly improving their transfer and oxygen reduction. As a result, an increased number of hydroxyl and superoxide radicals can form, improving the efficiency of the photocatalytic reaction. Br-UiO-66 accumulates fewer intermediates on its surface and still shows excellent photocatalytic activity and structural stability after 24 h of dynamic reaction. This work demonstrates the excellent adsorption and catalytic oxidation performance of Br-UiO-66 towards acetaldehyde and may provide new ideas for researching catalysts in the photocatalytic degradation of pollutants.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xinyu Hu,Yao Zhang,Mingrong Lu,Min Yang,Jianmin Li,Zhengmei Wang,Guizhen Li,Hongbin Wang
In the present work, Ce-UiO-66, namely cerium-organic framework was prepared through rapid one-step solvothermal method, uncovering it potency to effectively get rid of tetracycline (TC) from an aqueous solution. The morphology and structure of Ce-UiO-66 materials were characterized by typical traditional methods such as FESEM, XRD , FTIR, and XPS. The process performance in terms of TC removal was investigated at different operating conditions. Specifically, when the dose, pH value, adsorption time, and temperature were 20 mg, 9, 180 min, and 25 ℃ respectively, the removal effect of TC was the best. The adsorption process of TC was described using the Freundlich model and the quasi second order model, respectively. The removal efficiency of TC by UiO-66 before modification was only 40.37%, and the adsorption amount was 44.38 mg⋅g −1 , while the removal efficiency of TC adsorption by Ce-UiO-66 could reach about 90% under the optimal adsorption conditions, and the maximum adsorption amount was 86.95 mg⋅g −1 . The data showed that Ce-UiO-66 exhibits good TC adsorption performance. And TC adsorption process was spontaneous and endothermic multi molecular layer chemical adsorption . Ce doping increased the quantity of active sites, and promoted the synergistic effects of electrostatic attraction, π-π conjugation, and hydrogen bonding between the adsorbent and TC, thus improving the adsorption effect of TC. As everyone knows that the application of UiO-66 in the adsorption field can be broadened by doping other metal ions , which prove that the metal skeleton adsorption material has broad development prospects in the next few years.
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TALANTA
·
2022
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IF 6.556
Pengfei Zhao,Sisi Tang,Xiaodan Wu,Yu Chen,Kangling Tang,Jinli Fu,Huibin Lei,ZhaoXia Yang,Zhaohui Zhang
Development of method with micro-volume reagent usage and high selectivity for rapid determination of valuable disease-related biomarkers is of great importance for disease surveillance. Herein, a novel ratiometric fluorescence capillary imprinted sensor was developed for highly selective fluorescence determination of sialic acid (SA) based on luminescent metal-organic framework (UiO-66-NH 2 ). In this strategy, the imprinted pre-polymer with double emissions was sucked into the capillary to grow imprinted layer on the inner wall of the capillary. In presence of SA, the blue fluorescence (440 nm) served as fluorescence response signal was quenched due to the electron transfer mechanism between metal organic framework and SA while the red fluorescence (655 nm) served as the reference signal was remained. Within SA concentration linear range of 1.0 × 10 −7 –3.0 × 10 −4 M, the ratiometric fluorescence capillary imprinted sensor was applied to detect SA in human serum and saliva samples successfully with a detection limit of 2.5 × 10 −8 M. A sensitive and selective fluorescence method with micro-volume sample consumption (15 μl) for determination of SA in practical samples was established.
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CARBOHYDRATE POLYMERS
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2022
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IF 10.723
Zhi Chen,Zhi-Bo Zhang,Jun Zeng,Zhi-Jie Zhang,Shan Ma,Cong-Ming Tang,Jun-Qiang Xu
In this work, a polyethyleneimine-modified chitosan/Ce-UIO-66 composite hydrogel (PEI-CS/Ce-UIO-66) was prepared using the ex-situ blend method. The synthesized composite hydrogel was characterized by SEM, EDS , XRD, FTIR, BET, XPS, and TG techniques, while the zeta potential was recorded for sample analysis. The adsorbent performance was studied by conducting adsorption experiments using methyl orange (MO), which showed that PEI-CS/Ce-UIO-66 exhibited excellent MO adsorption properties (900.5 ± 19.09 mg/g). The adsorption kinetics of PEI-CS/Ce-UIO-66 could be explained by the pseudo-second-order kinetic model , and its isothermal adsorption followed the Langmuir model. Thermodynamics showed that the adsorption was spontaneous and exothermic at low temperatures. MO could interact with PEI-CS/Ce-UIO-66 via electrostatic interaction , π–π stacking, and hydrogen bonding . The results indicated that the PEI-CS/Ce-UIO-66 composite hydrogel could potentially be used for the adsorption of anionic dyes.
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ANALYST
·
2022
·Vol. 147
·期 24
·5655-5662
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IF 5.227
Ying Zhou,Ruichun Li,Guomei Zhang,Yan Zhang,Caihong Zhang,Shaomin Shuang
Metal–organic frameworks (MOFs) have emerged as interesting nanomaterials owing to their large surface area, high porosity, tunable pore architecture and easy functionalization. However, an inferior electrical conductivity hinders their application in electrochemical sensing. In this paper, gold–palladium alloy/UiO-66-NH2/graphene (AuPd/UiO-66-NH2/GN) composites were synthesized by loading alloys on the surfaces of MOFs and then attaching them to the graphene surface. The addition of metal nanoparticles and graphene enhanced the electron transfer ability of MOFs. Then, composites were used to modify a glassy carbon electrode (GCE) to construct a sensitive dopamine (DA) electrochemical sensor. The developed sensor manifested two linear relationships in lower concentration ranges and in higher concentration ranges with a 0.21 × 10−6 mol L−1 low detection limit (3σ/k) under optimal conditions. The results certified that the constructed sensor had high selectivity, excellent reproducibility and good stability, and had been used successfully for DA detection in actual human serum samples.
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PLoS One
·
2022
·Vol. 17
·期 8
·e0271075
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IF 3.752
Bicun Jiang,Fuqiang Liu,Yang Pan,Yan Tan,Chendong Shuang,Aimin Li
Tetracycline (TC) is widely-used antibiotic pollutant with high toxicity, refractory, persistence and bacteriostasis, and its removal from water needs to be enhanced. In this work, a novel Graphite-UiO-66(Zr)/Ti electrode was successfully prepared and evaluated for electrochemical oxidation degradation of TC. The electrochemical performance tests indicate the Graphite-UiO-66(Zr)/Ti electrode had higher electrochemical oxidation activity, which achieved higher TC removal efficiency (98.1% ± 1.5%) than Ti plate (65.2% ± 3.5%), Graphite-MIL-53(Al)/Ti electrode (79.5% ± 2.9%) and Graphite-MIL-100(Fe)/Ti electrode (89.0% ± 2.6%). The influence of operating condition was also systematically studied, and the optimized condition was pH 5.0, 20 mA/cm 2 current density and 0.1 M electrolyte (Na 2 SO 4 ). Through the liquid chromatography mass spectrometry (LC-MS), the TC degradation pathway by Graphite-UiO-66(Zr)/Ti electrode oxidation was proposed. Under the •OH free radical oxidative decomposition effect, the double bond, phenolic group and amine group of TC were attacked. TC was transformed into intermediate product ① (m/z = 447), then was further degraded to intermediates ② (m/z = 401) and ③ (m/z = 417). The latter was fragmented into small fractions ④ (m/z = 194), ⑤but-2-enedioic acid (m/z = 116) and ⑥oxalic acid (m/z = 90, the proposed intermediate). In addition, TC removal remained at 89.6% ± 2.7% in the sixth cycle of operation, which confirmed the efficient reusability and stability for antibiotics removal from water.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Ting Du,Jing Wang,Liang Zhang,ShaoChi Wang,Chengyuan Yang,Linxuan Xie,Zhaoli Liu,Yongsheng Ni,XiangHong Xie,Jing Sun,Wentao Zhang,Jianlong Wang
The creation of defects into luminescent MOFs allows for manipulation of fluorescent properties and thus leads to the enhanced detection performance for technological applications. Herein, a modulator-induced defect formation strategy was proposed to introduce missing-linker defect into lanthanide-based metal–organic framework (Eu@UiO-MOFs) and the enhanced detection properties was investigated. Notably, the missing-linker numbers in per Zr 6 cluster were calculated to facilitate comparison and quantitively interpretation. By elaborately tailoring defect numbers, the resultant Eu@UiO-MOFs-2 sensor with 0.53 missing linkers per Zr-O cluster showed a remarkably enhanced response slope and realized excellent trace detection under the range of 0–10 ppm with ultralow detection limit to 5.67 × 10 −7 M (114 ppb), acting as a powerful signal amplifier for trace detection of Cd 2+ . Moreover, the relationship between structural change and defect numbers of Eu@UiO-MOFs-X has been studied to understand the positive effect of the improved enrichment for the optical behavior. As far as we know, this is the first experimental demonstration of missing-linker defects in luminescent MOFs for regulation of optical sensing, offering a unique approach to explore innovative technologies for precisely detecting of heavy metal ion pollutants.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
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IF 7.2
Pengxiao Liu,Yan Jia,Yao Ning,Xiaocheng Zhang,Shuhui Tian,Fan Yang,Weiyu Song,Ying Zhang
This study demonstrates the significant effect of incorporating inexpensive transition metal nanoparticles into metal-organic frameworks (MOFs) to improve their room-temperature hydrogen storage properties. Low-cost nanoparticles (Cu, Ni, and CuNi) were incorporated into UiO-66(Zr) via the double-solvent approach (DSA) plus chemical reduction processes. All composites exhibited higher hydrogen storage capacity compared to pure UiO-66 at both room temperature and 60 bar. Notably, the hydrogen spillover efficiency of CuNi nanoparticles loaded in UiO-66 was comparable to that of MOF adsorbents embedded with noble metals such as Pd and Pt. The hydrogen storage capacity of CuNi@UiO-66 was significantly increased from 0.20 wt% to 0.74 wt%. DFT calculations showed that the CuNi alloys facilitated the adsorption and dissociation of hydrogen molecules in comparison to the single metal nanoparticles , thus favoring the hydrogen spillover effect and improving the hydrogen storage performance. This work demonstrates the potential of designing MOF loaded with inexpensive metal nanoparticles for optimized room-temperature hydrogen storage.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
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IF 4.2
Wei Zhang,Runtang Liu,Longwen Lei,Binbin Nian,Shipin Yang,Yi Hu
Efficient and stable catalysis has always been a fundamental concept in enzyme-catalyzed industrial processes. However, the poor stability of laccase has hindered its application in industry. The conventional methods of immobilization have proven to be ineffective in achieving both stability enhancement and the maintenance of high activity simultaneously. To address this challenge, we have constructed a magnetic core–shell structured metal–organic framework doped with copper ions (MCIL@Cu-UiO-66-NH2), which leverage the synergistic effects of copper ion activation and covalently binding to immobilize laccase. The resulting immobilized laccase exhibited high activity recovery (89%) and stability, retaining 90% relative activity after 30 days of storage and 66% of its initial activity after being exposed to a temperature of 60 °C for 6 h. The application of immobilized laccase in the removal of aqueous organic pollutants was also investigated. The results demonstrate that immobilized laccase can remove 2,4-dichlorophenol completely within 8 h and maintains approximately 90% removal efficiency after undergoing five cycles. Moreover, immobilized laccase also exhibited favorable results in the removal of other phenolic pollutants and typical aromatic pollutants, which are difficult to degrade, such as indole and anthracene. The copper ion-doped magnetic MOF composite novel introduced in this work demonstrated promising potential as an efficient carrier for laccase immobilization, and the immobilized laccase exhibits practical application prospects in the field of wastewater treatment.
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ChemistrySelect
·
2023
·Vol. 8
·期 43
·e202302665
·
IF 2.1
Muhammad Umair Ahmad,Guoying Zhao,Shahid Hussain
Graphical An efficient trifloalumiate supported MOF(UIO-67) catalyst was synthesized to promote the butyl levulinate formation from α-angelica lactone under mild reaction, resulting in remarkable conversion and selectivity. The catalyst was easily separated and could be recycled five times without significant activity loss. Herein, levulinate acid esters (LAEs) were efficiently synthesized from the α-angelica lactone (α-AL) esterification with trifloaluminate ionic liquids supported UIO-67 MOF as Lewis acidic catalyst. A series of UIO-67 catalysts with varied trifloaluminate ionic liquids loading were prepared via the post-modification method and exhibited excellent catalytic activity for α-AL esterification. Remarkable α-AL conversion (100 %) and LAEs selectivity (>99 %) were achieved by UIO-67 catalysts (0.2 mol %) with 12.4 %, trifloaluminate ionic liquids loading (UIO-67-TFA) at 70 °C and 90 min. The UIO-67-TFA catalyst can be reused at least 5 cycles without significant loss of catalytic activity. The UIO-67-TFA catalysts were fully characterized by XRD, SEM, XPS, TGA, IR, N 2 physisorption, etc. The results indicated that the well-distributed active trifloaluminate Lewis acid catalytic sites, high BET surface area, and good thermal stability could contribute to its excellent catalytic activity.
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