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SENSORS AND ACTUATORS B-CHEMICAL · 2022 · IF 9.221

One-step fabrication of high-density Si nanotips as SALDI-MS substrate for highly sensitive detection

Shuzhen Dou,Zhongshun Wang,Qiye Chen,Nan Lu

The high sensitivity of surface-assisted laser desorption/ionization mass spectrometry (SALDI-MS) analysis depends on the enhancement of the signal intensity and the reduction of the background. Here, high-density Si nanotips were prepared as SALDI-MS substrate by taking template-free reactive ion etching for sensitive detection . The high-density Si nanotips act as tiny antennas to concentrate the laser energy and generate photo-induced electrons on a small area, which promotes desorption and ionization of molecule, enhancing the signal intensity. Additionally, the high stability of Si nanotips under laser irradiation ensures low background interference. The applicability of the substrate was demonstrated by the detection of various small molecules, e.g., fatty acids, amino acids , environmental pollutants and drugs. In addition, this substrate can be successfully applied for detecting trace small molecules in complex sample, such as 10 −9 M verapamil in serum and 10 −12 M crystal violet in lake water. Moreover, the banned fungicides left on the fish skin was also detected. The substrate is compatible with imaging, and the endogenous and exogenous substances in fingerprint were visualized by MS imaging. These results demonstrate the easily prepared high-density Si nanotips SALDI-MS substrate is of high detection sensitivity and great value toward large-scale practical applications.

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PROGRESS IN ORGANIC COATINGS · 2023 · IF 6.6

Construction of eco-friendly multifunctional cashew nut shell oil-based waterborne polyurethane network with UV resistance, corrosion resistance, mechanical strength, and transparency

Jiawei Li,Chengyu Hong,Mengsong Liu,Yongquan Wang,Yutong Song,Ruixue Zhai,Jiaqi Zhang,Chao Zhou

Vegetable oil-based waterborne polyurethane possesses numerous advantages, including its sustainability, environmental friendliness, and economic benefits. Nevertheless, its application is constrained by inferior mechanical properties and a low glass transition temperature . Hereon, the renewable polyols of sorbitan monooleate/cytidine were incorporated into the anionic cashew nut shell oil-based WPU network through molecular structure design. Series of CNSL-based WPU with outstanding UV resistance, mechanical properties, corrosion resistance , and transparency were successfully synthesized. The effects of Ce/SP content on the performance of CNSL-based WPU dispersions and films were investigated. The results demonstrated a remarkable enhancement in the properties of the modified WPU films. Specifically, the tensile strength and T g were increased from 9.7 MPa to 23.9 MPa and 1.1 °C to 45.8 °C, respectively, while maintaining a toughness of 26 MJ/m −3 , which attained or even surpassed the current vegetable oil-based WPU systems. It was confirmed excellent UV resistance within the UVB and UVC spectrums. Furthermore, with the increase in Ce/SP content, the water contact angle of films increased slightly, enhancing its water resistance. The IE of WPU-Ce and WPU-SP films reached 97.93 % and 98.42 % respectively, indicating outstanding corrosion resistance. This work presented novel strategies for the advancement of high-performance bio-based WPU, which held promising potential in diverse areas including coatings, corrosion protection , inks, and wearable applications.

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ANALYTICAL SCIENCES · 2023 · IF 1.6

A comprehensive evaluation of a polymeric zwitterionic hydrophilic monolith for nucleotide separation

Lai Liang,Zhang Mengyun,Liu Chusheng,Qu Jiahuan,Xu Dongsheng,Jiang Zhengjin

Rapid and effective separation of nucleotides (NTs) and their derivatives is crucial for studying their physiological functions. In this work, we comprehensively evaluated the separation ability of a zwitterionic hydrophilic monolith, i.e., poly(N,N-dimethyl-N-(3-methacrylamidopropyl)-N-(3-sulfopropyl)ammonium betaine- co –N,N’-methylenebisacrylamide) (poly(SPP- co -MBA)) for NTs analysis, including its selectivity, chemical stability under extremely basic condition and compatibility with hydrophilic interaction liquid chromatography (HILIC) coupled with mass spectrometry (HILIC-MS). The poly(SPP- co -MBA) monolith exhibited excellent chemical stability, as evidenced by the low relative standard deviation of retention time (0.16–1.05%) after 4000 consecutive injections over one month under strong alkaline elution condition (pH 10). After optimizing the separation conditions, including buffer pH and concentration, organic solvent content and column temperature, four nucleoside triphosphates, five nucleoside diphosphates and five nucleoside monophosphates were baseline separated within 7 min. Additionally, the mixtures containing one nucleoside and its corresponding mono-, di-, and triphosphates were baseline separated within only 3 min, respectively. It is good HILIC-MS compatibility was also confirmed by the satisfactory peak shape and high response of nine NTs. Overall, the proposed poly(SPP- co -MBA) monolith exhibited good mechanical stability and compatibility of HILIC-MS, making it a promising technique for NTs analysis. Graphical Abstract

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JOURNAL OF CHROMATOGRAPHY A · 2021 · IF 4.759

Performance evaluation of silica microspheres functionalized by different amine-ligands for hydrophilic interaction chromatography

Houmei Liu,Pian Jin,Mi Jiang,Yu Duan,Guozheng Zhu,Hui Yu,Hongdeng Qiu

In this work, for the first time five amine-ligands including mono-amine, di-amine, tri-amine, secondary and tertiary amine, were functionalized on mesoporous micro-silicas and developed as stationary phases for hydrophilic interaction liquid chromatography (HILIC). The investigations about the retention mechanisms, effects of different chromatographic conditions and stability were systematically conducted. Three kinds of polar and hydrophilic compounds (saccharides, sulfonamides, nucleosides and nucleobases) were selected as probe molecules to evaluate their separation performances. Among the five stationary phases, only aminopropyl-bonded silica has already gained wide developments and applications. Whereas, there are no related researches about the other four to be utilized as separation media. By a series of chromatographic evaluations, the results revealed the other four mesoporous micro-silica materials functionalized with di-amine, tri-amine, secondary and tertiary amine, had great potential to be explored as novel stationary phases of HILIC. Particularly, the two stationary phases functionalized with di-amine and tri-amine exhibited outstanding separation and retention abilities. This work offered some insights on the understanding of retention in HILIC mode and provided us possibility to explore other amine-based HILIC stationary phases.

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MICROCHEMICAL JOURNAL · 2021 · IF 4.821

Preparation and application of Au nanoparticles-decorated SO3H-cofunctionalized silica stationary phase for per aqueous liquid chromatography

Tong Chen,Liang Xu,Guangsan Song,Yuan Li,Hong Xu,Hongbin Zhou,Zhen Xiao,Ping Li

Au nanoparticles (Au NPs)-decorated SO 3 H-cofunctionalized porous silica particles was prepared as a novel mixed-mode stationary phase and used in Per aqueous liquid chromatography (PALC) mode. The obtained stationary phase was characterized by elemental analysis, FT-IR spectra, and transmission electron microscopy. To evaluate the retention behavior, the effect of a variety of chromatographic factors on the retention of different types of solutes was investigated. The obtained column exhibited a hydrophobic interaction/cation-exchange mixed-mode retention mechanism, and a typical PALC characteristic was observed in water-rich mobile phases. When the particle size of Au NPs was 10–20 nm, the analytes had a sharp peak shape and the column pressure was also moderate. Compared with the hydrophilic interaction liquid chromatography (HILIC) and C 18 column, some hydrophilic compounds such as six monosaccharides were baseline separated with the enhanced resolution of the obtained column under the PALC mode. Moreover, the efficiency of the Au-S/SO 3 H-SiO 2 -2 column was significantly higher than that of the HILIC column. PALC mode was a green annlysis method and suitable for the replacement of hydrophilic interaction liquid chromatography.

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MICROCHEMICAL JOURNAL · 2020 · IF 3.594

A paper-based fluorescent test for determination and visualization of cysteine and glutathione by using gold-silver nanoclusters

Yuanyuan Zhang,Mei Yang,Zeyu Shao,Hedan Xu,Yan Chen,Yuling Yang,Wenfeng Xu,Xiaoling Liao

A method is described for fluorometric determination of cysteine (Cys) and glutathione (GSH), either in solution by using a fluorescence spectrometer, or by using a paper-based test with visual observation. The method is based on the finding that the yellow fluorescence of the gold/silver nanoclusters (AuAg NCs), with excitation/emission maxima of 358/574 nm, is quenched by Cys and GSH via NCs aggregation. The method is selective for Cys and GSH. The limits of detection for both Cys and GSH are 0.74 nM in solution state and 5.0 μM on paper-based test. Response is linear in the range from 2.3 nM to 110 μM and from 2.3 nM to 63 μM in solution for Cys and GSH, respectively. The method is not interfered by other amino acids even if their concentrations are 10 times higher. It was successfully applied to the determination of Cys in spiked serum samples.

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JOURNAL OF CHROMATOGRAPHY A · 2020 · IF 4.049

A single-step preparation of carbohydrate functionalized monoliths for separation and trapping of polar compounds

Jincai Wang,Jialiang Guo,Haowen Chen,Xiaoling Huang,Govert W. Somsen,Fenyun Song,Zhengjin Jiang

A single-step copolymerization strategy was developed for the preparation of carbohydrate (glucose and maltose) functionalized monoliths using click reaction. Firstly, novel carbohydrate-functionalized methacrylate monomers were synthesized through Cu(I)-catalyzed 1,3-dipolar cycloaddition (alkyne-azide reaction) of terminal alkyne with azide of carbohydrate derivatives. The corresponding carbohydrate functionalized monolithic columns were then prepared through a single-step in-situ copolymerization. The physicochemical properties and performance of the fabricated monolithic columns were evaluated using scanning electron microscopy, Fourier-transform infrared spectroscopy, and nano-liquid chromatography. For the optimized monolithic column, satisfactory column permeability and good separation performance were demonstrated for polar compounds including nucleoside, phenolic compounds and benzoic acid derivatives. The monolithic column is also highly useful for selective and efficient enrichment of glycopeptides from human IgG tryptic digests. This study not only provided a novel hydrophilic column for separation and selective trapping of polar compounds, but also proposed a facile and efficient approach for preparing carbohydrate functionalized monoliths.

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JOURNAL OF LIQUID CHROMATOGRAPHY & RELATED TECHNOLOGIES · 2020 · IF 0.992

The fabrication of carboxylic acid-functionalized porous layer open tube column and its application in hydrophilic interaction chromatography for small polar molecules

Shiyun Tang,Yuanxing Duan,Feng Chang,Wei Jiang,Fengmei Zhang,Zhihua Liu,Yuting Yang,Chunbo Liu,Yingzhuang Chen

The porous layer open-tube (PLOT) columns, which were characterized by their considerable specific surface area and high permeability, have attracted a growing attention from researchers in liquid chromatography. In this work, a hydrophilic PLOT column rich in carboxylic acid functional groups was successfully synthesized in capillary with an inner diameter of 200 µm by thermally initiated aqueous two-phase polymerization. Methacrylic acid (MAA) areas monomers that responsible for the introduction of polar functional groups, and poly(ethylene glycol) diacrylate (PEGDA) are as cross-linker. The optimized PLOT column has a uniform, moderately thick porous layer, which is tightly bonded to the inner wall without any detachment. The hollow structure gives the PLOT column good permeability, which facilitates fast mass transfer. The systematical evaluations of the resulting PLOT columns were performed by using polar analytes including nucleosides, bases, amides, phenols and carboxylic acids. Those results demonstrated excellent separation performance for the small polar molecules. Compared to the poly(PEGDA) PLOT column, the hydrophilic retention of analytes on poly(PEGDA-co-MAA) porous layer open-tube column is significantly improved by the introduction of carboxylic acids. Furthermore, with modified nucleosides and chlorophenols being disease markers and the persistent pollutant of wide concern, respectively, the separation was optimized and the linear range of the quantitative analysis was examined for both targets. which indicates the potential application of such PLOT column for analysis of real samples.

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Analytical Methods · 2020 ·Vol. 12 ·期 46 ·5635-5641 · IF 2.596

Preparation of a boronate-affinity monolithic column for adsorption of nucleosides

Dan Liu,Lili Meng,Liping Huang,Shipeng Luo,Guohua Zhang

Chitosan is a considerably versatile and promising biomaterial and can easily form a 3D hierarchical porous scaffold. In this work, a novel boronate-affinity monolithic column modified with a boronic acid–chitosan complex was prepared and characterized by different methods such as Fourier transform infrared spectroscopy, scanning electron microscopy, thermal gravimetric analysis, specific surface area analysis and pore size distribution analysis. The synthesized monolithic column was used for polymer monolithic microextraction combined with high performance liquid chromatography for the simultaneous determination of cytidine, uridine, inosine, and guanosine in milk powder samples. Several parameters affecting extraction efficiency, including the eluent proportion, eluent flow rate, sample flow rate, sample volume, and sample pH were investigated. The boronate-affinity monolithic column showed high enrichment ability due to the selective formation of cyclic borate esters between nucleosides and boronic acid groups at high pH and the release of cyclic borates at low pH values. Under the optimum operating conditions, the linear range was 0.1–50 μg mL−1, and the correlation coefficients were in the range of 0.9993–0.9994. The LOD and LOQ were in the range of 0.0027–0.0034 and 0.0090–0.011 μg mL−1, respectively. In addition, the results of recovery and relative standard deviation were satisfactory.

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MICROCHIMICA ACTA · 2020 ·Vol. 187 ·期 7 ·1-11 · IF 6.232

β-Cyclodextrin covalent organic framework–modified organic polymer monolith as a stationary phase for combined hydrophilic and hydrophobic aqueous capillary electrochromatographic separation of small molecules

Ma Mingxuan,Du Yingxiang,Zhang Liu,Gan Jie,Yang Jiangxia

A β-Cyclodextrin covalent organic framework (β-CD COF) was successfully prepared under ambient temperature with a mild chemistry strategy from heptakis(6-amino-6-deoxy)-β-cyclodextrin and terephthalaldehyde. It was embedded into the poly[(glycidyl methacrylate)-co-(ethylene dimethacrylate)] [poly(GMA-co-EDMA)] monolith and served as the β-CD COF material–incorporated monolith. The synthetic materials were characterized by field emission scanning electron microscopy, energy-dispersive X-ray mapping analysis, transmission electron microscopy, thermogravimetric analysis, Fourier transform infrared spectroscopy, and N 2 adsorption-desorption isotherm. The β-CD COF material–incorporated monolith achieved baseline separation in capillary electrochromatographic separation of three amides, three amino acids, three nucleosides, four aromatic acids, and three positional isomers (with resolution values of three amides, 1.75 and 1.54; three amino acids, 5.24 and 1.75; three nucleosides, 2.56 and 1.77; four aromatic acids, 6.96, 2.74, and 1.64; three positional isomers, 1.61 and 1.50). In comparison with the original monolith, the β-CD COF material–incorporated monolith shows significantly enhanced resolution for mixed molecules. The effect of pH and concentration of buffer and applied voltage were discussed in detail. The fabricated monolith showed good stability and reproducibility (relative standard deviation (RSD) < 6.9%). Molecular modeling illuminated the interactions between the small molecules and stationary phase, and provided a sufficient theoretical basis for experimental data. Schematic presentation of the preparation of β-cyclodextrin covalent organic framework (β-CD COF) material–incorporated organic polymer monolith for separating the amides, amino acids, nucleosides, aromatic acids, and positional isomers. β-CD COF materials were synthesized and incorporated into the monolith as the stationary phase. Then, the incorporated monolith was applied in the capillary electrochromatography system for separating small molecules.

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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Rapid fabrication of versatile zwitterionic super-hydrophilic polymers by sole-monomer system for biomolecules separation

Qiqin Wang,Kun Peng,Ning Gan,Xiao Liu,Hao Huang,Huikai Shao,Hanying Jin,Jacques Crommen,Zhengjin Jiang

Zwitterionic super-hydrophilic polymers showed fascinating prospects because of their excellent biocompatibility, and antifouling characteristics. However, their commercial development and the application in different fields were limited by their tedious preparation process, unsatisfactory reproducibility and performance. In this study, a rapid fabrication approach based on a sole-monomer system (2-(methacryloyloxy)ethyl-[ N -(2-methacryloyloxy)ethyl]phosphorylcholine (MMPC) was simultaneously employed as monomer and crosslinker) was proposed for preparing the cell membrane biomimetic polymers within only 1 h, which is significantly faster than the conventional multi-monomers based approach (~12 h). Furthermore, the proposed strategy turns out to be very simple, time saving and reproducible. The super-hydrophilicity, excellent separation efficiency, biocompatibility and antifouling ability were also achieved on the resulting biomimetic polymers. It is worth noting that the versatile biomimetic polymers exhibited excellent enrichment capacity for N -glycopeptides or C-reactive protein (CRP) from complex biological matrices as well as great separation performance for small bioactive molecules although the PC analogous moiety is located in the middle of the MMPC molecule. In particular, a quite similar binding mode exists between the MMPC dimer and the natural PC ligands to CRP. Therefore, the sole-monomer system can not only simplify the preparation process and improve the reproducibility of the zwitterionic materials, but also combine the advantages of the biomimetic cell membrane surface and the zwitterionic super-hydrophilic polymers for the separation of biomolecules in complex biological fluids.

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MICROCHIMICA ACTA · 2020 ·Vol. 187 ·期 3 ·1-10 · IF 6.232

Colloidal photonic crystal array chip based on nanoparticle self-assembly on patterned hydrophobic surface for signal-enhanced fluorescent assay of adenosine

Guo Rui,Wang Dan-Ni,Wei Yun-Yun,Zhang Ying-Zhi,Yang Chun-Guang,Xu Zhang-Run

A controllable approach for preparing a portable colloidal photonic crystal (CPC) array chip is presented. The approach was inspired by the confinement effect of nanoparticle self-assembly on patterned surface. Hydrophobic polydimethylsiloxane substrate with reproducible micro-region array was fabricated by soft-lithography. The substrate was employed as the patterned template for self-assembly of monodisperse polystyrene nanoparticles. The CPC units can be prepared in several minutes, and exhibit consistent reflection wavelength. By adjusting the size of polystyrene nanoparticles and the shape of micro-regions, CPC units with multiple structure, colors and geometries were obtained. The CPC array chip features fluorescence enhancement owing to the optical modulation capability of the periodic nanostructure of the self-assembled CPC. With the reflection wavelength (523 nm) of green CPC units overlapping the emission wavelength (520 nm, with excitation wavelength of 490 nm) of 6-carboxyfluorescein-labeled DNA probe, the fluorescence intensity increased more than 10-fold. For signal-amplified assay of adenosine, the concentration range of linear response was 5.0 × 10 −5  mol L −1 to 1.0 × 10 −3  mol L −1 , and the limit of detection was 1.3 × 10 −6  mol L −1 . Because of the enhancement effect of photonic crystal, the fluorescence images were more readable from the CPC array chip, compared with those from the planar substrate. The chip has potential applications in multiplex determination with high-throughput via encoding strategy based on the tunable structure, color or geometric shape. Schematic diagram of signal-enhanced fluorescent detection of adenosine based on the colloidal photonic crystal array chip (PDMS, polydimethylsiloxane; PS NPs, polystyrene nanoparticles; CPC, colloidal photonic crystal; GO, graphene oxide; FAM, 6-carboxyfluorescein).

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