RSC Advances
·
2016
·Vol. 6
·期 69
·64895-64901
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IF 3.289
Fengli Qu,Lian Xia,Chuanxiang Wu,Lijie Liu,Guoliang Li,Jinmao You
A zirconium-based metal–organic frameworks (MOF), with 2-aminoterephthalic acid as linkers, named UiO-66-NH2, has been synthetized and characterized in a dispersive solid-phase extraction (DSPE) procedure in combination with high-performance liquid chromatography (HPLC) with fluorescence detection (FLD) for the pre-concentration and detection of sialic acids (SAs) in serum samples. In this study, UiO-66-NH2 was employed for the first time as a novel DSPE sorbent for sample pretreatment. Parameters which influence the extraction efficiency such as the amount of MOF, nature of the desorption solvent and its amount, adsorption time and desorption time were investigated and optimized. Under the optimized conditions, better extraction results were obtained by UiO-66-NH2 based DSPE for the extraction of SAs from serum samples than traditional sample preparation methods. Detection limits of the method as low as 0.16 pmol for N-glycolylneuraminic acid (Neu5Gc) and 0.11 pmol for N-acetylneuraminic acid (Neu5Ac) were obtained, with determination coefficients (R2) higher than 0.9995 for the range 10–1000 pmol L−1, average recoveries of >91.3% at three different spiked levels (1, 5 and 10 ng mL−1), and relative standard deviation (RSD) values below 3.4%. The proposed method was demonstrated to be sensitive enough for determination of SAs from bio-samples.
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RSC Advances
·
2016
·Vol. 6
·期 109
·107533-107541
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IF 3.289
Xinliang Fang,Shanfeng Wang,Yanxiao Li,Xiaoyun Liu,Xinxin Li,Shaoliang Lin,Zhong-Kai Cui,Qixin Zhuang
Novel Fe3O4/polyimide (PI) composite films with extraordinary dielectric properties were prepared via in situ polymerization of PI in the presence of 4,4′-diaminodiphenyl ether (ODA), pyromellitic dianhydride (PMDA) and compatible amine-functionalized carbon-coated Fe3O4 nanoparticles (Fe3O4@C–NH2). Fe3O4 nanoparticles prepared via solvothermal reaction were coated with crosslinked glucose and then surface-grafted via carbodiimide coupling. The core–shell structure of Fe3O4@C–NH2 was thereafter obtained with amine functionalities on the carbonized-glucose shell. Homogeneous dispersion of Fe3O4@C–NH2 and strong interfacial covalent bonding on the shell surface contributed to high dielectric constants (ε) and extremely low dielectric losses (tan δ) in the composite films. The highest dielectric constant of the composite films was 58.6 at 1 kHz when the Fe3O4@C–NH2 composition was 1.13 vol%, as well as a low dielectric loss of 0.0091 and a high breakdown strength of 126.5 ± 11.3 MV m−1 were observed without considerable sacrifice of the thermal stability and mechanical properties.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Guojun Li,Zheng Lian,Qiuqiu Lyu,Chenyu Zhu,Zhinian Liu,Shule Zhang,Qin Zhong
The efficiency of photocatalytic Nitric Oxide(NO) oxidation is limited by the lack of oxygen(O 2 ) active sites and poor charge carrier separation. To address this challenge, we developed a molecular Cobalt Phthalocyanine modified MIL-68(In)–NH 2 photocatalyst with a robust Built-in electric field(BIEF). In the 2 % CoPc-MIN sample, the BIEF strength is increased by 3.54 times and 5.83 times compared to pristine CoPc and MIL-68(In)–NH 2 , respectively. This BIEF facilitates the efficient S-scheme charge transfer, thereby enhancing photogenerated carrier separation. Additionally, the Co-N4(II) sites in CoPc can effectively trap the separated photoexcited electrons in the S-scheme system. In addition, the Co-N4(II) sites can also serve as active sites for O 2 adsorption and activation, promoting the generation of superoxide radical ( O 2 – ), thereby driving the direct conversion of NO to nitrate(NO 3 – ). Consequently, the 2 % CoPc-MIN sample exhibits a remarkable photocatalytic NO removal efficiency of 79.37 % while effectively suppressing the formation of harmful by-product nitrogen dioxide(NO 2 ) to below 3.5 ppb. This study provides a feasible strategy for designing high-efficiency O 2 activation photocatalysts for NO oxidation.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Tongtong Wang,Xuedan Song,Qunxing Luo,Xiaodong Yang,Siying Chong,Jie Zhang,Min Ji
In terms of ‘green chemistry’ and ‘atom economy’, the cycloaddition of CO 2 to yield cyclic carbonate without any additive is an eco-friendly way to utilize CO 2 . Unfortunately, the low CO 2 capture quantity of common catalysts limited its catalytic efficiency. Herein, a novel acid-base bifunctional catalyst was successfully prepared by immobilizing ionic liquid on MIL-101-NH 2 (IL/MIL-101-NH 2 ) and tested for propylene carbonate (PC) rapid and facile synthesis from CO 2 and propylene oxide (PO). The synergetic interaction between Lewis base with strong CO 2 chemical capture capacity and Brønsted acid with strong hydrogen bond donor leads to the high catalytic efficiency of IL/MIL-101-NH 2 for carbonate synthesis from CO 2 and PO without any additive. The immobilization mode between MIL-101-NH 2 and IL is energetically supported by the density functional theory (DFT) calculations. This design idea of specific catalyst and the acid-base synergetic strategy provides new insights into the design of powerful catalyst systems for the CO 2 conversion.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shuang Luo,Chenghua Zhang,Xingyan Liu,Yue Li,Lei Tang,Min Fu,Song Wang,Jie Wu,Mengmeng Xu,Xiaoping Wang,Youzhou He
A novel protonated NH 2 -MIL-125 was fabricated to introduce the moiety with charge and ample hydrogen (–NH 3 + Cl - group) into NH 2 -MIL-125 using HCl vapor obtained by natural volatilization of hydrochloric acid as a protonating reagent, which could exhibit excellent photocatalytic activity in both hydrogen production and NO purification under visible light irradiation. The hydrogen production and NO purification rate of the best protonated NH 2 -MIL-125 were 6762.80 μmol g −1 and 49.17%, respectively, which were 20.53 and 1.84 times as that of the original NH 2 -MIL-125. A series of characterizations, such as Mott-Schottky, PL, FT-IR and in situ DRIFTS , etc. were used to characterize the photoelectrochemical properties of the optimal catalyst, which demonstrated the protonation effect can not only enhance the electron migration rate, but also effectively accelerate photo-generated electron-hole pairs separation in the photocatalytic reaction process. This research believed that using HCl vapor as a facile protonation reagent to introduce the moiety with charge and ample hydrogen (–NH 3 + Cl - ) was a very effective method to decorate MOFs for hydrogen evolution and NO removal.
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FOOD CHEMISTRY
·
2025
·
IF 9.8
Zhiyang Qin,Tianyue Peng,Xinguang Qin,Gang Liu,Haizhi Zhang
Accurate detection of tetracycline residue is of great significance for ensuring product quality and protecting human health. Here, a colorimetric/fluorescent dual-mode biosensor was developed for the detection of tetracycline in honey by using metalloporphyrin [TCPP(Fe)] covalently modified NH 2 -MIL-101(Fe) [named NH 2 -MIL-101(Fe)@TCPP(Fe)]. The morphology, chemical structure and peroxidas-like activity of this hybrid nanozyme were comprehensively studied. Based on excellent catalytic activity and intrinsic fluorescence of NH 2 -MIL-101(Fe)@TCPP(Fe), a colorimetric/fluorescent dual-mode biosensor was developed for the detection of tetracycline. The primary mechanism for this dual mode biosensor was the inhibitory effect of tetracycline on on NH 2 -MIL-101(Fe)@TCPP(Fe) catalyzed chromatic reaction between H 2 O 2 and 3,3′,5,5′-tetramethylbenzidine (TMB)/ o -phenylenediamine (OPD), which was ascribed to the consumption of · OH by tetracycline and the adsorption of tetracycline on the surface of NH 2 -MIL-101(Fe)@TCPP(Fe). After effective validation, this colorimetric/fluorescent dual mode method was applied to detect tetracycline residues in three actual honey samples.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yibo Zhang,Peng Hu,Yaseen Muhammad,Ying Tang,Shan Shao,Zhu Gao,Jiaxing Wang,Ruimeng Wang,Yang Hu,Lihan Kuang,Zhongxing Zhao,Zhenxia Zhao
Hollow nano-sphere NH 2 -MIL88(Fe) (HS NMIL88(Fe)) with interfacial defects was fabricated to load laccase as a host. Through metal multi-coordination, dopamine engineered large amount of defective pores with large size on NH 2 -MIL88(Fe) interface. This defect-interfacial structure provided a high-density host for laccases, which efficiently protected enzyme from structure deformation and then inhibited inactivation. Besides, the unique hollow structure will help to fasten reactant diffusivity, and thus improved the catalytic reaction process. Experimental results showed that the maximum immobilized capacity and maximum activity recovery for laccase reached up to 213.2 mg/g and 75.8% beyond many state-of-the-art enzyme hosts, respectively. Meanwhile, the immobilized laccase exhibited better pH, thermal and storage stabilities on HS NMIL88(Fe) than free and loaded on NMIL88(Fe) ones. Thermal deactivation kinetics analysis showed that HS NMIL88(Fe)-Lac had much higher apparent activation energies of (105.2 kJ/mol) than that of free laccase (89.2 kJ/mol). Catalyzing decolorization performance of dye Remazol Brilliant Blue R (RBBR) was finally carried out and exhibited the decolorization rate of 1.8 times and 2.6 times faster than solid NMIL88(Fe)-Lac and free laccase, respectively. Moreover, the interaction mechanism of laccase for RBBR was investigated and revealed by molecular docking.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yanwei Sun,Chunshan Song,Xinwen Guo,Yi Liu
Preferred orientation has proven to exert a significant impact on the gas separation performance of metal–organic framework membranes. Nevertheless, realizing three-dimensional orientation control remains a challenging issue. In this study, well-intergrown NH2-UiO-66 membranes with both (111) out-of-plane and regional in-plane orientations were prepared by combining oriented deposition of seeds and solvothermal epitaxial growth. Dynamic air–liquid interface-assisted self-assembly method was employed to organize uniform octahedral-shaped NH2-UiO-66 seeds into closely packed monolayers with (111) out-of-plane and regional in-plane orientations, whereas the use of ZrS2 as the zirconium precursor during the solvothermal epitaxial growth was found indispensible for sealing the intercrystalline gaps while preserving the preferred orientation inherited from seed layers. In addition, compared with solvothermal heating, employing microwave heating led to poor intergrowth between neighboring NH2-UiO-66 crystals because of a lower dielectric loss factor of the reaction medium. Gas permeation results indicated that the prepared NH2-UiO-66 membranes exhibited H2/CO2 selectivity up to 5.5 times higher than their counterparts with random and/or mere out-of-plane orientations as well as H2 permeability 14.5 times higher than NH2-MIL-125(Ti) membranes with mere out-of-plane orientation under similar operating conditions.
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ANALYTICA CHIMICA ACTA
·
2026
·
IF 6.1
Ya Liu,Jiayi Hu,Huiqiong Huang,Xiaofang Yang,Xin Liu,Ning Lu,Shengchun Yang,Xiaodong Wen
Background Lead (Pb 2+ ) is a persistent and non-degradable pollutant that poses serious threats to human health and food safety. However, conventional methods are often limited by matrix interferences, sensitivity, and selectivity pose significant challenges for the direct quantification of trace metal ions in complex samples. Therefore, the development of efficient sample pretreatment techniques is necessary to address these limitations and enable reliable quantification of trace Pb 2+ in food and environmental samples. Results A novel method for the separation and enrichment of trace Pb 2+ in Angelica sinensis (Oliv.) Diels (AS) and water samples was developed, using a newly synthesized pH-responsive amorphous MIL-68(In)–NH 2 –TiO 2 (aMIL-68(In)–NH 2 –TiO 2 ) composite prepared with green deep eutectic solvents as a dispersive micro solid-phase extraction (DMSPE) adsorbent. At pH = 3, the composite showed excellent selectivity for Pb 2+ adsorption in multi-metal ion systems and achieves adsorption equilibrium within 3 min, providing a practical improvement over conventional extraction process and enhancing overall experimental efficiency. Under the optimized conditions, the method showed efficient extraction of Pb 2+ with an enrichment factor of 31, a limit of detection (LOD) of 0.1 μg L −1 , and a wide linear range (1–6000 μg L −1 ). Significance In this work, aMIL-68(In)–NH 2 –TiO 2 was prepared as a DMSPE adsorbent for the environmentally friendly, highly sensitive, and highly selective monitoring of trace Pb 2+ in AS and water samples, providing a novel strategy for the sensitive detection of metal ions, offering a promising approach for food and environmental monitoring.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Tingting Zhang,Xing Liu,Yanqiu Jiang,Xiaowei Zheng,Jian Zhang,Yudong Li,Defeng Li,Kaifeng Lin
Photo-Fenton reaction has received increasing attention in removing antibiotics in water. Herein, Fe 2 O 3 -on-ZrO 2 polypods were designed and synthesized via metal organic frameworks (MOFs) derivation strategy combined with reflux heating and baking. The experimental results showed that under Ultraviolet–visible (UV–vis) light irradiation, more than 95 % tetracycline hydrochloride (TC-HCl) was degraded by Fe 2 O 3 -on-ZrO 2 with Fe/Zr mole ratio of 1.3 in 25 min within full pH range. Mainly due to the following points, there were abundant Fe 2 O 3 -on-ZrO 2 heterojunctions, which conduced to transfer photo-induced electrons (e − ) from ZrO 2 to Fe 2 O 3 , thus accelerating the iron cycle. Besides, OH – adsorbed was oxidized to hydroxyl radicals (·OH) by holes (h + ) in the valence band (VB) of ZrO 2 , and ZrO 2 also enhanced the stability of the catalyst and reduced the leaching of iron ions. Finally, the reasonable degradation pathway and degradation mechanism were speculated by high performance liquid chromatography-mass spectrometry (HPLC-MS), electron spin resonance technology (ESR), scanning Kelvin probe (SKP), the conduction band (CB) and VB positions of Fe 2 O 3 -on-ZrO 2 , etc. This work exhibited a new structure and degradation mechanism, which would further encourage researchers to study the rational regulation of materials with special morphology and structure.
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JOURNAL OF MICROBIOLOGY AND BIOTECHNOLOGY
·
2020
·
IF 1.992
Jin Xu,Xuejia Shi,Xiaomeng Zhang,Zhenzhong Wang,Wei Xiao,Linguo Zhao
To efficiently recycle GH78 thermostable rhamnosidase (TpeRha) and easily separate it from the reaction mixture and furtherly improve the enzyme properties, the magnetic particle Fe 3 O 4 -SiO 2 -NH 2 -Cellu-ZIF8 (FSNcZ8) was prepared by modifying Fe 3 O 4 -NH 2 with tetraethyl silicate (TEOS), microcrystalline cellulose and zinc nitrate hexahydrate. FSNcZ8 displayed better magnetic stability and higher-temperature stability than unmodified Fe 3 O 4 -NH 2 (FN), and it was used to adsorb and immobilize TpeRha from Thermotoga petrophilea 13995. As for properties, FSNcZ8-TpeRha showed optimal reaction temperature and pH of 90°C and 5.0, while its highest activity approached 714 U/g. In addition, FSNcZ8-TpeRha had better higher-temperature stability than FN. After incubation at 80°C for 3 h, the residual enzyme activities of FSNcZ8-TpeRha, FN-TpeRha and free enzyme were 93.5%, 63.32%, and 62.77%, respectively. The organic solvent tolerance and the monosaccharides tolerance of FSNcZ8-TpeRha, compared with free TpeRha, were greatly improved. Using naringin (1 mmol/l) as the substrate, the optimal conversion conditions were as follows: FSNcZ8-TpeRha concentration was 6 U/ml; induction temperature was 80°C; the pH was 5.5; induction time was 30 min, and the yield of products was the same as free enzyme. After repeating the reaction 10 times, the conversion of naringin remained above 80%, showing great improvement of the catalytic efficiency and repeated utilization of the immobilized α-L-rhamnosidase.
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Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 30
·5998-6005
·
IF 6.331
Pan Li,Lixiang Zhang,Sheng Zhang,Chenchen Xu,Yinuo Li,Juan Qu,Shuai Li,Guojiang Mao,Hua Wang
A high-throughput and selective fluorimetric platform has been constructed for the analysis of ammonia in blood by using a polymer-stabilized metal–organic framework (MOF) of porous NH2-MIL-125, which was coated onto a wettable microwells array constructed on an indium tin oxide (ITO) substrate. It was found that the nitrogen plasma treatment for the ITO substrate could create a super-hydrophilic interface that combined with the hydrophobic pattern yielded a wettable microwells array, enabling the condensation-based enrichment of targets from the sample droplets. Moreover, the NH2-MIL-125 MOF encapsulated using polymers could be firmly coated onto the microwells to act as fluorescent probes for sensing NH3 with enhanced responses. In addition, the use of the polymer polyvinyl pyrrolidone could protect and stabilize the crystals of NH2-MIL-125 probe in aqueous media, revealing the improved hydrophilicity and significantly depressed signal background. The as-developed fluorimetric platform, containing a MOF-coated microwells array, can enable the detection of ammonia in blood, with concentrations ranging linearly from 0.10 to 300 μM. More importantly, this plasma treatment-based fabrication route may hold promise for designing different wettable microwells arrays for the high-throughput detection of multiple targets in the fields of biomedical analysis and environmental monitoring.
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