CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
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IF 3.898
Xueting Liu,Chunhui Hu,Jingjing Wu,Peng Cui,Fengyu Wei
In this study, a series of metal–organic frameworks (MOFs) NH 2 -UiO-66- x HAc catalysts were synthesized by solvothermal method using acetic acid (HAc) as a modulator, and were applied to the cycloaddition of CO 2 and epichlorohydrin (EPIC) under ambient pressure. Influences of the modulation by HAc on morphologies and structures of the MOFs are demonstrated via PXRD, FESEM, FTIR, N 2 adsorption–desorption, XPS and 1 H NMR characterizations. The results show that the MOFs containing mesoporous pores can be prepared by adjusting the concentration of HAc. By optimizing the amount of HAc added, the specific surface area of NH 2 -UiO-66-8HAc is as high as 879.17 m 2 ·g −1 , which is 28.3% higher than that of the original MOFs. And the evaluation of catalytic performance showed that HAc modulation enhanced the activity of NH 2 -UiO-66- x HAc under mild conditions. The exposure of Lewis acid sites, increased specific surface area and porosity via the modulation of HAc defective ligand can be supposed the key factors to determine the enhanced catalytic activities. In addition, considering the influence of gas concentration on the reaction, the concept of TOP (Turnover of Pressure, defined as the mass of conversions of a unit mass catalyst under unit pressure and unit time) was first proposed in this article.
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Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 44
·23666-23674
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IF 14.511
Mingna Chu,Yang Li,Ximing Chen,Guangyao Hou,Yan Zhou,Hongjun Kang,Wei Qin,Xiaohong Wu
Solar-driven carbon dioxide (CO2) reduction into valuable chemicals or feedstock is of great significance for the sustainable development of the environment and energy. Herein, we presented a photo-induced reduction method to synthesize catalysts by anchoring Zn single atoms (SAs) on UiO-66-NH2. Impressively, UiO-66-NH2-0.7Zn SAs had excellent performance in converting CO2 to carbon monoxide (CO), which was about a 5-fold improvement compared to pristine UiO-66-NH2 without a photosensitizer or hole sacrificial agent under UV-vis light. The remarkable photocatalytic CO2 reduction performance was attributed to the built-in electric field construction by anchoring highly dispersed Zn SAs on UiO-66-NH2. The built-in electric field could effectively promote the separation of photogenerated charges and activate CO2. Density functional theory (DFT) calculations revealed that low-coordination Zn–N2 sites could dramatically enhance the formation of COOH*, which was the rate-limiting step for CO generation. This study created a new opportunity to develop high-efficiency photocatalysts containing single-atom sites for photocatalytic CO2 reduction.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Hao Wang,Shuai Wang,Shixing Wang,Jiali Tang,Yingbi Chen,Libo Zhang
A new zirconium-based adsorption material (UiO-66-AMP) was prepared by modifying UiO-66-NH 2 with 5-adenosine to effectively remove Pb(II) and Cr(VI) from wastewater. The SEM, EDS, XRS and FT-IR characterization confirmed the successful synthesis of UiO-66-AMP. We conducted a sets of experiments to test the adsorption effectiveness of UiO-66-AMP for Pb(II) and Cr(VI). The maximum adsorption capacity of UiO-66-AMP for Cr(VI) (pH=2) and Pb(II) (pH=4) are 196.60 and 189.69 mg/g, respectively. The adsorption process conforms to the pseudo-second-order and Langmuir models, which indicates that the adsorption is a single-layer chemical process. Gibbs free energy ( ∆G) indicates that the adsorption of Pb(II) is an exothermic reaction , while the adsorption of Cr(VI) is an endothermic reaction . At the same time, the adsorbent maintains excellent adsorption capacity at least after 4 cycles. The good adsorption performance of UiO-66-AMP towards the metal ions was attributed to the surface complexation and electrostatic interactions. Therefore, the new adsorbent has obvious application prospect to remove Pb(II) and Cr(VI) from wastewater.
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Journal of Environmental Chemical Engineering
·
2020
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IF 4.3
Lei He,Lutao Yang,Luxia Zhang,Zhe Wang,Hongjie Cheng,Xiaoguang Wang,Jianrong Lv,Jun Zhang,Hong Mo,Jian Shen
The high salinity of oilfield-produced water caused by the presence of metal ions, such as Ca 2+ and Mg 2+ , has a significantly adverse effect on oil recovery. It is crucial to remove these metal ions efficiently before the oilfield wastewater is reinjected down into the oil wells. To address this issue, we prepared a PEG/Fe 3 O 4 /GO-NH 2 nanoadsorbent by aminating GO, incorporating magnetic Fe 3 O 4 nanoparticles and coating with PEG (PEG = poly(ethylene glycol); GO-NH 2 = aminated graphene oxide). We investigated the removal ratios of the nanoadsorbent for Ca 2+ and Mg 2+ . The respective removal ratios for Ca 2+ and Mg 2+ reached 69.8 % and 61.1 % at 10 min, indicating that the nanoadsorbent was capable of efficiently removing Ca 2+ and Mg 2+ . We also evaluated the reusability of the nanoadsorbent by recycling and reusing it 5 times. At the fifth recycling run, the nanoadsorbent retained relatively high reuse rates (79.1 % for Ca 2+ , 69.5 % for Mg 2+ ) and removal ratios (69.5 % for Ca 2+ , 64.3 % for Mg 2+ ), suggesting that the nanoadsorbent possessed relatively high reusability. Oilfield wastewater treated with the nanoadsorbent was employed for oil recovery in core displacement experiments. The oil recovery efficiency significantly increased by 11.8 % compared with untreated oilfield wastewater. Therefore, the PEG/Fe 3 O 4 /GO-NH 2 nanoadsorbent exhibits considerable potential for the treatment of oilfield wastewater to enhance oil recovery.
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Energy Technology
·
2020
·Vol. 9
·期 2
·2000957
·
IF 3.404
Bo Li,Jianhong Zhao,Qingjie Lu,Shiqiang Zhou,Haitang Wei,Tianping Lv,Yumin Zhang,Jin Zhang,Qingju Liu
Applying metal–organic framework (MOF) materials to perovskite solar cells (PSCs) is an innovative and promising direction in the current photovoltaic field, especially in low-cost carbon-based PSCs without hole transport layer. Herein, a novel mesoporous anatase TiO 2 nanocrystalline with pie morphology, large specific surface area (SSA), and outstanding wettability is successfully prepared by sintering the NH 2 -MIL-125 at 500 °C for 6 h. The TiO 2 derived from NH 2 -MIL-125 possesses excellent penetration and crystallinity of perovskite in the electron transporting layer (ETL), and exhibits appropriate work function which matches relatively better with the conduction band of perovskite. Meanwhile, the power conversion efficiencies (PCEs) of the two PSC devices based on the as-prepared TiO 2 are 13.49% and 12.55%, respectively. Moreover, both of these devices exhibit good stability.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Haojie Zeng,Zongxue Yu,Liangyan Shao,Xiuhui Li,Meng Zhu,Yuchuan Liu,Xiaofang Feng,Ximei Zhu
A composite membrane based on a novel strategy was prepared which using graphene oxide (GO), UiO-66-NH 2 and polyacrylic acid (PAA) as basic materials on the surface of nylon membrane by vacuum filtration self-assembly. The structure of the composite membrane was made of graphene oxide as vertical separation layer, the PAA@UiO-66-NH 2 (PAA@UiO) embedding between GO as horizontal capture material. The PAA@UiO-66-NH 2 /GO (PAA@UiO/GO) membrane was characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and atomic force microscopy (AFM). Compared with the GO membrane, PAA@UiO/GO membrane combined the effects of GO, UiO-66-NH 2 and PAA, which significantly enhances the separation performance of dye wastewater. In particular, the PAA@UiO/GO membrane can achieve complete removal of MB , RB and CR while the fluxes during filtration process can reach about 100 L ∙ m - 2 ∙ h - 1 . At the same time, PAA@UiO/GO membrane almost retained stable removal rate on all dyes under extreme pH and ionic strength conditions. In addition, after 10 cycles of experiments, PAA@UiO/GO membrane retained a removal rate and a flux more than 95% and 85 L ∙ m - 2 ∙ h - 1 for all dyes, respectively. Compared to a composite membrane based on intercalation, the unique structure of PAA@UiO/GO membrane with a large number of adsorption sites and screening structures, resulting a better removal rate for dyes. Furthermore, PAA@UiO/GO membrane has a great potential in practical applications and a solution to balance trade-off effect.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yuexin Wang,Zhen Zhong,Yaseen Muhammad,Hui He,Zhongxing Zhao,Shuangxi Nie,Zhenxia Zhao
Engineering of monodentate ligands induced defects was proposed to modify NH 2 -MIL-88B(Fe) in order to promote its synergetic photo-Fenton catalytic degradation performance for acetamiprid (ACTM) as model neonicotinoid insecticides. Three monodentate ligands with different coordination groups (benzoic acid, pyrrole and pyrrole-2-carboxylic acid) were applied to in-situ induce ligand vacancies on NH 2 -MIL-88B(Fe). Effect of defect coordination mode on its photo-Fenton catalytic performance was investigated through the ACTM degradation reaction. Ligand defects on NH 2 -MIL-88B(Fe) would generate three merits: (1) it can modulate surface properties to enhance adsorption affinity towards ACTM; (2) it can introduce large amount of monodentate ligands and ligand vacancies in MOFs to promote light absorption and electron-hole separation capacity for photo-catalysis; (3) it can increase the amount of Fe Lewis acid sites to improve redox capacity of Fe 2+ /Fe 3+ for Fenton-catalysis. In this work, Pyrrole-2-carboxylic acid (Pac) was proved to introduce more monodentate ligands in MOFs and generate more ligand vacancies as well. As a result, ACTM can be easily captured by defective NH 2 -MIL-88B(Fe) and degraded by in-situ triggered oxidative reaction through the synergistic “photo-Fenton catalysis”. Performance measurements showed that Pac-MIL88(Fe) achieved 7.3 times higher adsorption rate and 5.5 times higher catalytic rate for ACTM than that of pristine MIL88(Fe). Moreover, total organic carbon (TOC) conversion reached 97.0% within only 90 min using Pac-MIL88(Fe) as photo-Fenton catalyst, showing 1.7 times higher than pristine MIL88(Fe). Thus, the in-situ fabrication of ligand defect-containing MIL88(Fe) can be foreseen of potential for designing new MOFs for wider practical applications.
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MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 11
·1-11
·
IF 5.7
Li Dan,Gao Yanmei,Mu Mengyao,Zhu Shiping,Zhang Ning,Lu Minghua
Ionic liquid (IL)-modified UiO-66-NH 2 composite was prepared and used as sorbent of dispersed solid-phase extraction (dSPE) for extracting trace benzoylurea insecticides (BUs) from complex environmental matrices. The IL in framework endowed the prepared material had electropositive characteristics, which can produce interaction with electron rich guest molecules, such as BUs. The high thermal and chemical stability of UiO-66-NH 2 /IL enabled it to be reused for 16 times without significant reduction in adsorption performance. Due to the multiple forces including π-π, hydrogen bonding, and fluorine-fluorine interaction, UiO-66-NH 2 /IL showed good adsorption performance, short adsorption time (20 s) and rapid desorption ability (60 s) for BUs. Under the optimal conditions, the method exhibited wide linear range (0.02–500 ng mL -1 ) with correlation coefficient ( R 2 ) not worse than 0.9928, high enrichment factor (252–300), and low detection limit (0.005–0.4 ng mL -1 ). The dispersed solid phase extraction coupling with high-performance liquid chromatography-diode array detector (dSPE-HPLC-DAD) was successfully used to detection of BUs in real environmental samples and satisfactory recoveries were obtained (80.5%±2.4–118%±3.2). The results indicated that UiO-66-NH 2 /IL composite can be a potential sorbent for the preconcentration of trace insecticides in environmental samples. Graphical abstract
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JOURNAL OF SOLID STATE CHEMISTRY
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2023
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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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COLLOIDS AND SURFACES B-BIOINTERFACES
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2023
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IF 5.8
Ke Cai,Wei Pi,Jiangyang Qin,Chenxi Peng,Dandan Wang,Yingying Gu,Yong Mei
In this study, an electrochemical immunosensor was constructed to detect the cytokeratin 19 fragment antigen 21-1 (CYFRA 21-1) in human serum. CYFRA 21-1 is the most sensitive tumor marker of non-small cell lung cancer (NSCLC), its content in normal human serum should be less than 3.3 ng/mL. When lung cancer cells dissolve or die, a myriad of CYFRA 21-1 is released into a tumor patient’s blood circulation , and its serum content elevates strikingly. Consequently, detecting CYFRA 21-1 by an electrochemical biosensor is expected to provide a new method for the early detection and prevention of lung cancer. In this study, a composite of UiO-66-NH 2 and carboxylated multi-walled carbon nanotubes (CMWCNTs) was used as the substrate material of a sensor; the resulting sensor had a large specific surface area and strong electrical conductivity . Moreover, gold nanoparticles (AuNPs) were used to bind to antibodies through an Au-S bonds. Also, a supersensitive detection of CYFRA 21-1 was achieved through the specific bindings of antigens and antibodies. Under optimal detection conditions, the change of current signal intensity of the immunosensor was proportional to the logarithm of CYFRA 21-1 concentration and had a linear relation in the range of 0.005–400 ng/mL, while the detection limit was 1.15 pg/mL (S/N = 3). The proposed immunosensor had high precision, stability, and selectivity . More importantly, the sensor was been successfully applied to detect CYFRA 21-1 in human serum with high recovery, providing a new method for early screening and dynamic monitoring of lung cancer.
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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 MEMBRANE SCIENCE
·
2023
·
IF 9.5
Zhihong Lin,Ziyi Yuan,Kaifang Wang,Xuezhong He
Novel mixed matrix membranes (MMMs) with superior CO 2 /N 2 separation properties are of great importance for post-combustion CO 2 capture from flue gas . Metal-organic frameworks (MOFs) as one of the most attractive porous fillers for MMMs fabrication, are considered to provide a solid molecular sieving mechanism for enhancing CO 2 /N 2 selectivity. However, it causes the reduction in gas permeability and limits its further industrialization. Herein, we proposed a new strategy for filler functionalization by doping silver ions (Ag + ) into UiO-66-NH 2 nanoparticles through the double-solvent method and used for the preparation of advanced MMMs. The double-solvent method is benefits for the enrichment of Ag + in the hydrophilic pores of UiO-66-NH 2 . As a result, the prepared novel MMMs called Ag + @UiO@PIM-1 with the polymers of intrinsic microporosity (PIMs) as polymer matrix , show outstanding CO 2 permeability. According to the mixed gases (CO 2 /N 2 = 10:90) permeation experiments under 25 °C and 2 bar, the membrane with 30%Ag + @10%UiO loading achieves more than 65% increase in CO 2 /N 2 selectivity (∼30) and 120% in CO 2 permeability (>15,000 Barrer) compared to the pristine PIM-1 membrane. By optimizing the Ag + doping amount and Ag + @UiO loading content, the separation performance exceeds the 2019 CO 2 /N 2 upper bound. To figure out the separation mechanism, the pore texture properties and CO 2 affinity of the functional filler (Ag + @UiO) together with the membrane structure were characterized by XPS , PXRD , SEM, gas sorption , etc. The synergistic mechanisms by combing CO 2 facilitated transport and molecular sieving from pore regulation were identified to enable advanced CO 2 /N 2 membrane separation .
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