JOURNAL OF COORDINATION CHEMISTRY
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2023
·
IF 1.9
Jinyan Tan,Na Zhang,Ling Wang,Liduo Chen,Cuiqin Li,Jun Wang
Metal-organic framework MIL-125(Ti)-NH2 was prepared and coordinated with salicylaldehyde and NiCl2·6H2O to create a heterogeneous catalyst for ethylene polymerization. The structure of the products was characterized by a variety of physical methods, such as Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM), inductively coupled plasma mass spectrometry (ICP-MS), and nitrogen adsorption-desorption. The catalytic performance of MIL-125(Ti)-NH2-Sal-Ni was also investigated. The results showed that the reaction temperature, Al/Ni molar ratio, and ethylene pressure influenced on the catalytic activity and product selectivity. Under optimal reaction conditions, the catalytic activity of MIL-125(Ti)-NH2-Sal-Ni for ethylene oligomerization could reach 5.90 × 104 g·(mol Ni·h)−1 using cyclohexane as the solvent and MAO as the co-catalyst; the main products were C4 and C6. In addition, MIL-125(Ti)-NH2-Sal-Ni had good catalytic stability and recycling, which could be reused at least twice without significant loss of activity. Moreover, based on the evaluation of catalytic performance, the catalytic ethylene oligomerization mechanism of MIL-125(Ti)-NH2-Sal-Ni was also deduced.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Minjun Ma,Yu Liu,Honghong Chang,Yingxiong Wang,Yan Qiao
Ofloxacin is one of the most potent antibiotics. But its low solubility in water has limited its use in site targeted delivery and topical applications. This study investigates the PAMAM-NH 2 (amine-terminated polyamidoamine dendrimers) delivery of ofloxacin in water based on host-guest chemistry and reveals the interaction mechanism of PAMAM-NH 2 with ofloxacin by utilizing NMR techniques including 1D chemical shift titration, 2D 1 H– 13 C HSQC titration, NOESY technique, STDD method, and 2D DOSY analysis. Ofloxacin interacts with surface amine groups of PAMAM-NH 2 via ionic interactions, and ofloxacin is also encapsulated into the PAMAM interior cave through hydrophobic interactions. An overall mechanism was proposed for the PAMAM-NH 2 adsorption of ofloxacin, and then the binding affinity was determined. The experimental data demonstrate the potential of the PAMAM-NH 2 for the drug molecules delivery.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Jun-Qing Ye,Yan-Zi Dai,Shu-Ying Xu,Pin-Xi Wang,Zhong-Hua Sun,Jun-Feng Qian,Qian Liang,Ming-Yang He,Qun Chen
The construction of efficient photocatalysts for water splitting to enable H2 evolution is pivotal to alleviate energy issues and environmental concerns. In this work, carbon dots (CDs) were prepared by employing “green solvent” ionic liquids as carbon sources and then combined with Pt/NH2-MIL-125, resulting in the emergence of a high-efficiency photocatalyst termed CDs-Pt/NH2-MIL-125 for the first time. This composite photocatalyst exhibited outstanding photocatalytic activity in H2 production under visible light irradiation. Notably, the H2 production rate of CDs100-Pt/NH2-MIL-125 reaches up to 951.4 μmol/g/h, which was 3.1 times that of Pt/NH2-MIL-125. The characterization results indicate that CDs and Pt uniformly dispersed on the surface of NH2-MIL-125 and fabricated a synergistic compact structure, providing a high BET surface area (985 m2 g–1) and a suitable band gap. Furthermore, the distinctive embeddable-dispersed CDs and Pt, as dual cocatalyst, can harvest light and facilitate the transfer of photogenerated electrons, thereby significantly augmenting the exploitation of visible light. The plausible mechanism of photocatalytic H2 evolution over the CDs-Pt/NH2-MIL-125 catalyst was also discussed. This work introduces a promising strategy for designing high-performance CDs-MOFs-based photocatalysts, an innovative step toward achieving efficient photocatalytic water splitting for H2 production.
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JOURNAL OF HAZARDOUS MATERIALS
·
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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Journal of Environmental Chemical Engineering
·
2022
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IF 7.968
Tiantian Feng,Qing Liu,Can Yang,Guiju Li,Jin Liu
Considering the stability and hazard of chromium complexes, their removal and recovery from industrial wastewater is a worthy goal. Membrane capacitive deionization (MCDI) can effectively reduce co-ion adsorption compared with CDI technology and has been demonstrated to be a promising deionization technology. In this study, functionalized activated carbon (AC@SiO 2 -NH 2 ) was applied as a MCDI eletrode. The AC@SiO 2 -NH 2 adsorbs chromium complexes (Cr(Ⅲ)-EDTA) through electrostatic gravitation of protonated amino groups (-NH 3 + ). With applied voltage of 1.2 V, solution flow rate of 20 mL min −1 and initial concentration of 300 mg L −1 , the electrosorption capacity of the AC@SiO 2 -NH 2 electrode for Cr(Ⅲ)-EDTA was 17.70 mg g −1 . The Ragone curves verified that the electrosorption rate (SER) of the AC@SiO 2 -NH 2 electrode was positively correlated with voltage and initial concentration. Moreover, the effects of competing ions (K + , Na + , and Mg 2+ ) in a series of single electrolyte solution by the AC@SiO 2 -NH 2 electrode were investigated. It was also verified that the optimum pH was 3 for electrostatic attraction. The energy consumption of the MCDI process is calculated as 0.251 kWh m 3 and 0.039 kWh g −1 Cr at 1.2 V. We envisage that the use of AC@SiO 2 -NH 2 electrodes will pave the way for efficient operation of MCDI as well as the preferential recovery of Cr(Ⅲ)-EDTA.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 60
·90738-90751
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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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FUEL
·
2022
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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
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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
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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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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Shirui Pang,Yuxin Liu,Zhe Zhang,Yuxin Li,Chunguang Li,Zhan Shi,Shouhua Feng
The transmembrane diffusion of soluble lithium polysulfides (LiPS) is the main cause of capacity loss and negative electrode corrosion in lithium-sulfur (Li-S) batteries. In order to suppress the shuttle effect of LiPS, a selective permeability membrane was constructed by introducing functional materials with negative charge groups. Herein, a functional separator with high ion conductivity is obtained by casting the environmentally friendly MOF material sulfonic acid functionalized amino-MIL-101 (S-MIL-101) onto the separator. It is found that the functionalized sulfonic acid group not only accelerates the conduction of the lithium-ion but also repels the polysulfide anion through electrostatic interactions . With this functionalized separator, the initial capacity of batteries is 1444.6 mAh·g −1 at 0.2C and remains 990.4 mAh·g −1 after 100 cycles. Meanwhile, the batteries still deliver a high initial discharge capacity of 895.7 mAh·g −1 even with the high-sulfur-loading cathode (4.7 mg cm −2 ) at 0.2C.
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Sustainability
·
2023
·Vol. 15
·期 18
·13382
·
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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