NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 32
·15405-15413
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IF 3.925
Yuzhu Zhai,Yijing Li,Qin Hou,Yuanhong Zhang,Enlong Zhou,Houshen Li,Shiyun Ai
A phosphate ion (Pi) is usually considered as an important index of eutrophication in water and can cause great harm to the water ecological environment. In this work, MOF-808(Zr/Ce) was synthesized simply for phosphate detection and removal. MOF-808(Zr/Ce) with oxidase-like activity can oxidize 3,3′,5,5′-tetramethylbenzidine (TMB). The colorimetric sensing of phosphate was performed based on the enhancement of the oxidase-like activity of MOF-808(Zr/Ce). The linear detection range for phosphate detection was 11–581 μM, and the detection limit (LOD) was 3.7 μM. The MOF-808(Zr/Ce)/CNF (cellulose nanofibers) flexible film synthesized by the filtration method also enables the rapid identification of phosphate. Besides, the phosphate adsorption performance of MOF-808(Zr/Ce) was also investigated. The adsorption capacities are 54.9, 65.1, and 68.5 mg g−1 at 298, 308, and 318 K, respectively. The results show that MOF-808(Zr/Ce) has great potential for phosphate detection and removal.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Xiaoya Zhao,Jilin Zhang,Zi Dai,Yunyun Lei,Xiaoxun Liu,Guixia Liu
Excess fluoride in drinking water from groundwater can cause dental and skeletal fluorosis affecting millions of people worldwide. Adsorption is an appealing strategy for defluoridation due to its simple operation and environmental friendliness. However, conventional adsorbents exhibit low adsorption capacity because few exposed active sites. In this work, La anchored Zr-based metal-organic framework (La-UiO-66-(COOH) 2 ) adsorbent with dual-metal sites was designed and synthesized to remove fluoride effectively. The doping of La(III) using uncoordinated carboxyl group of UiO-66-(COOH) 2 increased the adsorption capacity. The morphology, composition, structure, surface area, and thermal stability of adsorbent were carefully characterized by powder X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), energy dispersive X-ray spectrometer (EDX), fourier transform infrared (FT-IR), thermogravimetric analysis (TGA), and X-ray photoelectron spectroscopy (XPS) techniques. The adsorbent is a polyhedral shape with aggregated and smaller crystalline particles and La is uniformly distributed over the adsorbent, favoring the effective adsorption of fluoride. La-UiO-66-(COOH) 2 showed excellent adsorption performance in a wide pH range of 3–9, and the maximum adsorption capacity was 57.23 mg g −1 . The fluoride removal rate of as-prepared adsorbent reached as high as 87 % within 5 min. The adsorption process conformed to the pseudo-second-order equation model and the Freundlich isotherm model. Thermodynamic research indicated that the adsorption process was spontaneous and endothermic. After four adsorption-desorption cycles, the fluoride removal rate of the adsorbent was still retained at 79.7%. The design of dual-metal site adsorbents provides a potential strategy for highly efficient removal of fluoride.
研究领域:
环境科学
·
材料科学
·
水处理
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Wenqi Ji,Wen Shen,Jiahui Li,Renjie Miao,Lianhao Li,Yaxin Zhang,Guining Chen,Guozhen Liu,Gongping Liu,Wanqin Jin
Metal-organic framework (MOF) with rich chemical functionality and tunable pore system has shown great potential for molecular separation. Facile construction of MOF membrane with precisely tailored pore structure for achieving high-efficiency liquid separation (e.g., organic solvents dehydration) remains a challenge. Herein, we proposed a ligand modulation strategy to construct Zr-MOF membranes with tunable pore structure for dimethyl carbonate (DMC) dehydration by pervaporation. Regulating the length and bulkiness of carboxylate ligands (1,4-benzenedicarboxylic acid, H 2 BDC; 1H-pyrazole-3,5-dicarboxylic acid, H 2 PZDC; fumaric acid, H 2 FUM) was applied to prepare a series of Zr-MOF membranes. The employed linear H 2 FUM ligand with the shortest length enhanced membrane surface hydrophilicity and narrowed pore size, thus facilitating the fast and selective transport of water molecules. The resulting Zr-FUM-MOF membrane exhibited an excellent dehydration performance of 2 wt% DMC/water mixtures at 35 °C with a flux of ∼5100 g m −2 h −1 and a separation factor of ∼2030, beyond the separation performance of state-of-the-arts membranes. This work paves a facile way to manipulate pore structure of MOF membranes for molecular separation.
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RSC Advances
·
2021
·Vol. 11
·期 55
·34754-34765
·
IF 3.361
Wei Qin,Kaixuan Xu,Junwei Wang,Xiaofeng Cui,Jianli Zhang,Yaqing Weng
To overcome the urgency of zirconium and hafnium separation, a novel mesoporous silica sorbent (PS-G1.0-MSNs) modified with phosphorous-functionalized G1.0 PAMAM dendrimers was prepared. The adsorption and separation behaviors of PS-G1.0-MSNs adsorbent on Zr(IV) and Hf(IV) were perfromed as a function of acidity, contact time, temperature, and ion concentrations by batch sorption methods. The maximum adsorption capacities for Zr(IV) and Hf(IV) were 25.7 mg g−1 and 5.36 mg g−1 under optimal experimental conditions, respectively, and the separation factor βHf/Zr = 2.0 > 1 demonstrated that the prepared sorbent had preferential selectivity for Hf(IV) in rich Zr(IV) solution. Moreover, kinetic data indicated that the sorption process on Zr(IV) and Hf(IV) achieved equilibrium within 120 min, and followed the pseudo-first-order model with a rate-determining step. The adsorption amount increased as temperature raised from 283 K to 303 K and the isothermal data plotted with the Langmuir model was better than the Freundlich model with monolayer behavior. Thermodynamic data analysis indicated that the sorption process was spontaneous and endothermic. Furthermore, XPS analysis revealed that the metal ion adsorption was mainly induced by the chemical coordination of Zr(IV) and Hf(IV) ions with N, O, P atoms of amide and phosphate groups. The present work provides good guidelines on the design of high efficient sorbent for the separation of Hf(IV) from Zr(IV) solutions.
研究领域:
材料科学
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化学工程
·
环境科学
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MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING
·
2020
·
IF 4.652
Yingnan Shi,Zheng Lu,Li Yu,Rui Xie,Yuhang Ren,Guang Yang
Oxide dispersion strengthened (ODS) FeCrAl alloys have been considered as the promising candidate fuel cladding materials for the Gen-IV fission reactors due to excellent radiation tolerance, mechanical properties and corrosion resistance , but their manufacturing is complex process. Laser engineered net shaped (LENS) technology followed by post-build heat treatment was employed successfully to fabricate Zr-containing ODS-FeCrAl alloy. The microstructure of as-deposited and heat-treated alloys was characterized by optical microscope (OM), electron backscatter diffraction (EBSD), scanning electron microscope (SEM) and high-resolution transmission electron microscope (HRTEM). The tensile tests were carried out at room temperature. The results show that the coarse columnar grains with preferred orientation ([001] fibre texture) are obtained after LENS deposit and are remained after post-build heat treatment. The average width of columnar grains for both as-deposited and heat-treated samples is ~180–190 μm. A slag-like layer which is made up of Y 3 Al 5 O 12 , ZrO 2 and Al 2 O 3 is observed at the surface of deposited sample. Some coarse appendage oxides which consist of Al 2 O 3 and Y 4 Zr 3 O 12 are distributed in the matrix of as-deposited sample. Post-build heat treatment produces high-density nanoscale Y 4 Zr 3 O 12 oxides in the matrix. The formation mechanism of different type oxides is explained. Both as-deposited and heat-treated samples present anisotropic tensile properties . After post-build heat treatment, the tensile strength is improved significantly by the formation of high-density nanoscale Y 4 Zr 3 O 12 .
研究领域:
材料科学
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增材制造
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核材料
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金相学
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力学性能
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 20
·2213999
·
IF 19
Yizhong Zhang,Liuchang Wang,Ruichi Zhang,Chao He,Lixia Jia,Xunliang Wang,Xuemin Feng,Tianxiang Jiang,Baolong Xie,Xiaolei Ma,Junrui Cao,Yuhui Ma,Xin Tan,Tao Yu
Because of spontaneous agglomeration effect and undesirable electronic state of Zr sites on the surface, zirconium (hydro)oxides generally exhibit suboptimal defluoridation capacity. Herein, a template confinement-ligand anchoring strategy is developed by utilizing confined growth of zirconium hydroxide (ZH) inside chitosan hydrogel beads (CHB) and subsequent anchoring of fumaric acid (fm) on its surface Zr sites in a monodentate mononuclear coordination mode. This technique leads to uniform dispersion of ultrafine fmZH (≈3.4 nm) and tunable electron density at the Zr sites. Due to the electron-withdrawing ability of fm, electron-delocalized Zr sites increase the orbital energy level matching and vacate Zr 4d orbitals to promote hybridization with the F 2p orbitals. Ultimately, robust Zr F bond can be formed as a result of reduced the adsorption energy toward fluoride ions. The defluoridation capacity shows positive linear relationship with the electron extraction ability of ligands. The saturation adsorption capacity and dynamic treatment capacity of CHB@fmZH are 10.8 and 45.9 times higher than that of CHB@ZH, respectively, owing to high electron extraction (0.098 e − ) of fm. This study offers a novel insight into the design and synthesis of high-efficiency metal oxide adsorbents by steering its surface metal sites’ electronic state through ligand effect.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Di Zhang,Hongli Hu,Ji-an Wei,Xin Xu,Lei Chen,Xiaohui Wu,Qianqian Yu,Bo-xing Zhang,LinGe Wang
Titanium dioxide (TiO 2 ) is well known for its photocatalytic and antibacterial properties which are widely used in organic pollutants treatment and antibacterial. However, the fast recombination of electron-hole pairs of TiO 2 and the wide bandgap energy during photocatalysis progress are prominently degrades its photocatalytic efficiency. In this study, we designed and investigated Zr-doped TiO 2 ceramic nanofibrous membranes with enhanced photocatalytic properties for dye scavenging and bacteria inactivation. A mixture solution of poly(acrylonitrile) (PAN) and preceramic polymers (Zr-doped polytitanoxane) was electrospun to fabricate Zr-doped TiO 2 ceramic nanofibrous membranes, which were then carbonized in argon at 600 °C and calcined in air at 400 °C. It was found that the morphologies, structures, and characteristics of ceramic nanofibrous membranes were significantly influenced by the composition and content of preceramic polymers. The doping of Zr element improved photocatalytic activity of ceramic nanofibrous membranes and achieved efficient antibacterial activity . This work demonstrates a new strategy for the fabrication and application of multifunctional TiO 2 composites by incorporating with ceramic nanofibrous membranes.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Jing Zhang,Beier Hu,Zhongli Guo,Hongqiang Luo,Rui Wang,Mingpo Li,Mengyu Chen,Cheng Li
The poor stability of metal halide perovskite seriously affects the large-scale commercial application of perovskite solar cells (PSCs). Here, a large-particle Zr-based metal–organic framework (Zr-MOF), e.g. UiO-66 (NH 2 ), is added to the precursor solution of SnO 2 electron transport layer (ETL), realizing a cross-layer modification of (1) ETL, (2) perovskite active layer and (3) theirs interface simultaneously. We find that the SnO 2 particles are dispersed into the ordered porous scaffold of Zr-MOF, to form an ETL with improved crystallinity , reduced defect states and increased contact area with active perovskite film. For the subsequently deposited perovskite layer, the crystallization along the vertical direction is significantly optimized, and the defects are passivated by the bottom-up infiltrated Zr-MOF, so as to suppress the ion migration process. The power conversion efficiency (PCE) of one-step fabricated Zr-MOF-modified MAPbI 3 based PSCs is optimized from 17.48% to 18.25%, and remaining 99% of its initial value after storage for 800 h under ambient conditions with the relative humidity over 60%. This work provides a simple cross-layer passivation strategy to improve the performance and stability of PSCs using highly designable MOF materials.
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 7
·2101-2107
·
IF 5
Jianhao Qiu,Lu Zhang,Guanglu Xia,Dingliang Dai,Yong Tang,Jianfeng Yao
Different ligand functionalized UiO-66 (UiO-66-X, X = OH, (OH)2 and NH2) were prepared and then modified by ZnIn2S4 lamellas to form ZnIn2S4/UiO-66-X heterostructures for visible-light-driven H2O2 evolution in pure water. The H2O2 yields using ZnIn2S4/UiO-66-NH2, ZnIn2S4/UiO-66-(OH)2 and ZnIn2S4/UiO-66-OH are 799, 733 and 165 μmol L−1, respectively, which are 9.5, 8.7 and 2.0 times that of ZnIn2S4/UiO-66. The high performance of ZnIn2S4/UiO-66-NH2 and ZnIn2S4/UiO-66-(OH)2 is ascribed to the benign visible-light response and Z-scheme heterostructures, and the H2O2 evolution abides by indirect O2 reduction with ˙O2− as an intermediate species. Additionally, H2O2 yields using ZnIn2S4/UiO-66-NH2 on tap water and Xuanwu Lake (Nanjing, China) water can be comparable to that on the above-deionized water. This study sheds light on the great promise of functionalized MOFs and their applications on green (photo)catalytic energy conversion.
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Progress in Natural Science-Materials International
·
2023
·
IF 4.7
Xuechun Wang,Zeming Dai,Xuan Zhou,Hao Chen,Yu Cao,Jianhua Hou,Xiaozhi Wang
In general, majority of MOFs are powder, which limit their applications. In this study, the highly stable Zr-based MOF-808 and its thiol-modified MOF-808-SH were selected as precursors, and then they were wrapped by sodium alginate hydrogel via a dripping strategy. Based on these, MOF/hydrogel composite beads (Alg-MOF-808, Alg-MOF-808-SH) with 3D network structure were prepared successfully. Due to its excellent adsorption properties and easy recovery, they were employed as effective environmental functional materials for the adsorption of Hg (II). The adsorption capacities of Hg (II) were 170.52 mg‧g −1 and 221.73 mg‧g −1 respectively and they can achieve adsorption equilibrium in a short time. The adsorption stability of Alg-MOF-808-SH was studied at different pH as well. In addition, the removal efficiency of composite beads for Hg (II) was almost unaffected by other coexisting ions, displaying good adsorption selectivity. Furthermore, the removal efficiency only decreased by 10.4% after 5 cycles, indicating that the as-prepared materials have high recycling efficiency. The results demonstrated that the MOF/hydrogel composite beads have a certain application potential for mercury removal in actual wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jie Yin,Wendi Fu,Jinrui Zhang,Xinyu Liu,Xinmiao Zhang,Chao Wang,Jing He,Wei Jiang,Hongping Li,Huaming Li
Porous ionic liquids are a novel category media that possesses the catalytic activity of porous solids and the extraction property of ionic liquids. Herein, a new type of porous ionic liquids (denoted as UiO-66-T3PILs) was fabricated by employing UiO-66(Zr) as the pore generator and the ionic liquid ([P 6,6,6,14 ][NTF 2 ]) as the size-excluded solvent for extraction coupled catalytic oxidative desulfurization (ECODS) using hydrogen peroxide (H 2 O 2 , 30 wt%) as an oxidant. Furthermore, several significant reaction parameters such as UiO-66 loading in porous ionic liquids, reaction temperatures, molar ratio of H 2 O 2 /DBT and sulfide species as well as recyclability were investigated in detail. As UiO-66-T3PILs exhibited higher efficiency (95.3%) than the summarized efficiency of UiO-66 and [P 6,6,6,14 ][NTF 2 ], there did exist a synergistic effect between the UiO-66(Zr) moiety and the ionic liquid moiety in UiO-66-T3PILs. With the assistance of density functional theory calculations, a possible mechanism was proposed that aromatic sulfur compounds in the oil phase were first extracted into ionic liquids moiety phase via C-H···π interactions and then rapidly oxidized by OH radicals in the presence of the UiO-66 moiety. This work will pave the way for the rational design of novel porous ionic liquids towards catalysis.
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AICHE JOURNAL
·
2023
·Vol. 69
·期 9
·e18181
·
IF 3.7
Yanling Guo,Yan Wei,Miao Chang,Dan Wang,Jie-Xin Wang,Jian-Feng Chen
Zr-based metal-organic framework (Zr-MOF) nanoparticles (NPs) have attracted extensive research thanks to their outstanding thermal and chemical stability, but their efficient synthesis is still challenging. Here, high-quality Zr-MOF NPs with tunable and uniform particle sizes can be successfully fabricated within 30 min by high-gravity technology with high yields. Significantly, the rapidly milder preparation of UiO-66 NPs can also be achieved at 90 or 70°C. This strategy has been extended to the synthesis of other Zr-MOF NPs. Furthermore, the water vapor adsorption properties of obtained UiO-66 NPs display a size-dependent effect. The 70 nm UiO-66 NPs have the highest adsorption capacity of 625 mg g −1 among unmodified UiO-66 reported so far, and manifest 2.0–2.8 times faster water adsorption rate than the micron ones. This study provides a feasible method for the efficient and mild preparation of MOFs nanoparticles, which may promote the synthesis and applications of nano-sized MOFs.
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