JOURNAL OF SEPARATION SCIENCE
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2018
·Vol. 41
·期 9
·2046-2055
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IF 2.415
Yulan Deng,Ruiqi Zhang,Di Li,Peng Sun,Ping Su,Yi Yang
Here, we describe a simple one-pot solvothermal method for synthesizing MIL-101(Fe)@polydopamine@Fe 3 O 4 composites from polydopamine-modified Fe 3 O 4 particles. The composite was used as a magnetic adsorbent to rapidly extract sulfonylurea herbicides. The herbicides were then analyzed by high-performance liquid chromatography. The best possible extraction efficiencies were achieved by optimizing the most important extraction parameters, including desorption conditions, extraction time, adsorbent dose, salt concentration, and the pH of the solution. Good linearity was found (correlation coefficients >0.9991) over the herbicide concentration range 1–150 μg/L using the optimal conditions. The limits of detection (the concentrations giving signal/noise ratios of 3) were low, at 0.12–0.34 μg/L, and repeatability was good (the relative standard deviations were <4.8%, n = 6). The method was used successfully to determine four sulfonylurea herbicides in environmental water and vegetable samples, giving satisfactory recoveries of 87.1–108.9%. The extraction efficiency achieved using MIL-101(Fe)@polydopamine@Fe 3 O 4 was compared with the extraction efficiencies achieved using other magnetic composites (polydopamine@Fe 3 O 4 , Hong Kong University of Science and Technology (HKUST)-1@polydopamine@Fe 3 O 4 , and MIL-100(Fe)@polydopamine@Fe 3 O 4 ). The results showed that the magnetic MIL-101(Fe)@polydopamine@Fe 3 O 4 composites have great potential for the extraction of trace sulfonylurea herbicides from various sample types.
研究领域:
环境科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yuhang Ren,Yu Tian,Yating Lu,Dongyu Nie,Huayi Zhu,Xia Yang
Malathion (MA) is a widely used organophosphorus pesticide globally. Developing efficient photocatalysts is crucial for eliminating MA pollution in water by photocatalytic technology. This study focuses on preparing a series of H-PDI supermolecule/NH 2 -MIL-101(Fe) (PM) materials by amidating NH 2 -MIL-101(Fe) with the more stable H-PDI supermolecule, forming a covalent O C–NH bond. Among these materials, 40 %PM (indicating a mass percentage content of 40 % H-PDI supermolecule in PM) exhibited the best performance for degradation of MA. Under simulated sunlight irradiation of a 10 mg·L 1 MA solution for 180 min, the reaction rate constants of 40 %PM were 5.95 times and 3.13 times higher than those of NH 2 -MIL-101(Fe) and H-PDI supermolecule, respectively. The enhanced performance is attributed to the formation of Z-scheme heterojunctions in the 40 %PM composite lead to fast separation of photogenerated e − and h + . Combining the results of HPLC-MS with Fukui Function, the HOMO, LUMO, and pathway of degradation of MA attracted by 1 O 2 , •OH, and h + were speculated. The pathway involves oxidation, demethylation, P-S bond breakage, decarboxylation, and final conversion to some inorganic molecules. The toxicity of the degradation byproducts were lower than that of MA estimated by Toxicity Estimation Software Tool.
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
DALTON TRANSACTIONS
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2022
·Vol. 51
·期 34
·13085-13093
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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.
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
ANALYTICA CHIMICA ACTA
·
2020
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IF 5.977
Qinzhi Wang,Zhan Shi,Zhi Wang,Yijian Zhao,Jianuo Li,Huifan Hu,Yaowen Bai,Zhihao Xu,Hui Zhangsun,Li Wang
Acid orange II (AO II), a typical azo pigment, is strictly controlled by legislation and prohibited in foodstuffs. Herein, we prepared gold nanoparticles decorated amino-functionalized Cr-based metal-organic frameworks [NH 2 -MIL-101(Cr)@Au] via an in-situ reduction method as a surface-enhanced Raman scattering (SERS) substrate for simultaneous adsorption and detection of AO II. Gold nanoparticles are uniformly dispersed on the surface of NH 2 -MIL-101(Cr) owing to its three-dimensional (3D) structure and the interaction between –NH 2 and Au ions , providing more SERS-active “hot spots”. These NH 2 -MIL-101(Cr)@Au nanocomposites exhibited selective and high adsorption performance (419.85 mg g −1 ) for AO II, and could be used as superior SERS substrates for the detection of AO II with a low limit of detection (LOD) of 0.05 mg L −1 and wide detection range of 0.05–50 mg L −1 using portable Raman spectrometer. Furthermore, this SERS assay has been successfully used to determine AO II in orange juice and chili powder with good sensitivities.
研究领域:
材料科学
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环境科学
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分析化学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2021
·
IF 5.909
Malcom Frimpong Dapaah,Baojian Liu,Liang Cheng
Metal-organic frameworks (MOFs) are of particular interest in the adsorption of organic pollutants . This study investigated the adsorption of aniline (ANI), furfural (FUR), and bisphenol A (BPA) in aqueous solution using MIL-101(Cr)-X (X = –H, –NO 2 , –NH 2 and, –N-2-pyc), MIL-100(Cr, Fe), HKUST-1, and ZIF-8. For the first time, an imino-functionalized MOF was used to adsorb organic compounds in water. MOFs were characterized by XRD, N 2 adsorption-desorption, SEM , TEM, elemental analysis, and FTIR. MIL-101-N-2-pyc demonstrated the highest adsorption capacity of 460.8, 126.5, and 100.7 mg/g towards 500 mg/L BPA, ANI, and FUR respectively. The adsorption isotherms better suited the Langmuir model than the Freundlich model. Importantly, 98% of BPA (100 mg/L) was removed and the kinetic data correlated well with the pseudo-second-order model (R 2 > 0.998). Binary adsorption of FUR and acetic acid (AA) were determined for industrial relevance. MIL-101-N-2-pyc outperformed commercial activated carbon and the other MIL-101s with an impressive co-adsorption of 66.1 mg/g FUR and 62.5 mg/g AA. Overall, the adsorption mechanism was due to hydrogen bonding, π-π interaction, and electrostatic attraction. Moreover, MIL-101-N-2-pyc exhibited remarkable structural stability and less than 0.01 wt% Cr leached into water. The adsorbent regeneration was improved after 4 cycles in methanol.
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
CATALYSIS COMMUNICATIONS
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2015
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IF 3.699
Yong Liu,Shao-Yi Jia,Song-Hai Wu,Ping-Li Li,Chun-Jiang Liu,Yi-Ming Xu,Feng-Xiang Qin
Highly dispersed metallic nanoparticles immobilizing inside the pores of MIL-101(Cr) were prepared using double solvent method (DSM). The particle size of Au, Ag, Pd, and AuPd NPs were 2.9 ± 0.7 nm, 1.9 ± 0.6 nm, 2.1 ± 0.6 nm and 2.8 ± 0.7 nm, respectively. The catalytic activity determined by the reduction of p-nitrophenol by NaBH 4 to p-aminophenol of Pd and AuPd prepared by DSM is 9.6 and 8.3 times higher than that of Pd and AuPd prepared by conventional impregnation method. The structure and activity of the catalysts prepared by DSM have no significant changes after three cycles.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
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2024
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IF 5.6
Shen Zhang,Yaxian Qiao,Shiwei Luo,Bingbing He,Jingliang Xu
We reported a bifunctional site-isolated Lewis acid-Brønsted base metal-organic frameworks (NH 2 -Mo-MIL-101(Al)) for selective epimerization and isomerization of glucose to mannose and fructose. The yields of mannose and fructose were 34.09 % and 19.25 %, respectively, at 120 °C for 40 min. The sum selectivity of mannose and fructose was 95.64 %. System characterization showed that the excellent catalytic performance may attribute to the synergistic effect of Lewis acid (MoO 2 and MoO 3 ) sites and Brønsted base (-NH 2 ) sites on NH 2 -Mo-MIL-101(Al). The composition of the catalyst before and after catalysis experiment was characterized by ICP-MS. Results showed that no Mo specie was leached from NH 2 -Mo-MIL-101(Al) after 5 times re-used. 97 % of catalytic efficiency was retained after 5 times reusing compared to origin NH 2 -Mo-MIL-101(Al). The N-Mo chemical bonding between Mo active sites with NH 2 -MIL-101(Al) skeleton enhanced the hydro-stability and hydrothermal cyclic stability. Notably, 94.13 % of total sugar recovery was achieved from reaction solution by sample crystallization process without requiring chromatographic separation. High purity of glucose (91.27 %) and mannose (88.53 %) were recovered from reaction solution. This study provided a green and feasible catalytic and recovery process for industrial production of high-yield mannose and fructose from glucose.
研究领域:
化学工程
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生物化学
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产品关联
DOI
高影响因子
Materials Today Communications
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2025
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IF 4.5
Lifeng Chi,Xiutong Wang,Siyao Guo,Meipeng Ren,Hua Guo,Mingchun Wang,Youbo Nan,Jinguo Wang
Photocathodic protection has obtained enormous attention in the field of metal corrosion control as an efficient and eco-friendly technology. Developing the photoelectrode with good photoelectrochemical properties is a prerequisite for achieving satisfactory photocathodic protection performance. Here, the NH 2 -MIL-101(Cr)/TiO 2 heterostructures are prepared. Meanwhile, the organic linkers and metal ions from NH 2 -MIL-101(Cr) are used to synthesize the N- and Cr-doped TiO 2 anodes, respectively. The UV–vis DRS, photoluminescence spectra and photoelectrochemical tests conducted under visible light demonstrate the enhanced light absorption, suppressed photoinduced charge carrier recombination, and accelerated separation and transfer rates of photoinduced electron-hole pairs in the TiO 2 composites. The 304 stainless steel connected with NH 2 -MIL-101(Cr)/TiO 2 heterostructures shows the most negative potential (about −0.72 V vs. SCE) and satisfied stability in a 3.5 wt% NaCl solution. The result can be explained by the significantly enhanced optical and photoelectrochemical properties and the strong electric field intensity in the composite heterojunctions. Besides, it has been observed that the NH 2 -MIL-101(Cr)/TiO 2 heterostructures exhibit the best photocathodic protection performance than Cr and N-doped TiO 2 anodes. This research broadens the application scope of MOFs in corrosion resistance and helps to assess the effect of heterostructure construction and element doping on TiO 2 .
研究领域:
材料科学
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电化学
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腐蚀与防护
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产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2025
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IF 4.7
Jian Luo,Yonghui Lin,Yanfeng Liu,Siliang Wang,Yiduo Chen,Xudong Tian,Weiting Yang,Zhongmin Su
Roxarsone (3-nitro-4-hydroxyphenylarsenic acid, ROX) is easily converted into highly toxic inorganic arsenic compounds, therefore, the development of highly efficient adsorbents for the removal of ROX from wastewater is necessary but remains challenging. In this study, NH 2 -MIL-101 (Fe) was synthesised and modified with TPA-CHO (4-(N, N-diphenylamine) benzaldehyde) to obtain TPA-MIL-101(Fe) with triphenylamine functionalised groups. The modified TPA-MIL-101(Fe) exhibits the very high adsorption capacity (728.2 mg g −1 ) and fast adsorption equilibrium (2 h). The TPA-MIL-101(Fe) showed excellent selectivity, and the adsorption efficiency hardly decreased in the presence of competing ions (Cl − , NO 3 − , SO 4 2− ). The TPA-MIL-101(Fe) showed good adsorption performance for ROX at pH 3–13, with the best performance at pH = 9. In addition, TPA-MIL-101(Fe) was able to remove trace amounts of ROX from actual water samples (<5 mg L −1 ) with an efficiency of 99.46 %, and the remaining ROX content meets the international drinking water standards of the World Health Organization (29 μg L −1 ). The mechanism studies have shown that the Fe-O-As coordination and the π-π stacking interaction between TPA-MIL-101(Fe) and ROX greatly enhance its adsorption performance. In conclusion, this work provides a promising material for effective removal of ROX from the environmental water.
研究领域:
环境科学
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材料科学
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环境污染与控制
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水处理技术
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配位化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2025
·
IF 3.5
Tongxin Xiao,Kangyue Qiao,Guodong Hao,Songyao Du,Yue Wang,Chao Sui
This study employed a solvothermal method to prepare an NH 2 -MIL-101(Fe, Co) bimetallic organic framework composite catalyst aimed at enhancing the photocatalytic reduction performance of Cr(VI). The experimental results show that introducing Co into the single-metal NH 2 -MIL-101(Fe) does not alter the material's octahedral structure. However, the bimetallic synergistic effect shifts the light absorption range to the red end of the spectrum, reduces the bandgap, and significantly improves carrier separation efficiency. Under visible light irradiation, the NH 2 -MIL-101(Fe, 0.15Co) catalyst exhibited outstanding photocatalytic performance, achieving a reduction efficiency of 94.7% for Cr(VI) within 40 minutes and 100% within 50 minutes, with a reaction rate constant 4.7 times that of the single-metal NH 2 -MIL-101(Fe). Free radical capture experiments further revealed that ·O 2 - is the key active species in the Cr(VI) reduction process, while photo-generated holes in the valence band can oxidise OH - to ·OH, synergistically participating in the reaction. Additionally, cyclic stability experiments showed that the catalyst maintained 85.8% reduction efficiency after five cycles, demonstrating excellent stability and practical application potential.
研究领域:
环境科学
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催化
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材料科学
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化学工程
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产品关联
DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 71
·41003-41011
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IF 2.936
Wen Bing Wu,Sun Xue,Jian Hua Chen,Xiao Li
Membrane separation technologies have great promising potential for applications in several industries. Metal–organic frameworks (MOFs), for their large surface areas, low framework densities, transition-metal ions in the skeleton and high pore volumes relative to other porous matrices, have great potential for the removal of sulfur from gasoline with high efficiency. In the present study, a novel porous membrane adsorbent MIL-101(Cr)/SA was prepared by immobilizing MIL-101(Cr) onto sodium alginate (SA) matrix, which can combine the size/shape selectivity of MIL-101(Cr) with the processability and mechanical stability of SA polymer. The physico-chemical properties of MIL-101(Cr)/SA were investigated by FT-IR, SEM, BET, XRD and EDX methods. To investigate the effects of some important factors on the adsorption behavior for thiophene, a batch of experiments were performed by changing the concentration of porogen polyethylene glycol in the MIL-101(Cr)/SA, solution temperature, initial thiophene concentration and contact time. Meanwhile, benzothiophene, thiophene and 3-methyl thiophene were used to test the selectivity of MIL-101(Cr)/SA. The MIL-101(Cr)/SA showed an excellent uptake capacity of 671 mg g−1 under the optimal adsorption conditions. Selectivity testing indicated that the uptake capacity of MIL-101(Cr)/SA follows the order of benzothiophene > thiophene > 3-methyl thiophene. Kinetics experiments indicated the pseudo-second-order model displayed good correlation with adsorption kinetics data. The Crank model showed that the intraparticle solute diffusion is the rate-controlling adsorption step. Regeneration experiment result shows that the prepared MIL-101(Cr)/SA has excellent adsorption and desorption efficiencies.
研究领域:
化学工程
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材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 39
·24453-24461
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IF 3.108
Chaocheng Zhao,Pei Dong,Zongmei Liu,Guangrui Wu,Shuaijun Wang,Yongqiang Wang,Fang Liu
An active Fe3O4/MIL-101 hybrid material was prepared via a simple in situ solvothermal method and characterized as a heterogeneous Fenton-like catalyst for Rhodamine B (RhB) degradation. The Fe3O4/MIL-101 exhibited enhanced catalytic performance for RhB degradation in a neutral solution. Under optimized conditions, almost 100% removal of 10 mg L−1 RhB was achieved in 30 min using 0.5 g L−1 Fe3O4/MIL-101 and 20 mM H2O2 at initial pH 7. The reusability of Fe3O4/MIL-101 was also investigated after four runs. On the basis of the characterization of the catalyst, the results of metal leaching, the effects of radical scavengers, and hydroxyl radical (˙OH) determination, it was concluded that RhB is decomposed mainly by the attack of the hydroxyl radical (˙OH), generated by the reaction of Fe2+ species with H2O2. MIL-101 showed a significant synergistic effect with Fe3O4, in which it played the role of a solid-acid catalyst with Lewis acid sites on its surface, ensuring that a Fenton-like reaction occurred in the neutral solution.
研究领域:
环境科学
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材料科学
✓ 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）