BIOCHEMICAL ENGINEERING JOURNAL
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2022
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IF 4.446
Jiacong Wu,Yi Wang,Juan Han,Lei Wang,Chunmei Li,Yanli Mao,Yun Wang
In this work, a mesoporous Zr-based MOF (MP-UIO-66) was first synthesized by biomineralization method using dextran as template and the resultant particles were applied in the immobilization of cellulase . Compared with conventional UIO-66, MP-UIO-66 has more mesoporous channels (4.6 nm) that allow cellulase (3.4 * 12.4 nm) to be entrapped into the channels, improving loading capacity and stability of immobilized enzyme . Specifically, the results showed that MP-UIO-66 had an excellent loading capacity (265 mg g −1 ) for cellulase, and the residual enzyme activity of PVP-cellulase@MP-UIO-66 (PCMU) was still about 83% after 6 cycles. Moreover, the suitable pore structure exposes the active center of cellulase to the external environment, which facilitates the mass transfer of the substrate. Based on Michaelis-Menten constant analysis, the substrate affinity (13.355 mg mL −1 ) and catalytic efficiency (1.311 mL mg −1 min −1 ) of PCMU were better than those of free cellulase (14.525 mg mL −1 , 0.732 mL mg −1 min −1 ).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Lingchao Kong,Jun Zhang,Yi Wang,Qinlin Yan,Jiayu Xu,Xi Quan,Charles B. Andrews,Zuotai Zhang,Chunmiao Zheng
Hazardous oxyanions in water bodies are potentially toxic to aquatic life, and the coexistence of multiple anions aggravates the toxicity. Herein, bowknot-like Zr/La bimetallic organic frameworks (Zr/La-BTC) were developed with superior hazardous oxyanion adsorption capacities, i.e., approximately 102 mg/g for arsenate and 159 mg/g for phosphate, respectively. The molar ratio of Zr to La in Zr/La-BTC plays a significant role in the structure and the adsorption efficiencies. Notably, the experiment-derived adsorption capacities of various Zr/La-BTC samples were consistent with their adsorption energies calculated by density-function theory (DFT). Further mechanism analysis revealed that coordination of Zr/La atoms with the target anion groups occurred during adsorption. The positive shift of binding energies in La 3d and Zr 3d XPS spectra and Bader charge analysis unveiled that back-donation interactions dominated the adsorption process . The reliable adsorption selectivity and reusability of 0.1Zr/La-BTC were verified with anion competition experiments and four adsorption-desorption cycles. Overall, this study provides significant insight into the design of high-performance bimetallic organic frameworks for the enhanced removal of hazardous oxyanions from water.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Jinliang Song,Chao Xie,Zhimin Xue,Tiejun Wang
Meerwein–Ponndorf–Verley (MPV) reduction of biomass-derived carbonyl compounds is a greatly promising route for biomass valorization. Robust, facile-prepared, and cost-effective inorganic Zr-based catalysts for this transformation remain highly desirable. Herein, Zr-containing montmorillonite (denoted as Zr-MMT) was constructed by the ion exchange of Zr4+ with the interlayer cations of montmorillonite (MMT). Very interestingly, as an inorganic catalyst, the prepared Zr-MMT showed high catalytic activity for MPV reduction of various biomass-derived carbonyl compounds. Systematic investigations revealed that the excellent performance of Zr-MMT predominantly originated from more positively charged Zr species ([Zrx(OH)y(H2O)n](4x−y)+), which could boost the activation of the carbonyl group and simultaneously promote the hydrogen transfer process assisted by suitable basic sites on MMT. Notably, the preparation of Zr-MMT avoided the utilization of surfactants or expensive organic ligands, and the prepared Zr-MMT showed better or comparable catalytic performance than most reported Zr-containing catalysts, significantly enabling it to be more practical.
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TALANTA
·
2022
·
IF 6.556
Jingyu Li,Yexin Dai,Jinran Cui,Halayit Abrha,Ning Kang,Xianhua Liu
Overuse of antibiotics posed a global threat to human health and the ecological environment. Efficient detection and control of antibiotic pollution demand novel sensory materials. Here, a dual-luminescent material FS@UIO66 was successfully synthesized by encapsulating fluorescent molecules (fluorescein sodium , FS) in UIO66 based on the in-situ encapsulation method. We found that the dual emission peaks of FS@UIO66 at 369 and 515 nm can be sensitively and synchronously quenched by tetracycline (TET). Interestingly, these two peak intensities were switched anisotropically by levofloxacin (LEV), in which the signal at 515 nm was enhanced. Photophysical analysis revealed that there may exist a competition and replenishment mechanism in the sensing processes. The ratiometric fluorescent feature was employed for rapid detection of TET and LEV, with detection limits of 0.2444 μM and 0.2808 μM for TET and LEV, respectively. The superior sensitivity, high selectivity, and excellent recyclability of FS@UIO66 in sensing TET and LEV were demonstrated in this work. In addition, TET and LEV were also successfully detected by FS@UIO66 in water from real water environment. The results indicate that FS@UIO66 composites are favorable for TET and LEV detection, presenting a great sensing platform for antibiotic detection.
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JOURNAL OF MEMBRANE SCIENCE
·
2021
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IF 8.742
Zimo Wang,Jiamo Ren,Yuxuan Sun,Li Wang,Yong Fan,Jifu Zheng,Huidong Qian,Shenghai Li,Jianing Xu,Suobo Zhang
The dispersion and compatibility of metal–organic frameworks (MOFs) in polymeric matrices significantly influence the properties of composite membranes . However, the modification and functionalization of the node structures of MOFs to improve their dispersion in the polymeric matrix have been rarely studied. In this work, the node structures of UiO-66-NH 2 frameworks were modified by the introduction of F species, and abundant Zr–F bonds and pore blocking effects were generated, which significantly affected the comprehensive performances of the composite membranes, including the dispersion, mechanical properties , proton conductivities, swelling ratios, and water uptake. Due to the good dispersion of the fluorinated MOF nanoparticles in the Nafion matrix, the composite membranes had high proton/methanol selectivity and low methanol permeability, which exhibited superior fuel cell performances in DMFCs (24.9–26.8 mW cm −2 ) to that of recast Nafion (20.4 mW cm −2 ). Notably, this was the first time that the node structures of MOF-based nanoparticles were fluorinated to improve their dispersion in a polymeric matrix, providing a simple strategy for developing high-performance composite membranes.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
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IF 5.455
Mengmeng Zhang,Jiaying Lou,Rui Xu,Peng Li,Yunfei Sha,Hui Zhang,Yu Jia,Zhenxia Chen,Da Wu,Yun Ling,Yaming Zhou
Metal-organic frameworks (MOFs) featuring a fcu-type net based on 12-connected [Zr 6 (μ 3 -O) 4 (μ 3 -OH) 4 ] cluster have received considerable interest for the fundamental investigation of structure-property relationships in a wide range of catalytic reactions . In this work, the bipyridine (bpy) chelate group was introduced into the fcu-type framework of UiO-67, giving UiO-67bpy as the catalyst support. Then, FeCl 3 was post-synthetically anchored to the bpy group, resulting into the isolation of FeCl 3 /UiO-67bpy. Catalyzed hydrolysis of 5-hydroxylmethoxyfurfural (HMF) into levulinic acid (LA) was then explored and revealed that it can efficiently and selectively catalytic convert HMF into LA, which is superior to that of FeCl 3 /UiO-67 where FeCl 3 is encapsulated in the cage of UiO-67 and dispersed on the pore surface. The recyclability studies further confirmed the importance of anchored FeCl 3 where there is no significant decrease in catalytic activity as compared with that of FeCl 3 /UiO-67. Taking the detailed textural porosity and catalytic results of isomorphous structures in consideration, our studies revealed that narrowing the pore size with anchored FeCl 3 on the skeleton of the fcu-type Zr-MOF rather than encapsulating FeCl 3 inside the cage is more favored for the rehydration reaction of HMF to LA.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Fan Xiao,Ming Cao,Rongrong Chu,Xiaoyu Hu,Wenxiong Shi,Yingbo Chen
A new type of composite membrane was prepared through the vacuum filtration self-assembly, in which, graphene oxide (GO) was the basic material, and the horizontal insertion material is product of perylene-3, 4, 9, 10-tetracarboxylic dianhydride (PTCDA) and UiO-66-NH 2 (PTCDA-UiO-66-NH 2 ). The leading role of Π-Π conjugate, auxiliary effect of hydrogen bonding during membrane preparation have been confirmed through Fourier transform infrared spectroscopy (FTIR), UV–visible spectrophotometer, Raman spectroscopy, and X-ray diffraction (XRD). The prepared GO@PTCDA-UiO-66-NH 2 membrane had new nodular structure compared to GO membrane by scanning electron microscopy (SEM) and atomic force microscopy (AFM), which promoted the water transport. In addition, the insertion of PTCDA-UiO-66-NH 2 narrowed the actual filtration spacing between GO sheets, and PTCDA-UiO-66-NH 2 could also adsorbed dye laterally. Experiments showed that the permeance of GO@PTCDA-UiO-66-NH 2 membrane was 1.7 times of GO membrane, and the removal of methyl blue, congo red, crystal violet and disperse black 9 was close to 100%. Under extreme pH, high salt concentration and multiple recycling, its separation ability was still excellent. The GO@PTCDA-UiO-66-NH 2 membrane constituted a unique synergistic structure of vertical-screening and horizontal-adsorption, which successfully overcame the trade-off effect and obtained excellent stability of structure and performance. Therefore, GO@PTCDA-UiO-66-NH 2 membrane had great potential in practical applications.
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RSC Advances
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2020
·Vol. 10
·期 68
·41283-41295
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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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CHEMICAL ENGINEERING JOURNAL
·
2020
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IF 10.652
Jiali Tang,Jiling Zhao,Shixing Wang,Libo Zhang,Minghu Zhao,Zhen Huang,Yuting Hu
In this study, a novel metal organic framework (MOF) was prepared by pre-modification strategy and used as adsorbents to recover palladium ions in wastewater. The characterization indicates that the adsorbents have been successfully synthesized. The effects of various factors on the adsorption behavior of the adsorbents for Pd(II) was studied. Experimental research shows that the optimal pH of the adsorption process is 4.0. The adsorption kinetics and isotherms of Pd(II) on the adsorbents show that it conforms to pseudo-second-order and Langmuir models, respectively. Therefore, the adsorption reaction is a single layer adsorption on the uniform surface of the adsorbent, and chemical adsorption is the main rate-limiting step. According to thermodynamic analysis, the adsorption process is entropiezunahme, spontaneous and endothermic. The adsorption mechanism of Pd(II) on the adsorbents is mainly through the electrostatic action and chelation of Pd(II) with N and O atoms, and the reduction of Pd(II) to Pd(0) by N and O functional groups. The adsorbents can selectively uptake palladium ions from multi-ion wastewater, and after five adsorption–desorption cycles, the adsorption efficiency is still high. This new adsorbent has a wide application prospect in the field of palladium ion separation.
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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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Environmental Science-Nano
·
2019
·Vol. 6
·期 12
·3590-3600
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IF 7.704
Yunyun Xu,Jiaxin Lv,Yao Song,Xiaoyu Zhou,Chen Tian,Xujia Hong,Yuepeng Cai,Cunyuan Zhao,Zhang Lin
As an emerging micropollutant, organoarsenic has caused global ecosystem pollution, due to its degradation to highly toxic inorganic arsenic in the environment. Therefore, to remove the low-concentration organoarsenic from arsenic compounds from water, materials with high adsorption affinity are in urgent need. Herein, we reported an amino-modified metal–organic framework (MOF) with defects (UiO-66-D-NH2) to adsorb two typical organoarsenic forms p-arsanilic acid (p-ASA) and roxarsone (ROX). The adsorption affinity of UiO-66-D-NH2 was 3.8 and 3.0 times higher than that of original UiO-66 and defective UiO-66 without amino modification (UiO-66-D), while the removal rate exceeded 99.1% when the initial concentration of organoarsenic decreased to 1 mg L−1. UiO-66-D-NH2 also showed excellent adsorption behavior in simulated wastewater, with residual arsenic concentrations lower than 0.54 μg L−1. Mechanism studies showed a cooperation of the defects and –NH2 groups in UiO-66-D-NH2. The defects provided more Zr–OH sites in the metal node, leading to transformation of the As–O–Zr coordination from monodentate mononuclear to bidentate binuclear configuration, while –NH2 groups formed hydrogen bonds with both p-ASA and ROX as a secondary interaction to further reinforce the as-formed As–O–Zr complex. This work revealed that making cooperation by defect creation and amino modification could be an effective method to enhance the adsorption affinity of MOFs to low-concentration organoarsenic.
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NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 43
·16981-16989
·
IF 3.069
Bingying Jia,Miaojiang Wu,Hua Zhang,Yi Zeng,Gongying Wang
Titanates are frequently used as precursors to prepare transesterification catalysts with TiIV species. Unfortunately, it is challenging to control the dispersity of TiIV active sites on supports. Herein, a series of TiIV species is anchored on abundant linker vacancy sites by introducing point and large scale defects in UiO-66(Zr/Ti) with hierarchical-pore structure. The catalyst functionalized by titanium(IV) oxide bis(2,4-pentanedionate) shows excellent catalytic performance in the transesterification of dimethyl carbonate with phenyl acetate. The catalysts are characterized by XRD, FT-IR, N2 adsorption–desorption, XPS, SEM and STEM-HAADF techniques. The results demonstrate that the delicate mesopores in the support can not only exhibit a large surface area for the distribution of the active sites, but also provide better mass transfer performance. Meanwhile, the introduction of octahedral TiIV ions raises the activity of the catalyst via more coordinatively unsaturated ZrIV sites. Furthermore, using titanium(IV) oxide bis(2,4-pentanedionate) as a Ti source can effectively prevent the condensation of tetrahedral TiIV species anchored on the hierarchical-pore UiO-66(Zr/Ti) support.
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危险品化学品经营许可证（带存储）