JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Yu Zhang,Hong Zheng,Pengyi Zhang,Xianming Zheng,Qi Zuo
Heavy metals are seriously hazardous contaminants and drinking water has been identified as an important route of human exposure to them. Herein, to efficiently and selectively remove trace heavy metal ions , a facile method was reported to achieve the slow polymerization of dopamine in the cages of MIL-100 (Fe) via ultrasonic treatment followed by the hydrolysis of the urea. X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), Brunner-Emmet-Teller (BET) and pore size distribution determination confirmed the formation of the polydopamine (PDA) and binding with the unsaturated Fe 3+ site in MIL-100 (Fe) pores. The composite not only retained pore structure of MOFs but also contained abundant reactive functional groups. When initial lead concentration was 150 ppb and 20 ppm calcium coexisted at pH of 6.5 ± 0.25, the effluent lead concentration met the safe drinking water standard in several tens of seconds, and decreased to 1.13 ppb in 10 min. The adsorption rate reached 99.35%. The synthetic strategy effectively overcomes mass transfer resistance of trace heavy metal ions and provides a facile approach to prepare adsorption materials for efficient and selective removal of trace heavy metal ions from drinking water.
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JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Meng Wang,Xiaoxu Wang,Bo Feng,Yuanhua Li,Xinchen Han,Zijie Lan,Huajun Gu,Huamin Sun,Meng Shi,Hexing Li,Hui Li
Acquisition of chiral amines is a very important item in scientific research. Chemoenzymatic catalyst combination of Pd nanoparticles supported on the external surface of the ethylenediamine-functionalized MIL-101 ( [email protected] ) with layered cross-linked enzyme aggregates of Candida antarctica lipase B (CALB-CLEAs) was established for the first time. This combination served as an ultra-efficient chemoenzymatic catalyst system for one-pot dynamic kinetic resolution (DKR) of rac -1-phenylethylamine leading to optically pure product (>99% ee value) with almost full conversion and excellent selectivity (>99%) without the aid of any additive. Significantly, aliphatic amines can be also efficiently converted to enantiomerically pure products, making this robust and heterogeneous combination one of the most powerful chemoenzymatic platforms for microwave-assisted one-pot DKR of amines available up to now.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
He Xiao,Wenyao Zhang,Qiushi Yao,Liulian Huang,Lihui Chen,Bruno Boury,Zhongwei Chen
Metal organic frameworks (MOFs) are exploited in many applications of materials science and very recently were investigated as precursors or reagents for material synthesis. In a new way different from previous approaches, here we introduce for the first time the synthesis of metal oxide M x O y in the presence of M-free MOF acting partially as a sacrificial template and as a provider of doping metal atom. We demonstrate this approach in the case of ZnO prepared by a simple hydrothermal method in the presence of a Zn-free MOF like MIL-53(Al) or MIL-125(Ti). The resulting ZnO show low content of Al or Ti < 2% and properties are significantly different depending on whether MIL-53(Al) or MIL-125(Ti) are used or if no MOF is present. The nature and presence of MOF has different major effects on the morphology, the specific surface area of as prepared ZnO and also on the oxygen defects in its crystal structure. Corroborating the XPS, UV–vis DRS, PL, EPR and DFT studies evidence the role of such O-defects on band gap narrowing for samples calcined at 400 °C. These exhibit high efficiency in photodegradation of methyl orange (MO) compared to ZnO prepared in MOF-free conditions or previous literatures. The kinetics of MO degradation is different depending on the morphology, the specific surface and oxygen defects. The present data open the door to a new approach of the synthesis of metal oxides and a control of their properties.
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TALANTA
·
2016
·
IF 4.035
Meng Chen,Ning Gan,You Zhou,Tianhua Li,Qing Xu,Yuting Cao,Yinji Chen
An ultrasensitive electrochemical aptasensor for simultaneous detection of oxytetracycline (OTC) and kanamycin (KAN) has been developed based on metal ions doped metal organic frame materials (MOFs) as signal tracers and RecJ f exonuclease-catalyzed targets recycling amplification. The aptasensor consists of capture beads (the anti-single-stranded DNA Antibody, as anti-ssDNA Ab, labeled on Dynabeads) and nanoscale MOF (NMOF) based signal tracers (simplified as Apts-MNM, the NMOF labeled with metal ions and the aptamers). Particularly, the MOF (UiO-66-NH 2 ), with large internal surface areas, ultrahigh porosity and abundant amine groups in the pores, was employed as substrates to carry plenty of metal ions (Pb 2+ or Cd 2+ ) and label aptamers of OTC or KAN. Thus, the aptasensor is formed by the specific recognition between anti-ssDNA Ab and aptamers. In the presence of targets (OTC and KAN), aptamers prefer to form targets-Apts-MNM complexes in lieu of anti-ssDNA Ab-aptamer complexes, which results in the dissociation of Apts-MNM from capture beads. With the employment of RecJ f exonuclease, targets-Apts-MNM in supernatant was digested into mononucleotides and liberated the target, which can further participate in the next reaction cycling to produce more signal tracers. After magnetic separation, the enhanced square wave voltammetry (SWV) signals were produced from signal tracers. The aptasensor exhibited a linear correlation in the range from 0.5 pM to 50 nM, with detection limits of 0.18 pM and 0.15 pM (S/N=3) toward OTC and KAN respectively. This strategy provides specificity and sensitive approach for multiplex antibiotics detection and has promising applications in food analysis.
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Materials Today Chemistry
·
2024
·
IF 6.7
Jian Gou,Yousong Hu,Luxin Xing,Jun Xu,Fengzhi Yue,Lina Zhang,Lei Jia
Traditional luminescent materials for anti-counterfeiting usually adopt encryption of low-level systems with limited security, which seriously hinders their application in preventing counterfeiting and information leakage. Therefore, it is urgent to develop materials for higher-level anti-counterfeiting. In this work, a stimulus-responsive intelligent luminescent material (AC@CDs-Eu-MOFs) was prepared by co-loading green-fluorescence CDs and red-fluorescence Eu-MOFs on Amino clay (AC). 5D security barcodes, which were easy to observe while difficult to clone, were ulteriorly designed based on the nanocomposite owing to the tunable fluorescence by optical stimulation and chemical stimulus. Owing to the large capacity, low cost, and easy authentication, the 5D security barcodes possess enormous potential in optical data storage and multi-dimensional information encryption. In addition, the chemical stimulus-response enables the nanocomposite achievable in detection of Cu 2+ and Bacillus anthracis. Particularly, quantitative determination of copper in environmental water samples could be realized with a detection limit as low as 10.67 nM. Therefore, the material shows potential for detection of environmental pollutants besides advanced anti-counterfeiting.
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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
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2024
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IF 3.1
Qiuhua Zhang,Youjia Wu,Pingping Wu,Liying Huang,Lingyi Huang
Luteolin is one of the bioactive components from the compound Anoectochilus roxburghii (Wall.) Lindl. oral liquid (CAROL), which was reported to have excellent hepatoprotective and anti-inflammatory activities. However, the enrichment and quantitation of luteolin from CAROL is challenging due to the low content and complex aqueous matrix. In this study, a bifunctional monomer surface molecularly imprinted polymer (MIP) with metal–organic frameworks (MOFs) as cores was prepared for the selective adsorption of luteolin from the aqueous system CAROL. Compared with conventional MIPs, this unique nanocomposite adsorbent (MOF@MIPs) has the advantages of short kinetic equilibrium time, good selectivity, and high adsorption capacity in aqueous solution. The theoretical maximum adsorption capacity of MOF@MIPs for luteolin was 36.99 mg/g. After adsorption enrichment of luteolin from CAROL using MOF@MIPs, liquid chromatography–tandem mass spectrometry was applied to analyze the target. The corresponding linearity range for analyte was 10–6000 ng/mL with good linearity (R 2 =0.9992), and the added recoveries varied from 85.70% to 99.25%. The present method has been successfully employed for the analysis of luteolin in five different batches of CAROL. Notably, we found no significant difference in the content of luteolin between these batches, which proved that the composition was stable between batches. The novel structure MIPs are suitable for the specific recognition of template molecules in aqueous solution. Therefore, this study provides a technical reference for the special identification and determination of trace components in complex samples, while the novel MOF@MIP nanocomposite can also provide valuable references for the extraction and purification methods of specific substances in traditional Chinese medicine and expand the application environment of MIPs material.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Yin-Xia Sun,Bo-Tao Ji,Jiang-Hai Chen,Lu-Lu Gao,Yu Sun,Zhe-Peng Deng,Biao Zhao,Jin-Guo Li
Diquat (DQ) is a typical bipyridine herbicide widely used to control weeds in fields and orchards. The severe toxicity of diquat poses a serious threat to the environment and human health. Metal-organic frameworks (MOFs) have received widespread attention due to their unique physical and chemical properties and applications in the detection of toxic and harmful substances. In this work, a two-dimensional (2D) Tb(III) functionalized MOF Tb(III)@ 1 ( 1 = [Cd(HTATB)(bimb)] n ·H 2 O (Cd-MOF), H 3 TATB = 4,4′,4″-triazine-2,4,6-tribenzoicacid, bimb = 1,4-bis((1H-imidazol-1-yl)methyl)benzene) has been prepared and characterized. Tb(III)@ 1 has excellent optical properties and high water and chemical stability. After the Tb(III) is fixed by the uncoordinated -COO- in the 1 framework, Tb(III)@ 1 emits the typical green fluorescence of the lanthanide ion Tb(III) through the “antenna effect”. It is worth noting that Tb(III)@ 1 can be used as a dual emission fluorescence chemical sensor for the ratio fluorescence detection of pesticide DQ, exhibiting a relatively low detection limit of 0.06 nM and a wide detection range of 0–50 nM. After the addition of DQ, a rapid color change of Tb(III)@ 1 fluorescence from green to blue was observed due to the combined effects of IFE, FRET and dynamic quenching. Therefore, a simple test paper box has been designed for direct on-site determination of pesticide DQ. In addition, the developed sensor has been successfully applied to the detection of DQ in real samples (fruits a Yin-Xia Sun and Bo-Tao Ji contributed equally to this work and should be considered co-first authors.nd vegetables) with satisfactory results. The results indicate that the probe developed in this study has broad application prospects in both real sample detection and actual on-site testing.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Shuming Yu,Kedi Cai,Hao Zhao,Tan Wang,Tingting Qu,Lan Li,Jianbin Li,Chuangang Yao,Xiaoshi Lang
Potassium-oxygen (K-O 2 ) batteries can offer high energy density and low cost, but suffer from poor cycle life due to low efficiency and slow kinetics. Therefore, the development of efficient catalysts is the key to solve the problems. In this study, an efficient Ag/MnO 1.1 @C composite is designed as a catalytic cathode for K-O 2 batteries via calcining MnAg-MOFs precursors. The porous chain structure of the material facilitates the storage of discharge products and diffusion of oxygen, while the oxygen vacancies enhance the adsorption of O 2 and catalytic activity. Furthermore, the interfacial electron transfer between Ag and MnO 1.1 induces surface charge redistribution, facilitating improved electrochemical reaction kinetics that effectively promote both formation and decomposition of the discharge product. And then, the coupling effect between Ag and MnO further promotes the electron transfer in the K-O 2 battery, which greatly enhances the ORR and OER activities. As a result, the Ag/MnO 1.1 @C composite as an air cathode for K-O 2 batteries show a specific initial discharge capacity of 2328 mAh g −1 (200 mAh g −1 limiting capacity) and 145 stable cycles.
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JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 34
·16171-16183
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IF 3.553
Liu Shengjun,Zou Qichao,Ma Yan,Sun Wen,Li Yu,Zhang Jian,Zhang Cheng,He Lifang,Sun Yudie,Chen Qian,Liu Bo,Zhang Hexin,Zhang Kui
Metal–organic frameworks (MOFs) are a new type of porous crystal materials that have been widely used in various fields. Owing to their adjustable porous structure, MOF photocatalysts with high catalytic activity have become a research hotspot. In this study, NH 2 -MIL-125/CoS x samples were investigated as a novel visible light-responsive catalyst for the removal of organic dye. The NH 2 -MIL-125/CoS x -20 composites showed the best photodegradation efficiency, where photodegradation of the rhodamine B reached 95.4% in 45 min. CoS x was able to effectively extend the wavelength absorption range of NH 2 -MIL-125 and effectively separate the photogenerated electrons and holes and that could lead to the improved photocatalytic performance of the composites. The reactive superoxide radical ( · O 2− ) was identified as the main active species using reactive species capture experiments, and a reasonable photocatalytic mechanism was proposed. This paper is intended to guide the development of organic–inorganic hybrid materials for environmental remediation.
研究领域:
材料科学
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环境科学
·
化学
·
纳米技术
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Molecular Catalysis
·
2019
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IF 2.938
Xuewei Li,Tianqinji Qi,Jing Wang,Wei She,Guijie Mao,Pengfei Yan,Weizuo Li,Guangming Li
Rational design and development of stable nitrogen-doped carbon supported non-noble metal based nanocatalysts with unique natures of active species and support for highly chemoselective hydrogenation of nitroarenes to arylamines remains a grand challenge. Here, firstly, an N, Fe-containing metal-organic frameworks (MOFs) has been designed and synthesized. Furthermore, an efficient N-doped carbon fiber supported FeO x -based nanocatalyst (FeO x @CN- hpes ) was prepared via pyrolysis of MOF@polymer composite towards electrospun nanofiber crosslinked N, Fe-containing MOFs. Remarkably, the developed FeO x @CN- hpes enables the hydrogenation of nitrobenzene to aniline with unprecedented performance (215.8 h −1 ) compared to those of FeO x @CN- hp (176.2 h −1 ) and FeO x @CN- pes (45.2 h −1 ) catalysts prepared by conventional approaches. The comparative characterizations have revealed that the high dispersion of FeO x species, enhanced basicity, and more structural defects and Fe-N x species towards FeO x @CN- hpes are responsible for the high performance. Moreover, the effect of the pyrolysis temperature towards FeO x @CN- hpes on the performance of hydrogenation reaction was also systematically investigated. The results indicated that the FeO x @CN- hpes -400 catalyst prepared at 400 °C was identified as the best hydrogenation catalyst. More importantly, the FeO x @CN- hpes -400 catalyst exhibited excellent activity and exclusive selectivity for the hydrogenation of functionalized nitroarenes to corresponding arylamines, as well as successive recyclability without any loss in both activity and selectivity. Therefore, this work provides a feasible strategy for the synthesis of other heterogeneous MOFs-based derived catalysts with superior catalytic performance for diverse industrial processes.
研究领域:
催化化学
·
材料科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Menghan Guo,Wenqing Wang,Jing Zhang,Pengfei Qi,Yifan Yan,Rui Wang
As a substitute for petroleum-based polymers, polylactic acid (PLA) always attracts great interest due to its unique eco-friendly properties and versatile applications. However, the inherent high flammability and slow natural degradation are still challenging for its wide usage. In this study, a multi-level sushi roll structured flame retardant (B@(D + E)@P-Fe) composed of boron nitride nanosheets (BNNS), iron metal-organic frameworks (Fe-MOFs), and phytic acid (PA) was synthesized through self-assembly technology and create a flame retardant PLA system. Loading of 6 wt % B@(D + E)@P-Fe enabled the PLA composites reached UL-94 V-0 rating and increased the LOI value up to 30 %. Cone calorimetry tests revealed that, compared with pure PLA, PLA composite exhibited a 32.6 % reduction in peak heat release rate and a 17.5 % reduction in total heat release. In addition, the composite material increased its crystallinity up to 51.2 % and maintained excellent mechanical properties with the modulus increasing from 2704.16 to 3448.52 MPa. Meanwhile, the as-synthesized flame retardant could be recycled with yield up to 81 %, and the purity of recovered lactic acid was 85.2 %, realizing a full life cycle of biodegradable PLA materials. This work presents a facile and eco-friendly strategy to fabricate renewable plastic with both good flame retardancy and high degradation efficiency.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Yanping Zhang,Yinian Zhu,Yinming Fan,Shengpeng Mo,Xiaobin Zhou,Zongqiang Zhu
A set of MOFs-derived Co 3 O 4 @MnO x hollow-sphere were synthesized to develop a catalyst for the photothermal catalytic removal of NO using acetone as a reducing agent. The study systematically investigated the impact of organic ligands and photoactive substances on energy transfer and photothermocatalytic reactions involving acetone and NO under 5 vol % H 2 O with the catalysts. At 240°C, sample C-5/1 (with an organic ligand added and Co/Mn molar ratio of 5/1) demonstrated 75 % NO conversion and 65 % acetone conversion. The highest catalytic performance was observed in the L-Py sample (with photoactive substance was added), achieving 80 % NO and 69 % acetone conversion at 240°C. The catalyst demonstrated low crystallinity, and the introduction structural defects through ligands adjusted the ratio of active components. Meanwhile, enhanced catalytic performance was attributed to light energy scattering in the inner space of microspheres, resulting in the efficient transfer of 2.17 eV energy with the addition of two photoactive substances. The elevated concentration of surface-active oxygen facilitated oxidation, while M n /M n+1 (Mn 3+ /Mn 4+ and Co 2+ /Co 3+ ) redox cycling supplied surface oxygen in the photothermal low-temperature response. The proposed mechanism for the simultaneous degradation of acetone and NO was elucidated using Density Functional Theory calculations.
研究领域:
环境科学
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材料科学
·
催化化学
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