INORGANIC CHEMISTRY
·
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
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Omega
·
2020
·
IF 2.87
Fengqing Xiong,Danni Chen,Chenglong Ma,Limei Cao,Ji Yang
Electrochemical oxidation has been considered as an efficient method to degrade pharmaceuticals and personal care products. Maintaining low power consumption while increasing the number of oxidation intermediates is deserving of exploring. Herein, Ti/SnO2–Sb/Zr0.3Ir0.7O2 was prepared by Zr doped into IrO2 and used for Sulfamethoxazole (SMX) degradation. The addition of Zr significantly increased the electrochemically active area and facilitated the catalyst to degrade SMX dramatically at a lower overpotential. The extremely outstanding lifetime of catalysts can reach 800 h during the accelerated life test, which showed excellent stability and developmental prospects. The overpotential at 10 mA·cm–2 is about 329 mV, indicating that this electrode has a high oxygen evolution reaction activity. Furthermore, the electrical efficiency per log order for the electrode is only 8.50 kW h m–3 at 4 V. Our research provides new anode electrochemical catalysts for the degradation of organic pollutants.
研究领域:
环境科学
·
材料科学
·
电化学工程
✓ 已验证
DOI
高影响因子
Materials Today Communications
·
2022
·
IF 3.662
Liyu Chen,Jiaxin Yang,Youjian Yang,Yifan Zhang,Zhaowen Wang
In this study, we investigated the thermodynamics and kinetics of the aluminothermic reduction of ZrO 2 . The results of thermal analysis and isothermal heat treatment showed that the aluminothermic reduction of ZrO 2 was an exothermic reaction that occurred at . 958.8°C. The aluminothermic reduction process does not produce metal Zr, but when the stoichiometric number of Al:ZrO 2 was 13:3, Al 3 Zr and Al 2 O 3 can be obtained by the reaction. The activation energy of the reaction was 1589.89 kJ/mol, and the reaction order was 1.90. The aluminothermic reduction process and mechanism of ZrO 2 in the presence of potassium cryolite as the molten salt medium was also studied. The results showed that ZrO 2 dissolved in potassium cryolite molten salt and participated in the reduction reaction in the form of Zr–O–F complex ions, while the by–product Al 2 O 3 also dissolved in potassium cryolite to further promote the formation of the Al–Zr alloy.
研究领域:
冶金学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Beibei Zhang,Lihua Zhang,Jin Li,Jiawen Fu,Xiwei Qu
In the present work, a series of PVA and CS blend membranes were studied. These prepared membranes were evaluated by binary mixture gases of CO 2 /N 2 and CO 2 /CH 4 . The optimum ratio of PVA/CS for CO 2 permeance was achieved at 5:5. It recorded a CO 2 permeability of 20.8 GPU (1 GPU = 1 × 10 -6 ·cm 3 (STP)·cm −2 ·s −1 ·cmHg −1 ) with CO 2 /N 2 selectivity of 89.7, as well as CO 2 permeability of 10.2 GPU and CO 2 /CH 4 selectivity of 56.3. Secondly, two kinds of nanoparticle UiO-66 and UiO-66-NH 2 were used to prepare mixed matrix membranes. The effects of nanofiller content and chemical groups on gas permselectivity were investigated. Results show that the addition of nanoparticles can effectively improve the permselectivity of membrane. The mixed matrix membranes addition with UiO-66-NH 2 achieved the optimum CO 2 performance and these were following the order of PVA(5)/CS(5)-UiO-66-NH 2 > PVA(5)/CS(5)-UiO-66 > PVA(5)/CS(5). For all these membranes, the permeance and selectivity present initial increased and then decreased. Mixed matrix membranes addition UiO-66-NH 2 (containing 3.75 wt%) exhibits a CO 2 permeance of 32.77 GPU and CO 2 /N 2 selectivity of 93.47, as well as CO 2 permeance of 25.57 GPU and CO 2 /CH 4 selectivity of 70.1, which was beyond the 2008 Robeson upper bound.
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
Nanomaterials
·
2019
·Vol. 9
·期 5
·675
·
IF 4.034
Lei Zhu,Xi Li,Zhiying Liu,Lin Yao,Peng Yu,Ping Wei,Yanhua Xu,Xingmao Jiang
Mn-Ce-Zr-O catalysts doped with varying Mn content were prepared and assessed for the catalytic combustion of chlorobenzene (CB). Nanosized MCZ-0.67 catalyst with amorphous phase exhibited a high and stable catalytic activity among the studied catalysts, achieving 90% CB conversion at 226 °C and withstanding stability tests, including time-based stability and the successive influence of various operating conditions. Meanwhile, the MCZ-0.67 catalyst used showed good recyclability by calcination in air. Characterization results suggested that Mn doping played a dominant role in improving the catalytic performance, resulting in larger surface area, better redox properties and greater amounts of surface active oxygen. In addition, the introduction of Zr was also indispensable for maintaining the good catalytic performance of catalysts. Finally, trace amounts of polychlorinated by-products during CB oxidation were monitored and the oxidation process was discussed.Keywords:MnOx-CeO2-ZrO2;catalytic combustion;chlorobenzene;active oxygen;product analysis
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Green Processing and Synthesis
·
2023
·Vol. 12
·期 1
·
IF 4.3
Qinhui Ren,Yufu Ma,Fuhua Wei,Lan Qin,Hongliang Chen,Zhao Liang,Siyuan Wang
Zr-metal-organic frameworks (Zr-MOFs) were prepared by a solvothermal method and characterized by X-ray diffraction, scanning electron microscopy, and thermogravimetry. Zr-MOFs were used to remove doxycycline hydrochloride (DOC) from wastewater. According to the experimental results, the maximum adsorption capacity of DOC by Zr-MOFs within 5 h was 148.7 mg·g −1 . From the pseudo-second-order kinetics model, all R
2 values were greater than 0.99, which proved that the adsorption of DOC by Zr-MOFs was consistent with practice. According to the Freundlich isotherm model, the adsorption of DOC by Zr-MOFs proceeded via multilayer adsorption. The aforementioned results show that Zr-MOFs have good application prospects for removing DOC from wastewater.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
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.
研究领域:
材料科学
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化学工程
·
催化
✓ 已验证
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
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
·
催化化学
✓ 已验证
DOI
高影响因子
MICROCHIMICA ACTA
·
2024
·Vol. 192
·期 1
·1-11
·
IF 5.3
Chen Xueke,Huang Tongfu,Wang Xin,Wu Chunyan,Yi Fei,Wan Ziqiang,Zou Bao,Xiong Wei,Liao Fusheng,Fan Hao,Yin Zhaojiang
The ultrahigh-sensitive detection of H 2 S is reported using a novel dual-ligand metal–organic framework (MOF) electrochemiluminescence (ECL) sensor. By combining tetrakis(4-carboxyphenyl) porphyrin (TCPP) and 1,3,6,8-tetrakis(4-carboxyphenyl) pyrene (TBAPy) as ligands and employing zirconium as the metal source, a spindle-shaped Zr-PyTCPPMOF was successfully designed and synthesized. Notably, the multiple nitrogen structures of porphyrin provided abundant binding sites for sulfur (S), further enhancing the ECL signal of Zr-PyTCPPMOF. The sensor shows a good linear relationship in the 0.01–100 μM range, with a detection limit reaching 1.18 nM (S/N = 3). When analyzing actual serum samples, the recovery was between 96.6 and 106.2%. Ultimately, the dual-ligand ECL platform based on Zr-PyTCPPMOF achieved trace detection of H 2 S, which is expected to provide reliable technical support for early environmental monitoring and disease diagnosis. Graphical abstract
研究领域:
分析化学
·
环境科学
·
生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2024
·
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
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Zhuoxue Li,Yunlei Shi,Yimian Ding,Dazhen Xiong,Zhiyong Li,Huiyong Wang,Jikuan Qiu,Xiaopeng Xuan,Jianji Wang
A Pickering emulsion is a natural microreactor for interfacial catalysis in which an emulsifier is critical. Recently, a metal–organic framework (MOF) has attracted attention to emulsify water–organic mixtures for constructing a Pickering emulsion. However, a few stimuli-responsive Pickering emulsions based on MOFs have been reported, and the MOF emulsifiers cannot be regenerated at room temperature. Herein, the Zr-MOF with a rodlike morphology is synthesized using ionic liquid as a modulator and then modified with n-(trimethoxysilylpropyl)imidazole (C3im) to prepare a series of functionalized Zr-MOFs (MOF-C3im). It is found that MOF-C3im is an excellent emulsifier to construct stable and CO2-responsive Pickering emulsions even at low content (>0.20 wt %). Notably, the emulsification and demulsification of the emulsions can be easily and reversibly switched by bubbling of CO2 and N2 alternatively at room temperature because CO2 and imidazole molecules anchored on the Zr-MOF underwent a reversible acid–base reaction, resulting in an obvious change in the wettability of the emulsifier. As a proof of concept, the reduction reactions of nitrobenzene have been successfully carried out in these Pickering emulsions, demonstrating the efficient integration as a microreactor for chemical reaction, product separation, and emulsifier recycling under ambient conditions. This strategy provides an innovative option to develop stimulus-responsive Pickering emulsions for sustainable chemical processes.
研究领域:
材料科学
·
化学工程
·
催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Liangjun Zhou,Wenxi Wang,Dekang Xu,Zhenyu Wang,Zhibin Yi,Min Wang,Zhouguang Lu
Thermal quenching of luminescence is the most critical problem for rare earth doped phosphors used in light-emitting diodes (LEDs). Herein, we demonstrate that thermal quenching can be considerably suppressed via the negative thermal expansion effect in Zr(WO 4 ) 2 that serves as host for Eu 3+ red emission. The photoluminescence (PL) intensity is surprisingly enhanced by 130% when the temperature is raised from room temperature to 100 °C. As temperature further increases to 160 °C, the PL intensity turns to reduce, which is still 1.4 times of that at room-temperature. Moreover, Zr(WO 4 ) 2 :15%Eu phosphor has good durability, which still exhibits strong red luminescence (only 13% loss) after being kept in 85 °C/85% relative humidity chamber for 240 h. The anti-thermal quenching of Eu 3+ luminescence can be ascribed mainly to the following two factors: first one is the thermal-enhanced energy transfer between Eu 3+ ions induced by the contraction of Zr(WO 4 ) 2 unit-cell volume that leads to the strong structural rigidity of host lattice; second one would be electron traps in the host that favors the increase of electrons on the excited energy levels. This important anti-thermal quenching effect induced from the negative thermal expansion of the host matrix may stimulates a novel and efficient approach to design highly thermal stable phosphors for next-generation LEDs.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）