Molecular Catalysis
·
2022
·
IF 5.089
Ji Wang,Shuqing Zhang,Yiming Han,Lilei Zhang,Qingyin Wang,Gongying Wang,Xiaoming Zhang
PET (poly(ethylene terephthalate)) is one of the most important type of thermoplastic polyesters and widely used in various fields. Titanium-based catalysts are environmentally friendly and have higher catalytic activity than antimony-based catalysts when used in industry. However, titanium-based catalysts are prone to hydrolysis and result in discolored products. UiO-66 (Zr/Ti) with different Ti 4+ contents were successfully synthesized via one-step method. The material was characterized by XRD, SEM, FT-IR, XPS, BET and TG techniques. The results demonstrates that Ti 4+ was integrated into the UiO-66 framework. NH 3 - in situ DRIFTS, pyridine-IR, and NH 3 -TPD were used to explore the acidic properties of the samples, which proved that stable Lewis acidic sites are present in the samples even at 300 °C. The catalytic performance of UiO-66 (Zr/Ti) containing different Ti 4+ was explored under different conditions. At the same time, the scale-up experiment was carried out in a 5 L reactor, and the PET chips obtained had a lower b value. The catalytic reaction mechanism of UiO-66(Zr/Ti) was demonstrated by DFT calculations and the catalytic performance was close to Sb-based catalysts.
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高影响因子
FUEL
·
2018
·
IF 4.908
Xiong-Fei Zhang,Zhongguo Wang,Yi Feng,Yuxia Zhong,Jiaqiang Liao,Yaquan Wang,Jianfeng Yao
Metal organic frameworks (MOFs) have recently emerged as promising candidates for efficient removal of sulfur-containing compounds (SCCs) from liquid fuels. In this study, adsorptive desulfurization (ADS) is performed by adsorbing thiophene (TP) and benzothiophene (BT) from model fuels over pristine and functionalized UiO-66 (Zr). The introduction of amino ( NH 2 ) and carboxylic ( COOH) groups reduces the porosity of UiO-66. However, the adsorption capacities of functionalized UiO-66 improved remarkably. Especially for the adsorbent functionalized with amino moieties (UiO-66-NH 2 ), its maximum adsorption capacities for TP (29.5 mg S/g) and BT (35.7 mg S/g) are 1.7 and 1.8 times to that of bare UiO-66. The superior performance of UiO-66-NH 2 is ascribed to the higher availability of hydrogen-bond donor sites in the surface and the favorable interactions between H atoms of NH 2 and sulfur species. UiO-66-COOH is beneficial for the adsorption of SCCs than that of pristine UiO-66 because of the existence of acid-base interactions. Moreover, the reusability of UiO-66-NH 2 is confirmed by regenerating it via a simple solvent washing.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2017
·
IF 3.133
Fan Yang,Weiyang Li,Bohejin Tang
An amorphous metal-organic framework (aMOF) UiO-66 (Zr-MOF) was prepared directly from synthesis, different from experiments involving heating, pressure, and ball-milling by other researchers. The as-prepared amorphous UiO-66 has been successfully used as a supercapacitor electrode material, exhibiting a high specific capacitance (920 F g −1 at 10 mV s −1 ) superior to crystalline UiO-66. It has been verified that the material after reaction can still remain amorphous state by transmission electron microscopy (TEM). The capacitance of amorphous UiO-66 can maintain 610 F g −1 after 5000 cycles, suggesting its promising potential as a supercapacitor electrode material.
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高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Yan Yin,Yueyang Xu,Konglu Guo,Peng Zhang,Yongping Zeng
Adsorptive desulfurization is one of the alternative technologies for the effective removal of sulfides from fuels. Functionalization of metal-organic frameworks (MOFs) with Cu + is extremely desirable for adsorption separation via π-complexation interaction with adsorbed molecules. Here we report that Cu + cation is significant and highly effective for adsorption desulfurization in a new type of Cu + - modified UiO-66(Zr). First, Cu 2+ was introduced via ion-exchange with H + of UiO-66-SO 3 H. Then, Cu + cation was obtained from the reduction of Cu 2+ by using vapor-induced reduction, in which vapors of reducing agents diffuse into the pores of MOFs at a lower temperature. The resulted UiO-66-SO 3 Cu(I)− 0.15 has a better adsorption capacity for thiophene compared to pure UiO-66. In the presence of toluene, the UiO-66-SO 3 Cu(I)− 0.15 also exhibits high adsorption capacity for thiophene. After recycling four times, UiO-66-SO 3 Cu(I)− 0.15 still remains a high adsorption capacity.
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RSC Advances
·
2019
·Vol. 9
·期 65
·37733-37738
·
IF 3.049
Yanghe Fu,Jieyu Wu,Rongfei Du,Ke Guo,Rui Ma,Fumin Zhang,Weidong Zhu,Maohong Fan
Defect engineering can be a promising approach to improve the photocatalytic performance of metal–organic frameworks (MOFs). Herein, a series of defective NH2-UiO-66(Zr) materials were synthesized via simply controlling the synthesis temperature, with concentrated HCl as the modulator and then these as-prepared samples were used to systematically investigate the effects of their structural defects on photocatalytic CO2 reduction. Remarkably, these MOFs with defects exhibit significantly enhanced activities in photocatalytic CO2 reduction, compared with the material without defects. The defect engineering creates active binding sites and more open frameworks in the MOF, and thus facilitates the photo-induced charge transfer and restrains the recombination of photo-generated charges efficiently. The current work provides an instructive approach to improve the photocatalytic efficiency by taking advantage of the structural defects in MOFs, and could also inspire more work on the design of advanced defective MOFs.
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DOI
PubMed
高影响因子
FUEL
·
2017
·
IF 4.601
Xiaotian Zhang,Pengcheng Huang,Aili Liu,Mingyuan Zhu
Owing to the high prices and other shortcomings associated with the existing methods of complex catalyst preparation, we used the UIO-66(Zr) metal–organic frameworks to directly catalyze the oxidative desulfurization (ODS) reaction. The synthesized UIO-66(Zr) was characterized using nitrogen adsorption–desorption isotherm analysis, X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. Under optimal reaction conditions, the ODS conversion of dibenzothiophene (DBT) reached 100%. This excellent catalytic activity was attributed to the unsaturated coordination of Zr, which may produce beneficial Lewis acid sites.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Konglu Guo,Yueyang Xu,Yan Yin,Yongping Zeng
Adsorption desulfurization can effectively remove thiophene-containing compounds in fuels. UiO-66 is a potential candidate for adsorption desulfurization due to the excellent chemical stability and resistances to acids and alkali. However, the adsorption capacity is relatively low for the big molecules of sulfide (such as thiophenes) because of the pore size in the microporous structure. We used Zn 4 O(BC) 6 as a template to synthesize a new π-complexation adsorbent (H-UiO-66-SO 3 Cu(I)) via ion-exchange and steam-induced reduction, with hierarchical porous (microporous and mesoporous) structure. The adsorbent was characterized by FT-IR, XRD , SEM , TEM and N 2 adsorption-desorption isotherms. The results show that H-UiO-66-SO 3 Cu(I) has the stable structural properties with the new mesopores . H-UiO-66-SO 3 Cu(I) has a good adsorption performance for thiophene and benzothiophene in the model fuel. The regeneration results show that H-UiO-66-SO 3 Cu(I) can be recycled four times and still has good adsorption performance.
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RSC Advances
·
2015
·Vol. 6
·期 5
·3671-3679
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IF 3.84
Aoning Wang,Yingjie Zhou,Zhoulu Wang,Miao Chen,Luyi Sun,Xiang Liu
A UiO-66-type metal–organic framework (MOF) fabricated with titanium was successfully prepared via a facial modified post-grafting method. The as-prepared samples were characterized by X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), ultraviolet-visible adsorption spectroscopy (UV-vis), and photoluminescence spectroscopy (PL) techniques. The introduction of titanium enhanced the optical properties of UiO-66 via the formation of oxo-bridged hetero-Zr–Ti clusters, but led to a sacrifice in crystallinity. The removal of methylene blue (MB) over these samples could be attributed to the dual function of the adsorption and photo-degradation mechanisms. The highest MB removal efficiency of 87.1% was achieved over UiO-66(1.25Ti) under simulated sun-light irradiation.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Zai-Dong Shao,Peng Wu,Fang Liu,Qi-Jun Zhang,Chao-Yang Guo,Rui-Sang Liu,Jiang Lu,Xiao-Meng Ren,Yu-Ming Zheng
Sulfur dioxide (SO 2 ) emissions present significant environmental and health risks, yet efficiently capturing SO 2 remains challenging due to its corrosive nature and the limited performance of conventional adsorbents. In this study, we developed multivariate metal-organic frameworks (MTV-MOFs) based on UiO-66(Zr) for effective SO 2 capture. Through systematic ligand functionalization with -OH, -NH 2 , -SO 3 H, and -(NH 2 ) 2 groups on terephthalic acid linker, we developed a series of MTV-UiO-66 materials with tailored pore environments and adsorption characteristics. UiO-66-NH 2 exhibited superior performance with an SO 2 uptake of 252.9 mL g −1 at 298 K and 1 bar. Ideal adsorbed solution theory (IAST) calculations demonstrated improved selectivity for SO 2 over N 2 (847) and CO 2 (31), surpassing that of the parent UiO-66. Dynamic breakthrough experiments further confirmed the practical viability of MTV-UiO-66 materials for SO 2 capture under both dry and humid (50 % RH) conditions, with UiO-66-NH 2 retaining a capacity of 30.73 mL g −1 in dry settings and exhibiting robust performance in moisture-rich environments. Grand Canonical Monte Carlo (GCMC) simulations and density functional theory (DFT) calculations provided molecular-level insights into the adsorption mechanisms, revealing that functional groups play a crucial role in modulating binding interactions through hydrogen bonding, dipole-dipole interactions, and spatial confinement effects. The computational binding energies corroborated the experimental isosteric heats of adsorption, validating the integrated experimental-computational approach.
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高影响因子
MICROCHEMICAL JOURNAL
·
2025
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IF 5.1
Daidai Wang,Ying Cao,Moustafa Zahran,Xinchun Liu,Xiaoyue Hui,Ahmed S. Abou- Elyazed,Hui-Ying Qu,Xiaolin Li
This study reports a novel electrochemical sensor based on a metal-organic framework (MOF) derivative to measure urea in sweat. The MOF structure, UiO-66(Zr), was greenly synthesized using a solvent-free thermal method, functionalized with molybdenum disulfide (MoS 2 ), and then thermally treated to form carbon-coated UiO-66(Zr)@MoS 2 . The MOFs were characterized by X-ray diffraction, an N 2 adsorption instrument, scanning electron microscopy, and an X-ray photoelectron spectrometer. Among the prepared MOFs, the carbon-coated UiO-66(Zr)@MoS 2 showed many crystal defects, providing more active sites required to improve the electrocatalytic activity, and high carbon content to enhance the electrical conductivity of the stainless steel (SS) electrode. The electrocatalytic activity of the MOFs was evaluated using cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and square wave voltammetry (SWV). CV studies showed poor catalytic activity of bare SS electrode and its modifiers, UiO-66(Zr), carbon-coated UiO-66(Zr), and UiO-66(Zr)@MoS₂, towards urea (0.1 mM) oxidation. In contrast, the carbon-coated UiO-66@MoS₂ modifier exhibited a urea oxidation peak with a current value of 5 μA, confirming its high electrocatalytic activity. Compared to CV, SWV exhibited a higher oxidation peak current (7.5 μA). Additionally, the EIS showed a 38.4 % reduction in the electron transfer resistance after SS electrode modification with the carbon-coated UiO-66(Zr)@MoS₂. The SWV sensor exhibited lower detection and quantification limits of 0.4 and 1.4 μM, respectively. Additionally, it showed high selectivity in the presence of possible interfering substances, such as glucose, lactic acid, ascorbic acid, cortisol, and sodium chloride. Moreover, its efficacy for measuring urea in artificial sweat samples was proved with acceptable recovery values.
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高影响因子
TURKISH JOURNAL OF CHEMISTRY
·
2026
·Vol. 50
·期 3
·285-299
·
IF 2
LI JUANHONG,WANG SUQIN,LIU XIN,LIU FENG
A [H]-accelerated catalytic Fenton system was developed using Pd/UiO-66(Zr)-F4 as the catalyst. This system enabled the regeneration of Fe²⁺ and facilitated the continuous generation of both ·OH and 1O2 through [H]-mediated electron transfer at ambient temperature and pressure. Under the conditions of 0.2 g L−1 catalyst (Pd loading 0.516 wt%), 25 μM Fe2+, 60 mL min−1 H2 flow (as the [H] source), 20 mM H2O2, and pH 3, approximately 89% of carbamazepine (initial concentration 20 mg L−1) was degraded within 3 h using trace iron. However, the catalytic activity of Pd/UiO-66(Zr)-F4 gradually declined from 89% to 53% over six reaction cycles. This decrease was likely due to loss of specific surface area caused by microstructural degradation associated with hydrogen spillover effects.
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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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