ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 31
·期 42
·2104629
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IF 18.808
Li Xin,Dezhu Zhang,Kai Qu,Yuqin Lu,Yixing Wang,Kang Huang,Zhaohui Wang,Wanqin Jin,Zhi Xu
Membrane with ordered channels is the key to controlling ion sieving and proton conductivity in flow batteries. However, it remains a great challenge for finely controlling the nanochannels of polymeric membranes. Herein, two types of acid-stable Zr-metal organic framework (MOF-801 and MOF-808) with variable pore structures and channel properties are introduced as fillers into a non-fluorinated sulfonated poly (ether ether ketone) (SPEEK). The membrane incorporated with MOF-801 of a smaller triangular window (≈3.5 Å) successfully translates the molecular sieving property into the flow battery membrane, resulting in enhanced coulombic efficiency (98.5–99.2%) at 40–120 mA cm −2 compared with the pristine SPEEK membrane (97.1–98.5%). In contrast, more protophilic internal interconnected channels of MOF-808 yield faster proton highway, leading to a significant increase of voltage efficiency (93.7–84.1%) at 40–120 mA cm −2 compared with the pristine SPEEK membrane (91.7–78.9%). By regulating the ion sieving and proton conductivity, MOF-801/MOF-808 binary composite membrane exhibits synchronously improved performance in the vanadium redox flow battery system. The revealed structure–property relationship in the Zr-MOFs-based membranes provides a general guideline to design new proton exchange membranes with ordered channels for flow battery application.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2021
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IF 4.098
Xiaoting Zhang,Ying Li,Lei Zhang
Dyes detection remains a serious task because of their high toxicity. In present work, designed Eu 3+ functionalized Zr-metal-organic framework (Eu 3+ @Zr-MOF-808) as fluorescent probe was constructed via post-synthetic modification (PSM) for rapid monitoring four most commonly used dyes (malachite green (MG), brilliant green (BG), alizarin red S (ARS), indigo red (IDR)). Systematic exploring on the sensing mechanism reveals that fluorescence resonance energy transfer (FRET) for BG, MG and IDR and inner filter effect (IFE) for ARS contribute to the realization of the fluorescence quenching process. It exhibits excellent sensing performances with low limit of detection (LOD) of 32, 58, 77 and 133 nM for BG, IDR, MG and ARS, respectively. The as-constructed Eu 3+ @Zr-MOF-808 was demonstrated to be a highly sensitive probe for screening of MG in fish pond and IDR in printing wastewater with satisfying results. Moreover, a portable test reagent bottle has been developed for visual on-site screening of sample containing dyes with naked eyes under UV light. This is the first attempt to construct the Eu 3+ @Zr-MOF-808 probe for sensing multiple dyes in real samples and demonstrates promising applications in water quality monitoring.
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PubMed
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Reaction Chemistry & Engineering
·
2020
·Vol. 5
·期 9
·1833-1844
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IF 3.441
Guochao Yang,Lingtao Wang,Haoxi Jiang
Upgrading bio-ethanol into high value chemicals is an important issue in biomass conversion, and conversion of ethanol into butadiene is one of the most feasible methods. Here Zr-incorporating mesoporous SBA-15 (Zr–SBA-15) materials with different Si/Zr ratios were successfully synthesized by a one-pot method and were employed as catalysts for the conversion of the ethanol (EtOH)–acetaldehyde (AcH) mixture to butadiene. The textural structure and acidity of Zr–SBA-15 were investigated by using XRD, N2 adsorption, TEM, FT-IR, UV-vis, XPS, NH3-TPD and Py-IR, and the results of these characterizations indicated the mesoporosity of Zr–SBA-15 and confirmed the incorporation of Zr into the framework. Zr–O–Si bonds were formed by the incorporation and exhibited Lewis acidity predominantly. The influence of the Si/Zr ratio and reaction conditions (temperature, EtOH/AcH ratio and WHSV) showed that a suitable Si/Zr ratio was needed to balance the butadiene selectivity, by-product selectivity and total conversion. Amongst the prepared catalysts, Zr–SBA-15-20 achieved the best butadiene selectivity of 74.0% at a relatively low temperature (275 °C). The good catalytic performance could be attributed to the homogeneous dispersion of Zr species and Zr–O–Si bond generated by Zr incorporation. Furthermore, EtOH-TPD and AcH-TPD experiments proved the essential role of acetaldehyde addition and the well-accepted reaction pathway.
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CHEMICAL PHYSICS LETTERS
·
2020
·
IF 2.029
Zijun Sun,Guisong Fang,Jinglin Li,Jiahuan Mo,Xiong He,Xu Wang,Zhiqiang Yu
Hematite (α-Fe 2 O 3 ) is one of the promising photoanode materials for photoelectrochemical (PEC) water splitting, but its poor bulk charge transfer has been challenging towards its practical application. Herein, we have synthesized the (Ti, Zr) co-doped hematite by a facile hydrothermal method. The cooperation of (Ti, Zr) co-doped hematite yields photocurrent density of 1.51 mA cm −2 at 1.23 V vs. RHE and IPCE of 17.3% at 400 nm. The structural and PEC analysis indicate that the considerably PEC performance improvement is contributed to the higher carrier density and enhanced charge transfer of the synergistic effect of Ti and Zr co-doping.
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RSC Advances
·
2019
·Vol. 9
·期 65
·37733-37738
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IF 3.049
Yanghe Fu,Jieyu Wu,Rongfei Du,Ke Guo,Rui Ma,Fumin Zhang,Weidong Zhu,Maohong Fan
Defect engineering can be a promising approach to improve the photocatalytic performance of metal–organic frameworks (MOFs). Herein, a series of defective NH2-UiO-66(Zr) materials were synthesized via simply controlling the synthesis temperature, with concentrated HCl as the modulator and then these as-prepared samples were used to systematically investigate the effects of their structural defects on photocatalytic CO2 reduction. Remarkably, these MOFs with defects exhibit significantly enhanced activities in photocatalytic CO2 reduction, compared with the material without defects. The defect engineering creates active binding sites and more open frameworks in the MOF, and thus facilitates the photo-induced charge transfer and restrains the recombination of photo-generated charges efficiently. The current work provides an instructive approach to improve the photocatalytic efficiency by taking advantage of the structural defects in MOFs, and could also inspire more work on the design of advanced defective MOFs.
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PubMed
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Shushu Jia,Ping Lin,Yue Li,Yakun Teng,Jing Wang,Tianyi Yang,Lijuan Li,Ce Wang,Xiang Li
The efficient removal of pharmaceutical pollutants in groundwater has become an urgent issue in sewage treatment. β-cyclodextrin (β-CD), a polysaccharide and rich in raw materials, has broad applications in adsorption and separation due to its host–guest interaction with many molecules. In this paper, a flexible and water-insoluble UiO-67(Zr)-modified cyclodextrin-based nanofiber membrane (UiO-67@β-CD-NP) was synthesized via a combination of electrospinning and solvothermal methods. By virtue of the synergetic adsorption effect of cyclodextrin and MOFs, the UiO-67@β-CD-NP shows excellent performance for ibuprofen (IBP) removal. The adsorption of IBP onto UiO-67@β-CD-NP was well-fitted with the pseudo-second-order kinetic model and Freundlich isothermal model, yielding an adsorption capacity of 226.24 mg/g. Furthermore, the UiO-67@β-CD-NP nanofibers demonstrate a high removal rate of 100 % and exhibit good regenerability in dynamic adsorption experiments. After the filtration of UiO-67@β-CD-NP, the chemical oxygen demand (COD) concentration of IBP has evidently reduced below the discharge standard of pharmaceutical sewage. This study provides a simple and novel strategy for preparing low-cost and high-performance composite nanofiber membrane incorporating cyclodextrin and MOFs. This membrane holds great potential as a candidate for adsorption applications in practical pharmaceutical sewage treatment.
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NUCLEAR ENGINEERING AND DESIGN
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2023
·
IF 1.7
Guanghui Wang,Yulong Du,Meng Zhang,Caishan Jiao,Hui He
In the nuclear spent fuel reprocessing, zirconium dibutyl phosphate (Zr-DBP) is deposited on the surface of stainless steel equipment, making spent fuel reprocessing difficult. Therefore, in this study, hydrazine carbonate ((N 2 H 5 ) 2 CO 3 ) was used to dissolve Zr-DBP. The effects of solid–liquid ratio, different mass fractions of (N 2 H 5 ) 2 CO 3 solutions, and (N 2 H 5 ) 2 CO 3 solutions containing different concentrations of hydrogen peroxide (H 2 O 2 ) on the dissolution of Zr-DBP were investigated. The corrosion rates of different dissolution solutions on stainless steel were also investigated. When the mass fraction of (N 2 H 5 ) 2 CO 3 in solution was increased from 1 % to 20 %, the concentration of Zr(IV) at dissolution equilibrium increased from 1.05 g/L to 1.61 g/L, respectively. When the dissolution temperature was kept in the range of 25 °C to 65 °C, the increasing temperature promoted the dissolution of Zr-DBP. The presence of H 2 O 2 induced the production of the white precipitates zirconium hydroxide (Zr(OH) 4 ). In addition, the corrosion rate of stainless steel gradually increased from 0.00153 mm/a to 0.0138 mm/a when the concentration of H 2 O 2 in the (N 2 H 5 ) 2 CO 3 solution was increased from 0 M to 1.5 M. The dissolution ability of Zr-DBP in different carbonate solutions was (N 2 H 5 ) 2 CO 3 ≥ ammonium carbonate ((NH 4 ) 2 CO 3 ) > sodium carbonate (Na 2 CO 3 ) ≥ potassium carbonate (K 2 CO 3 ).
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Arabian Journal of Chemistry
·
2023
·
IF 6
Hongru Zhao,Chengqiang Hu,Na Sui,Xinyu Liu,Junlian Wang
Zr/Hf separation has always been a great challenge. Although the methyl isobutyl ketone (MIBK)-thiocyanic acid (HSCN) extraction system selectively extracts Hf over Zr and can realize Zr/Hf separation, it has the following disadvantages: it has a strong smell; it is easy to burn; and there is large loss of extractant during extraction due to the low boiling point (115.7 °C), low flashing point (13 °C), and high solubility of MIBK in water (1.7 % at 25 °C). In this study, Zr/Hf separation performance by MIBK homologues — of which one side of C = O is iso pentyl, iso hexyl, n -pentyl, n -hexyl or n -heptyl, while the other side are all methyl — were studied and compared with MIBK. Effects of HSCN pre-extraction, HCl concentration, NH 4 SCN concentration on Zr, Hf extraction and separation performance were investigated. Relationships between methyl alkyl ketone structure and their Zr/Hf separation performance were revealed. A new Zr/Hf separation system MNPK (methyl n -pentyl ketone)-HSCN was found. MNPK has a higher boiling point (151 °C), a higher flashing point (47 °C) and a lower solubility in water (0.43 % at 20 °C) than MIBK. Compared to MIBK, it is safer, more friendly operation environments and less extractant loss during extraction. MNPK has as fast extraction kinetics as MIBK. It also has good anti-emulsification performance. Its maximum β Hf/Zr can reach to 12.61. The loaded Zr and Hf in MNPK have very similar stripping behaviors with those loaded in MIBK by HCl and H 2 SO 4 solutions, respectively. MNPK is the most possible candidate to replace MIBK from HSCN media in Zr/Hf separation industry.
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JOURNAL OF MOLECULAR STRUCTURE
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2023
·
IF 3.8
Jiayin Li,Runze Liu,Pengfei Liu,Hu Zhou
The reactive oxygen species (ROS) level as an hopeful strategy for cancer therapy, mainly including photodynamic therapy (PDT) and chemodynamic therapy (CDT). It is well known both PDT and CDT greatly rely on oxygen reliance, inherent flaws of traditional photosensitizers, and lowly selectivity between normal cells and tumor cells. Herein, we reported Zr(IO 3)4 nanoparticles as a biocompatible nanozyme with effective ROS supply by Feton-like reaction and Brady reaction. The Zr(IO 3 ) 4 exhibiting a remarkable selectivity between normal cells and tumor cells. Importantly, the Zr(IO 3 ) 4 , H 2 O 2 -responsive and GSH-depleted nanozymes, were explored for tumor therapy. Nanozyme is highly important from the deep cancer therapy point of view. In this work, we prepared Zr(IO 3 ) 4 by a simple method. The obtained Zr(IO 3 ) 4 samples showed obvious performance in treatment of cancer. It was confirmed by the electron spin resonance (ESR) as well as the fluorescence probe results of Zr(IO 3 ) 4 that the treatment of cancer due to the reactive oxygen species.
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CATALYSIS COMMUNICATIONS
·
2023
·
IF 3.7
Haoxi Jiang,Xinyi Ni,Angjiong Jiang,Guochao Yang,Lingtao Wang
Zr-β zeolites were modified with second metals to catalyze the conversion of ethanol/acetaldehyde to 1,3-butadiene. The incorporation of Ta increases the Lewis acidity of Zr-β zeolite, resulting in higher catalytic activity than that of In, Y and Ce. Furthermore, the Zr-β zeolite that was first incorporated with Zr and then Ta with a Ta/Zr molar ratio of 1.5 exhibited greater catalytic activity of 57% conversion and 75% selectivity. Activity descriptors were proposed to calculate the reactivity of key reaction steps, which served as evidence that Ta incorporation enhances the aldol condensation and MPV reduction reaction activity, thus improving catalytic performance.
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Molecular Catalysis
·
2023
·
IF 4.6
Jianhong Zheng,Xi Chen,Xiaoxiao Yin,Kai Chen,Aili Liu,Xiaochun Yu,Shun Wang,Zhongwei Chen
A highly efficient and organic solvent-free synthetic strategy for the selective oxidation of anilines to azoxybenzenes was developed by employing porous Zr-MOFs as catalysts in aqueous hydrogen peroxide solution. The impact of cluster nodes, pore size, and linker functionalities on the catalytic performance of Zr-MOFs was fully evaluated and discussed. Featuring abundant bridging Zr-OH-Zr catalytic sites and confined microenvironments, the pristine UiO-66(Zr) could create abundant reactive oxygen species (ROS) with high H 2 O 2 efficiency, affording quantitative yield of azoxybenzene under mild conditions. Furthermore, the UiO-66(Zr)/H 2 O 2 heterogeneous catalytic system exhibited broad and size-selective substrate scope and excellent stability in consecutive catalytic cycles. Mechanism studies demonstrated that the azoxybenzenes were produced through radical pathway on bridging Zr-OH-Zr sites. This study provided alternative strategies exploiting green catalytic systems with porous MOFs, which might further expand the potential application of the MOFs family.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2023
·
IF 3.8
Fuhua Wei,Haiyan Liu,Qinhui Ren,Lu Yang,Lan Qin,Hongliang Chen,Yufu Ma,Zhao Liang,Siyuan Wang
Zr-MOF was prepared under solvothermal conditions using zirconium acetate as the metal ion and 2,5-dihydroxyterephthalic acid as the organic ligand. It was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), and thermogravimetry (TG). Zr-MOF was used as an adsorbent to remove norfloxacin from aqueous solutions. The experimental results were fitted, and the results showed that the pseudo-second-order kinetics model was appropriate for studying the removal of norfloxacin. We investigated the adsorption capacity of Zr-MOF under different masses, concentrations, and pH values. At pH 10, the maximum adsorption capacity after 5 h was 134.5 mg/g.Compared with another adsorbent,the adsorption capacity of Zr-MOF was higher.The removal of norfloxacin from an aqueous solution using Zr-MOF was feasible, inexpensive, and effective. Our findings indicate that Zr-MOF has broad application prospects for the purification of an aqueous solution.
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