Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Qinglian Sun,Sheng Huang,Zaoyuan Li,Donghua Su,Jinfei Sun
Metal-organic frameworks (MOFs) effectively remove hazardous contaminants and are widely used for wastewater treatment . In this work, Co-doped bimetallic MIL-88B(Fe/Co) was synthesized via the hydrothermal method to activate potassium persulfate (KPS) for methylene blue (MB) degradation. XRD , IR, XPS, and SEM were conducted to investigate the crystalline structure, chemical valence state, and morphology of MIL-88B(Fe/Co). The synthesis time and Fe 3 + /Co 2 + molar ratio were optimized. Results showed that 10% Co-doped MIL-88B(Fe/Co) could efficiently activate KPS to achieve 100% MB removal in 15 min, thereby indicating that Co 2 + could accelerate metal-to-metal charge transfer during activation. A quadratic model was established by fitting the experimental data to optimize the degradation parameters. The reaction system with a temperature of 70 °C, KPS concentration of 30 mM, MOFs concentration of 0.8 g/L, and initial pH of 10 could effectively remove 99.85% MB in 5 min. Quenching experiments and EPR analysis revealed that·OH, 1 O 2 , and·O 2 − were the dominant reactive oxygen species (ROS) during MB degradation. The active sites (N15, N7, S10, and N18) most vulnerable to ROS attack in MB were identified by DFT calculation. MB degradation intermediates were identified through MALDI.
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JOURNAL OF MEMBRANE SCIENCE
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2022
·
IF 10.53
Wenji Zheng,Dongyue Wang,Xuehua Ruan,Yan Dai,Xiaoming Yan,Xiujuan Zhang,Xiangcun Li,Xiaobin Jiang,Gaohong He
Reducing the effective pore size of MOFs is necessary to improve gas screening of mixed matrix membrane (MMMs). However, continuous and precise regulation on pore size of MOFs is still challenging. In this work, dopamine (DA) monomers are proposed to polymerize in situ into pore cages of UIO-66, achieving the tuning of effective pore size for CO 2 screening. Meanwhile, the abundant hydroxyl and amino groups in polydopamine (PDA) offer high affinity with CO 2 to improve the selective permeation of CO 2 . Furthermore, additional PDA existing outside UIO-66 at longer polymerization time can intensify the interface compatibility to promote CO 2 /N 2 selectivity. Through increasing PDA content in the cage by prolonging polymerization time, the effective pore size and total pore volume of UIO-66 are decreased by 13.2% and 59.2%, respectively, compared with pure UIO-66. Correspondingly, PDA@UIO-66/Pebax MMM presents greatly improved CO 2 separation performances, especially the CO 2 /N 2 selectivity, compared with UIO-66/Pebax MMM. Specifically, both the permeability and selectivity of CO 2 increase with the PDA content into the cages increasing, which is attributed to the synergy of reduced pore size and abundant CO 2 -philic groups in PDA. The PDA 10.3 @UIO-66/Pebax MMM shows the best CO 2 /N 2 selectivity of 70.55 and CO 2 permeability of 94.56 Barrer, 29.2% and 27.9% higher than those of UIO-66/Pebax MMM, respectively. The proposed PDA@UIO-66 based MMMs exhibit superior CO 2 separation performance, especially high CO 2 /N 2 selectivity compared with most reported UIO-66 based MMMs. Together with the good long-term stability, the proposed regulating strategy on effective pore engineering of MOFs is promising and competitive in CO 2 screening of MOFs based MMM.
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Journal of Environmental Sciences
·
2022
·
IF 6.796
Wan-Yi Zeng,Minzhong Huang,Minglai Fu
Compared with the traditional liquid–liquid extraction method, solid-phase extraction agents are of great significance for the recovery of indium metal due to their convenience, free of organic solvents, and fully exposed activity. In this study, P 2 O 4 (di-2-ethylhexyl phosphoric acid) was chemically modified by using UiO-66 to form the solid-phase extraction agent P 2 O 4 -UiO-66-MOFs (di-2-ethylhexyl phosphoric acid-UiO-66-metal-organic frameworks) to adsorb In(III). The results show that the Zr of UiO-66 bonds with the P-OH of P 2 O 4 to form a composite P 2 O 4 -UiO-66-MOF, which was confirmed by X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FT-IR). The adsorption process of indium on P 2 O 4 -UiO-66-MOFs followed pseudo first-order kinetics, and the adsorption isotherms fit the Langmuir adsorption isotherm model. The adsorption capabilities can reach 192.8 mg/g. After five consecutive cycles of adsorption-desorption-regeneration, the indium adsorption capacity by P 2 O 4 -UiO-66-MOFs remained above 99%. The adsorption mechanism analysis showed that the P=O and P-OH of P 2 O 4 molecules coated on the surface of P 2 O 4 -UiO-66-MOFs participated in the adsorption reaction of indium. In this paper, the extractant P 2 O 4 was modified into solid P 2 O 4 -UiO-66-MOFs for the first time. This work provides a new idea for the development of solid-phase extractants for the recovery of indium.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Jiaojiao Cao,Yubo Lian,Huatao Weng,Zhenyu Chen
The effect of an external DC electric field on the inhibition behavior of Zn-MOFs in 0.5 mol/L NaCl solution for copper was investigated via electrochemical measurements and various characterization techniques. Results indicated that the corrosion inhibition efficiency of the Zn-MOFs decreased under strong electric field intensities, which went from 94.2% to 61.7%. The corrosion inhibition efficiency of the materials decreased with increasing electric field duration when maintained at a certain electric field intensity. When the electric field duration time was 6 h, 12 h, 18 h and 24 h, the corresponding efficiency was 90.4%, 86.8%, 78.2% and 61.7% respectively. The effect of an electric field on the corrosion inhibition performance of the Zn-MOFs could essentially be attributed to changes in the structure of the material framework.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Yuxin Li,Li Liu,Wei Li,Yeqing Lan,Cheng Chen
In this study, a novel Co 3 O 4 -La 2 O 2 CO 3 @C composite was fabricated via the calcination of Co-La bimetallic MOFs at 500 °C, and was employed to efficiently activate peroxymonosulfate (PMS) for simultaneous oxidation of roxarsone (ROX) and adsorption of concomitant inorganic arsenic. Approximately 100% of ROX (50 μmol L −1 ) was degraded by PMS (0.5 mmol L −1 ) activated with Co 3 O 4 -La 2 O 2 CO 3 @C (0.2 g L −1 ) at initial pH 6 within 10 min. Meanwhile, the produced inorganic arsenic was almost completely adsorbed within 90 min. The maximum adsorption capacity of As(V) by Co 3 O 4 -La 2 O 2 CO 3 @C was determined to be high up to 275.4 mg g −1 . Co 3 O 4 -La 2 O 2 CO 3 @C also exhibited superior stability. During 6 rounds, the degradation efficiency of ROX and the removal efficiency of the total As maintained almost 100% and more than 97%, respectively. SO 4 − and OH were confirmed to be the reactive oxygen species (ROS) in charge of the degradation of ROX and the conversion of As(III) to As(V). The investigation of the adsorption mechanism revealed that the As species were combined with La species via ligand and anion exchange, resulting in the formation of La-O-As bond. Furthermore, the practical application potential of Co 3 O 4 -La 2 O 2 CO 3 @C in the ROX degradation and the in-situ adsorption of the released arsenic were further evaluated in a continuous flow column reactor. The Co 3 O 4 -La 2 O 2 CO 3 @C composite as catalyst and adsorbent may offer a feasible strategy for the implementation of organoarsenic degradation and produced inorganic arsenic adsorption.
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TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
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2021
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IF 2.917
Lei HUANG,Zhi-hui YANG,LÜ-ji YAN,Sikpaam Issaka ALHASSAN,Hai-yin GANG,Ting WANG,Hai-ying WANG
2D carbon ribbon/Al 2 O 3 was synthesized with two-dimensional metal organic frameworks 2D-MOFs as precursors using the solvothermal and calcination methods. Batch experiments of adsorption parameters such as pH, liquid/solid ratio, adsorption kinetics, adsorption thermodynamics, and anions competitions were investigated to understand the adsorptive behavior of fluoride on carbon ribbon/Al 2 O 3 and nitrogen-doped carbon ribbon/Al 2 O 3 . The adsorption of fluoride on carbon ribbon/Al 2 O 3 could be described as the chemical and multilayer adsorption, while the adsorption of fluoride on nitrogen-doped carbon ribbon/Al 2 O 3 followed the chemical and monolayer adsorption phenomenon. The fluoride on nitrogen-doped carbon ribbon/Al 2 O 3 had a much faster adsorption rate of 3.1×10 −7 m/s than carbon ribbon/Al 2 O 3 , which was 1.2×10 −7 m/s. The nitrogen-doping on carbon ribbon enhances structural defects and improves the adsorption performance of fluoride. Also, the diacetylene linkages (—C≡C—) and pyridinic-N were studied to understand their influences on removing fluoride. The result indicates that carbon ribbon and nitrogen-doped ribbon could serve as good adsorbents for removing fluoride.
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FOOD CHEMISTRY
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2021
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IF 7.514
Yukun Yang,Zhuo Shi,Yuanyuan Chang,Xiaomin Wang,Ligang Yu,Caixia Guo,Jinhua Zhang,Baoqing Bai,Dandan Sun,Sanhong Fan
In order to solve inherent problems of traditional molecularly imprinted electrochemical sensors (MIECS), a novel platform of surface molecularly imprinted magnetic metal-organic frameworks (mMOFs@MIPs) was coupled with magneto electrode to establish magnetic MIECS for the recognition of oxytetracycline (OTC). mMOFs@MIPs were synthesized using layer-by-layer modification method for the recognition of OTC . With the help of magneto electrodes, mMOFs@MIPs can be magnetically modified on the electrode surface, forming the electrochemical sensing interface. The imprinted cavities of mMOFs@MIPs can act as the electron channel of the probe to realize label-free detection of OTC. A linear response was obtained within the OTC concentration range of 1.0 × 10 −9 g mL −1 -1.0 × 10 −4 g mL −1 . The applicability of the sensor was estimated using the spiking and recovery method in milk samples with the recoveries ranging from 89.0% to 103.1%. It has potential applications in food safety analysis with high throughput detection capability, high specificity and good stability.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 15
·6865-6871
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IF 3.591
Pengcheng Li,Enze Xu,Jiamin Zhang,Lei Chen,Zhenjie Sun,Li Wang,Yang Jiang
Transition metal sulfides (TMSs), especially cobalt-based sulfides have great potential use in battery anode materials. However, low coulombic efficiency and poor cycle stability limit their application in battery fabrication. In this work, a two-dimensional MOF material ZIF-9 was treated by a two-step calcination method that obtained a flower-shaped carbon skeleton coated with Co-vacancy, Co1−xS nanoparticles. The skeleton effectively restrains the volume expansion that happens on electrodes, which improved the electrical conductivity of the compound. The cobalt vacancy changes the local electronic structure and atomic populations; the DFT calculation also proves that this structure is beneficial to the migration of sodium ions and provides good cycling performance under high current density. According to our electronic experiments, Co1−xS@C exhibited good electrochemical performance, which maintains a capacity of about 300 mA h g−1 at a high current density of 5 A g−1 after 250 cycles. All results indicate the outstanding electrochemical performance of our composite material, especially under a high current density. This work may provide a method in MOFs-derived TMSs compounds to stimulate the potential of transition metal sulfide materials in energy storage.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2021
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IF 6.953
Yuqi Wang,Hiba Shaghaleh,Youself Alhaj Hamoud,Shuangsheng Zhang,Pengfei Li,Xu Xu,He Liu
In order to circumvent the water eutrophication caused by nitrogen loss in agriculture, slow-release and high-water containing fertilizers have captured much attention. Considering the unstable release of traditional slow-released fertilizers, novel strategies need to be designed to meet the steady release of fertilizers. Herein, by integrating cellulose-based hydrogel with MIL-100(Fe), a pH-sensitive Cellulose/MOFs hydrogel (CAM) with a high surface area (45.25 m 2 /g) was devised. The volume changes and the water adsorption of the hydrogels were uncovered from pH 3 to pH 11, where the highest water adsorption (100 g/g) was achieved at pH 11. Besides, a pH-sensitive urea slow release fertilizer (U-CAM) was also designed. The urea release of the U-CAM at pH 11 was much slower than that of the U-CAM at pH 3, which indicated its potential application in arid regions. In parallel with a favorable water-holding capacity, the totally loss of the soil moisture loaded with U-CAM was slowed down by 18 days as compared with the pure soil. The positive effect of the U-CAM on the growth of wheat was indexed with the germination rate, number of tillers, photosynthetic rate and chlorophyll content of the crop, which verified their further application in irrigating farming.
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JOURNAL OF CATALYSIS
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2020
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IF 7.888
Yanyan Gong,Ye Yuan,Cheng Chen,Somboon Chaemchuen,Francis Verpoort
Facile strategies for noble metal dispersion in the shell-layer of core–shell structured metal–organic frameworks based on Zr-MOFs (UiO-66@Pd-UiO-67-BPY) was developed. The robust structure of the core-structure UiO-66 was firstly synthesized before covering up with a shell-structure of UiO-67-BPY obtaining the core–shell structure (UiO-66@UiO-67-BPY). The metallation with active palladium species (Pd II ) was designed on the shell-layer of core–shell MOFs via a post-synthetic method. The Pd species were coordinated explicitly in a bidentate manner to the bipyridyl linkers of the shell-structure (UiO-67-BPY). Excellent dispersion of Pd in the shell structure was obtained, resulting in UiO-66@Pd-UiO-67-BPY, as confirmed from characterizations. Taking advantage of the designed catalyst, the synthesized UiO-66@Pd-UiO-67-BPY was examined for the catalytic hydrogenation reaction. The results revealed an excellent catalytic performance of UiO-66@Pd-UiO-67-BPY compared with the traditional catalyst Pd-UiO-67-BPY. Moreover, the designed catalyst structure exhibited outstanding performance and paved the way towards a cost-effective catalyst synthesis based on MOFs combined with a noble metal.
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BIOCONJUGATE CHEMISTRY
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2021
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IF 4.774
Chunxiao Sui,Rui Tan,Yiwen Chen,Guotao Yin,Ziyang Wang,Wengui Xu,Xiaofeng Li
Metal–organic frameworks (MOFs) derivatives had been widely explored in electronic and environmental fields, but rarely evaluated in the biomedical applications. Herein, Fe–N codoped carbon (FeNC) nanoparticles were synthesized and characterized via facile pyrolysis of precursor ZIF-8 (Fe/Zn) nanoparticles, and their potential applications in tumor therapy were assessed in this investigation both in vitro and in vivo. After PAA (sodium polyacrylate) modification, the FeNC@PAA nanoparticles were able to initiate a Fe-based Fenton-like reaction to generate ·OH and O2 for chemodynamic therapy (CDT) and O2 evolution. Meanwhile, the porphyrin-like metal center in the FeNC@PAA nanoparticles could be used as a photosensitizer for photodynamic therapy (PDT) of tumors, which could be enhanced by O2 generated in CDT. Furthermore, the FeNC@PAA nanoparticles were also found to be effective in photothermal therapy (PTT) with a photothermal conversion efficiency of 29.15%, owing to a high absorbance in the near-infrared region (NIR). In conclusion, the synthesized FeNC@PAA nanoparticles exhibited promising applications in O2 evolution and CDT/PDT/PTT synergistic treatment of tumors.
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JOURNAL OF MEMBRANE SCIENCE
·
2020
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IF 7.183
Zixing Guo,Wenji Zheng,Xiaoming Yan,Yan Dai,Xuehua Ruan,Xiaochen Yang,Xiangcun Li,Ning Zhang,Gaohong He
Cage-type MOFs based Mixed-matrix membranes (MMMs) hardly exhibit screening effect of gas molecules due to the flexible aperture. Regulation of nanocages of MOFs by Ionic Liquid (IL) has been proved to be effective. Therefore, in this work, an IL adsorption/infiltration two-step strategy is proposed to confine IL into the nanocages of MOFs, achieving fine tuning of effective cage size for screening gas pair with similar size. [Bmim][PF 6 ] are first adsorbed on the outer-surface of ZIF-8, then through heat treatment, the aperture of ZIF-8 is dilated, and the bigger [Bmim][PF 6 ] molecules infiltrate through the dilated aperture into the nanocage driven by thermodynamics and differential concentration. When the temperature is down to room temperature, the aperture is narrowed to 3.4 Å, thus [Bmim][PF6] are confined into nanocages, which are confirmed by PXRD , TGA and FT-IR characteristics. By controlling IL content in the cage, the effective cage size of ZIF-8 is tuned to specific slope among dynamic diameters of CO 2 over N 2 , which is perfectly reflected in the CO 2 /N 2 separation. Compared with ZIF-8/Pebax MMMs, the IL@ZIF-8/Pebax MMMs exhibit improved CO 2 /N 2 selectivity but decreased CO 2 permeability, demonstrating effectiveness of cage size adjustment. Furthermore, with the IL molecules inside ZIF-8 cage increasing, the CO 2 /N 2 selectivity of the MMMs continues to rise, indicating cage size screening effect of ZIF-8 by IL infiltration . Especially, the IL 8 @ZIF-8/Pebax MMMs exhibit the best gas separation performances with CO 2 permeability of 117 Barrer and CO 2 /N 2 selectivity of 84.5, beyond the 2008 Robinson upper bound. The proposed strategy provides an effective but facile way to confine IL into the cages of MOFs to precisely screen gas pairs with similar size and can be easily expanded to other IL and MOFs system.
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