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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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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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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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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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yuling Ma,Airong Li,Cheng Wang
Metal-organic frameworks (MOFs) with a high specific surface area, an adjustable pore structure, and functionalized pore environment have a broad application prospect in gas adsorption and separation. In this work, a series of defective UiO-66 (UiO-66-monocarboxylic acid) samples were prepared by adding different monocarboxylic acids during the synthesis of UiO-66. UiO-66-monocarboxylic acid samples (UiO-66-formic acid, UiO-66-acetic acid, UiO-66-benzoic acid, UiO-66-acrylic acid, and UiO-66-cyanoacetic acid) had a high specific surface area (1200–1400 m 2 /g) and a good thermal stability (560 °C). In the desulfurization experiment of simulated flue gas (SO 2 /CO 2 /O 2 /N 2 , 0.3/10.0/5.5/84.2 vol%), the breakthrough time of UiO-66-cyanoacetic acid for SO 2 was higher (194 min/g), and the selectivity of SO 2 /CO 2 reached 33.8. Through optimizing the moles of cyanoacetic acid added, the breakthrough time of SO 2 on 18-UiO-66-cyanoacetic acid increased to 251 min/g. At a pressure of 1.0 bar and a temperature of 298 K, the adsorption capacity of SO 2 by 18-UiO-66-cyanoacetic acid reached 762.1 mg/g. In addition, the adsorption behavior of 18-UiO-66-cyanoacetic acid for SO 2 was considered as a combination of chemical and physical adsorption, and fractional chemisorption sites was provided by cyanoacetic acid.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Shenglong Tian,Zede Yi,Junqing Chen,Shiyu Fu
The capture of radioactive iodine is an inevitable requirement in nuclear industry for environmental protection. Metal-organic frameworks (MOFs) are a new generation of sorbents that have wide applications for iodine adsorption and recovery. Although the loading of MOFs on wood can avoid the drawbacks of the powder form of MOFs in implementation, the dense structure of wood results in the lower loading, even after delignification, which limits the adsorption capacity. Herein, a hierarchically porous UiO-66-NH 2 @WCA composite was fabricated by in-situ synthesis of UiO-66-NH 2 in wood-derived cellulose aerogel (WCA) that was further removed hemicellulose from delignified wood. UiO-66-NH 2 @WCA exhibited a high loading (36 wt%) of UiO-66-NH 2 crystals and a high adsorption capacity of 704 mg/g for iodine vapor and 248 mg/g for iodine aqueous solution. The adsorption behavior in iodine aqueous solution was well predicted by the Freundlich isotherm and pseudo-second-order kinetic model. The adsorption capacity of UiO-66-NH 2 @WCA was highest in solution when the pH was 6, while the ionic strength had little effect. The hydroxyl groups on the WCA matrix had a charge transfer effect with iodine, providing additional sites for iodine capture . Furthermore, a packed column system was applied to demonstrate the excellent recyclability and potential for practical application.
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CHEMOSPHERE
·
2022
·
IF 8.943
Bin Zhao,Min Sun,Zhiqiang Guo,Liang Wang,Yiran Qian,Xiaojia He,Jixiang Li
Endocrine disrupting compounds (EDCs) have been increasingly detected in drinking water sources, and pose severe threat to human health. Polyamide (PA) based nanofiltration (NF) membrane has great potential for EDCs removal from water, but the removal of hydrophobic EDCs is not satisfying due to strong hydrophobic affinity. In this study, UiO-66-NH 2 /PA membranes were prepared by predepositing hydrophilic UiO-66-NH 2 onto the substrate prior to interfacial polymerization. The UiO-66-NH 2 aggregates increased the permeable area and strengthened the “gutter effect”. Therefore, the pure water flux of UiO-66-NH 2 /PA increased by 115% compared with that of the thin-film composite (TFC) membrane, and its rejection of Na 2 SO 4 was 96%. The hydrophilicity-enhanced PA film reduced its adsorption of EDCs and decreased the driving force for EDCs diffusion. Moreover, the UiO-66-NH 2 -induced hydrophilic nanochannels, including the interfacial gaps between PA film and UiO-66-NH 2 aggregates, the gaps in UiO-66-NH 2 aggregates, and the inherent pores in UiO-66-NH 2 crystals, alleviated the hydrophobic affinity and effectively restricted EDCs diffusion. The rejection rates of methylparaben, propylparaben, bisphenol A, and benzylparaben by the optimal UiO-66-NH 2 /PA were 50%, 67%, 75%, and 85%, respectively, and the water/benzylparaben selectivity was 4.4 times as high as that of TFC. The results demonstrate that incorporating hydrophilic metal-organic frameworks (MOFs) can improve the membrane hydrophilicity and create hydrophilic nanochannels, and is an effective strategy to enhance EDCs removal by nanofiltration.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 60
·90738-90751
·
IF 5.19
Zhang Xiaoting,Han Runping
In this study, a zirconium elemental organic framework (UiO-66-NH 2 ) was prepared by a green synthesis method and showed a good adsorption performance for removing 2,4-dichlorophenoxyacetic acid (2,4-D) from water. UiO-66-NH 2 was analyzed by a variety of characterization methods and the adsorption properties of 2,4-D on UiO-66-NH 2 were investigated by static adsorption experiments. The results showed that the adsorption of 2,4-D had a wide pH range (2–10) and good salt tolerance with the adsorption equilibrium time about 2 h. The maximum adsorption capacity from Langmuir was up to 652 mg g −1 at 303 K. The isotherms can be described by Langmuir model and the adsorption kinetics was consistent with pseudo-second-order kinetic model and Elovich model. The regeneration efficiency was still 95% after 5 cycles with 0.01 mol L −1 NaOH as desorption solution. The feasibility of practical application of UiO-66-NH 2 was explored by simulating actual wastewater at different pH. UiO-66-NH 2 is promising to remove 2,4-D from water. Graphical abstract
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
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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FUEL
·
2022
·
IF 8.035
Ping Lu,Huaifang Li,Mantian Li,Jie Chen,Changshen Ye,Hongxing Wang,Ting Qiu
In this work, acidic ionic liquid (AIL) was grafted into NH 2 -UiO-66 through acid-base interaction. And the novel heterogeneous catalyst x AIL@NH 2 -UiO-66 ( x means the mass ratio of AIL to NH 2 -UiO-66) was first applied in the field of biodiesel production. The optimal catalyst 3AIL@NH 2 -UiO-66 with good wettability (with reactants) and high acidity was prepared successfully. Accordingly, the 3AIL@NH 2 -UiO-66 can be widely applied in biodiesel production from different raw materials. The conversion of free fatty acids (FFAs) in esterification was above 90%, as well as the biodiesel yield in transesterification was above 80%, showing excellent catalytic activities of 3AIL@NH 2 -UiO-66. And the 3AIL@NH 2 -UiO-66 also revealed excellent reusability, with the conversion of oleic acid decreases from 96.86% to 90.42% after 6 runs. In addition, the interaction between any two of the three factors (catalyst dosage, reaction time and molar ratio) on the oleic acid conversion was revealed with 3D response surface technology. By the mechanism investigation, the good wettability with reactants and high acidity of the catalysts are identified as key factors for biodiesel production. The method of anchoring ionic liquids with organic linkers for the application of MOFs in biodiesel production offers abundant possibilities.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Zan Chen,Zongping Hong,Hong Wu,Cheng Li,Zhongyi Jiang
Hybrid membranes based on the Tröger’s base polyimide (PI-TB) as a rigid microporous polymer matrix containing a kinked N-heterocycle and a kind of CO2-philic porous UiO-66-NH2 nano-filler were successfully fabricated for gas separation. This new hybrid membrane exhibits good interfacial compatibility through hydrogen bonds and charge transfer interactions between the PI-TB matrix and the UiO-66-NH2 nano-filler, thus enabling a relatively high loading and well dispersion of nano-filler. Meanwhile, the as-synthesized UiO-66-NH2 nanoparticles increase the average inter-chain spacing distance of PI-TB by interfering with the packing of polymer chains and thus providing additional transport pathways in the membranes. The pure gas permeabilities and ideal selectivities for CO2/CH4, CO2/N2, and O2/N2 systems were investigated at 35 °C and a feed pressure of 1 bar. Among them, the hybrid membrane containing 30 wt % UiO-66-NH2 exhibits the optimal gas separation performance with enhanced permeabilities of CO2 and O2 increased by ∼166% (415 and 92.3 Barrer, respectively) while maintaining comparable CO2/CH4, CO2/N2, and O2/N2 gas pair selectivities (25.0, 18.9, and 4.2, respectively) with the pristine PI-TB membrane. This work enriched the studies on the post-modification of PI-TB as a potential candidate membrane material for gas separation.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 20
·6813-6822
·
IF 4
Ruowen Liang,Shihui Wang,Yuzhou Xia,Ling Wu,Renkun Huang,Zhoujun He
Designing frustrated Lewis pair (FLP)-structured photocatalysts is a new challenge in catalysis. In particular, the relationship between the active sites and photocatalytic charge transport mechanism over FLP-structured photocatalysts is still ill-defined. In this study, a novel perylene-3,4,9,10-tetracarboxylic diimide/UiO-66(Ti/Zr)–NH2 (denoted as PDI/TUZr) photocatalyst is successfully constructed using an ammoniation process. The PDI/TUZr heterojunction is equipped with a unique “Zr/Ti SBUs-ligand-PDI” FLP structure and exhibits remarkable catalytic FLP properties. In this “Zr/Ti SBUs-ligand-PDI” structure, the Zr/Ti bimetal centers and PDI serve as Lewis acid and base sites, respectively, and the C–N chemical bond provides a channel for electron transmission, and a bimetallic system facilitates electron transfer from excited ligand to Zr/Ti-SBUs nodes. These superior microstructural designs cooperate to promote substrate activation for photocatalytic antibacterial reactions. Accordingly, 2.2-fold enhancement is achieved in visible photocatalytic antibacterial activity on Staphylococcus aureus for 4%PDI/0.2TUZr composite compared with unadorned UZr. This study provides insights into the formation and carrier transfer behaviors of solid FLP on MOFs and illustrates a rational strategy for the construction of highly efficient photocatalysts.
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