Frontiers in Chemistry
·
2022
·
IF 5.545
Zhao Kangyu,Xiang Yanping,Sun Xiaoao,Chen Linjiao,Xiao Jiafu,Liu Xianxiang
In this study, a novel sulfonic acid-modified catalyst for MOFs (UIO-66-SO3H) was synthesized using chlorosulfonic acid as a sulfonating reagent and first used as efficient heterogeneous catalysts for the one-pot conversion of fructose into biofuel 5-ethoxymethylfurfural (EMF) in a cosolvent free system. The physicochemical properties of this catalyst were characterized by Fourier transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM), and powder X-ray diffraction (XRD). The characterization demonstrated that the sulfonic acid group was successfully grafted onto the MOF material and did not cause significant changes to its morphology and structure. Furthermore, the effects of catalyst acid amount, reaction temperature, reaction time, and catalyst dosage on reaction results were investigated. The results showed that the conversion of fructose was 99.7% within 1 h at 140°C, while the EMF yield reached 80.4%. This work provides a viable strategy by application of sulfonic acid-based MOFs for the efficient synthesis of potential liquid fuel EMF from renewable biomass.
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PubMed
高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 153
·期 3
·836-849
·
IF 2.936
Jiang Haoran,Xue Changhao,Sun Weijie,Gong Zhaoxiang,Yuan Xia
The esterification of cyclohexene with formic acid is the first step in synthesizing cyclohexanol via the indirect hydration of cyclohexene. In this work, we improved the efficiency of the esterification reaction by constructing a sulfonic-acid-functionalized UiO-66 solid-acid catalyst containing defect sites. By using acetic acid as the modulator, ZrCl 4 as the zirconium source, and 2-sulfoterephthalic acid monosodium salt as the ligand, a sulfonic-acid-functionalized UiO-66-SO 3 H with defect sites was prepared using a solvothermal synthesis method. Additionally, we also prepared UiO-66 with defect sites for comparison. We then investigated the regulation effects of acetic acid addition amount on the defect structures and acidity of the as-prepared materials. The results showed that the addition of acetic acid caused lattice defects in the as-prepared materials with a missing linker, and the specific surface area, pore volume, pore size, and particle size of the material changed significantly. The number of defect sites was determined by thermogravimetric analysis. Additionally, pyridine infrared spectroscopy and X-ray photoelectron spectroscopy (XPS) analysis indicated that the ratio of Lewis acid to Brønsted acid sites, and the total acid content in the defect materials, greatly increased compared to pure UiO-66 and UiO-66-SO 3 H, which greatly enhanced the acid catalytic performance of the material. Among these, UiO-66-SO 3 H(20), which was prepared by adding 20 mL of acetic acid, exhibited the best catalytic activity. The conversion rate of cyclohexene reached 83.4%, the selectivity toward cyclohexyl formate was 99.8%, and the catalyst could be reused three times. Graphical Abstract The purpose of this work was to improve the efficiency of the esterification reaction of cyclohexene with formic acid by constructing a sulfonic acid-functionalized UiO-66 solid acid catalyst containing defective sites. The regulation effect due to the amount of acetic acid added on the defect structure and acidity of the as-prepared materials was investigated.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2022
·Vol. 139
·期 24
·52332
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IF 3.057
Xibin Wu,Zhimei Wei,Jie Yang,Gang Zhang,Shengru Long,Xiaojun Wang
The purification of dye wastewater plays a critical role in water pollution treatment. Adsorption is a cheap and effective separation technology but is limited by the reuse of adsorption materials. Ultrafiltration membranes have a relatively high flux but their pores are too large to reject small dye molecules. In this study, negatively charged oxidized poly (arylene sulfide sulfone) (O-PASS) membrane, NMP pretreatment oxidized O-PASS (N-O-PASS) membrane, and O-PASS@UiO-66-NH 2 /O-PASS composite membranes were fabricated to retain cationic methylene blue (MB) from wastewater by combining ultrafiltration and adsorption techniques. The increased porosity of the N-O-PASS membrane provides more available adsorption sites for an equilibrium MB adsorption amount of 22.5 (mg g −1 ) and 100% rejection in the first 10 min during ultrafiltration with a pure water flux of 162.32 (L m −2 h −1 bar −1 ). Due to the enhanced hydrophilicity and separating property by deposited UiO-66-NH 2 particles and PASS resin, O-PASS@UiO-66-NH 2 /O-PASS composite membrane shows a flux of 170.32 (L m −2 h −1 bar −1 ) and a 100% MB rejection in 60 min with great reusability. The O-PASS@UiO-66-NH 2 /O-PASS composite membrane is a new promising membrane for the removal of dyes from wastewater. Meanwhile, the superior solvent resistance endows it great adaptability in wide applications, especially in harsh conditions.
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Polymers
·
2022
·Vol. 14
·期 2
·283
·
IF 4.967
Wei Chen,Ping Zhu,Yating Chen,Yage Liu,Liping Du,Chunsheng Wu
Iodine has been widely used as an effective disinfectant with broad-spectrum antimicrobial potency. However, the application of iodine in an antibacterial polymer remains challenging due to its volatile nature and poor solubility. Herein, iodine immobilized UiO-66-NH2metal-organic framework (MOF) (UiO66@I2) with a high loading capacity was synthesized and used as an effective antibacterial additive for poly(ε-caprolactone) (PCL). An orthogonal design approach was used to achieve the optimal experiments’ conditions in iodine adsorption. UiO66@I2nanoparticles were added to the PCL matrix under ultrasonic vibration and evaporated the solvent to get a polymer membrane. The composites were characterized by SEM, XRD, FTIR, and static contact angle analysis. UiO-66-NH2nanoparticles have a high iodine loading capacity, up to 18 wt.%. The concentration of iodine is the most important factor in iodine adsorption. Adding 0.5 wt.% or 1.0 wt.% (equivalent iodine content) of UiO66@I2to the PCL matrix had no influence on the structure of PCL but reduces the static water angle. The PCL composites showed strong antibacterial activities againstStaphylococcus aureusandEscherichia coli. In contrast, the same content of free iodine/PCL composites had no antibacterial activity. The difference in the antibacterial performance was due to the different iodine contents in the polymer composites. It was found that MOF nanoparticles could retain most of the iodine during the sample preparation and storage, while there was few iodine left in the free iodine/PCL composites. This study offers a common and simple way to immobilize iodine and prepare antibacterial polymers with low antiseptic content that would reduce the influence of an additive on polymers’ physical properties.Keywords:UiO-66-NH2metal-organic framework;iodine;poly(ε-caprolactone);antibacterial
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Jiajun Yu,Xiao Wang,Lu Chen,Guanhong Lu,Gansheng Shi,Xiaofeng Xie,Yan Wang,Jing Sun
The development of photocatalytic materials with both promising adsorption capacity and high visible-light activity is essential for the highly-efficient and stable photocatalytic degradation of toluene. In this work, a series of carbon quantum dots (CQDs) decorated UiO-66 metal–organic-frameworks gel (MOG) composites (CQDs/UiO-66 MOG) with hierarchical pore structures were prepared. The introduction of CQDs effectively improved the light utilization and promoted the separation of photo-induced electrons and holes, which were beneficial for the generation of active free radicals. Besides, benefiting from the hierarchical pore structure of UiO-66 MOG and the new adsorption sites provided by CQDs, 0.5 wt% CQDs/UiO-66 MOG showed a high toluene adsorption capacity (29.06 μmol/g) and its enhanced degradation efficiency for toluene was 4.4 times higher than that of pristine UiO-66 MOG. Both in-situ Fourier transform infrared (FTIR) and Gas Chromatography–Mass Spectrometer (GC–MS) were conducted to give the possible degradation pathways. Toluene was firstly converted into xylene and benzene, and then degraded into acids, aldehydes, alcohols before fully mineralized into carbon dioxide. A relatively high CO 2 conversion ratio (85%) of toluene was obtained when applying 0.5 wt% CQDs/UiO-66 MOG as the photocatalyst, together with less intermediates detected, confirming the positive role of CQDs decoration in the effective mineralization of toluene. This work sheds new light on MOG material optimization and degradation of low-concentration flowing toluene.
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RENEWABLE ENERGY
·
2021
·
IF 8.001
Hui Li,Yongbo Wang,Xiaoling Ma,Min Guo,Yan Li,Guoning Li,Ping Cui,Shoujun Zhou,Mingzhi Yu
Ca 2+ ion leaching and poor pore structure are obstacles of CaO for biodiesel production . To this end, a typical Zr–based metal organic framework, UiO–66(Zr) is adopted to support calcium acetate to prepare CaO/ZrO 2 catalyst. For comparison, catalyst precursor is activated in nitrogen (UCN) and air (UCA) atmosphere, respectively. Preparation factors including calcium acetate addition and activation temperature are evaluated. Moreover, effects of transesterification parameters on oil conversion are investigated and the optimized parameters are further used to examine catalyst reusability . Meanwhile, catalysts are characterized with TG, XRD, XPS , FTIR, Hammett indicator titration, N 2 adsorption and desorption. Results reveal UCN calcined at 650 °C (UCN650) and UCA calcined at 700 °C (UCA700) separately exhibits the best catalytic performance. The maximum conversion of 96.99% is achieved by UCN650 with catalyst amount of 6 wt% and molar ratio of methanol to oil of 9 at 65 °C for 60 min. Even after being used 3 cycles, conversion of 92.76% is still achieved by UCN650. By contrast, UCA700 shows lower conversion of 92.94% at the first cycle with catalyst amount of 8 wt% and molar ratio of methanol to oil of 9 at 65 °C for 60 min.
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OPTICAL MATERIALS
·
2023
·
IF 3.9
Siyue Wang,Xiaoman Teng,Chao Liu,Hanfei Zhu,Hongbu Cheng,Jing Yan,Li Wang,Zhenyan Liang,Jun Ouyang
Due to a synergistic effect of piezo-catalysis and photocatalysis , piezo-photocatalysis is gaining popularity as an effective approach to remove organic pollutants. In this work, single-component piezo-photocatalytic nanoparticles of UiO-66-NH 2 (Hf) metal-organic frameworks were prepared by a hydrothermal process with an average diameter of ∼52.6 nm. An ultrafast piezo-photocatalysis degradation of RhB solution was achieved by using the UiO-66-NH 2 (Hf) nanoparticles . Under UV light and ultrasound irradiation, the percentage of dye degradation for an initial RhB concentration of 5 mg/L reached 91 % in 60 s. The removal mechanism of RhB was investigated via capture experiments of active species, which revealed that the hydroxyl radicals and hole play a key role in the degradation of RhB. This work provides a reference for the piezo-photocatalytic capability and the underlying mechanism of single-component metal-organic framework based nanomaterials , promoting their further development in technological applications involving highly efficient catalysts.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Huimin Ruan,Nengxiu Pan,Chao Wang,Lu Yu,Junbin Liao,Jiangnan Shen
Metal–organic frameworks (MOFs) have a good separation potential due to their uniform pore size, easy functionalization, and adjustable structure. Therefore, we make use of this feature of MOFs for the separation of Cl–/SO42– systems with different charges and sizes. In this work, two kinds of UiO-66 membranes with different functional groups were synthesized and applied to the monovalent perm-selective separation of the Cl–/SO42– system in electrodialysis (ED). UiO-66-NH2 membranes were used to investigate the influence of current density and initial solution concentration on perm selectivity. A layer of UiO-66-NH2 was first grown on the anodic alumina oxide (AAO) disks. After that, short chains containing sulfonic acid groups were grafted onto the amino groups by the ring-opening reaction of 1,3-propanesulfonate. The structural stability of the MOF layer was confirmed by XRD analysis of the membrane surface after the ED test. Ion exchange capacity (IEC) and elemental mapping were used to confirm the comparison changes in the degree of sulfonation. It was found that UiO-66-NH2 membranes exhibited a higher monovalent anion perm selectivity with a peak value of 36.23 (initial mixture solution of 0.05 M NaCl and 0.05 M Na2SO4) at lower current density (2.5 mA·cm–2). The perm selectivity of UiO-66-SO3H membranes increased with running time under 24 h of sulfonation time. In particular, with low IEC value of 0.10–0.16, it still showed a good performance on perm selectivity. Compared with published polymer ion exchange membranes (perm selectivity < 5) for ED, it has higher perm selectivity, more convenient functionalization, and resistance to organic solvents.
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高影响因子
ACS Applied Energy Materials
·
2026
·
IF 5.5
Wang Jiaxuan,Zhang Tongtong,Kawi Sibudjing,Li Yinhui
The development of high-energy-density lithium-metal batteries (LMBs) has imposed increasingly stringent requirements on the thermal stability, ionic conductivity, and interfacial compatibility of separators. To address the inherent drawbacks of conventional polypropylene (PP) separators, such as inadequate thermal stability and poor electrolyte wettability, a polyimide (PI) separator was fabricated via the nonsolvent induced phase separation (NIPS) method in this work. Furthermore, by introducing metal-organic framework (MOF) materials (UiO-67) into PI slurry, a PI/UiO-67 composite separator was successfully constructed, which achieves the synergistic optimization of the pore structure, surface morphology, and mechanical properties of the separator. The results demonstrate that the PI/UiO-67 composite separator retains the excellent thermal stability of the PI matrix, with no thermal shrinkage observed at 200 ° C, while simultaneously exhibiting significantly improved electrode–electrolyte interfacial compatibility. Compared with the commercial PP separator (bulk resistance 2.97 Ω, interfacial impedance 165 Ω), the composite separator possesses a lower bulk resistance (2.28 Ω) and interfacial impedance(122 Ω). Additionally, integrating UiO-67 considerably improves the wettability of the electrolyte and the lithium-ion transference number (0.61) in the separator, which in turn markedly boosts the electrochemical stability and the long-cycle performance of LMBs. LMBs utilizing the PI/UiO-67 separator achieve a notable capacity retention of 87.4% after 150 cycles at a rate of 0.5 C. In tests conducted with lithium symmetric cells, stable cycling performance is observed for more than 600 h at a current density of 0.2 mA cm –2 . This study offers a valuable composite approach and theoretical insights for advancing the development of separators that ensure high safety and performance in LMBs.
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高影响因子
International Journal of Low-Carbon Technologies
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2023
·
IF 2.3
Wang Tingting,Yue Xiaoju,Han Lin,Wang Jinnong,Zhang Yuzhen,Tang Xiaofeng,Wang Shifeng
We reported anchoring mesoporous silica onto the microporous metal–organic frameworks (MOF) (UiO-66-NH2) to obtain a hierarchical porous framework (UiO-66-NH2@SiO2). This strategy maintains the high specific surface area (SA) of the MOF and addresses the mass transfer issue frequently encountered in microporous materials, providing more possibilities for subsequent modified structural frameworks. The structural characteristics of UiO-66-NH2@SiO2 were evaluated by Fourier transform infrared spectroscopy, X-ray diffraction, thermogravimetric analysis, scanning electron microscopy, surface analysis and X-ray photoelectron spectroscopy. In this work, the specific SA of the composite material was 196.667 m2/g, which decreased due to the occupation of some pores by anchored silica. Adsorption experiments showed that the composite material had a better adsorption effect (Congo red, 393.83 mg/g; bromophenol blue, 446.46 mg/g) than UiO-66-NH2, with electrostatic interaction and hydrogen bonding being the main driving forces. Therefore, this is a material that has a positive impact on dye adsorption. The strategy proposed in this work has potential applications not only in the construction of new materials but also in the exploration of dye adsorbents.
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高影响因子
Journal of Physical Chemistry C
·
2023
·
IF 3.7
Huan-Yu Chen,Xing-Biao Liu,Qi-Xin Guan,Can-Jun Zou,Ping-Ping Fang
The detection of antibiotics has attracted great attention among scientists and health researchers in the past decades. However, it is still difficult to realize the sensitive and selective detection of antibiotics with similar structures. Herein, the antibiotic molecules of oxytetracycline (OTC) can be sensitively and selectively detected by surface-enhanced Raman spectroscopy (SERS) on NH2–UiO-66(Zr)@Au nanoparticles (NPs). The SERS substrate of NH2–UiO-66(Zr)@Au NPs realizes a detection sensitivity of 1 × 10–12 g·L–1 for 4-mercaptobenzoic acid, indicating its high SERS activity. A high detection sensitivity of 10–11 g·L–1 is obtained for OTC on such a SERS substrate. Besides the high sensitivity, NH2–UiO-66(Zr)@Au NPs can also selectively detect OTC from streptomycin sulfate, salicylic acid, and ofloxacin by SERS on NH2–UiO-66(Zr)@Au NPs, with a selective detection limit of 10–10 g·L–1. Furthermore, OTC can be selectively detected in a real sample of river water with a detection limit of 1.0 × 10–10 g·L–1. Therefore, this study provides an effective way to enrich and detect antibiotics in real samples in the environment.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 40
·18865-18871
·
IF 3.3
Chao Liu,Gang-Gang Chang,Ting-Ting Luo,Yi-Tian Wang,Shi-Tian Xiao,Yao Yao,Hong-Jian Xu,Ge Tian,Christoph Janiak,Hai-Hu Yu,Xiao-Yu Yang
Metal–organic frameworks (MOFs) have great potential for producing photoelectrocatalyzed hydrogen and degrading pollutants, owing to several factors such as high porosity and tunable semiconductor-like properties. Wide band gaps, which restrict their use to only UV light induced reactions, and low efficiencies for the separation of photogenerated charge carriers (electrons and holes) pose significant challenges to the widespread applications of MOFs. In this study, a hierarchical hollow Pt@H-UiO-66-NH2/CdS ternary catalyst was designed and synthesized. The immobilized CdS nanoparticles (NPs) in this catalyst endow the MOF H-UiO-66-NH2 with high visible light absorption ability and the Pt NPs serve as electron sinks to improve charge carrier separation. Furthermore, the hierarchical hollow structure of H-UiO-66-NH2 in the composite contributes to boosting light absorption and shortening the distance for charge transfer. As a proof of principle, Pt@H-UiO-66-NH2/CdS catalyzes methylene blue (MB) degradation with a high rate constant of 1.025 × 10−2 and hydrogen production with a rate of 12 810 μmol g−1 h−1, the latter of which is about 2.3, 11.7 and 173 times higher than those of Pt@UiO-66-NH2/CdS, H-UiO-66-NH2/CdS and Pt@H-UiO-66-NH2, respectively.
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危险品化学品经营许可证（带存储）