Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Shuya Liu,Xinjie Ma,Yuxin Liu,Weiwei Chen,Yuejie Ai,Kexin Li,Xiushen Ye,Ming Fang,Xiaoli Tan
To fully utilize the customizable characteristics of metal-organic framework (MOF) materials in environmental applications, it is important to precisely modulate the branching groups of MOFs for improved performance. In this work, MIL-53(Al) was modulated by different numbers of nitrogen atoms and carboxyl groups/phosphite groups (MOF-N 2 -(COOH) 3 , MOF-N 3 -(COOH) 4 , and MOF-N 2 -(PO(OH) 2 ) 3 ) via a post-synthesis modification method, and the influence of functional groups and chain length on adsorption and the mechanism of modified groups on the adsorption of uranium (U) are demonstrated. Batch experiments suggest the removal of U(VI) reaches 37%, 27%, and 90% for MOF-N 2 -(COOH) 3 , MOF-N 3 -(COOH) 4 and MOF-N 2 -(PO(OH) 2 ) 3 , respectively (pH = 4.0, T = 25 ℃, I = 0.01 M NaNO 3 ). The surface complexation between UO 2 2+ and the surface of functional groups on the modulated MOF dominates the adsorption. Nevertheless, the steric hindrance in MOF porous structure can explain the inferiority of U(VI) adsorption on MOF-N 3 -(COOH) 4 (27%) to MOF-N 2 -(COOH) 3 (37%). MOF-N 2 -(PO(OH) 2 ) 3 is more conducive to uranyl adsorption than MOF-N 2 -(COOH) 3 or MOF-N 3 -(COOH) 4 , which is due to better affinity of U(VI) to phosphate group than the carboxyl group by density functional theory (DFT) calculation. Moreover, the excellent regeneration performance and U(VI) adsorption of MOF-N 2 -(PO(OH) 2 ) 3 in natural water or wastewater further confirmed the practical application of modulated MOFs in practical application.
研究领域:
环境科学
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材料科学
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化学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Meng Xia,Longqi Li,Xiaocong Wang,Kaihao Xu,Shuai Zhang,Chengxue Zhang
During CO2/HCO3– reduction with renewable biomass, achieving high-efficiency production of the target products is vital but challenging. In this study, an NH2– functional-group-modified MIL-53(Fe) catalyst was synthesized using a facile and efficient method. Under the action of the NH2-MIL-53(Fe) catalyst, a clear synergistic effect was exhibited on the transformation of glucose and NaHCO3 into formic acid with a high yield of 50% at a low reaction temperature (190 °C) via a three-pronged route, which mainly involved the decomposition of intermediates of glucose to gradually reduce NaHCO3 to formic acid under hydrothermal conditions. An in-depth analysis of the catalytic mechanism and density functional theory calculations demonstrated that the increased alkalinity of active sites by the NH2– functional group incorporation into the catalytic system enhanced the crucial reaction steps and reduced the activation energy of the crucial reactions, including glucose isomerization, aldehyde intermediate retro-aldol condensation, and redox of aldehyde compounds and NaHCO3 to formic acid, thereby promoting the generation of target products and suppressing side products. This study addresses the challenge of reducing NaHCO3 from renewable biomass to commercial formic acid by constructing multifunctional active sites, thus providing a new strategy for achieving carbon cycling.
研究领域:
化学工程
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催化科学
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可再生资源转化
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
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IF 2.7
Xia Zhang,Jialong Chu,Yifang Zhang,Fei Li,Chen Wang,Tiemei Li,Jing Fan
A novel microporous iron-based MIL-101@MIL-53 Z-scheme heterojunction photocatalyst was synthesized via a one-pot solvothermal strategy. Composition, structure, morphology and optical properties of the prepared photocatalyst were characterized using XRD, SEM, FT-IR, XPS and UV-vis DRS. The formation mechanism of the iron-based MIL-101@MIL-53 Z-scheme heterojunction was proposed to be attributed to the gradual transformation from MIL-101 to MIL-53. The in situ formation of an iron-based MIL-101@MIL-53 Z-scheme heterojunction facilitated the electron transfer from MIL-53 to MIL-101. Therefore, the separation of photogenerated charge carriers was enhanced. The removal efficiency of 300 mg L−1 tetracycline hydrochloride reached 99.6% in 90 min under simulated solar light irradiation. Radical capturing experiments showed that ˙O2− was the main active substance for the degradation of tetracycline hydrochloride. This work provided strategies for development and application of iron-based MIL-101@MIL-53 Z-scheme heterojunction and efficient treatment of wastewater with a high tetracycline hydrochloride concentration.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2019
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IF 4.978
Zhenjiang He,Yuxi Yang,Peng Bai,Xianghai Guo
Selective adsorption and separation of three xylene isomers of seven stable metal-organic frameworks (MOFs) were investigated, where MIL-53(Cr) manifested the highest adsorption capacity and apparent preference for o -xylene. Further detailed studies with MIL-53(Cr) showed that pseudo-second-order model fit best with adsorption kinetics of xylene isomers, and the isotherms were perfectly fitted by Langmuir isotherm model. The adsorption was proved to be a quick process, and both the changes of entropy and enthalpy contributed to the o -xylene selectivity, but which mainly resulted from the entropy effect. The adsorption capacity of preferable isomer o -xylene, on account of better packing efficiency, was record-breaking 8.19 mmol/g, and selectivity of OX/PX, OX/MX and MX/PX were 13.75, 8.01 and 1.72, respectively. Both the adsorption capacity and OX selectivity on MIL-53(Cr) in liquid phase adsorption and breakthrough experiments were super high, which discriminated it from zeolites and other materials reported so far. Combined with extremely short equilibrium time and high stability, MIL-53(Cr) can be a promising adsorbent for separation of xylenes in industrial process.
研究领域:
化学工程
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材料科学
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物理化学
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产品关联
DOI
高影响因子
INORGANICA CHIMICA ACTA
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2022
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IF 3.118
Yan Wang,Wenpei Feng,Jinjun Li,Zhixiong You
Metal-organic frameworks (MOFs) have shown attractive advantages in adsorbing dyes from wastewater. However, their complex synthesis processes and poor stability have limited their applications. Herein, we proposed a novel two-step route to prepare NH 2 -MIL-53(Fe) at room temperature and investigated its dye adsorption performance. The prepared NH 2 -MIL-53(Fe) displayed high water stability in the pH range of 3–11. Moreover, NH 2 -MIL-53(Fe) showed a significantly higher adsorption capacity and faster adsorption rate towards congo red (CR) than the other selected dyes, with more than 99 % of CR being removed by NH 2 -MIL-53(Fe) within 20 min. The maximum adsorption capacity of NH 2 -MIL-53(Fe) for CR was 1877 mg·g −1 . Besides, the removal efficiency of CR could maintain higher than 80 % within the tested pH range (3 to 11), and removal efficiency was consistently higher than 95 % at different NaCl concentrations (0 to 0.4 M). The dynamic CR adsorption process matched the pseudo-second-order kinetic model and fitted well using the Langmuir model, suggesting that the adsorption of CR onto NH 2 -MIL-53(Fe) was a monomolecular-layer chemical adsorption process. More importantly, NH 2 -MIL-53(Fe) showed high removal efficiency and good reusability towards CR in both synthetic and model wastewater. Mechanistic studies suggested that the removal of CR was attributed to the synergistic effects of the π-π stacking interactions, hydrogen bonds and electrostatic interactions between CR and NH 2 -MIL-53(Fe). Overall, the present study provides a novel strategy for the facile synthesis of NH 2 -MIL-53(Fe), highlights the excellent adsorption performance and reusability towards CR and underlies the adsorption mechanisms involved.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2022
·Vol. 169
·期 9
·097508
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IF 4.386
Xiaomin Guo,Pinghua Chen,Hualin Jiang,Xiaoqiu Tang,Yiping Huang,Guanghui Wu,Jian Zhang
Due to the strong toxicity of heavy metal ions to public health and the environment, it is a great challenge to develop a method for ultra sensitive capture and determination of heavy metal ions effectively. Herein, a novel heterostructure composite (MIL-53(Fe)/Ag2CrO4, named MA(1:x)) was prepared by a simple method successfully. MA(1:x) modified GCE was applied to detect heavy metals ions simultaneously. Significantly, the designed MA(1:1)/GCE sensors performed outstanding detection performances. The wide ranges of 7.49 ∼ 320.00 μmol l−1 and 7.49 ∼ 320.04 μmol l−1 are obtained for Pb(II) and Cu(II) ions, respectively. The LOD of the MA(1:1)/GCE sensor was determined to be 27.40 nmol l−1 (5.68 ppb) for Pb(II) and 86.96 nmol l−1 (5.52 ppb) for Cu(II) ion simultaneously, which are lower than the allowable level of drinking water stipulated by the World Health Organization (WHO). Possible detection mechanism by the MA(1:1)/GCE was discussed. The MA(1:1)/GCE was successfully applied to monitor heavy metal ions locate in tap and river water. The recoveries are in the range of 93.86%–104.4%, which further proves the potential in analyzing real samples. Moreover, the MA(1:1)/GCE also showed excellent stability, selectivity, reproducibility. A novel method was provided to construct sensitive sensors for simultaneous analysis of different metal ions.
研究领域:
环境科学
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分析化学
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DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2024
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IF 3.7
Sijia Wang,Ye Liu,Liang He,Yu Sun,Qing Huang,Shoudong Xu,Xiangyun Qiu,Tao Wei
Solid polymer composite electrolytes possess the benefits of superior compatibility with electrodes and good thermal characteristics for more secure energy storage equipment. Herein, a new gel polymer electrolyte (GPE) containing NH 2 -MIL-53(Al), [PP 13 ][TFSI], LiTFSI, and PVDF-HFP was prepared using a simple method of solution casting. The effects of encapsulating different ratios of ionic liquid ([PP 13 ][TFSI]) into the micropores of functionalized metal-organic frameworks (NH 2 -MIL-53(Al)) on the electrochemical properties were compared. XRD, SEM, Nitrogen adsorption-desorption isotherms and electrochemical measurements were conducted. This GPE demonstrates a superior ionic conductivity of 8.08×10 –4 S cm –1 at 60 °C and can sustain a discharge specific capacity of 156.6 mAh g –1 at 0.2 C for over 100 cycles. This work might offer a potential approach to alleviate the solid-solid contact with the solid-state electrolyte and electrodes, and broadens up new window for the creation of all-solid-state batteries.
研究领域:
材料科学
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能源存储技术
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产品关联
DOI
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2017
·Vol. 409
·期 22
·5239-5247
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IF 3.431
Xie Lijun,Liu Shuqin,Han Zhubing,Jiang Ruifen,Zhu Fang,Xu Weiqin,Su Chengyong,Ouyang Gangfeng
The fiber coating is the key part of the solid-phase microextraction (SPME) technique, and it determines the sensitivity, selectivity, and repeatability of the analytical method. In this work, amine (NH 2 )-functionalized material of Institute Lavoisier (MIL)-53(Al) nanoparticles were successfully synthesized, characterized, and applied as the SPME fiber coating for efficient sample pretreatment owing to their unique structures and excellent adsorption properties. Under optimized conditions, the NH 2 -MIL-53(Al)-coated fiber showed good precision, low limits of detection (LODs) [0.025–0.83 ng L -1 for synthetic musks (SMs) and 0.051–0.97 ng L -1 for organochlorine pesticides (OCPs)], and good linearity. Experimental results showed that the NH 2 -MIL-53(Al) SPME coating was solvent resistant and thermostable. In addition, the extraction efficiencies of the NH 2 -MIL-53(Al) coating for SMs and OCPs were higher than those of commercially available SPME fiber coatings such as polydimethylsiloxane, polydimethylsiloxane–divinylbenzene, and polyacrylate. The reasons may be that the analytes are adsorbed on NH 2 -MIL-53(Al) primarily through π – π interactions, electron donor–electron acceptor interactions, and hydrogen bonds between the analytes and organic linkers of the material. Direct immersion (DI) SPME–gas chromatography–mass spectrometry methods based on NH 2 -MIL-53(Al) were successfully applied for the analysis of tap and river water samples. The recoveries were 80.3–115% for SMs and 77.4–117% for OCPs. These results indicate that the NH 2 -MIL-53(Al) coating may be a promising alternative to SPME coatings for the enrichment of SMs and OCPs.
研究领域:
分析化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
·
2024
·Vol. 149
·期 10
·4505-4516
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IF 3
Liu Huimin,Deng Lisha,Zhao Ziheng,Sun Xiaoyan,Zhou Ru,Shu Chi-Min,Jiang Juncheng
An iron-based metal–organic framework, MIL-53(Fe), was synthesized and added as a synergist to high-density polyethylene (HDPE), and its flame-retardant effect with aluminum diethyl hypophosphite (ADP) and aluminum hypophosphite (AHP) in HDPE was investigated to further improve the flame-retardant efficiency. FTIR results showed that the ADP, AHP, and MIL-53(Fe) were successfully incorporated into the HDPE. The LOI of HDPE-3 and HDPE-7 with 0.75 mass% MIL-53(Fe) was 48.9% and 34.8% higher than that of the pure sample. The combustion grades reached V-0 and V-1. HDPE/MIL-53(Fe)/ADP exhibited more superior flame-retardant properties than HDPE/MIL-53(Fe)/AHP. A synergistic effect between ADP and both AHP and MIL-53(Fe) changes the decomposition process of HDPE. In addition, the FGI value of the composites decreased after the addition of MIL-53(Fe). MIL-53(Fe) enhances the thermal stability of HDPE composites, and improves the quality of the char residue. Experimental results show that MIL-53(Fe) can be used as a flame retardant and is a novel material in polymer flame-retardant research. The new synthetic material shown here may contribute to environmental safety.
研究领域:
材料科学
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聚合物工程
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燃烧科学
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产品关联
DOI
高影响因子
JOURNAL OF FOOD ENGINEERING
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2025
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IF 5.8
Sihang Li,Xun Zhou,Jiahao Cui,Xingjian Zou,Zijian Li,Wirote Youravong,Ming Li,Haihua Wang,Zhenyu Li
Residual Alicyclobacillus acidoterrestris severely impacts juice quality. Conventional thermal treatments fail to completely eliminate bacteria and simultaneously cause the loss of heat-sensitive components. Ultrafiltration (UF) has been a nonthermal alternative to conventional thermal process for the sterilization of apple juice. However, membrane fouling, particularly biofouling is an obstacle for deployment of UF in food processing. In order to tackle the challenging issue of membrane biofouling while ensuring food safety, functionalized UF membrane was developed by multi-stage modifications including metal chelator coating and chlorogenic acid-encapsulated MIL-53(Fe) microparticle grafting. The engineered membrane was applied for cold sterilization of apple juice to remove Alicyclobacillus acidoterrestris . Results showed that (i) the engineered membrane could release chlorogenic acid in response to pH stimulation, (ii) the steady state flux of engineered membrane was maintained higher than the pristine membrane after filtration with contaminated apple juice. Only 4.9% viable bacteria were observed on the membrane surface, (iii) the antibacterial mechanism of engineered membrane was mainly due to the disruption of cellular structural integrity and enhanced permeability of cell membranes, which caused the damage to A. acidoterrestris cell, (iv) after filtration, the Fe 3+ concentration in the permeate solution was almost undetectable. The engineered membrane can simultaneously exclude and inactivate A. acidoterrestris in apple juice, while demonstrating excellent anti-adhesion and anti-biofouling properties. Furthermore, the engineered membrane complies with food safety requirements, which verifies that this metal-organic framework modification method has the potential for practical application in food processing.
研究领域:
食品科学
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膜技术
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微生物学
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食品加工
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纳米技术
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Luan Minh Nguyen,Ngoan Thi Thao Nguyen,Thuy Thi Thanh Nguyen,Dai Hai Nguyen,Duyen Thi Cam Nguyen,Thuan Van Tran
The global occurrence of textile dyes pollution has recently emerged, posing a serious threat to ecological systems. To abate dye contamination, we here developed a novel magnetic porous CoFe 2 O 4 @MIL–53(Al) nanocomposite by incorporating magnetic CoFe 2 O 4 nanoparticles with MIL–53(Al) metal–organic framework. This nanocomposite possessed a surface area of 197.144 m 2 g −1 and a pore volume of 0.413 cm 3 g −1 . The effect of contact time (5–120 min), concentration (5–50 mg L −1 ), dosage (0.1–1.0 g L −1 ), and pH (2–10) on Congo red adsorption was clarified. CoFe 2 O 4 @MIL–53(Al) could remove 95.85% of Cong red dye from water with an accelerated kinetic rate of 0.6544 min −1 within 10 min. The kinetic and isotherm models showed the predominance of Bangham and Temkin. According to Langmuir, the maximum uptake capacities of CoFe 2 O 4 @MIL–53(Al), CoFe 2 O 4 , and MIL–53(Al) adsorbents were 43.768, 17.982, and 15.295 mg g −1 , respectively. CoFe 2 O 4 @MIL–53(Al) was selected to optimize Cong red treatment using Box–Behnken experimental design. The outcomes showed that CoFe 2 O 4 @MIL–53(Al) achieved the highest experimental uptake capacity of 35.919 mg g −1 at concentration (29.966 mg L −1 ), time (14.926 min), and dosage (0.486 g L −1 ). CoFe 2 O 4 @MIL–53(Al) could treat dye mixture (methylene blue, methyl orange, Congo red, malachite green, and crystal violet) with an outstanding removal efficiency of 81.24% for 30 min, and could be reused up to five cycles. Therefore, novel recyclable and stable CoFe 2 O 4 @MIL–53(Al) is recommended to integrate well with real dye treatments systems.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
POLYMERS FOR ADVANCED TECHNOLOGIES
·
2019
·Vol. 30
·期 9
·2458-2467
·
IF 2.162
Zhongwei Chen,Tingting Chen,Yuan Yu,Qingwu Zhang,Zhiquan Chen,Juncheng Jiang
Metal-organic framework MIL-53 (Fe)@C/graphite carbon nitride hybrid (MFeCN), a novel flame retardant, was synthesized by hydrothermal reaction and subsequently added into unsaturated polyester resin (UPR). The structure, morphology, and thermal stability of MFeCN were characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDS), and thermogravimetric analysis (TG). The thermal stability and flammability of the UPR composites were characterized by TG and cone calorimeter tests (CCT). The results of CCT demonstrated that the peak heat release rate (pHRR), total heat release (THR), peak smoke production rate (pSPR), and total smoke production (TSP) of UPR/MFeCN-4 were reduced by 39.8%, 10.2%, 33.3%, and 14.5%, respectively, comparing with UPR. The results of TG and CCT indicated that MFeCN could improve the thermal stability, flame retardancy, and smoke suppression properties of the UPR composites. The residues after CCT were then characterized by laser Raman spectroscopy (LRS), XPS, and SEM. Finally, based on the above experimental results and analysis, the flame retardancy mechanism of MFeCN was proposed.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子