JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Kunpeng Liu,Nan Wang,Jianhua Li,Fanglin Du,Baorong Hou,Ruiyong Zhang
Electrochemical two-electron water oxidation reaction (2e − WOR) to produce H 2 O 2 has been widely concerned. However, four-electron competition reaction causes the large overpotential and low production rates of 2e − WOR, which restrict its’ development and application. Herein, we prepared N-TiO 2 derived from NH 2 -MIL-125 by the hydrothermal combined with calcination method. We found that N-TiO 2 as photoanode exhibited the well properties of photoelectrocatalysis water oxidation, which gave an overpotential of 630 mV at 1 mA cm −2 . The overpotentials of N-TiO 2 was approximately 130 mV (at 1 mA cm −2 ) lower than NH 2 -MIL-125, and even lower than the previous reported TiO 2 , which may attribute to the increased oxygen vacancy with the calcination process and N doping. In addition, we investigated the degradation performance of the prepared catalysts to degrade methylene blue by photoelctrocatalysis on-site the preparation of H 2 O 2 . It was shown that N-TiO 2 performed high degradation efficiency (∼91%) and excellent stability. The possible mechanism was speculated due to the increased oxygen vacancy and N doping. This work provides a new idea for photoelectrocatalysis water oxidation materials and points out a new way for on-site H 2 O 2 production for direct use.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Yuzhen Jiao,Yajie Chen,Wei Han,Shumei Liang,Wei Li,Guohui Tian
Metal-organic frameworks-based hybrids with desirable components, structures, and properties have been proven to be promising functional materials for photocatalysis and energy conversion applications. Herein, we proposed and prepared ZnSe sensitized hierarchical TiO 2 nanosheets encapsulated MIL-125(Ti) hollow nanodisks with sandwich-like structure (MIL-125(Ti)@TiO 2 \ZnSe HNDs) through a successive solvothermal and selenylation reaction route using the as-prepared MIL-125(Ti) nanodisks as precursor. In the ternary MIL-125(Ti)@TiO 2 \ZnSe HNDs hybrid, TiO 2 nanosheets were transformed from MIL-125(Ti) and in situ grown on both sides of the MIL-125(Ti) shell, forming sandwich-like hollow nanodisks, and the ratio of MIL-125(Ti)/TiO 2 can be tuned by changing the solvothermal time. The ternary hybrids possess the advantages of enhanced incident light utilization and abundant accessible active sites originating from bimodal pore-size distribution and hollow sandwich-like heterostructure, which can effectively promote CO 2 photoreduction reaction. Especially, the formed multi-channel charge transfer routes in the ternary heterojunctions contribute to the charge transfer/separation and extend the lifespan of charge-separated state, thus boosting CO 2 photoreduction performance. The CO (513.1 μmol g −1 h −1 ) and CH 4 (45.1 μmol g −1 h −1 ) evolution rates over the optimized ternary hybrid were greatly enhanced compared with the single-component and binary hybrid photocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Ning Yao,Jinfeng Chen,Ren Feng,Zhipeng Liu,Yu He,Zhuwu Jiang
N -nitrosodiethylamine (NDEA) is a disinfection by-product (DBP) and is classified as a probable carcinogen by the International Agency for Research on Cancer. Its concentration is lower but its toxicity is higher than other DBPs. Designing a new adsorbent with a high adsorption effect on low concentrations of NDEA instead of traditional materials will be useful. To the best of our knowledge, this is the first study to investigate metal-organic frameworks (MOFs) for the adsorption of NDEA. Two novel Al-based MOFs were synthesized by modifying MIL-96 with amino and thiol groups. Their adsorption performances at low concentrations of NDEA in water were compared using adsorption kinetics and isotherm models. It was observed that MIL-96 modified with thiol groups (MIL-96-M) followed the Langmuir and pseudo-second-order models and exhibited the best adsorption performance. Owing to the well-matched pore size and hydrophobicity, the Langmuir adsorption capacity of MIL-96-M for NDEA was achieved at 1004.71 μg/g. The parameters of the adsorption performance were investigated using the Box-Behnken response surface methodology, and on the basis of which, the performance under different conditions was predicted. The experimental data suggested that the increase in temperature and time was beneficial for the adsorption performance, whereas an increase in dosage was not beneficial. It was identified that the adsorption mechanism between MIL-96-M and NDEA involves van der Waals forces, electrostatic interactions, and nucleophilic reactions by characterization and density functional theory (DFT).
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POLYHEDRON
·
2022
·
IF 2.975
Chunqing Wang,Na Xia,Siming Zhu,Lin Chen,Liang Chen,Zhendong Wang
In this study, α- l -rhamnosidase was immobilized on magnetic Fe 3 O 4 /MIL-101 (Cr) nanoparticles using MIL-101(Cr) as precursor by crosslinking method. The crosslinking agent concentration ratio and crosslinking time were EDC/NHS 1:1 and 2 h, respectively. The immobilized materials were characterized by FT-IR, XRD, SEM and VSM. The saturation magnetization of the prepared magnetic nanoparticles was 46.2 emu/g. The optimum pH and temperature of immobilized enzyme were 6 and 60 °C. The application of immobilized enzyme in the preparation of hesperidin dihydrochalcone glucoside (HMGDC) by hydrolysis of hesperidin dihydrochalcone (HSDDC) was studied. The results showed that immobilized enzyme had better temperature resistance, repeatability and stability than free enzyme. The immobilized enzyme activity was 293.55 U/g, and the recovery was 116.03%. After treatment at 60 °C for 4 days, the enzyme activity remained at 24.6%. The conversion rate of HSDDC reached 93.1%.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Yichen Jiang,Dazhi Li,Yifei Zhao,Jianmin Sun
Hydrogen bond donor functionalized poly(ionic liquids) were incorporated into MIL-101 framework for synthesis of composites PIL-R@MIL-101 (R = COOH, OH, NH 2 ). The effect of different hydrogen bond donors on CO 2 -epoxide cycloaddition reaction was discussed through XPS, NH 3 -TPD characterizations. Thereinto, PIL-COOH@MIL-101 showed efficient catalytic performance in the cycloaddition reaction of CO 2 and epichlorohydrin , 92.7% substrate conversion was obtained under 70 °C, 1.0 MPa, cocatalyst- and solvent-free conditions for 2.5 h. The improved activity was benefited from the synergistic effects of Lewis acidic Cr centers, carboxyl group, and nucleophilic Br - , together with the high surface area (1178 m 2 /g), and good CO 2 affinity. In addition, PIL-COOH@MIL-101 also showed facile recovery method by easy centrifugation and good recycling stability. Considering the good CO 2 affinity, excellent catalytic performance in CO 2 cycloaddition reaction, better thermal and recycling stabilities, the facilely prepared functionalized poly(ionic liquid)@MIL-101 composite would exhibit promising application prospect in CO 2 capture and conversion.
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JOURNAL OF NANOBIOTECHNOLOGY
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2022
·Vol. 20
·期 1
·1-12
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IF 9.429
Hong Liping,Pan Mingfei,Yang Xiao,Xie Xiaoqian,Liu Kaixin,Yang Jingying,Wang Shan,Wang Shuo
In this study, a thermo-sensitive molecularly imprinted fluorescence sensor was developed for the specific detection of β-Lactoglobulin (β-LG) allergen in milk products. The metal–organic frameworks (MIL-100) with a high specific surface area was coated on the surface of upconversion micro-particles (UCMPs). As the core, an imprinted polymer layer allowing for swelling and shrinking with response to temperature was prepared, which exhibited high adsorption and mass transfer capabilities for β-LG allergen. The fluorescence intensity of UCMPs@MIL-100@MIP decreased linearly with the concentration of β-LG in the range of 0.1–0.8 mg mL−1, and the limit of detection was 0.043 mg mL−1. The imprinting factor reached 3.415, which indicated that excellent specificity of the UCMPs@MIL-100@MIP for β-LG allergen. In the analysis of β-LG allergen in actual milk samples, the proposed UCMPs@MIL-100@MIP fluorescence sensor produced reliable and accurate results (recovery: 86.0–98.4%, RSD: 2.8–6.8%), closely related to the results of standard HPLC method (correlation coefficient: 0.9949), indicating that its feasibility in the detection of β-LG allergen.Graphical Abstract
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ACS Catalysis
·
2021
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IF 13.084
Zhongjie Cai,Meng Huang,Jiajun Dai,Guowu Zhan,Fu-li Sun,Gui-Lin Zhuang,Yiying Wang,Pan Tian,Bin Chen,Shafqat Ullah,Jiale Huang,Qingbiao Li
Methanol synthesis from CO2 hydrogenation with H2 produced from renewable energy has emerged as a promising method for carbon neutrality. The supported Pd/In2O3 catalyst has attracted great attention due to its superior activity and methanol selectivity, but the formation of the In–Pd bimetallic phase upon over-reduction would lead to quick catalyst deactivation. In this work, we elucidate the reduction behavior of Pd/In2O3 catalysts by using TCPP(Pd)@MIL-68(In) as precursors. During catalyst fabrication, metalloporphyrins (viz., TCPP(Pd)) served as both a capping agent for the growth of MIL-68(In) and a shuttle for transporting the Pd2+, which enhanced the dispersion of Pd0 species on In2O3–x during the calcination and reduction treatments and prevented the formation of In–Pd bimetallic phase by over-reduction. With a low Pd loading of 0.53 wt %, the resultant Pd/In2O3 catalyst exhibited a maximum methanol space–time yield of 81.1 gMeOH h–1 gPd–1 with a CO2 conversion of 8.0% and a methanol selectivity of 81% over 50 h on stream (295 °C, 3.0 MPa, 19,200 mL gcat–1 h–1). In contrast, the comparative Pd/In2O3 catalyst prepared by the impregnation of PdCl2 in MIL-68(In) showed poor activity and stability due to the formation of InPd/In2O3–x surface structures. In addition, we found a strong connection between the reduced degree of In2O3 and the catalytic performance of the supported Pd/In2O3 catalysts by integrating catalyst characterization results with density functional theory (DFT) calculations. Interestingly, the surface In/O ratio detected by XPS can reflect information about both metal–support interaction and the amount of oxygen vacancy, which is highly related to the catalytic activity. The DFT calculation also shows that the Pd/In2O3 catalyst has excellent thermodynamic selectivity for the CH3OH product. This work provides an alternative synthetic strategy for Pd/In2O3 nanocatalysts and sheds light on the deactivation mechanism of the supported catalysts.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Chunyan Hu,Jinke He,Jianjun Liang,Tao Lin,Qiuliang Liu
A novel photo-Fenton catalyst α-Fe 2 O 3 @g-C 3 N 4 @NH 2 -MIL-101(Fe) (FGN) with dual Z-scheme heterojunction was successfully prepared by hydrothermal method to degrade tetracycline (TC). The preparation conditions were optimized by orthogonal test, and the successful synthesis was confirmed by characterization analyses. The prepared FGN showed better light absorption performance, higher photoelectrons-holes separation efficiency, lower photoelectrons transfer resistance, and higher specific surface area and pore capacity compared with α-Fe 2 O 3 @g-C 3 N 4 and α-Fe 2 O 3 . The effects of experimental conditions on the catalytic degradation of TC were investigated. The degradation rate of 10 mg/L TC could reach 98.33% within 2 h when the dosage of FGN was 200 mg/L, and the degradation rate could remain 92.27% after 5 times of reuse. Furthermore, the XRD spectra and XPS spectra of FGN before and after reuse were compared to explore the structural stability and catalytic active sites of FGN, respectively. According to the identification of oxidation intermediates, three degradation pathways of TC were proposed. Through H 2 O 2 consumption experiment, radical-scavenging experiments, EPR results, the mechanism of the dual Z-scheme heterojunction was proved. The improved performance of FGN was attributed to the dual Z-Scheme heterojunction effectively promoting the separation of photogenerated electrons from the holes and accelerating the electrons transfer , and the increase of the specific surface area.
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MICROCHEMICAL JOURNAL
·
2023
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IF 4.8
Wanlin Qin,Lufang He,Yuchi Zhang,Bohan Li,Le Han,Yan Xu
Construction of heterocompositional hybrid metal–organic frameworks (MOFs) by integration of more than two MOFs is a smart strategy for fine-tuning MOF properties. In this work, a novel yolk-shell MIL-88A@NiFe-PB heterostructure, in which MIL stands for Materials from Institute Lavoisier, and PB represents the coordination network of Prussian Blue, was fabricated through a fast wrapping and then inward-etching growth synthetic strategy under mild stirring condition. The thickness of the outmost layer of NiFe-PB and the internal core structure of MIL-88A can be controlled by tuning the concentration of K 4 [Fe(CN) 6 ]·3H 2 O in the assembly system. A rational growth mechanism for the yolk-shell MIL-88A@NiFe-PB heterostructure was proposed. The as-prepared yolk-shell MIL-88A@Ni 10 Fe PB-50 architectures were then explored for non-enzymatic glucose sensing. The results show that the designed glucose sensor exhibits a high sensitivity of 1963.2 μA mM −1 cm −2 over a wide linear range of 0.005–1.0 mM, a low detection limit (0.12 μM), as well as a fast reaction time (<2 s) and long-term stability for non-enzymatic glucose detection. Also, it shows good applicability in real serum samples. This work provides a “wrapping-inward-etching” synthetic strategy for construction of hybrid MOFs with exceptional outstanding non-enzymatic glucose sensing performance, providing a reasonable guide for construction of other MOF on MOF intriguing structures for electrochemical sensing applications.
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JOURNAL OF SOLID STATE CHEMISTRY
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2023
·
IF 3.3
Rui Zhao,Cheng Cheng,Xiurong Wu,Xueyan Bai,Fenghuan Wang
Due to the excellent pore structure , MOFs as the stationary phase was playing an important part in chromatography . In this work, the shell-core MIL-101(Al)@SiO 2 composites post-synthetic modified by ligands with different polarities were fabricated for separation of estrogens. The structure and morphology of these materials were characterized by X-ray diffraction (XRD), Fourier transform infrared spectrum (FTIR), scanning electron microscope (SEM) and Brunauer-Emmett-Teller (BET). In order to investigate the influence of the ligand polarity on chromatographic separation performance of estrogens, alkyl molecules with different chain length were introduced as the ligands. With the hydrophobicity and chain length of the ligands increasing, the resolutions of the MIL-101(Al)@SiO 2 columns for the separation of estrogens exhibited the tendency of a parabola. Best result was achieved on the C4-MIL-101(Al)@SiO 2 column. On that basis, the possible retention mechanism on C4-MIL-101(Al)@SiO 2 column was elucidated by studying the mobile phase effect on separation behavior.
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Energy & Environmental Materials
·
2021
·Vol. 6
·期 1
·e12254
·
IF 15.122
Ailin Li,Jian Xiong,Ye Liu,Liming Wang,Xiaohong Qin,Jianyong Yu
MIL-101(Cr) is a promising moisture absorbent for solar-driven water harvesting from moisture to tackle the worldwide water shortage issue. However, the MIL-101(Cr) powder suffers from a long ab/desorption cycle due to the crystal aggregation caused by its inherent powder properties. Here, we demonstrate a MIL-101(Cr) nanofibrous composite membrane with a nanofibrous matrix where MIL-101(Cr) is monodisperse in the 3D porous nanofibrous matrix through a simple spray-electrospinning strategy. The continuous porous nanofibrous matrix not only offers sufficient sites for MIL-101(Cr) loading but also provides rapid moisture transport channels, resulting in a super-rapid ab/desorption duration of 50 min (including an absorption process for 40 min and a desorption process for 10 min) and multicycle daily water production of 15.9 L kg −1 d −1 . Besides, the MIL-101(Cr) nanofibrous composite membrane establishes a high solar absorption of 92.8%, and excellent photothermal conversion with the surface temperature of 70.7 °C under one-sun irradiation. In addition, the MIL-101(Cr) nanofibrous composite membrane shows excellent potential for practical application due to its flexibility, portability, and use stability. This work provides a new perspective of shortening MOF ab/desorption duration by introducing a porous nanofibrous matrix to improve the specific water production for the solar-driven ab/desorption water harvesting technique.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Chan Zhou,Lei Zhu,Lin Deng,Haojie Zhang,Hanxuan Zeng,Zhou Shi
For improving the catalytic activity and recyclability of CuS in Fenton-like reaction processes, novel sulfur vacancies-enriched CuS@MIL-101(Fe) was constructed, characterized, and examined as heterogeneous catalysts for activating peroxymonosulfate (PMS) to degrade coumarin (COU). Thanks to the redox pairs of Fe 3+ /Fe 2+ , Cu + /Cu 2+ , S 2− /S 2 2− /S 0 /sulfate species, copper-iron synergistic effect and sulfur vacancies, the CuS@MIL-101(Fe) realized a complete removal of COU (30 μM) in 10 min with reaction rate constant of 0.577 min −1 , which was 11.1 and 17.0 times of CuS and MIL-101(Fe), respectively. The effect of various experimental conditions (i.e., initial pH, CuS@MIL-101(Fe) dosage, PMS concentration, and background anions) on COU degradation was discussed, and the stability and versatility of CuS@MIL-101(Fe) was studied as well. Radical scavenging experiments and electron paramagnetic resonance (EPR) spectroscopy identified • OH and 1 O 2 as the main reactive oxygen species (ROS). Finally, the possible mechanism of higher COU degradation efficiency in the CuS@MIL-101(Fe) activated PMS system and the degradation pathways were also deeply explored. Consequently, this work provided a novel insight into construction of sulfur vacancies-enriched heterogeneous catalysts for efficiently activating PMS for refractory organic pollutants elimination.
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