Sustainability
·
2023
·Vol. 15
·期 18
·13382
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IF 3.9
Qihang Dai,Ju Liu,Junjie Zheng,Bo Fu
Metal–organic frameworks (MOFs) hold great potential for efficient removal of particulate matter (PM) due to their high porosity and tunable surface groups. In this work, sustainable bacterial cellulose (BC) was employed as a substrate for Zr-based MOF (i.e., UiO-66-NH2) deposition. Specifically, the UiO-66-NH2@BC aerogel exhibits a multi-level pore structure with a specific surface area of 103 m2/g. Pristine BC aerogels indicated a removal efficiency of 50.6% for PM2.5, with a pressure drop of 22.8 Pa. While UiO-66-NH2@BC aerogels showed a PM2.5removal efficiency of 96.9%. The filtration mechanism can be assigned to the following reasons: (i) the interception/impaction of PM with the fibrous and porous aerogel network; and (ii) the presence of polar amine groups that boost electrostatic interactions between PM and MOFs. Moreover, as-prepared filters can be regenerated in a facile way with good reusability and long-term stability.
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Catalysts
·
2023
·Vol. 13
·期 5
·876
·
IF 3.9
Huan He,Xusheng Wang,Qin Yu,Wenbin Wu,Xinya Feng,Deyu Kong,Xiaohui Ren,Junkuo Gao
Cr(VI) is one of the most toxic heavy metals, posing multiple threats to humans and ecosystems. Photoreduction of toxic Cr(VI) to para-toxic Cr(III) is one of the most effective ways to remove heavy metal chromium but is still challenging. Herein, Ti3C2/UiO-66-NH2composites with different ratio of Ti3C2were synthesized via an in situ solvothermal process and used for the enhanced photocatalytic removal of Cr(VI) for the first time. The UiO-66-NH2nanoparticles were dispersed on the surface and slits of accordion-like Ti3C2homogeneously. A strong interfacial interaction between Ti3C2and UiO-66-NH2was formed, which was indicated by the XPS. The Fermi level of the MXene cocatalyst is lower than UiO-66-NH2; thus, Ti3C2can serve as the electron sink and accumulate photogenerated electrons from UiO-66-NH2on its surface. A depletion layer was also formed due to the different Fermi levels of UiO-66-NH2and Ti3C2, which prevents electrons from flowing back to UiO-66-NH. The strong interfacial interaction and formed depletion layer are beneficial for the following charge transfer from UiO-66-NH2to Ti3C2after light irradiation and for suppressing the photogenerated charge recombination. With suitable band positions and enhanced charge separation ability, Ti3C2/UiO-66-NH2composites exhibited better photoreduction efficiency of Cr2O72−than pure Ti3C2and UiO-66-NH2, with optimized samples reaching 100% in 40 min. The photoreduction kinetics of Cr2O72−by 2-T/U was also studied, with a photoreduction rate of 0.0871 min−1, which is about 2.6 times higher than that of the pure UiO-66-NH. This research provides a new type of efficient and environmentally friendly photocatalysts for the photoreduction of Cr2O72−.Keywords:metal–organic frameworks;photocatalysis;MXene;Cr(VI);photocatalyst;photoreduction;porous materials
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Mengya Guo,Feng Wang,Mingwei Zhang,Li Wang,Xiangwen Zhang,Guozhu Li
Encapsulation of clean metal nanoparticles (NPs) into interior of metal–organic framework (MOF) is of great importance to remarkably improve the stability and tune the catalytic performance of metal NPs. Herein, highly dispersed Pt NPs are encapsulated in UiO-66 with different functional groups on linker (UiO-66-X, X = F, H, NH 2 , OH) through enhanced electron attraction of metal precursor by MOF node and proper reduction by H 2 /Ar gas. Compared with traditional impregnation method, the encapsulation method gives well-defined Pt NPs and controllable microenvironment. Detailed characterizations reveal that functional group of the linker can effectively tune the microenvironment and electronic properties of guest Pt NPs. In situ FTIR was utilized to investigate the adsorption capability and strength of reactants on the catalysts. The electron-deficient Pt species and appropriate surface hydrophobicity match well with the reactants, which is responsible for enhanced catalytic hydrogenation activity of C C and nitro groups. The surface hydrophobicity plays a major role in promoting alkyne hydrogenation. This work is devoted to rationalize the relationship between hydrogenation performance and catalyst property of UiO-66 encapsulated Pt NPs, in terms of energy adaptability in electronic state and structure adaptability in surface chemistry. Rational design strategy of Pt-confined-in-MOF composites through molecular level regulation is provided for hydrogenation.
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MATERIALS CHEMISTRY AND PHYSICS
·
2023
·
IF 4.6
Lin Yang,Tingjiao Liu,Zheng Li,Changqing Liu,Feifeng Wang,Chunshan Wu
The application of metal organic frameworks (MOFs) for the recovery of low concentrations of rare-earth elements (REEs) has attracted increasing attention due to the precious value of REEs resources. In this study, UiO-66-COOH was modified by trifluoroacetic acid (TFA) to not only promote material crystallization and the pore structure verified by XRD and SEM characterization, but successfully enhance its adsorption capacity and achieve perfect selectivity for Lanthanum ion (La 3+ ). The adsorption capacity for UiO-66-COOH-24TFA was increased by 58% compared to unmodified material. The adsorption mechanism and application were comprehensively investigated. By adsorption kinetics , isotherm and thermodynamic studies, it was found that the adsorption process mainly exhibited monolayer adsorption with spontaneous endothermic-chemisorption characteristics, and –COOH of the modified materials (UiO-66-COOH-24TFA) played an important role, which was confirmed by XPS. Moreover, UiO-66-COOH-24TFA was applied to REEs actual wastewater by successive six-stage adsorption process , where the overall recovery rate on La 3+ reached 94.1% under the coexisting conditions of multiple ions. The application of this acid modified material in the field of the separation and recovery of REEs is of great promise.
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高影响因子
Frontiers of Chemical Science and Engineering
·
2023
·Vol. 17
·期 10
·1389-1398
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IF 4.5
Kou Zongliang,Sun Guanlun,Ding Qiuyan,Li Hong,Gao Xin,Fan Xiaolei,Ou Xiaoxia,Pan Qinhe
Hydrothermal and catalytic stability of UIO-66 MOFs with defective structures are critical aspects to be considered in their catalytic applications, especially under the conditions involving water, moisture and/or heat. Here, we report a facile strategy to introduce the macromolecular acid group to UIO-66 to improve the stability of the resulting UIO-66—PhSO 3 H MOF in aqueous phase catalysis. In detail, UIO-66—PhSO 3 H was obtained by grafting benzenesulfonic acid on the surface of the pristine UIO-66 to introduce the hydrophobicity, as well as the Brønsted acidity, then assessed using catalytic hydrolysis of cyclohexyl acetate (to cyclohexanol) in water. The introduction of hydrophobic molecules to UIO-66 could prevent the material from being attacked by hydroxyl polar molecules effectively, explaining its good structural stability during catalysis. UIO-66—PhSO 3 H promoted the conversion of cyclohexyl acetate at ca. 87%, and its activity and textural properties were basically intact after the cyclic stability tests. The facile modification strategy can improve the hydrothermal stability of UIO-66 significantly, which can expand its catalytic applications in aqueous systems.
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CRYSTENGCOMM
·
2019
·Vol. 21
·期 11
·1772-1779
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IF 3.382
Zheng Deng,Xinsheng Peng,Yu-Jia Zeng
Modulators were frequently employed to synthesize UiO-66 with improved crystallinity, enhanced porosity, and controlled size and morphology. However, little attention was paid to the functionality of modulators themselves. We showed that ferrocenecarboxylic acid (FcCOOH) was not only an efficient modulator for UiO-66 synthesis but also endowed UiO-66 with redox properties. FcCOOH significantly reduced the size of UiO-66 from 400 nm intergrown crystals into 50 nm individual ones, and at the same time remarkably improved their crystallinity, micro-pore volume (0.56 cm3 g−1), and BET surface area (1364 m2 g−1). In addition, FcCOOH in UiO-66 served as a reducing agent for in situ incorporation of Pd nanoparticles into UiO-66 under mild conditions and was used as an efficient heterogeneous catalyst for the Suzuki–Miyaura reaction.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2018
·
IF 5.091
Liang Zeng,Ling Xiao,Yangke Long,Xiaowen Shi
In this study, POM@UiO-66 nanoparticles were fabricated by encapsulation of POM (K 6 P 2 W 18 O 62 polyoxometalate) into mesoporous UiO-66 metal organic framework through a solvothermal method with trichloroacetic acid as a modulator to promote the defects formation of UiO-66. The as-prepared samples were characterized by TEM , SEM, PXRD , TG, XPS , and EDX elemental mapping, and the successful combination of POM and UiO-66 was confirmed. Two cationic dyes, rhodamine B and malachite green , and one anionic dye orange G were employed to investigate the adsorption performance of POM@UiO-66. The adsorption data showed that the removal process of cationic dyes by POM@UiO-66 matched well with the pseudo-second-order model and Langmuir isothermal model. The resulting POM@UiO-66 nanoparticles exhibited high adsorption to cationic dyes but low adsorption to anionic dyes, and the adsorption capacities of rhodamine B, malachite green, and anionic dye orange G were 222.6, 190.6 and 40 mg g −1 , respectively. Furthermore, the cationic dyes could be selectively removed from a cationic-anionic dye binary system. These results suggested that the novel polyoxometalate-based UiO-66 material is a promising candidate for the adsorption of cationic dyes from effluent.
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PubMed
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2024
·
IF 4.1
Mingtao Wang,Shijie Wang,Zhenzi Li,Xuepeng Wang,Liping Guo,Haixia Liu,Lijun Liao,Wei Zhou
Photocatalysis is an alternative for antibiotics removal from wastewater for the sustainable development of human society. However, applying photocatalysts for antibiotics (e.g., tetracycline) degradation under practical conditions is highly restricted by the low reaction efficiency due to the prompt charge recombination. Constructing porous heterojunctions is an efficient way to regulate the electron transfer path and accelerate charge migration efficiency. Herein, TiO 2 /defective UiO-66 porous octahedral S-scheme heterojunctions are successfully fabricated through an in-situ growth strategy. The strong interaction and charge migration behavior between TiO 2 and defective UiO-66 have been studied using X-ray photoelectron spectroscopy and electron paramagnetic resonance measurements. The photocatalytic removal efficiency of tetracycline is notably improved by forming TiO 2 /defective UiO-66 porous heterojunctions. The promoted photocatalytic performance can be ascribed to the strong interaction between TiO 2 and defective UiO-66, and the accelerated charge separation and transfer efficiency due to the formation of S-scheme heterojunctions, thus generating abundant reactive oxygen species, including O 2 − and OH. The optimized 38-TiO 2 /UiO-66-300 can eliminate 97.9 % of tetracycline in 60 min with a reaction constant rate of 0.0425 min −1 , which is approximately 4 and 10 times that of pristine TiO 2 and UiO-66-300, respectively. This work provides an alternate strategy for preparing highly active heterojunction photocatalysts for environmental applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Xingxing Wang,Jian Gao,Shuaichuan Cui,Shihan Liu,Yifan Huang,Yifan Zhang,Pengyang Deng
Separation membranes with high solvent permeation and rejection are attractive for energy conservation in waste solvents separation. Herein, ultra-high flux dye separation membrane was firstly obtained by in situ growing continuous thin MOF membranes on commercial non woven fabrics, which overcome the “trade-off” effect of traditional separation membranes. The continuity of MOF membrane is closely related to the grafting density of maleic anhydride (MAH), and the thickness and surface morphology of continuous thin UiO-66-NH 2 membrane (CTUM) can be controlled by tuning reaction time. The CTUM exhibits a molecule weight cut-off of 950 Da and organic solvents permeation of > 2200 L m −2 h −1 bar −1 with the rose bengal (RB) rejection of 99.39 %. The selectivity of CTUM depends on the size screening and electrorepulsion effect, and the permeation of CTUM is at least 10 times higher than conventional separation membranes. Meanwhile, the CTUM is durable under mechanical friction and during filtration. Our work represent a reliable way to make durable MOF membranes for ultra-high permeation organic solvent filtration, which lay a foundation for further exploration of high performance separating membranes.
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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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MATERIALS RESEARCH BULLETIN
·
2017
·
IF 2.446
Aisheng Huang,Linlin Wan,Jürgen Caro
In a detailed study, the influence of microwave irradiation, synthesis time and temperature, addition of acetic acid (HAc) as a modulator on the morphology, crystallinity and stability of UiO-66-NH 2 is investigated to develop a reliable and reproducible strategy for the preparation of well-shaped UiO-66-NH 2 . The UiO-66-NH 2 were characterized by powder X-ray diffraction (PXRD), field emission scanning electron microscopy (FESEM), thermogravimetric analysis (TGA), and gas adsorption. It is found that well-shaped UiO-66-NH 2 with a high CO 2 adsorption capacity can be synthesized in a short time by microwave heating. The UiO-66-NH 2 crystals synthesized by microwave heating are of high quality and show a superior CO 2 adsorption capacity (5.8 mmol/g at 273k and 1 bar) due to the strong interactions between the −NH 2 group and CO 2 . The CO 2 /N 2 selectivity of the obtained UiO-66-NH 2 at 298 K and 1 bar is 66, which is much higher than that of the pristine UiO-66 of 17.8.
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高影响因子
CATALYSIS LETTERS
·
2015
·Vol. 146
·期 1
·117-125
·
IF 2.307
Dong Wenhuan,Feng Cheng,Zhang Li,Shang Ningzhao,Gao Shutao,Wang Chun,Wang Zhi
Abstract
In this paper, the palladium nanoparticles were successfully encapsulated in metal–organic framework material, UiO-66, by a facile approach. Based on the microwave-assisted method, the pores of UiO-66 were activated and the metal precursors were reduced at the same time in the presence of reducing agent. The obtained Pd@UiO-66 was characterized via transmission electron microscopy, powder X-ray diffraction, N 2 adsorption and X-ray photoelectron spectroscopy. The Pd@UiO-66 exhibited efficient catalytic activity for the Suzuki–Miyaura coupling reactions at mild condition. Graphical Abstract The palladium nanoparticles were successfully encapsulated in metal–organic framework material, UiO-66, by a facile approach. Based on the microwave-assisted method, the pores of UiO-66 were activated and the metal precursors were reduced at the same time in the presence of reducing agent. The obtained Pd@UiO-66 exhibited efficient catalytic activity for the Suzuki–Miyaura coupling reactions at mild condition.
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