JOURNAL OF SOLID STATE CHEMISTRY
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2022
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IF 3.656
Lichuan Tan,Peng Wang,Ruowei Lu,Siwen Feng,Guangsong Yuan,Cuijuan Wang
Hollow MOFs nanoreactors with controlled shape, size, pore volume , and shell thickness have been considered as emerging materials for a variety of applications. Selecting environmentally friendly and cheap colloidal carbon (CNs) as the template, bimetallic hollow Ce/Zr-UiO-66 nanoreactors were synthesized. The PXRD , TEM , EDS and other characterization analysis proved that hollow structure was formed, accompanied with incorporating of Ce(III) in UiO-66 and the crystal morphology was good. Furthermore, bimetallic hollow Ce/Zr-UiO-66 was studied as a catalyst to catalyze the conversion of furfural (FF) to furfuryl alcohol (FAL) without exogenous hydrogen. The results showed that the hollow structure and bimetallic UiO-66 was beneficial to the catalytic reaction by modulating the ratio of Ce(III) and Zr(IV). Among then, the 1:4 ratio of Ce(III) and Zr(IV) displayed good catalytic activity, the conversion rate of FF was 95% and selectivity of FAL was 94%. This study opens a new avenue for further rational design and construction of well-performing MOFs nanoreactors.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
DALTON TRANSACTIONS
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2024
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IF 3.5
Zhengyan Wang,Chenhao Yuan,Dong Yang,Mifen Cui,Jihai Tang,Zhuxiu Zhang,Xu Qiao
It is of great significance to develop catalysts for the degradation of hexachlorobenzene from the industrial thermal process. In this paper, formic acid was used as a modulator to generate defect sites in Ce/Zr-UiO-66 with intrinsic Brønsted acidity. The defective formate ligands were removed through methanol–water vapor treatment to expose additional open metal sites with Lewis acidity. The intrinsic Brønsted acid sites of the resulting Ce/Zr-UiO-66-FA-P achieved a hexachlorobenzene degradation efficiency of 99.5% at 250 °C. The generated Lewis acid sites facilitated the C–C cleavage of degradation intermediates. More than 95.0% of the final products were CO2/CO, coupled with chlorinated alkanes/alkenes, which outperformed other benchmark metal oxide catalysts. The Ce/Zr-UiO-66-FA-P catalyst maintained its catalytic activity in the model industrial flue gas and humid environment. The degradation pathway of hexachlorobenzene was tracked using in situ FT-IR spectra.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
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2021
·
IF 5.097
Haojie Zhao,Beili Yi,Xiaomeng Si,Lei Cao,Longxing Su,Yanli Wang,Lien-Yang Chou,Jin Xie
Perfect crystals do not exist; however, the introduction of defects can tailor the physical and chemical properties of materials. Defects in metal–organic frameworks (MOFs) have been demonstrated to be important in many applications, including but not limited to catalysis, gas separation, and energy storage. While a few liquid-phase synthesis methods have been reported to prepare defect-rich UiO-66, the heavy use of organic solvents may cause irreversible environmental problems. Here, we present a green, rapid, and facile solid-state synthesis approach to prepare UiO-66. All UiO-66 crystals remain in the nanometer size due to the limited diffusivity of growth species in solid-state synthesis without a large quantity of the solvent. The defect concentrations can be fine-tuned by the content of ethanol addition. Defect-rich UiO-66 shows excellent catalytic activity to the ring opening of epoxides with alcohols. This work provides insights into the large-scale production of defect-rich MOFs.
研究领域:
材料科学
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催化化学
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环境科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Yun Fan,Haijun Zhang,Meihui Ren,Yichi Zhang,Yun Li,Longxing Wang,Jiping Chen
It is of great significance to develop the low-temperature catalysts for the reduction in emission of chlorinated aromatic hydrocarbons (CAHs) from the industrial thermal processes. In this work, the bimetallic Ce-Zr/UiO-66 catalysts were synthesized by a solvothermal method to degrade CAHs. Powder X-ray diffraction, Fourier transform infrared spectra and X-ray photoelectron spectroscopy analyses showed that cerium was successfully incorporated into the lattice of Zr/UiO-66 without destroying the structure of metal–organic frameworks. The activities of Ce-Zr/UiO-66 catalysts for CAHs degradation varied with the concentration of cerium. Ce 0.2 Zr 0.8 /UiO-66 with the highest surface area (1502 m 2 g −1 ) presented the highest efficiency (>85%) for hexachlorobenzene degradation at low heating temperature (100–150 °C) with less formation of polychlorinated dibenzo- p -dioxins and dibenzofurans. Appropriate amount of water (5 wt%) and nitrogen atmosphere were beneficial to improve degradation efficiency. The degradation products proved that hydrodechlorination and oxidation of CAHs both occurred on the catalysts.
研究领域:
环境化学
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催化
·
材料科学
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
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2022
·
IF 5.436
Haojie Zhao,Beili Yi,Xiaomeng Si,Wenda Bao,Lei Cao,Longxing Su,Yanli Wang,Lien-Yang Chou,Jin Xie
Metal–organic frameworks (MOFs), a new type of porous material, have shown many possible applications in gas storage and separation, biomedicine, catalysis, and so on. While most MOFs are synthesized through solvothermal synthesis where a large quantity of organic solvent is used, the green synthetic approach using a minimized amount of solvent is important to prevent irreversible environmental compacts. In this study, we successfully synthesized Zr-MOFs with SBUs (e.g., UiO-66 and MIL-140A) using a simple metal source and investigated the role of organic modulators in modulating the MOF structures during solid-state synthesis. Meanwhile, UiO-66 rich in defects synthesized via a solid-state conversion strategy shows good catalytic performance for the ring-opening of epoxides with alcohols. This work contributes to the understanding of the role of organic modulators in the solid-state synthesis of MOFs.
研究领域:
材料科学
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环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
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2021
·
IF 4.126
Xianxian Kong,Qianqian Pan,Shuang Song,Zhiqiao He,Tao Zeng,Yan Yu
The development of low-cost, high-performance, and stable photocatalytic materials is vital to achieving highly efficient solar-to-fuel conversion. We report the fabrication of a metal-doped Zr-UiO-66-NH2 ((M/Zr)-UiO-66-NH2) catalyst using a one-pot hydrothermal method via a single-step reaction. The optimized 0.5(Co/Zr)-UiO-66-NH2, 0.5(Ni/Zr)-UiO-66-NH2, and 0.5(Fe/Zr)-UiO-66-NH2 photocatalysts exhibit significant hydrogen evolution performance approximately 35.22, 13.84, and 1.58 times higher than Zr-UiO-66-NH2 under simulated solar light. The enhanced hydrogen production efficiency can be ascribed to the metal-to-metal charge-transfer excitation between Co (Fe or Ni) and Zr species and the improved light harvest. Their cooperating function favors the excitation and separation of photogenerated carriers, which leads to a marked increase in catalytic activity.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
OPTICAL MATERIALS
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2023
·
IF 3.9
Xiandi Yu,Qianshu Xia,Peng Liu,Yan Xu
Lanthanide-doped upconversion (UC) nanomaterials with zero background auto-fluorescence are of extensive interest in optical fields. Here, a NaYF 4 :Yb 3+ /Er 3+ @Zr-UiO-66 nanostructure was prepared by simultaneously encapsulating NaYF 4 :Yb 3+ /Er 3+ nanoparticles (NPs) and promoting the nucleation of UiO-66 under solvothermal condition. Traditional nanosize-surface induced defects and grain boundaries of NaYF 4 :Yb 3+ /Er 3+ upconversion nanoparticles (UCNPs) were greatly minimized; enabling a highly efficient energy transfer confirmed by the prolonged fluorescence lifetime and enhanced UC emission of NaYF 4 :Yb 3+ /Er 3+ @Zr-UiO-66 nanocomposite. The optical thermometry property of nanocomposite was investigated based on the fluorescence intensity ratio (FIR) technique in the temperature range of 303–393 K. The maximum relative temperature sensitivities (S r ) were calculated to be 1.02 and 0.73% K −1 based on a pair of thermally coupled energy levels (TCLs) of ( 2 H 11/2 → 4 I 15/2 , 4 S 3/2 → 4 I 15/2 ) and another pair of non-thermally coupled energy levels (NTCLs) of ( 2 H 11/2 → 4 I 15/2 , 4 F 9/2 → 4 I 15/2 ), respectively. Besides, it exhibited effective internal optical heating property due to the thermal excitation between the two adjacent TCLs of 2 H 11/2 and 4 S 3/2 in NaYF 4 :Yb 3+ /Er 3+ UCNPs as heated by increasing the laser power. This work demonstrates a feasible confined synthesis of NaYF 4 :Yb 3+ /Er 3+ @Zr-UiO-66 nanocomposite with extreme UC emitting performance, and it holds great potential acting as both ratiometric thermometer and optical heater for multifunctional applications.
研究领域:
材料科学
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光学工程
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Fangfang Li,Jinjin Wang,Ying-Hua Zhou
Metal-organic frameworks (MOFs) possess highly tunable structures, making them promising heterogeneous catalysts for efficient CO 2 conversion reactions. In this work, cerium-modified zirconium-based metal-organic frameworks (ZrCe-UiO-66) were engineered and post-synthetically functionalized with dicationic ionic liquid moieties, enabling the simultaneous introduction of strong Lewis acidic sites and nucleophilic ionic liquid units without the need for external co-catalysts. The resulting ZrCe 0.5 -UiO-66-DIL(n-PyRIm) ( n = 2, 3, 4; R = Et, Pr, Bu, Pe) functionalized MOFs were prepared via a modular grafting approach and exhibited remarkable catalytic performance. Among them, ZrCe 0.5 -UiO-66-DIL(2-PyBuIm) converted epichlorohydrin into the corresponding cyclic carbonate with 96% yield and 98% selectivity under solvent-free conditions at 110 °C and a CO 2 pressure of 0.1 MPa. This outstanding activity arises from a cooperative activation mechanism, in which the mixed Zr 4+ /Ce 4+ activate the epoxide substrate through Lewis acid coordination with the epoxide oxygen, thereby facilitating C O bond activation, while the bromide anions embedded in the ionic liquid moieties promote nucleophilic ring opening. In addition to high catalytic efficiency, the MOF hybrids demonstrated excellent recyclability and broad substrate tolerance. Combined CO 2 adsorption measurements and in situ infrared spectroscopy further revealed key surface intermediates, enabling a plausible mechanistic pathway for the cycloaddition process to be proposed.
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Yunlong Li,Miao Liu,Yixian Liu,Lilong Zhou,Jilong Han,Zhengjie Li,Jimmy Yun,Runjing Liu
Two kinds of Ce-doped UiO-66 were synthesized by using CeCl 3 ·7H 2 O and (NH 4 ) 2 Ce(NO 3 ) 6 as cerium precursors, namely Ce(III)- and Ce(IV)-UiO-66. The effect of valence states of cerium precursors on adsorption performance towards Rhodamine B (RhB) was investigated for the first time. Ce atoms are in two valence states of +3 and + 4, where Ce 3+ ions turn their surfaces negatively charged. The higher cerium content (24.8%) and ratio of Ce 3+ /Ce 4+ ions (1.4:1) of Ce(IV)-UiO-66 made its surface more negatively charged, which is contributed to form stronger electrostatic interaction with cationic dyes. The adsorption amounts of RhB were 239.5 mg/g and 431.7 mg/g for Ce(III)- and Ce(IV)-UiO-66, which are 2.38 and 5.11 times higher than pristine UiO-66, respectively. The well-fit Langmuir model and pseudo-second-order model suggest a monolayer chemisorption process. The adsorption mechanism suggests that the electrostatic interaction and the complexation interaction between Ce 3+ and RhB are dominant factors affecting RhB adsorption. Since Ce 3+ severed as adsorption sites, the higher Ce content and stronger electrostatic interaction of Ce(IV)-UiO-66 together promoted its RhB adsorption than Ce(III)-UiO-66. The obtained results help to understand how the mixed-valences of incorporated metals affect the adsorption behaviors of bimetallic MOFs deeply.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
FOOD CHEMISTRY
·
2024
·
IF 8.5
Yiming Dong,Yu Zhang,Puyue Liu,Shiyi Zhu,Xuewen Peng,Xiaobo Hu,Xiya Zhang,Yiping Chen
Ensuring the safety of animal-derived foods requires the reliable and swift identification of enrofloxacin residues to monitor the presence of antibiotics. In this regard, we synthesized, tuned, and investigated the optical properties of a bimetallic metal–organic framework (Ce/Zr-UiO 66). The investigation was facilitated by employing a polydopamine-coated pipette tip with high adsorption efficiency, serving as an immunoreactive carrier. Subsequently, an immunofunctionalized variant of Ce/Zr-UiO 66, referred to as Ce/Zr-UiO 66@ Bovine serum albumin-enrofloxacin, was developed as an optical probe for the rapid and sensitive identification of enrofloxacin across a variety of samples. The method can accurately detect enrofloxacin at concentrations as low as 0.12 ng/mL, with a determination time of under 15 min; furthermore, it demonstrates exceptional efficacy when applied to food, environmental, and clinical samples. The implementation of this methodology offers a valuable means for cost-effective, rapid, and on-site enrofloxacin determination.
研究领域:
分析化学
·
食品安全
·
材料科学
·
生物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）