Journal of Materials Chemistry A
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2020
·Vol. 8
·期 16
·7870-7879
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IF 11.301
Rongming Xu,Qinghua Ji,Pin Zhao,Meipeng Jian,Chao Xiang,Chengzhi Hu,Gong Zhang,Chaochun Tang,Ruiping Liu,Xiwang Zhang,Jiuhui Qu
Metal–organic frameworks (MOFs) have attracted increasing interest for adsorption applications due to their ultrahigh porosity and specific surface area. However, their adsorption performance in liquids, particularly for water treatment, is significantly limited by the poor accessibility of micropores inside the MOF matrix to most molecules and deficient active sites. Herein, we use a facile strategy, ligand selective thermolysis, to create oxygen vacancies and construct mesopores in water stable UiO-66. The obtained hierarchically porous UiO-66 (HP-UiO-66) has tunable oxygen vacancies and mesopores, and outperforms the state-of-the-art MOF based adsorbents reported so far in removing arsenic, achieving an ultrahigh adsorption capacity of 248.75 mg g−1 under neutral conditions. Extended X-ray absorption fine structure (EXAFS) and X-ray absorption near-edge structure (XANES) analysis and density functional theory (DFT) calculations reveal that arsenic is mainly captured by forming bidentate Zr–O–As bonds between arsenate and HP-UiO-66 via occupying coordinatively unsaturated zirconium atoms. This study offers a new strategy for designing ultrahigh performance MOF based adsorbents.
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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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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 20
·6813-6822
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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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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2023
·
IF 6.1
Cong Li,Chang Li,Le Sun,Pushuang Xing,Ronglan Zhang
In this article, composite materials PMoV 2 @UiO-66-X (X = H, NH 2 , NO 2 , SO 3 H) are prepared by using hydrothermal synthesis method, and then the surfaces of the composite materials are coated with mSiO 2 shell to obtain three-layer coated catalysts PMoV 2 @UiO-66-X@mSiO 2 . The prepared catalysts were characterized by FT-IR, XRD, N 2 adsorption desorption isotherms, SEM, and TEM. The catalytic oxidation desulfurization performance of the catalyst was studied using GC–MS, and the optimal reaction conditions of the catalysts were explored, including temperature, stirring rate, catalyst dosage, and oxidant dosage. The results indicate that at 800 ppm of simulated fuel, PMoV 2 @UiO-66-NO 2 @mSiO 2 has the highest catalytic activity, with a total desulfurization efficiency of 98 % under optimal conditions. After eight cycles, the efficiency can still reach 94 %, which is attributed to the strong acidity provided by PMoV 2 , the electron donating effect of the –NO 2 group, and the stable core–shell structure after coating with mSiO 2 .The paper further confirmed the high catalytic activity of the catalyst through UV–Vis analysis.
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Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Li He,Zichang Yang,Xingkai Lu,Yuyao Xu,Xiaolong Yao,Changming Li,Chao Wu,Zhiliang Yao
Defective UiO-66 by metal doping exhibits considerable promise in the photocatalytic degradation of environmental contaminants, albeit how different metal doping affect formation of defects and its efficacy in the degradation of methyl mercaptan has yet to be comprehensively explored. In this study, a one-step solvothermal method was employed to successfully synthesize six distinct metal-doped UiO-66 with variations of defects by incorporating Ce, Al, Cu, Cr, Mg, and Fe. A systematic examination of the structural and photochemical attributes of these metal-doped UiO-66 materials was conducted through a series of characterisations. Metal doping creates defects in UiO-66, changes its colour and morphology and increases its specific surface area. Subsequently, the adsorption and photocatalytic degradation characteristics of these nanomaterials concerning methyl mercaptan were investigated. In comparison to pristine UiO-66, all metal-doped UiO-66 variants exhibited enhanced adsorption and photocatalytic degradation capabilities towards methyl mercaptan. Notably, among the prepared materials, FeUiO-66 demonstrated the most exceptional photocatalytic degradation performance, followed by CuUiO-66, AlUiO-66, CeUiO-66, CrUiO-66, and MgUiO-66 in that order. 1.0FeUiO-66 exhibiting the most remarkable performance, achieving a 99 % degradation of methyl mercaptan within 30 min. This represented a degradation rate 36.8 times higher than that of pure UiO-66, attributable to the incorporation of low-valence metals into the UiO-66 framework, resulting in the creation of oxygen vacancy defects. Furthermore, the presence of these metals facilitated electron transport, thereby enhancing the efficiency of photocatalytic degradation. This study underscores the potential of various metals-doped UiO-66 for adsorption and photocatalytic elimination of methyl mercaptan.
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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
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2023
·Vol. 13
·期 5
·876
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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
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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
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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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CRYSTENGCOMM
·
2019
·Vol. 21
·期 11
·1772-1779
·
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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