JOURNAL OF PHYSICAL CHEMISTRY B
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2024
·
IF 2.8
Hong-Jie Zhang,Xue-Bin Shang,Xu-Ran Wang,Chen-Xi Zhang,Qing-Lun Wang
SCPEEK@MOF proton exchange membranes, where SCPEEK is sulfinyl chloride polyether ether ketone and MOF is a metal–organic framework, were prepared by doping Fe-MIL-101-NH2 into polymers. The amino group in the MOF and the -SOCl2 group in thionyl chloride polyether ether ketone cross-link to form a covalent bond through the Hinsberg reaction, and the prepared composite membrane has stronger stability than other electrostatic interactions and simple physical doping composite membranes. The formation of covalent bonds improves the water absorption of the composite membrane, which makes it easy for water molecules to form hydrogen bonds. Moreover, SPEEK as a proton conductive polymer and the synergy of MOFs improve the proton conductivity of composite membranes. The composite membranes were characterized by Fourier transform infrared spectroscopy, powder X-ray diffraction, scanning electron microscopy, and atomic force microscopy. The swelling rate, water absorption, mechanical stability, ion exchange capacity, and proton conductivity of the pure sulfonated polyether ether ketone (SPEEK) membrane were compared with those of the mechanically doped SPEEK/MOF membrane and the composite membrane SCPEEK@MOF doped with different ratios of Fe-MIL-101-NH2, and all of the SCPEEK@MOF showed superior performance. When the Fe-MIL-101-NH2 loading rate of the composite membrane is 2%, the proton conductivity of the composite membrane can reach 0.202 S cm–1 at 363 K and a 98% relative humidity, which is much higher than that of the SPEEK/MOF membrane obtained by simple physical doping under the same conditions.
研究领域:
材料科学
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化学工程
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2019
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IF 4.084
Guoru Li,Xiaobo He,Fengxiang Yin,Biaohua Chen,Huaqiang Yin
The development of highly efficient electrocatalysts with low cost for oxygen reduction reaction (ORR) is urgently required for metal-air batteries and fuel cells. In this work, Fe Co/MIL-101(Cr) with various molar ratios of Fe/Co as hybrid catalysts was prepared by a facile and mild impregnation method. MIL-101(Cr) increased the specific surface areas of the hybrid catalysts, thus improving the dispersion of Fe and Co species at their surfaces. The effects of Fe and Co species on ORR activity of the hybrid catalysts were investigated. It is found that the synergistic effects between the well-dispersed Fe and Co species contribute mainly to ORR activity. More specifically, Fe species exert a partial-charge-transfer-activation effect on Co ones, which reduces the charge transfer resistance and thus improves the catalytic activity . As a result, Fe Co/MIL-101(Cr) showed the excellent ORR activity, in which Co 50 Fe 50 /MIL-101(Cr) exhibited the superior ORR activity to the other prepared hybrid catalysts.
研究领域:
材料科学
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电化学
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DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 4
·2198-2208
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IF 3.119
Hui Su,Jiaxin Lv,Liansheng Yang,Li Feng,Yongze Liu,Ziwen Du,Liqiu Zhang
The pollution of aromatic organophosphorus flame retardants (aromatic OPFRs) in aquatic environments has drawn great attention over the last few years. Two MIL-101-based metal–organic frameworks (Cr-MIL-101 and Fe-MIL-101-NH2) which possess ordered mesoporous cavities (2.9 and 3.4 nm) and aromatic structures were chosen and prepared to selectively adsorb a typical aromatic OPFR [triphenyl phosphate (TPhP)] from aqueous solution. Pore distribution analysis showed that Cr-MIL-101 and Fe-MIL-101-NH2 had both a mesoporous structure (2–3.5 nm) and microporous structure (1–2 nm), conducive to diffusion and adsorption of TPhP molecules. Compared with Fe-MIL-101-NH2 as well as commercial activated carbon, Cr-MIL-101 showed rapid and efficient adsorption for TPhP, and its initial sorption velocity (v0) calculated from the pseudo-second-order model was up to 568.18 μmol g−1 h−1. The adsorption equilibrium of TPhP on the Cr-MIL-101 was almost achieved within 12 h, while the equilibrium time of other adsorbents required more than 48 h. The study of selective adsorption found that Cr-MIL-101 had a higher sorption amount for aromatic OPFRs than alkyl-OPFRs and other aromatic compounds with different chemical structures. Cr-MIL-101 was able to keep a steady selective adsorption for TPhP in the presence of co-existing aromatic compounds. Based on the analysis of Kow, molecular structure and further density functional theory calculations, hydrophobic interactions may play a dominant role in the selective adsorption process of TPhP, and π–π interactions may be also involved. Cr-MIL-101 exhibits reusability and promising potential to rapidly and selectively remove aromatic OPFR in environmental remediation.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2026
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IF 7.3
Chunxia Ma,Limin Ma,Yaoyao Chen,Rui Han,Dongming Xu,Huanhuan Xing,Shasha Lu,Dewen Wang,Xiurong Yang
A major hurdle in nanozyme design is the difficulty of rationally tuning the coordination and electronic states of active sites, which are typically locked by the material’s rigid framework or surface composition. In this study, we address this limitation by developing a series of Fe-based quasi metal–organic framework nanozymes having a succulent appearance, denoted as Qx-MIL, through controlling the calcination of MIL. Partial decomposition of terephthalic acid ligands during heating increases the electron density of Fe active centers, reduces their coordination number, and generates asymmetric unsaturated Fe sites. These structural modifications enhance electron transfer, improve intermediate adsorption, promote the hydroxyl radical formation, and lower the energy barrier of the rate-determining step. As a result, Q400-MIL exhibits remarkable peroxidase-like activity and enhanced reaction kinetics. Leveraging this superior enzyme-mimicking performance, we constructed a galactose-oxidase-cascade colorimetric biosensor for the sensitive and selective detection of galactose. This work not only validates the high enzymatic activity and bioapplication potential of quasi MOF nanomaterials but also provides a simple and effective strategy for precisely engineering the active sites of nanozymes to broaden their functional scope.
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DOI
PubMed
高影响因子
Nanomaterials
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2020
·Vol. 10
·期 10
·2000
·
IF 4.324
Yongpan Shan,Chunli Xu,Hongjun Zhang,Huiping Chen,Muhammad Bilal,Shujun Niu,Lidong Cao,Qiliang Huang
Recently, metal–organic frameworks (MOFs) have become a dazzling star among porous materials used in many fields. Considering their intriguing features, MOFs have great prospects for application in the field of sustainable agriculture, especially as versatile pesticide-delivery vehicles. However, the study of MOF-based platforms for controlled pesticide release has just begun. Controlled pesticide release responsive to environmental stimuli is highly desirable for decreased agrochemical input, improved control efficacy and diminished adverse effects. In this work, simple, octahedral, iron-based MOFs (NH2-Fe-MIL-101) were synthesized through a microwave-assisted solvothermal method using Fe3+as the node and 2-aminoterephthalic acid as the organic ligand. Diniconazole (Dini), as a model fungicide, was loaded into NH2-Fe-MIL-101 to afford Dini@NH2-Fe-MIL-101 with a satisfactory loading content of 28.1%. The subsequent polydopamine (PDA) modification could endow Dini with pH-sensitive release patterns. The release of Dini from PDA@Dini@NH2-Fe-MIL-101 was much faster in an acidic medium compared to that in neutral and basic media. Moreover, Dini@NH2-Fe-MIL-101 and PDA@Dini@NH2-Fe-MIL-101 displayed good bioactivities against the pathogenic fungus causing wheat head scab (Fusarium graminearum). This research sought to reveal the feasibility of versatile MOFs as a pesticide-delivery platform in sustainable crop protection.Keywords:metal–organic framework;polydopamine;pesticide;pH-sensitive release;fungicidal activity
研究领域:
农业科学
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材料科学
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植物保护
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DOI
PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Chenxi Lu,Yuanzhuo Zhou,Liangzhi Li,Hongwei Chen,Lishi Yan
Catalytic production of 5-hydroxymethylfurfural (5-HMF) from glucose is a promising routine for generation of varied value-added chemicals. Herein, Mixed-Metal metal–organic frameworks (MOFs)–Fe/MIL-101(Cr) and MIL-101(Cr, Fe) obtained from post-synthesis modification and one-pot synthesis approach respectively were applied for catalytic converting glucose to 5-HMF. The synthesized Mixed-Metal MOFs were characterized by PXRD, SEM, N 2 adsorption–desorption analysis, TGA, XPS and NH 3 -TPD. Cr-and Fe-containing Mixed-Metal MOFs Fe/MIL-101(Cr) and MIL-101(Cr, Fe) presented synergistic effect with enhanced catalytic ability for glucose transformation to 5-HMF compared with typical single-metal MOFs and sulfonic acid-functionalized MOFs. Moreover, these two Mixed-Metal MOFs also presented better thermal stability than single-metal MOFs like MIL-101(Cr). Fe/MIL-101(Cr) was found to possess higher catalytic performance than MIL-101(Cr, Fe). 55.8 % 5-HMF yield was obtained with Fe/MIL-101(Cr) at 170 °C for 2 h in DMSO/water system. In addition, Fe/MIL-101(Cr) demonstrated desired recyclability for five times without incredible loss in its activity. This study provides a Mixed-Metal strategy on MOFs for improving catalytic efficiency of glucose conversion to 5-HMF.
研究领域:
化学工程
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材料科学
·
催化
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DOI
高影响因子
SYNTHETIC METALS
·
2019
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IF 2.87
Zhengsong Yu,Na Li,Xiaosong Hu,Yulin Dong,Yawei Lin,Hongwei Cai,Zhizhong Xie,Deyu Qu,Xi Li
Based on the electrode modified by the carboxyl-functionalized graphene, a highly sensitive electrochemical sensor for Pb 2+ detection was proposed by using 8–17 DNAzyme as the recognition element and the reaction of H 2 O 2 catalyzed by Fe-MIL-101 as the signal probe. Due to the high selectivity of the 8–17 DNAzyme to Pb 2+ , the excellent catalytic ability of Fe-MIL-101 and the advantages of graphene, the proposed electrochemical sensor exhibited an excellent sensing performance with a wide linear range of 10 −13 to10 −7 mol·L −1 , a lower detection limit of 1.74 × 10 −14 mol·L −1 and high selectivity to Pb 2+ . Tap water and river water were analyzed by the developed sensor with satisfying recoveries and RSD, demonstrating a promising practicability for the determination of Pb 2+ in the real sample analysis. Furthermore, the proposed strategy could be extended to the determination of other metal ions just by changing the specific DNAzymes.
研究领域:
分析化学
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环境科学
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纳米技术
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生物传感器
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 50
·108774-108782
·
IF 5.8
Xu Jinjie,Li Yongli,Yu Lihong,Pang Yuehong,Shen Xiaofang,Liu Jun
In this work, metal–organic frameworks (MOFs) including Fe-MIL-101 and Ti-MIL-125 were prepared and fixed on the melamine foam (MF) by polyvinylidene fluoride (PVDF) to prepare MF/PVDF/MOFs, which was used as adsorbents in pipette-tip solid-phase extraction (PT-SPE) for rapid extraction of organophosphorus pesticides (OPPs). Then, a gas chromatograph-flame thermionic detector (GC-FTD) was used for simultaneous analysis of Dimethoate (DMT), Iprobenfos (IBF), Parathion-methyl (PAM), and Chlorpyrifos (CPF). The morphology, crystal structure, and functional groups of MF/PVDF/MOFs were characterized, indicating that Ti-MIL-125 and Fe-MIL-101 were successfully synthesized and distributed on MF. The Fe-MIL-101 and Ti-MIL-125 showed good extraction ability for OPPs, which was mainly due to the π-π interaction and the multiple porous structures. Under the optimal conditions, the limit of detection (LODs) of four OPPs was 0.03–0.14 μg L −1 and the RSDs were less than 9.9%. The developed PT-SPE method showed a short extraction time (<3 min). The recoveries in fruits and vegetables (Celery, cabbages, and oranges) ranged from 75.3%–118.8% (RSDs<9.6%). The prepared MF/PVDF/MOFs demonstrated the efficient extraction performance of OPPs, contributing to the rapid pretreatment of OPPs from food and the environment.
研究领域:
分析化学
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环境科学
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食品科学
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产品关联
DOI
PubMed
高影响因子