Sustainable Chemistry and Pharmacy
·
2023
·
IF 6
Qiuyun Zhang,Yaping Wu,Xingyue Hong,Zhenying Li,Yanting Lei,Rongfei Yu,Taoli Deng,Yutao Zhang,Peihua Ma
Different ligand functionalized bimetallic organic framework ((Zr/Ce)UiO-66- X ( X = H, NO 2 , NH 2 and (OH) 2 ) solids-supported phosphotungstic acid (HPW) has been fabricated through a facile impregnation process, and used in the esterification of methanol with oleic acid (OA). The obtained composites were characterized by FTIR , XRD, NH 3 -TPD, SEM-EDS, N 2 adsorption-desorption isotherm, TG , Py-FTIR, and XPS. The characterization analysis shows that the HPW/(Zr/Ce)UiO-66-NO 2 composite possesses the proper catalytic features, such as the greatest number of both strong Brønsted and Lewis acid sites, wider pores, relatively high surface area, and the existence of synergistic catalytic effects between HPW and (Zr/Ce)UiO-66-NO 2 framework. In the screening, the maximum OA conversion rate using (Zr/Ce)UiO-66-NO 2 , HPW/(Zr/Ce)UiO-66-NO 2 , HPW/(Zr/Ce)UiO-66, HPW/(Zr/Ce)UiO-66-NH 2 , HPW/(Zr/Ce)UiO-66-(OH) 2 catalysts is 13.7%, 91.6%, 81.6%, 80.7%, and 72.6% at 110 °C for 3 h, respectively. Moreover, the HPW/(Zr/Ce)UiO-66-NO 2 catalyst presents the better reusability over four cycles. Besides these, the HPW/(Zr/Ce)UiO-66-NO 2 catalyzed esterification reaction is estimated to have an activation energy of 33.7 kJ/mol. This present study provides an effective route for realizing biofuel production on an industrial scale involving heteropolyacids/bimetallic MOFs synergistic catalysts.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2016
·
IF 3.349
Xing Chu,Dan Zhou,Dan Li,Kun Xia,Ning Gan,Xinhuan Lu,Renfeng Nie,Qinghua Xia
This work has firstly constructed purely Lewis acidic sites on MCM-41 successfully, for which Zr-MCM-41 catalysts with different Zr contents are prepared through the hydrolysis of ZrOCl 2 on MCM-41, followed by calcination . Thus-prepared materials possess typical hexagonal mesostructures, irregular morphologies, large surface areas, and large pore sizes, as revealed by XRD , SEM, TEM, N 2 adsorption, and DRIFT FTIR. UV–vis, Raman and XPS spectra prove the formation of isolated species in high dispersion on the surface of MCM-41. NH 3 -TPD analysis shows that the acid intensity of the catalysts is proportional to the content of Zr, and the acidity of Zr-MCM-41 with the Zr content of <0.5% is very weak. Pyridine-IR spectra show that the surface acidity is mainly consisted of Lewis acidity, and solely Lewis acidic sites are constructed on Zr-MCM-41(550) with a low Zr content < 0.5 wt%. More Lewis acidic sites exposed on the surface of Zr-MCM-41 are considerably important for promoting the titled Prins condensation.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Wei He,Ru Yan,Xiang Gao,Yan Wang,Xinxiao Sun,Houyi Ma
Most Zr conversion coatings are prepared on Al alloys , with Al 3+ from the substrate contributing significantly to the film growth process. Thus, the effect of Al 3+ on the electrochemical characteristics, surface microstructure and film-formation mechanism of Zr-based conversion coatings on old- rolled steel (CRS) substrates was investigated by growing the coatings with and without Al 3+ as an additive. Electrochemical tests indicated that the anticorrosion performance of the Zr-Al coatings prepared in the presence of Al 3+ was greatly superior to that of Zr conversion coatings obtained in the absence of Al 3+ . Field-emission scanning electron microscopy and X-ray photoelectron spectroscopy analysis indicated that adding of Al 3+ in the conversion bath changed the surface microstructure of the Zr coating, greatly promoted the deposition of Zr and F on the CRS substrate and increased the film thickness and density. Both coatings were embedded into the etched CRS substrates. The presence of Al 3+ additive induced the formation of different coating components . The Zr coating mainly consisted of ZrO 2 and some FeF x , whereas the Zr-Al coatings comprised of ZrO 2 , ZrO x F y , Al 2 O 3 , AlF x and some FeF x . The present study results confirm the key role of Al 3+ as an additive in the film formation and growth process of Zr coatings and its effect on enhancing the anticorrosion performance of CRS substrates in NaCl solutions.
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JOURNAL OF FOOD SCIENCE
·
2024
·
IF 3.2
Xi Wu,Chenggang Geng,Weiwei Cheng,Zhenjiong Wang,Yan Zhang,Di Wu,Xiaozhi Tang
In this work, an ultrasensitive electrochemical sensor based on Zr-MOF-SH/rGA/NPG was developed for the first time for the rapid determination of mercury ions. First, nanoporous gold (NPG) film was covered on the glassy carbon electrode (GCE) to offer a desirable substrate. Then, Zr-MOF-SH/rGA composites were dropped on the NPG film to form a modified electrode. Mercapto functionalized MOFs (Zr-MOF-SH) showed strong adsorption capability toward mercury ions, and the unique structure of reduced graphene oxide aerogel (rGA) provided various sites for coupling with Zr-MOF-SH as well as improved the electrochemical activity. As a consequence of the synergistic effect of Zr-MOF-SH, rGA, and NPG, the optimized Zr-MOF-SH/rGA/NPG/GCE sensor showed excellent detection performance toward mercury ions with a linear range from 0 to 200 nM and a low limit of detection of 1.4 nM. Meanwhile, the fabricated electrochemical sensor exhibited outstanding stability, reproducibility, and anti-interference ability. To verify the practical applicability, the Zr-MOF-SH/rGA/NPG/GCE was applied for the determination of mercury ions in real rice samples with desirable recovery rates ranging from 98.8% to 108.3%.
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Food Bioscience
·
2025
·
IF 5.9
Hai Chi,Yue Xiao,Xuefei Wen,Houqi Ning,Xingzhong Zhang,Hongrui Chen,Jie Tang
This study developed an electrochemical sensor incorporating a dual recognition strategy that integrates molecularly imprinted polymer (MIP) and aptamers for the ultra-sensitive detection of zearalenone (ZEN) in grains. Exploiting the high specific surface area of the Cu-Zr bimetallic metal-organic framework-818 (MOF-818), aptamers were covalently immobilized on the olefin-functionalized MOF-818 surface via thioenol reaction. Employing 3-thiopheneacetic acid functionalized gold nanoparticles (3-TAA@AuNPs) as functional monomers, nanoscale molecularly imprinted cavities were electro-polymerized onto the modified electrode surface in the presence of the ZEN template. This synergistic recognition system integrates the aptamer's specific binding capability with the spatial complementarity of MIP, displaying an excellent linear response over a concentration range of 10 −13 to 10 −5 g/L and a detection limit as low as 2.8 × 10 −14 g/L. Analysis of real samples exhibited ZEN recoveries ranging from 96.5 % to 105.0 % (RSD <5.2 %) in corn and wheat matrices, confirming its practical applicability for rapid screening of fungal toxins in agricultural commodities.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Tiantian Si,Jilong Zhao,Jie Li,Guoying Zhang,Shuai Wang,Yong Guo,Xiaojing Liang,Yong Yang,Rong Rong
Because of the intricacy of traditional Chinese medicine, the extraction and separation for active components is restricted by current analytical techniques. The Zr-based metal–organic framework was strategically integrated into a “defective” structure, and pore size adjustment strategy was employed to fashion a dispersive, hierarchically porous composite. This composite has been utilized as a carrier in traditional Chinese medicine, particularly in conjunction with high-performance liquid chromatography, for the identification of active components. It exhibited significant selectivity in the absorption and separation for targeted analytes including alkaloids and carbohydrates via in-situ capture and separation, emphasizing the critical role played by the defective structure. The approach yielded recoveries of 81.5–101.4 % with a detection limit of 0.25 μg·L −1 . The approach demonstrated repeatability and stability, evidenced by the low relative standard deviations in efficiency measurements for separation, specifically below 0.8 % and 0.9 %, respectively. It offers distinctive insights and a versatile methodology for the extraction and separation of active ingredients from intricate matrices.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhizhou Liu,Le Ma,Xueyan Nan,Xiang Zhao,Liang He,Tong Wang,Pengli Bai
Non-specific binding was a critical bottleneck in biosensing field and hindered the implementation of biosensors in bioassays. Thus, various approaches were developed to minimize the non-specific binding of biosensors. However, the rational utilization of non-specific binding will also produce generous returns. Herein, the first universal cell surface barcoding strategy for mass cytometry independent on particular cell surface molecules was developed based on nano-sized UIO-66 typed metal organic framework (MOF). Profiting from the 9 abundant stable isotopes of Zr and Hf, up to 84 mass barcode combinations can be achieved theoretically through the non-specific binding between positively charged UIO-66 and negatively charged cells. Clearly distinguished individual population sets were obtained when the cell samples were barcoded with UIO-66(Zr), UIO-66(Hf), and UIO-66(Zr/Hf) mixture. UIO-66 can also be used for flow cytometry barcoding and imaging after the modification with a fluorescent dye. Furthermore, the UIO-66 barcoding showed high compatibility with metal chelated polymer (MCP) mass tags in single-cell multiplexing and 16-fold higher sensitivity than MCP based barcoding agents. This work opens new opportunities for MOFs in mass cytometry applications and will also prompt people to evaluate the nasty non-specific binding in another perspective.
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GREEN CHEMISTRY
·
2021
·Vol. 23
·期 7
·2640-2651
·
IF 10.182
Zhicheng Jiang,Mi Gao,Javier Remón,Wei Ding,Changwei Hu,Bi Shi
This work addresses the manufacturing of a pioneering chrome-free tanning agent, consisting of ‘Al–Zr-oligosaccharides’ produced from biomass. First, a microwave-assisted AlCl3–H2O2–H2O reaction system was used for the simultaneous degradation and oxidation of hemicellulose in corncob. The obtained aqueous solution containing ‘Al-oligosaccharides’ was then combined with Zr to produce water-soluble ‘Al–Zr-oligosaccharides’. These species behaved as a ‘Trojan horse’, allowing the uniform and controlled penetration of Al and Zr into the leather, avoiding their accumulation on the surface. The effects of the reaction temperature and the AlCl3 and H2O2 concentrations used during the synthesis were systematically analyzed. Increases in the temperature and AlCl3 concentration improved the hemicellulose conversion, while the use of high H2O2 concentrations augmented the amounts of –CHO/–COOH functionalities in the oligosaccharides, with both phenomena being paramount for the efficient formation of ‘Al–Zr-oligosaccharides’. However, more severe reaction conditions led to the formation of an undesirable species, negatively influencing the tanning performance and chromaticity of the tanning agent. Given this, these parameters were optimized, and it was found that it is possible to convert up to 72 wt% of the hemicellulose present in corncob into an ‘advanced Trojan horse tanning agent’ contained in a colorless water solution, conducting the synthesis at 129 °C with a solvent comprising 56 mM AlCl3 and 2.6 vol% H2O2. The application of this solution for leather tanning provided leather with a shrinkage temperature as high as 87 °C, thus meeting the restrictive requirements of the leather industry. Therefore, these results are a landmark achievement in this field and represent a step forward to a sustainable and renewable leather industry.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Xin Li,Xiangheng Niu,Peng Liu,Xuechao Xu,Dan Du,Yuehe Lin
Phosphate ion (Pi) is an inorganic anion widely distributed and commonly regarded as a significant indicator of water eutrophication, and thus it is urgent to develop convenient, cost-effective and reliable analytical approaches for the monitoring of Pi for water quality control. In this work, we propose the high-performance dual-channel ratiometric colorimetric sensing of Pi based on the analyte-triggered differential oxidase-mimicking activity changes of oxidized Ce-Zr bimetal-organic frameworks (oxidized UiO-66(Ce/Zr)). By integrating two types of metal nodes with different functions into one framework structure, the proposed oxidized UiO-66(Ce/Zr) not only exhibits excellent activity to catalyze the chromogenic oxidation of both 3,3′,5,5′-tetramethylbenzidine (TMB) and 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS) due to oxidase-like active Ce 4+ /Ce 3+ sites but also provides main Zr 4+ sites to specifically recognize Pi. When Pi is in presence, it is rapidly adsorbed onto oxidized UiO-66(Ce/Zr) and changes the surface chemistry of the latter, leading to differential enzyme-like activity changes towards the two chromogenic substrates TMB and ABTS. Based on this finding, a dual-channel ratiometric colorimetric method was established for the sensitive determination of Pi. Compared to conventional single-signal colorimetric sensors, our method offered a widened linear detection scope from 3.3 to 666.7 μM. Also, robust and accurate analysis of Pi in various water matrices was demonstrated, indicating our method’s great potential in practical applications.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Chuan Guo,Jianwei Yang,Zhiyuan Cui,Shuo Qi,Qianqian Peng,Weiwei Sun,Li-Ping Lv,Yi Xu,Yong Wang,Shuangqiang Chen
With great superiorities in energy density, rate capability and structural stability, Na 3 V 2 (PO 4 ) 2 F 3 (NVPF) has attracted much attentions as cathode of sodium ion battery (SIB), but it also faces challenges on its poor intrinsic electronic conductivity and the controversial de/sodiation mechanism. Herein, a series of Zr-doped NVPF coated by N-doped carbon layer (~5 nm in thickness, homogenously) materials are fabricated by a sol–gel method, and the optimized heteroatom-doping amounts of Zr and N doping improve intrinsic properties on enlarging lattice distance and enhancing electronic conductivity, respectively. Specifically, among all samples of Na 3 V 2− x Zr x (PO 4 ) 2 F 3 /NC (NVPF-Zr- x /NC, x = 0, 0.01, 0.02, 0.05, and 0.1), the optimized electrode of NVPF-Zr-0.02/NC delivers high reversible capacities (119.2 mAh g −1 at 0.5 C), superior rate capability (98.1 mA h g −1 at 20 C) and excellent cycling performance. The structural evolution of NVPF-Zr-0.02/NC electrode, in-situ monitored by X-ray diffractometer, follows a step-wise Na-extraction/intercalation mechanism with reversible multi-phase changes, not just a solid-solution-reaction one. Full cells of NVPF-Zr-0.02/NC//hard carbon demonstrate high capacity (99.8 mA h g −1 at 0.5 C), high out-put voltage (3.5 V) and good cycling stability. This work is favorable to accelerate the development of high-performance cathode materials and explore possible redox reaction mechanisms of SIBs.
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MICROCHEMICAL JOURNAL
·
2014
·
IF 3.583
Shengling Sun,Jie Li
A method has been developed for the determination of zirconium (Zr), hafnium (Hf), niobium (Nb), tantalum (Ta), molybdenum (Mo), tungsten (W), and tin (Sn) in seawater by quadrupole inductively coupled plasma-mass spectrometry (Q-ICP-MS). The method is based on separation of the seven elements by extraction chromatography using N-benzoyl-N-phenylhydroxylamine (BPHA) supported on a microporous acrylic ester polymeric resin. The optimized procedure indicates that the BPHA resin has high selective adsorption for Zr, Nb, Mo, Sn, Hf, Ta, and W (known as fluoride soluble elements), whereas other interference and matrix elements are minimally adsorbed. The optimized eluent mixture with their molarity gives satisfactory recoveries for all analytes. The recovery can be achieved 99% for Zr, 97% for Nb, 97% for Mo, 99% for Sn, 99% for Hf, 95% for Ta, and 98% for W, respectively, by eluting with 6 mL of 6 mol L − 1 HF/1 mol L − 1 HCl. Furthermore, the technique for separation and enrichment of these elements provides a low total method blank. The detection limits for this method are 0.5 ppt for Zr, 0.2 ppt for Nb, 1.7 ppt for Mo, 1.0 ppt for Sn, 0.1 ppt for Hf, 0.1 ppt for Ta, and 0.3 ppt for W, respectively. The validity of the method is evaluated by replicate analyses of seawater reference materials; the precision of the results is better than 3% (RSD, n = 4), and the results are in good agreement with certified values. The established procedure has proved to be both practical and effective for seawater sample analyses.
研究领域:
分析化学
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海洋化学
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环境地球化学
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痕量元素检测
·
质谱分析
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2023
·
IF 4.4
Chengxiang Chu,Xianfeng Wang,Yuanyi Deng,Yi Ma,Chengyue Zou,Mei Yang,Huibo Luo,Danqun Huo,Changjun Hou
A facile and rapid fluorescence sensor array based on Tb (III) and Eu (III) doped Zr (IV) metal–organic frameworks was proposed for Chinese green tea discrimination. According to large porosity of Tb@UiO-66-(COOH) 2 and Eu@UiO-66-(COOH) 2 , phenolic hydroxyl groups of tea polyphenols could coordinate with free carboxylic acid groups and was captured into the pores, which led to the disturbance of electronic structure of ligand and inhibited the energy transfer efficiency from ligand to Tb (III) and Eu (III) center, causing the fluorescence quenching effect. Based on Hierarchy Cluster Analysis and Linear Discrimination Analysis, the fluorescence sensor array was employed for successful tea polyphenols classification through the analysis of different fluorescence quenching effect to tea polyphenols. Green tea samples within different categories and grades were also successfully discriminated using this assay according to tea polyphenols, providing a new method for Chinese green tea identification.
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PubMed
高影响因子