CHEMOSPHERE
·
2021
·
IF 7.086
Peipei Huang,Lili Yao,Qing Chang,Yunhan Sha,Guodong Jiang,Shenghua Zhang,Zhe Li
The slow redox rate of Fe(III)/Fe(II) couples is a rate-limiting step for Fenton-like performance of Fe-MOFs. In this study, a series of catalysts (MIL-101) with various p-phthalic acid/2-aminoterephthalic acid (H 2 BDC/NH 2 –H 2 BDC) molar ratios were prepared using a simple and mild chemical method and applied for catalyzed degradation of bisphenol A (BPA). Interestingly, the –NH 2 modified MIL-101(Fe) can adjust Fe-Oxo node by increasing the electron density of Fe(III) in the presence of –NH 2 group with high electron density, thus forming Fe(II) in situ in MOFs. Meanwhile, the –NH 2 groups used as electron-donors can promote electron transfer , resulting in faster Fe(III)→Fe(II) half-reaction and active H 2 O 2 to continuously generate •OH radical. The BPA degradation and rate constant of Fe-BDC-NH 2 /H 2 O 2 system are 15.4-fold and 86.8-fold higher than that of Fe-BDC/H 2 O 2 system, respectively. The density functional theory (DFT) calculations showed that Fe-BDC-NH 2 possesses higher Fermi level energy (−4.88 eV) and lower activation energy barriers (0.32 eV) compared with Fe-BDC. Moreover, Fe-BDC-NH 2 showed good reusability and stability. This work offers a highly efficient and stable MOFs-based Fenton-like catalyst to rapidly degrade organic pollutants over a wide pH range for potential applications in wastewater treatment .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano Research
·
2020
·Vol. 14
·期 7
·2383-2389
·
IF 8.183
Zhang Yuwei,Liu Fei,Yang Zhichao,Qian Jieshu,Pan Bingcai
In the pursuit of heterogeneous catalysts with high reactivity, metal organic framework (MOF) nanomaterials have received tremendous attentions. However, many MOF catalysts especially Fe-based MOFs need to be utilized immediately after synthesis or being activated using high temperature, because of the easy loss of reactivity in humid environments resulting from the occupation of active Fe sites by water molecules. Here, we describe an inspiring strategy of growing MIL-101-Fe nanoparticles inside the three-dimensional confined space of graphene aerogel (GA), generating shapeable GA/MIL-101-Fe nanocomposite convenient for practical use. Compared to MIL-101-Fe, GA/MIL-101-Fe as catalyst demonstrates much higher reactivity in Fenton-like reaction, attributing to smaller MIL-101-Fe particle size, presence of active Fe(II) sites, and abundant defects in GA. Strikingly, the weakly hydrophobic nature of the composite greatly inhibits the loss of catalytic reactivity after being stored in humid air and accelerates the recovery of reactivity in mild temperature, by resisting the entrance of water molecules and helping to exclude water molecules. This work demonstrates that a delicate design of nanocomposite structure could not only improve the reactivity of the catalytic component, but also overcome its intrinsic drawback by taking advantage of the properties of host. We hope this functional nanoconfinement strategy could be extended to more scenarios in other fields.
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2018
·
IF 2.746
Man Gao,Wei Liu,Xuran Wang,Yanyan Li,Peipei Zhou,Liwan Shi,Buxing Ye,Randy A. Dahlgren,Xuedong Wang
Herein, we investigated in detail the relationship between surface properties and extraction performance of virgin and amino-functionalized MIL-101s(Fe) for the extraction of 10 bisphenols (BPs) and their derivatives. These BPs were used as model contaminants due to their different hydroxyl groups and contrasting polarities. The differential sorption efficiencies for relatively polar BPs (BPF, BPE, BPA , BPB , BPZ, BPAP and BPP) lies in the formation of hydrogen-bonding between OH of target analytes and NH 2 of two MIL-101s(Fe). However, the surface properties of MIL-101(Fe) and NH 2 -MIL-101s(Fe), such as S BET and pore structure , determined the extraction recoveries for BPs derivatives (BADGE, BADGE·2H 2 O and BFDGE·2H 2 O) due to lack of OH in their molecular structures. NH 2 -MIL-101s(Fe) nanosorbent was successfully applied to the preconcentration/extraction of trace BPs and their derivatives by dispersive solid-phase extraction (DSPE) method. Following optimization of the main factors, recoveries for BPs ranged from 90.8 to 117.8% and their LODs were 0.016–0.131 μg L −1 in environmental waters. Experimental precisions based on relative standard deviations were 0.9–4.9% for intra-day and 1.3–7.6% for inter-day analyses, respectively. These findings provide important information on how to design and modify nanosorbents for highly efficient extraction of pollutants having contrasting polarities. Moreover, the newly developed NH 2 -MIL-101s(Fe)-based DSPE method has a good application prospect in pretreatment of trace pollutants in real-world waters.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Tian Tian,Xuefeng Hu,Yao Huang,Huixian Du,Chao Wang,Mina Yang
The widespread utilization of fossil fuels has resulted in a significant increase in CO 2 emissions, leading to a variety of environmental issues. The photocatalytic conversion of CO 2 into fuel presents an effective solution to both the energy crisis and environmental warming. Therefore, the selection of a suitable catalyst is paramount. However, traditional photocatalysts often encounter challenges such as rapid electron-hole recombination and limited exposure of active sites. To improve these limitations, this study introduces AFM-X, a heterojunction catalyst composed of Au/Fe 3 O 4 /MIL-101(Fe)-X, which facilitates the formation of open metal sites (OMS) that enhance the effective separation of photogenerated carriers. In AFM-X, OMS function as Lewis acid sites, thereby enhancing CO 2 adsorption. The presence of Au nanoparticles (NPs) introduces additional active sites for CO 2 reduction. The synergistic effect between OMS and Au NPs increases the catalyst’s active sites, while the heterojunction construction promotes electron transfer, thereby enhancing CO 2 photocatalytic reduction efficiency. The CO generation rate of AFM-2 reached 98.8 μmol g −1 h −1 , surpassing those of FM, MIL-101(Fe), Fe 3 O 4 , and Au NPs, by 4.1, 6.3, 6.2, and 3.2 times, respectively. Furthermore, AFM-2 maintains stable performance over a 40 h cycle test. In-situ DRIFTS spectroscopy reveals that CO 2 reduction occurs through two parallel pathways. This study offers new insights into the design of composite photocatalytic materials, highlighting the effectiveness of OMS Lewis acid sites in significantly enhancing the photocatalytic reduction of CO 2 .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Shu-Huan Chen,Huma Javeria,Xu-Hui Sun,Zhen-Xia Du
With the proliferation of vehicles in households, people are spending more and more time in their cars, so it is important to ensure the air quality and safety of the car. In this research, environmentally friendly, green PET@PDA@MIL-101(Fe) (PPM) was prepared by in-situ solvothermal growth and acid etching methods, which was categorized by SEM, FTIR, XRD, XPS, and BET. PPM was used to adsorb benzene, toluene, and m-xylene at low concentrations. The maximum amount of adsorption of PET@PDA@MIL-101(Fe) (PPM) for benzene, toluene, and m-xylene was 68.72 mg/g, 91.63 mg/g, and 78.47 mg/g respectively. The adsorption process of PPM is well fitted by the pseudo-first-order kinetic model and Langmuir isothermal adsorption model. Furthermore, PPM exhibited excellent toluene removal performance in simulated vehicles and excellent cycling capability in adsorption-desorption experiments. As a result, PPM can be used to treat and manage toluene volatile organic compounds (VOCs) at low concentrations.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yiting Lv,Jinjuan Xue,Zhaoxia Chen,Jianan Qu,Kaiwen Huang,Mingxin Wang,Wei Sun
Photocatalytic production of H 2 O 2 has garnered significant attention, but the use of sacrificial reagents in H 2 O 2 photosynthesis and the subsequent limited H 2 O 2 activation efficiency would impede its practical application in water decontamination. In this work, hydrothermal carbonaceous carbon/NH 2 -MIL-101(Fe) (abbreviated as HTC-cf/NMIL-101(Fe)) heterojunction was fabricated through a solvothermal strategy, and serving as a self-sufficient photo-Fenton-like catalyst to in-situ generate and activate H 2 O 2 . Hydrothermal carbonaceous carbon derived from cost-effective waste coffee grounds, serving as a green and sustainable photocatalyst, demonstrated high H 2 O 2 production rate of 612 μmol/g/h without the need for sacrificial reagents or aeration assistance. Moreover, the excellent self-sufficient photo-Fenton activity for HTC-cf/NMIL-101(Fe) can be obtained, which ascribed to the synergistic effect of self-generated H 2 O 2 production as well as the in-situ catalytic H 2 O 2 decomposition of • OH by Fe species in NMIL-101(Fe) and photogenerated electrons. The optimized HTC-cf/NMIL-101(Fe) photocatalyst showed simultaneous improvements in both H 2 O 2 production and activation capabilities. Impressively, the effective circulation of Fe 3+ /Fe 2+ in NMIL-101(Fe), aided by photogenerated electrons, results in a 5-fold increase toward H 2 O 2 decomposition rate constant (K d ) compared to HTC-cf alone under light irradiation in open-air conditions. The enhanced charge separation and appropriate band structure of HTC-cf/NMIL-101(Fe) photocatalyst assured the high selectivity of two-electron O 2 -reduction to H 2 O 2 . HTC-cf/NMIL-101(Fe) displayed excellent photocatalytic sterilization efficiency against E. coli and S. aureus under visible light, and its sterilization application in actual water was also demonstrated. Notably, the adaptability of this system to ambient conditions, including open-air atmosphere, non-sacrificial reagents, and low leaching of Fe ions, highlights the promising practical utility of the HTC-cf/NMIL-101(Fe) photocatalyst.
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Jingjing Guo,Shu Wu,Yan Wang,Min Zhao
A label-free and high sensitive fluorescence biosensor for the detection of choline and acetylcholine (ACh) was developed based on the MIL-101(Fe) nanozyme with dual functions of mimetic peroxidase and fluorescent emission. This fluorescence sensing strategy involves the reaction of acetylcholinesterase (AChE) catalyzing the hydrolysis of ACh into choline that is in turn oxidized by choline oxidase (ChOx) to generate H 2 O 2 , and the as-produced H 2 O 2 is decomposed into highly reactive hydroxyl radicals under the catalysis of MIL-101(Fe) nanozyme, thereby the non-fluorescent organic ligand terephthalic acid of MIL-101(Fe) is oxidized by hydroxyl radicals to form a highly fluorescent 2-hydroxy terephthalic acid. By virtue of this finding, the label-free detection of choline and ACh via multienzyme cascade reaction was realized with low detection limits of 20.0 nM and 8.9 nM, respectively. Moreover, the practicality of the developed bifunctional MIL-101(Fe)-based sensing strategy was successfully validated through the detection of choline in milk and ACh in human plasma. This proposed assay not only exhibited high sensitivity and selectivity towards choline and ACh, but also simplified the sensing systems, reduced the detection cost, and avoided the potential risks caused by the fluorescent reagents, which opened a green avenue for the analysis of complex biological samples.
✓ 已验证
DOI
高影响因子
DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 34
·13085-13093
·
IF 4.569
Lijun Guo,Feifei Li,Jianxin Liu,Zehui Jia,Rui Li,Zhuobin Yu,Yawen Wang,Caimei Fan
The scaling relations between nitrogen adsorption and NHx destabilization are key challenges to the widespread adoption of the photocatalytic synthesis of ammonia. In this work, a FeII-rich MIL-101(Fe) (MIL-101(FeII/FeIII)) was synthesized using a one-step solvent thermal method with ethylene glycol (EG) as a reducing agent, which can break the scaling relationship by photoinduced FeII (high nitrogen adsorption ability) and FeIII (high NHz destabilization ability) cycling. XPS was used to detect the change in iron valence state in the MIL-101(FeII/FeIII) material. The photocatalytic nitrogen fixation efficiency of MIL-101(FeII/FeIII) under visible light without any sacrificial agent was 466.8 μmol h−1 g−1, five times that of MIL-101(Fe). After photocatalytic experiments, MIL-101(FeII/FeIII) retained an unchanged FeII/FeIII rate, indicating that this FeII/FeIII cycling can be maintained. DFT modeling of the FeII-rich MOF material showed that a FeII1 FeIII2 system has a higher N2 activation capacity than a FeIII3 system. The catalytic mechanism was further proved by in situ infrared spectra and N15 isotopic tracers. Therefore, the improvement of photocatalytic activity was mainly attributed to the change in the nitrogen adsorption capacity during the photoinduced FeII/FeIII cycling.
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhiqiang Guo,Xinmiao Wu,Juanjuan Meng,Xinxin Li,Yuan Li,Liangliang Hu
MIL-101(Fe) has received more and more attention in wastewater treatment, and how to further improve its stability and sorption capacity has become a research focus. In this study, metal Mg was used to dope MIL-101(Fe) to construct Mg@MIL-101(Fe) with bimetallic sites, which was then mixed with NH 2 -MIL-125(Ti) to successfully fabricate Mg@MIL-101(Fe)/NH 2 -MIL-125(Ti) (MOM) bis-MIL composites. MOM not only contains a large number of sorption sites but also exhibits excellent stability and reusability, realizing efficient sorption of Pb(II) from aqueous solution. In addition, the sorption performance and mechanism of Pb(II) on MOM were investigated by the characterizations of SEM, BET, TG, XRD, FTIR and XPS, as well as the kinetic and thermodynamic analyses. The sorption of Pb(II) on MOM is in accordance with the Langmuir isothermal model and pseudo-second-order kinetic model. The maximum sorption capacity of Pb(II) on MOM derived from the Langmuir model fitting is 320.941 mg·g −1 . The sorption of Pb(II) on MOM is strongly affected by pH, but not by ionic strength, which indicates that MOM has good resistance to salt interferences. The strong complexation of carboxyl, hydroxyl and amino functional groups with Pb(II) is the main sorption mechanism of Pb(II) on MOM, and electrostatic interaction and ion exchange also contribute to the sorption. In conclusion, MOM has strong practical application prospects in the treatment of Pb(II)-containing wastewater.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jin Liu,Zhirui Fan,Wenzhe Zhao,Peipei Song
Recently, escalating antibiotics contamination in aquatic environments has become a critical global threat to public health. In this study, a novel cathode catalyst (NH 2 -MIL-101(Fe)@Mel-MoPc/BC) was fabricated via hydrothermal method for efficient degradation of ofloxacin (OFX) through an electro-activated peroxymonosulfate (PMS) system. The incorporation of Mo-C and Fe/Mo-N substantially enhanced the electrocatalytic performance. The influence of various parameters, including the internal mass ratio of the catalyst, current, PMS concentration, OFX concentration, pH, as well as electrolyte concentration and type on OFX degradation were systematically evaluated. Under optimal conditions, OFX degradation reached 92.6 %, with 84.2 % total organic carbon removal, outperforming previous studies. The free radical quenching experiment and electron paramagnetic resonance analysis identified singlet oxygen ( 1 O 2 ) as the dominant active species. In situ Raman spectroscopy, high performance liquid chromatography-mass spectrometry and density functional theory calculation elucidated the degradation mechanism and pathways of OFX, including demethylation, decarboxylation, hydroxylation, and dehydrogenation, ultimately forming water, carbon dioxide, and inorganic ions. Furthermore, computational toxicology and seed germination tests confirmed significantly reduced wastewater toxicity after treatment by electro-activated PMS system based on NH 2 -MIL-101(Fe)@Mel-MoPc/BC cathode. Additionally, it also exhibited superior cyclic stability and excellent performance in various real water matrices and for other organic pollutants such as Rhodamine B, phenol, tetracycline, and dimethyl phthalate, demonstrating great application potential. This work provides valuable insights into cathode catalyst design and establishes a sustainable technology for antibiotic wastewater treatment.
✓ 已验证
产品关联
DOI
高影响因子
MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 6
·1-9
·
IF 6.232
Qin Peige,Zhu Wenli,Han Lizhen,Zhang Xiaowan,Zhao Bing,Zhang Xuebin,Lu Minghua
The monodispersed mesoporous SiO 2 @metal-organic framework (MSN@MIL-101(Fe)) composites were prepared by grafting MSN-NH 2 onto MIL-101(Fe) particles with a solvothermal method. The adsorption ability of the composites was greatly improved compared to that of pristine MSNs or MIL-101(Fe) for phytohormones (Phys). The MSN@MIL-101(Fe) composites were characterized by scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, energy dispersive spectrometer, and mapping analysis. Using MSN@MIL-101(Fe) composites as sorbent, a dispersive solid-phase extraction procedure (dSPE) was developed to extract three endogenous Phys (abscisic acid (ABA), indole-3-aceticacid (IAA), and indole-3-butyric acid (IBA)) and two exogenous Phys (1-naphthylacetic acid (1-NAA) and 2-naphthylacetic acid (2-NAA)) prior to HPLC-DAD analysis. The experimental parameters including sample volume, sorbent amount, adsorption time, adsorption pH, desorption time, and desorption solvent on extraction efficiency were optimized and evaluated. Under optimized conditions, the working range of 0.08 to 0.45 ng mL −1 with enrichment factors from 144 to 207 were achieved. The linear range is 0.75–200 ng mL −1 for IAA, 0.20–200 ng mL −1 for ABA, and 1.0–200 ng mL −1 for IBA, 1-NAA, and 2-NAA. With MSN@MIL-101(Fe) as sorbent for extraction of Phys and determination by HPLC-DAD, two endogenous Phys (IAA and ABA) were detected from mung bean sprouts which were made in a laboratory, and the results were further confirmed by high-resolution mass spectrometry. The composites can be applied to extract other small molecules, which have similar chemical structures with Phys in biological, environmental, and food samples.
Schematic presentation of a dispersive solid-phase extraction using monodispersed mesoporous SiO 2 @metal-organic framework composites (MSNs@MIL-101(Fe)) as the sorbent for extraction, clean-up, and preconcentration of phytohormones in mung bean sprouts prior to HPLC-DAD analysis.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2024
·
IF 4.1
Jingjing Chen,Zhixiang Li,Xiaoqi Li,Yingxiang Du
A fluorescence sensor was developed based on NH 2 -MIL-101(Fe) and silicon-doped carbon quantum dots for the analysis of copper ions. Copper ions enhanced the fluorescence intensity of doped silicon-carbon quantum dots and decreased the intensity of NH 2 -MIL-101(Fe). The addition of copper ions resulted in fluorescence resonance energy transfer, which caused a reverse change in the fluorescence signal. The sensor based on the above mechanism can eliminate false positive interference. The fluorescence sensing system had a remarkable linear range of 0.25–5 µM for copper ions and a detection limit of 11 nM. It was then applied to water samples, resulting in recoveries ranging from 95.43 % to 103.1 %. The successful construction of this optical sensor not only broadened the way to detect copper ions but also provided a new idea for the detection of other targets mediated by copper ions. Finally, an attempt was made to construct a smartphone-assisted colourimetric platforms to detect copper ions in daylight.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）