SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Yang Wang,Rongkai Ren,Fang Chen,Liming Jing,Zhenhua Tian,Zhijian Li,Jianzhi Wang,Chen Hou
The polyfuoroalkyl substances, especially perfluorooctanoic acid (PFOA), are emerging as harmful environmental micropollutants that are known to globally contaminate water, air, and soil resources. Herein considering the urgent demand for the sensitive detection and effective degradation of PFOA present in water environment, a novel molecular imprinting polymer (MIP) MOFs (Co/Fe)-driven carbon nanofiber (Co/Fe@CNF) electrode has been developed for electrochemical detection and electro-Fenton (EF) degradation of PFOA. MIP was formed by one-pot step by electro-polymerization of the pyrrole in the presence of PFOA template on the Co/Fe@CNF. The MIP has a strong adsorption force on PFOA for the special O–H-π hydrogen bond between PFOA and the imprinting site, helped PFOA to access the surface of electrode. Therefore, the resulting MIP Co/Fe@CNF was able to detect PFOA with a good linear response in the range of 1 × 10 -8 –9 × 10 -5 M, and the limit of detection (LOD) was reached 1.073 × 10 -9 M. Moreover, the imprinted cavity on MIP can precisely adsorb PFOA and its intermediates to shorten the transmission distance between free radicals and targets, which enhanced the degradation ability in the EF process, and the targeted degradation efficiency reached 93% with 180 min.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
·
IF 4.598
Qi Wang,Jinjin Zhang,Nannan Dou,Jianying Qu
In this work, a leaf-shaped iron-doped metal–organic framework (MOF) was synthesized in the aqueous phase and marked as Fe-L-ZIF-8. Fe-L-ZIF-8 was carbonized at high temperature under nitrogen atmosphere to obtain an iron and nitrogen doped carbon nanonets with unique three-dimensional network structure (Fe, N -CNs), which was characterized with XRD, SEM, EDS, FTIR and electrochemical impedance spectra. And a highly sensitive electrochemical sensor was constructed through modifying Fe, N -CNs on the surface of a glassy carbon substrate for simultaneous detection of catechol and hydroquinone. Under optimal conditions, both the linear ranges for detecting CC and HQ are 0.50–80.00 μM and the limits of detection are both 0.17 μM. In addition, the proposed sensor exhibited a wider linear range with good stability, reproducibility and selectivity, which has potential applications.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Shiang Li,Chao Feng,Yuehong Xie,Changyan Guo,Liugen Zhang,Jide Wang
Transition metal-based nitrogen-doped carbon materials have been proved to be a promising low-cost electrocatalyst for oxygen reduction reaction (ORR), which is a critical step in systems such as fuel batteries and zinc-air batteries. In this paper, transition metal (cobalt) N-doped carbon nanomaterials derived from metal-organic framework (MOFs) were synthesized by calcination of ZIF-67 precursors at high temperature (Co@NCNTs). Nitrogen atoms were introduced into the carbon matrix by capturing volatile CNx from dicyandiamide, and porous carbon nanotube structures with N-doped and uniformly dispersed active sites were obtained. The effects of different carbonization temperatures and molar ratio of Co/2-MI on the catalytic activity of materials for ORR reaction were studied. It was found that the Co@NCNTs prepared at 700 ℃ with the ratio of cobalt metal to dimethylimidazole of 1: 8 shows excellent ORR activity in both acidic and alkaline electrolytes . In alkaline conditions, the half-wave potential E 1/2 = 0.81 V, initial potential E onset = 0.89 V, and limiting current density even reaching 7.4 mA cm −2 . And in acidic electrolytes, E 1/2 = 0.66 V, while the limiting current density is 6.4 mA cm −2 , which is still better than that of Pt/C. Its excellent ORR performance is due to the synergistic effect of the porous carbon nanotube structure, N-doped carbon and Co-Nx active sites. Meanwhile, the optimum catalyst also shows better stability and methanol resistance than Pt/C in both acidic and alkaline electrolytes .
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LUMINESCENCE
·
2022
·Vol. 37
·期 12
·2050-2058
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IF 2.613
Xin Hou,Xiaohui Wen,Juan He,Xiandeng Hou
Lanthanide metal–organic frameworks Eu(BTB) MOFs was synthesized in low-temperature plasma produced by dielectric barrier discharge (DBD). This DBD synthesis possesses the characteristics of rapid reaction (within 20 min), mild condition (low temperature and atmospheric pressure) and simple operation compared with many traditional synthesis methods. The prepared Eu(BTB) MOF material exhibits typical red light emitting of europium (Eu 3+ ) at 617 nm, which can selectively and sensitively be quenched in the presence of trace iron(III) ion (Fe 3+ ). A simple, fast and sensitive fluorescence sensing strategy of Fe 3+ was thus constructed, with a limit of detection (LOD) of 0.5 μM. Compared with reported fluorescence probes, Eu(BTB) MOFs have also demonstrated the advantages of low cost, easy and fast preparation, great stability, and excellent optical properties, thus making them a promising fluorescence candidate for trace Fe 3+ sensing for the potential application in biological systems in the future.
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TALANTA
·
2022
·
IF 6.556
Jingyu Li,Yexin Dai,Jinran Cui,Halayit Abrha,Ning Kang,Xianhua Liu
Overuse of antibiotics posed a global threat to human health and the ecological environment. Efficient detection and control of antibiotic pollution demand novel sensory materials. Here, a dual-luminescent material FS@UIO66 was successfully synthesized by encapsulating fluorescent molecules (fluorescein sodium , FS) in UIO66 based on the in-situ encapsulation method. We found that the dual emission peaks of FS@UIO66 at 369 and 515 nm can be sensitively and synchronously quenched by tetracycline (TET). Interestingly, these two peak intensities were switched anisotropically by levofloxacin (LEV), in which the signal at 515 nm was enhanced. Photophysical analysis revealed that there may exist a competition and replenishment mechanism in the sensing processes. The ratiometric fluorescent feature was employed for rapid detection of TET and LEV, with detection limits of 0.2444 μM and 0.2808 μM for TET and LEV, respectively. The superior sensitivity, high selectivity, and excellent recyclability of FS@UIO66 in sensing TET and LEV were demonstrated in this work. In addition, TET and LEV were also successfully detected by FS@UIO66 in water from real water environment. The results indicate that FS@UIO66 composites are favorable for TET and LEV detection, presenting a great sensing platform for antibiotic detection.
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ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 34
·2204499
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IF 19.924
Yue Liu,Xinfeng Zhou,Zirui Jia,Hongjing Wu,Guanglei Wu
Polymeric metal-organic framework (MOF)-derived composites are promising functional materials because of their exceptional chemical homogeneity, designable components, and adjustable pore size. The modulation of oxygen and Mn vacancies via the introduction of heteroatoms and changes in the annealing temperature in MOFs-derived composites can be a possible solution to investigate the polarization loss mechanism, which facilitates the improvement of electromagnetic loss capacity. Herein, the design of laminate-stacked sphere-shaped trimetallic CoNiMn-MOFs is presented. The derived CoNi/MnO@C composites retain the original topography of the MOFs. The concentration of oxygen vacancies increases with the incorporation of heteroatoms, but decreases with annealing temperature, which prevails in the polarization loss mechanism rather than the contribution of Mn 2+ vacancies and heterogeneous interfaces. Therefore, the minimum reflection loss of the CoNi/MnO@C sample demonstrates −55.2 dB at 2.6 mm and the broad effective absorption bandwidth reaches 8.0 GHz at 2.1 mm. This work is expected to provide meaningful insights into the significant effect of ion vacancy modulation on the EM wave-absorbing performance of Mn-based MOFs-derived composites.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Xiu-Zhi Wei,Fentahun Wondu Dagnaw,Jianguo Liu,Longlong Ma
Carboxylic acid is one of the most crucial and widely used organic chemicals in daily human life activities. Hence preparation of this important chemical was performed under the application of the highly selective photo-catalysts through oxidation of alcohols to carboxylic acids. Herein, we have designed and disclosed a binary NH 2 -MIL-125(Ti)/ NaBr) catalyst system to realize the effective transformation of alcohols into carboxylic acids under visible light irradiation . Hence, derivatives of benzyl alcohol containing either electron withdrawing and donating groups as well as aliphatic primary alcohols were effectively converted into the corresponding carboxylic acids. Based on our findings, NH 2 -MIL-125(Ti) based photocatalytic system has shown efficient and highly selective activities for oxidation of alcohol especially the in-situ conversion of co-catalyst NaBr into the corresponding free radical can enhance the alcohol oxidation performance of the catalytic system.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
IF 7.139
Tao Zhao,Dazhong Zhong,Genyan Hao,Guang Liu,Jinping Li,Qiang Zhao
The development of efficient and stable electrocatalysts is of great significance for improving water splitting. Among them, transition metal oxyhydroxides show excellent performance in oxygen evolution reactions (OER), but there are certain difficulties in direct preparation. Recently, Metal–organic frameworks (MOFs) as precatalysts or precursors have shown promising catalytic performance in OER and can be decomposed under alkaline conditions. Therefore, using a mild and controllable way to convert MOFs into oxyhydroxides and retaining the original structural advantages is crucial for improving the catalytic activity . Herein, a rapid electrochemical strategy is used to activate well-mixed MOFs to prepare Co/Ni oxyhydroxide nanosheets for efficient OER catalysts, and the structural transformation in this process was investigated in detail by using scanning electron microscope , X-ray diffraction, Raman, X-ray photoelectron spectroscopy and electrochemical methods . It is discovered that electrochemical activation can promote ligand substitution of well-mixed MOFs to form porous oxyhydroxide nanosheets and tune the electronic structure of the metal (Co and Ni), which can lead to more active site exposure and accelerate charge transfer. In addition, the change of structure also improves hydrophilicity , as well as benefiting from the strong synergistic effect between multiple species, the optimal a-MCoNi–MOF/NF has excellent OER performance and long-term stability. More obviously, the porous CoNiOOH nanosheets are formed in situ during electrochemical activation process through structural transformation and acts as the active centers. This work provides new insights for mild synthesis of MOFs derivatives and also provides ideas for the preparation of highly efficient catalysts.
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Nano Research
·
2022
·Vol. 16
·期 5
·6067-6075
·
IF 10.269
Ding Jieting,Guo Danyu,Hu Anqian,Yang Xianfeng,Shen Kui,Chen Liyu,Li Yingwei
The preparation of supported high-density metal nanoparticles (NPs) is of great importance to boost the performance in heterogeneous catalysis. Thermal transformation of metal-organic frameworks (MOFs) has been demonstrated as a promising route for the synthesis of supported metal NPs with high metal loadings, but it is challenge to achieve uniform metal dispersion. Here we report a strategy of “spatial isolation and dopant anchoring” to resist metal aggregation in the pyrolysis of MOFs through converting a bulk MOF into dual-heteroatom-containing flower-like MOF sheets (B/N-MOF-S). This approach can spatially isolate metal ions and increase the number of anchoring sites, thus efficiently building physical and/or chemical barriers to cooperatively prevent metal NPs from aggregation in the high-temperature transformation process. After thermolysis at 1,000 °C, the B/N-MOFS affords B,N co-doped carbon-supported Co NPs (Co/BNC) with uniform dispersion and a high Co loading of 37.3 wt.%, while untreated bulk MOFs yield much larger sizes and uneven distribution of Co NPs. The as-obtained Co/BNC exhibits excellent electrocatalytic activities in both hydrogen evolution and hydrazine oxidation reactions, and only a voltage of 0.617 V at a high current density of 100 mA·cm −2 is required when applied to a two-electrode overall hydrazine splitting electrolyzer.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Yong Xue,Jing Shao,Guoqi Sui,Yuqin Ma,Hongji Li
In this paper, a novel SERS imprinted composite material was successfully synthesized with the aid of surface enhanced Raman scattering technology and molecular imprinting technology, which could be suitable for specific detection of organic dyes in the river. The UIO-66(NH 2 ) was wrapped with a thin layer of polydopamine (PDA), after loading Ag nanoparticles on rough surface, Ag@UIO-66(NH 2 )/PDA was synthesized and applied as the SERS substrate. In order to promote the ability of selective detection property in the practical sample, the molecularly imprinted polymer (Ag@UIO-66(NH 2 )/PDA-MIPs) was proposed. When the concentrations range changed between 10 −8 mol/L and 10 −10 mol/L, the intensity of characteristic peak at 1596 cm −1 exhibited a linear relationship with OII concentrations increasing. The limit of detection was low than 10 −10 mol/L, the correlation coefficient was 0.9985. The prepared SERS substrate could be available to the practical sample detection, which expanded SERS detection fields.
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CARBOHYDRATE POLYMERS
·
2021
·
IF 9.381
Shao-zhong Hu,Ting Huang,Nan Zhang,Yan-zhou Lei,Yong Wang
Metal organic frameworks (MOFs) have been considered to be robust adsorbent for the removing heavy metal ions from wastewater due to their unique properties such as large active sites, high specific surface area and high porosity, etc., however, their practical engineering application faces the problem of serious agglomeration. In this work, a new strategy of chitosan (CS) assisting MOF dispersion was proposed to develop the new generation of MOF-based adsorbents, namely, CS grafted UiO-66-NH 2 composite materials (CGUNCM). The UiO-66-NH 2 was selected and it was grafted onto the main chains of CS through covalent bonding interaction with the aid of glutaraldehyde , which was totally different from the common method that grafting molecular chains on the surface of MOFs resulting in the dramatic reduction of active adsorption sites. The results show that grafting MOFs onto CS main chains not only greatly improves the dispersion of MOFs but also reserves the morphology of MOFs as much as possible. The adsorption performances toward Cu(II) and Pb(II) were intensively studied by varying adsorbate concentration, ionic strength , the contact time, adsorption temperature and pH value of solution. The results show that the composite adsorbent exhibits high adsorption efficiency and the adsorption equilibrium can be reached within 45 min, and the maximum adsorption capacity toward Cu(II) and Pb(II) achieve 364.96 mg/g and 555.56 mg/g, respectively. Furthermore, the composite adsorbent shows good reusability. This work provides a new method of fabricating the MOF-based adsorbent and paves the way for the practical application of such adsorbents in wastewater treatment.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Wei She,Jing Wang,Xuewei Li,Jingfang Li,Guijie Mao,Weizuo Li,Guangming Li
Tuning of the metal–metal/oxide interaction is a vital route to enhance the performance of the supported catalysts. In this study, a Cu/Zn bimetallic MOFs was synthesized through a simple solvothermal method by using an adenine rigid biomolecule acted as organic linker. Furthermore, a ZnO/nitrogen-doped carbon composite supported Cu catalyst (named as Cu-ZnO/NC-BMOFs) derived from the bimetallic CuZn-MOFs was obtained via one-pot pyrolysis method. The developed Cu-ZnO/NC-BMOFs catalyst was tested for hydrogenation-amination tandem reaction. The bimetallic CuZn-MOFs with the uniformly dispersed Cu and Zn centers acted as a self-sacrificing template, which could facilitate the derived catalyst with strengthened Cu-ZnO interaction, high dispersity, and more N species. All of these advantages give the developed Cu-ZnO/NC-BMOFs catalyst with higher performance in hydrogenation-amination tandem reaction compared with traditional Cu/ZnO/NC-IWI (synthesized by incipient wetness impregnation) catalyst. The Cu-ZnO/NC-BMOFs exhibits good stability for the recycling experiments with a negligible loss in its performance. More importantly, the Cu-ZnO/NC-BMOFs catalyst could convert nitroarenes into the corresponding imines or secondary amines with excellent selectivity (>90.0%). This bimetallic MOFs-derived strategy may provide a way for fabricating NC supported catalysts in other tandem reactions.
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