SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Siyu Liu,Jianhua Zu,Gang Han,Xiaohan Pan,Yi Xue,Jingjie Diao,Qing Tang,Mingjie Jin
137 Cs is a radioactive pollutant in the production of wastewater from nuclear power plants. In this study, a rapid and simple in-situ synthesis new method was employed to prepare a novel AMP-functionalized UiO-66 composite material for the selective capture of 137 Cs from low-level radioactive wastewater. Characterization techniques such as SEM-EDS, FTIR, XRD, TG, and BET were used to confirm the successful loading of AMP on the surface of UiO-66. UiO-66/AMP showed a good removal effect in pH4-11. At pH7, the effects of different parameters, such as the initial Cs concentration, the ratio of the amount of adsorbent to the volume of solution, and the adsorption time were investigated. The adsorption efficiency is 96.7%, the maximum adsorption capacity is 94.9 mg/g and has fast adsorption kinetics (90% Cs + removal within 5 min). The adsorption data conformed to the pseudo-second-order kinetic model and Langmuir isotherm model, suggesting a monolayer homogeneous adsorption process. XPS helps confirm that the adsorption mechanism is the ion exchange between Cs + and NH 4+ ions. Particularly, in the adsorption experiments of 137 Cs, UiO-66/AMP demonstrated good selectivity (K d Cs : 5.8 × 10 3 ∼ 1.26 × 10 4 mL/g) towards trace Cs + in a mixed ion solution with a molar ratio of 1 (Cs): 2.18 × 10 15 (Na): 4.6 × 10 14 (K): 2 × 10 14 (Mg): 2 × 10 14 (Ca), indicating its potential for selective capture of 137 Cs from low-level liquid waste (LLLW).
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CHEMOSPHERE
·
2023
·
IF 8.8
Xiule Wang,Fanyong Yan,Ying Chen,Xinyi Bai,Yang Fu
Metal organic frameworks (MOFs) possess a large surface area, inherent porosity and high crystallinity . Nevertheless, they lack electron acceptors, which limit the exploitation of their photocatalytic properties. Carbon dots (CDs) known for excellent optical properties can serve as localized electron acceptors. As a novel hybrid nanomaterial , the structure of CDs@MOFs effectively facilitates charge separation and carrier transfer, bring about a marked improvement of photocatalytic activity. In this study, yellow-emission carbon dots (YCDs) were encapsulated within zirconium-based metal organic framework (UiO-66) via a dynamic adsorption method. Compared with blue carbon dots (BCDs), the YCDs@UiO-66 exhibited superior degradation performance. It demonstrates that incorporation of YCDs broadens the UV absorption range of UiO-66, thereby enhancing light utilization. The degradation efficiency of YCDs@UiO-66 was 92.6%, whereas UiO-66 alone achieved only 63.1%. Notably, the results of the radical quenching experiment and electron paramagnetic resonance (EPR) revealed that h + and •O 2 − played a prominent role in the photodegradation of tetracycline hydrochloride (TCH). This study highlights that the introducing YCDs in MOFs-mediated photocatalytic reactions is a viable strategy to improve catalytic efficiency.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 51
·111039-111050
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IF 5.8
Dong Shiwen,Liu Xuan,Kong Xianxian,Dong Feilong,Yu Yan,Wang Lizhang,Wang Da,He Zhiqiao,Song Shuang
Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) have been proved as efficient catalysts for photocatalytic hydrogen (H 2 ) evolution, thanks to their tunable functionalities, permanent porosity, excellent visible light response, and physicochemical stability. Herein, a series of photocatalysts (termed NUBC) was fabricated by loading different amounts of Zr-UiO-66-NH 2 (NU) onto a benzoic acid–modified covalent triazine–based framework (BC) based on post-synthetic covalent modification. The resulting NUBC catalysts exhibited a type-II Z-scheme heterojunction structure formed via the amide covalent bonds between the amine groups on NU and carboxyl groups on BC. The optimal loading of NU on BC is 30 wt.% (30NUBC) and the corresponding photocatalytic H 2 evolution rate was 378 μmol h −1 g −1 , almost 445 and 2 times than that of NU and BC, respectively. The synergistic effect between the type-II Z-scheme heterojunctions and amide bonds was conducive to boosting visible light harvesting and facilitating charge transportation and separation. Furthermore, the prepared NUBC catalysts show great reusability and stability. Overall, this work sheds light on the design of novel MOF/COF hybrid materials and provides a systematic exploration of their photocatalytic H 2 evolution properties.
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高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 12
·期 6
·3565-3574
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IF 11.9
Ling-Chan Tian,Geqian Fang,Yun Zhou,Wenjun Yu,Lin Li,Jin-Nian Hu,Haiyan Wang,Jin-Xia Liang,Chun Zhu,Xiaodong Wang,Jian Lin
Direct selective oxidation of methane (DSOM) to oxygenates under mild conditions is garnering increasing interest. UiO-66-H MOFs are effective for this reaction, while the active configuration of Zr-oxo nodes with adsorbed ˙OH species need further clarification from the atomic/molecular viewpoint. Here, we detect the evolution of the geometric and electronic structures of adsorbed oxygenic species on Zr-oxo nodes of UiO-66-H via the controlled ˙OH species. DFT calculations reveal a volcano-like curve relationship between the quantity of ˙OH species and the DSOM performance, which is further corroborated by experimental tests. Zroxo-˙OH is the main active configuration on Zr-oxo nodes of UiO-66-H at low ˙OH concentration, while it evolves to other oxygenic species (˙OOH, O2, and H2O) due to the self-reaction with the increase of ˙OH concentration, which leads to performance decrease. Furthermore, a critical descriptor of the p-band centers of O atoms in these oxygenic species on the Zr-oxo nodes is established, which can well represent the catalytic activity for the DSOM reaction.
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ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Xiangyu Wang,Min Jiang,Iseult Lynch,Zhiling Guo,Peng Zhang,Lisi Wu,Jun Ma
Although Fe/Fe 2 O 3 has potential application compared with nanoscale zero-valent iron (nZVI), its smooth structure largely limits the catalytic performance. To address this challenge, we innovatively constructed highly efficient composite Fe/Fe 2 O 3 @UiO-66 via employing an urchin-like core-shell structure of Fe/Fe 2 O 3 onto UiO-66 through a facile ion exchange precipitation method without inert gas protection. The characterization results show the urchin-like core-shell configuration can extend the life span of Fe 0 and produce more active sites. Besides, the absorption spectrum is broadened by Fe 2 O 3 which has narrow band gap and the high-efficiency separation of photogenerated electron-hole pairs is obtained with the load of Fe/Fe 2 O 3 . Moreover, Two-parameter pseudo-first-order decay model fits well with the reduction and adsorption of composites in the dark reaction, and a plausible pathway for tetracycline (TC) degradation is also proposed. The findings of this research provide a promising method for promoting the catalytic properties of MOF-based materials and Fe/Fe 2 O 3 .
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2023
·
IF 6.1
Qin Zhang,Lijiao Fan,Wenbin Liu,Yuming Xie,Jiangang Li,Guolin Huang
The core–shell structure UiO-66-NH 2 @Ni-MOF was prepared by in-diffusion growth of 2D Ni-MOF on UiO-66-NH 2 using PVP (polyvinylpyrrolidone) as a structural guide. It was applied to the adsorption of U(VI) in aqueous solution. The materials were characterized by powder X-ray diffraction (PXRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and energy dispersive spectrometer (EDS). The UiO-66-NH 2 @Ni-MOF adsorption to U(VI) was investigated experimentally. The study showed that the adsorption of U(VI) onto UiO-66-NH 2 @Ni-MOF was endothermic and spontaneous. At pH 5.00 and 308 K, the adsorption capacity was 581.40 mg/g according to Langmuir model. In addition, the adsorption process can be described by the pseudo-second-order kinetic model. The adsorption capacity was kept at 83.83% of its original one after five sorption–desorption cycles, a promising indication for repetitive usage.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Yunlong Li,Miao Liu,Yixian Liu,Lilong Zhou,Jilong Han,Zhengjie Li,Jimmy Yun,Runjing Liu
Two kinds of Ce-doped UiO-66 were synthesized by using CeCl 3 ·7H 2 O and (NH 4 ) 2 Ce(NO 3 ) 6 as cerium precursors, namely Ce(III)- and Ce(IV)-UiO-66. The effect of valence states of cerium precursors on adsorption performance towards Rhodamine B (RhB) was investigated for the first time. Ce atoms are in two valence states of +3 and + 4, where Ce 3+ ions turn their surfaces negatively charged. The higher cerium content (24.8%) and ratio of Ce 3+ /Ce 4+ ions (1.4:1) of Ce(IV)-UiO-66 made its surface more negatively charged, which is contributed to form stronger electrostatic interaction with cationic dyes. The adsorption amounts of RhB were 239.5 mg/g and 431.7 mg/g for Ce(III)- and Ce(IV)-UiO-66, which are 2.38 and 5.11 times higher than pristine UiO-66, respectively. The well-fit Langmuir model and pseudo-second-order model suggest a monolayer chemisorption process. The adsorption mechanism suggests that the electrostatic interaction and the complexation interaction between Ce 3+ and RhB are dominant factors affecting RhB adsorption. Since Ce 3+ severed as adsorption sites, the higher Ce content and stronger electrostatic interaction of Ce(IV)-UiO-66 together promoted its RhB adsorption than Ce(III)-UiO-66. The obtained results help to understand how the mixed-valences of incorporated metals affect the adsorption behaviors of bimetallic MOFs deeply.
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IRANIAN POLYMER JOURNAL
·
2023
·Vol. 32
·期 8
·979-990
·
IF 3.1
Fu Mengjie,Wang Chun,Lai Xing,Xiao Changfa,Ding Ying
In terms of nanofiltration (NF) membrane development, the properties of membrane substrates and thin-film composite (TFC) structures have become an important factor to determine the separation performances of NF membrane. In this paper, the method of interfacial polymerization assisted by spacer spraying was used to construct the striped structure at nanometer scale. Nanoscale striped structure was prepared successfully on PPTA (poly( p -phenylene terephthamide)) NF surface with 1.3 g/L of UiO-66-NH 2 in the aqueous phase, and the morphology gradually changed to “point shaped” structure when 2.6 g/L of UiO-66-NH 2 in the aqueous phase. The optimized PPTA/UiO-66-NH 2 NF (PU4) membranes were used for dye/salt separation of methylene blue (MB). Compared with the nascent PPTA NF membranes, it showed a higher MB rejection rate of 98.6%, along with permeation flux of 19.79 L/m 2 \(\cdot\) h \(\cdot\) MPa. The salt separation order of the PU4 membrane was Na 2 SO 4 > MgSO 4 > MgCl 2 > NaCl. The rejection rates were 96.3%, 85.4%, 53.2%, and 18.4%, respectively. Under strong acid and alkali conditions, the separation performance was rejected 86.5%, better under alkaline conditions. More importantly, after a six-time recycle, the PU4 membrane showed no significant change in separation performance, suggesting its excellent stability. The novel strategy in this study provided an approach to develop advanced UiO-66-NH 2 membranes toward sustainable molecular separation in environmental applications. Graphical abstract
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Wenqian Zhao,Xu Zhang,Chang Li,Lusheng Xu,Qin Meng,Guoliang Zhang
Adding nanomaterials such as metal–organic frameworks (MOFs) into a polyamide (PA) layer to prepare forward osmosis (FO) membranes for efficient desalination has attracted great attention. However, rational design and preparation of high-quality MOF-based PA nanocomposite forward osmosis membranes still remain a big challenge. In this study, a polyamine (PA) forward osmosis (FO) membrane was fabricated via interfacial polymerization (IP) with the assistance of a UiO-66 nanocomposite interlayer to enhance desalination and antifouling performances. Polydopamine (PDA) and polyethyleneimine (PEI) were codeposited with UiO-66 and formed a hydrophilic nanocomposite intermediate layer. The substrate with the PDA/PEI/UiO-66 interlayer had better hydrophilicity, restricting the diffusion of m-phenylenediamine (MPD) and promoting the formation of a defect-free active layer. In addition, the PDA/PEI/UiO-66 interlayer not only provided additional water channels but also enhanced the interaction of the substrate and PA layer. The water flux of the PA-PDA/PEI/UiO-66 membrane reached 40.0 L m–2 h–1 with a low reverse salt flux (3.2 g m–2 h–1). Moreover, the PA-PDA/PEI/UiO-66(0.1) membrane also possessed excellent antifouling performances with a high flux recovery of 98% and a low total fouling rate of 17%, which were 18.4% higher and 43.3% lower than those of the pristine TFC membrane, respectively. These results presented that the codeposition of the PDA/PEI/MOF interlayer greatly improved the desalination and antifouling performances of the PA FO membrane.
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Analytical Methods
·
2023
·Vol. 15
·期 16
·1953-1958
·
IF 3.1
Piaotong Liu,Rusi Hao,Wenliang Sun,Junhui Li
As an important trace element in the human body, the concentration of Cu2+ has an important impact on the environment and human health, and its quantitative determination is of great significance in the fields of environmental protection and food safety. Here, a ratiometric fluorescent probe based on Tb(III)-functionalized UiO-66-type MOFs has been synthesized via a facile post-synthetic modification method by employing mixed linkers containing terephthalic acid and 2,6-pyridinedicarboxylic acid for Cu2+ detection. The blue fluorescence intensity at 440 nm from the ligands of MOFs does not change much with increasing Cu2+ concentrations and can be used as a reference signal, while the green fluorescence of Tb3+ can be rapidly and selectively quenched, causing fluorescence intensity at 547 nm to decrease. The probe can be used as a ratiometric sensor for Cu2+ detection with a good linear response and low detection limit. The use of the probe for the determination of Cu2+ in real water samples and drinks shows good practicality. This method for Cu2+ detection is simple, specific and visualized to meet the needs of environmental monitoring and food analysis and provides a new strategy for the construction of new copper ion fluorescent sensors to analyze complex samples.
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Journal of Cleaner Production
·
2019
·
IF 6.395
Likang Fu,Shixing Wang,Guo Lin,Libo Zhang,Qiming Liu,Houhuang Zhou,Chenxia Kang,Shuyun Wan,Hongwei Li,Sheng Wen
A new metal organic framework UiO-66-RSA (UiO-66 with hydroxyl) was prepared by the post-modification of UiO-66-NH 2 (UiO-66 with amino) with resorcyl aldehyde and was employed for the efficient and selective separation and removal of Pb(II) in aqueous media . The maximum adsorption amount of UiO-66-RSA was 189.8 mg/g at an optimal pH of 4. The adsorption isotherm and kinetic were well described by Langmuir/Dubinin-Radushkevich and pseudo-second-order models respectively. Adsorption process was monolayer chemisorption . UiO-66-RSA was regenerated by thiourea/nitric acid and the removal rate was only decreased by 3.7% after five successive cycles. The analysis of X-ray photoelectron spectroscopy suggested the adsorption mechanism lay on the complexation reaction between hydroxyl/nitrogen-containing groups and Pb(II). The UiO-66-RSA bound Pb(II) by forming double/quadri coordinated complexes. Compared with a multitude of usual metal ions , viz., Zn(II), Co(IV), Ni(II), Mg(II), Cd(II), Cu(II) and Ca(II), the Pb(II) could be absorbed selectively by UiO-66-RSA. The results indicated that the UiO-66-RSA sorbent could be of great potential in the removal of Pb(II) from aqueous solutions.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Shipeng Wan,Man Ou,Qin Zhong,Xinming Wang
Base-on the excellent optoelectronic properties, perovskite CsPbBr 3 quantum dots (QDs) have been used on perovskite solar cells and LED devices, but little research has been focused on photochemical CO 2 reduction due to their poor moisture stability. Coincidentally, metal-organic frameworks (MOFs) materials have received tremendous attention for sustainable clean energy and environmental remediation. However, the design of excellent performed MOFs is still indispensable. Therefore, the CsPbBr 3 QDs/UiO-66(NH 2 ) nanocomposites that combine the advantages of CsPbBr 3 QDs and UiO-66(NH 2 ) have been successfully designed and fabricated for the first time. Then we employ the nanocomposites as photocatalysts to convert CO 2 to chemical fuels in nonaqueous media. The resultant nanocomposites exhibit significantly improved photocatalytic activity for CO 2 reduction. When CsPbBr 3 QDs content is 15 wt%, the amount of CO can reach 98.57 μmol·g −1 . The remarkable photocatalytic performance could be ascribed to the improved electron extraction and transfer between UiO-66(NH 2 ) and CsPbBr 3 QDs, large accessible specific surface area and enhanced visible light absorption capacity. Moreover, the nanojunction shows excellent reusability for photocatalytic CO 2 reduction. This work might supply new pathway to utilize halide perovskite QDs/MOF nanocomposite in energy conversion and environmental remediation.
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