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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Fabrication of double imprinted anchor points in cellulose nanocrystals-based hierarchical porous polyHIPEs for selective separation of flavoniods under physiological pH

Shucheng Liu,Zhi Hu,Xuan Zhang,Hao Huang,Jianming Pan,Hongxiang Ou

Previous research had proved that molecular imprinted polymers can be used as separation material for removing Naringin (NRG) from agricultural pomelo wastes effectively. But the adsorption amounts of NRG molecules from traditional MIPs was quite low by using boronic acid as functional monomer because of single affinity interaction. Therefore, we developed the new combination of bifunctional monomers (i.e. low pKa boronate affinity monomer 2,4-difluoro-3-formylphenylboronic acid and dopamine) based on cellulose nanocrystals (CNCs) mixed with polymerized high internal phase emulsion (polyHIPE, PH) through an double layer surface imprinted method. The introduction of polyethylenimine (PEI) can offer abundant anchor units for the growth of more anchor sites to immobilization template molecules. Importantly, largely improved selective adsorption amounts (50.79 μmol g −1 ), which may be attribute to the fabrication of the uniform growth of double imprinted layers onto the polydopamine (PDA)/boronic acid-based surfaces. In addition, the resulting double recognition molecular imprinted polymers (MIPs) based on hypercrosslinked PH (DR-HCLPH@MIPs) not only exhibited fast adsorption kinetic of NRG molecule, but also possessed excellent selectivity and high adsorption capacities at physiological pH. Meanwhile, the coarse NRG from pomelo waste can be high selectively extracted to 94.74%. Overall, this study provides a versatile approach for fabrication of the sandwich-biscuit-like double imprinting layer porous MIPs for precise identification and ultrafast transport separation of NRG from complex samples.

研究领域: 材料科学 · 分子生物学
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EUROPEAN POLYMER JOURNAL · 2018 · IF 3.741

Boronate affinity monolith via two-step atom transfer radical polymerization for specific capture of cis-diol-containing compounds

Qian Dong,Shuai-Shuai Chi,Xi-Yan Deng,Yao-Han Lan,Chao Peng,Lin-Yi Dong,Xian-Hua Wang

Boronate affinity (BA) monolith is an important tool for uniquely selective capture of cis -diol-containing compounds. However, most of BA monoliths suffer from limited binding sites. In this work, a high-capacity BA monolith was successfully synthesized via simple two-step atom-transfer radical polymerization method. Fourier transform infrared spectra, scanning electron microscope and Brunauer–Emmett–Teller surface area analyzer were used to characterize the resultant BA monolith. The BA monolith could selective capture of cis -diol-containing small molecular compounds and protein macromolecules with all aqueous mobile phase at pH of 8.5. Frontal analysis was applied to measure the adsorption data, and Scatchard equation was used to calculate the C (Q max ) and dissociation constants ( K d ). By using polymer chains to amplify the number of binding sites, the binding capacity of BA monolith had been effectively improved to 303.5 and 118.2 μmol g −1 for catechol and adenosine, respectively. Such binding capacity was the highest among already reported BA monoliths. Interestingly, the binding capacity was mainly depended on the molecular volume (or molecular weight) of cis -diol containing compounds with a significant negative correlation. Besides, via synergistic effect of double binding, the BA chains had enhanced the binding strength of BA monolith toward molecules with two cis -diol groups with K d value of 10 −5 M, which were lower than that of molecules with one cis -diol group by one order of magnitude. The results indicated that the binding capacity and strength depend on not only the property of BA materials but also the nature of cis -diol-containing compounds.

研究领域: 生物化学 · 材料科学
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JOURNAL OF CHROMATOGRAPHY A · 2014 · IF 4.258

Online micro-solid-phase extraction based on boronate affinity monolithic column coupled with high-performance liquid chromatography for the determination of monoamine neurotransmitters in human urine

Xiaoting Yang,Yufei Hu,Gongke Li

Quantification of monoamine neurotransmitters is very important in diagnosing and monitoring of patients with neurological disorders. We developed an online analytical method to selectively determine urinary monoamine neurotransmitters, which coupled the boronate affinity monolithic column micro-solid-phase extraction with high-performance liquid chromatography (HPLC). The boronate affinity monolithic column was prepared by in situ polymerization of vinylphenylboronic acid (VPBA) and N , N ′-methylenebisacrylamide (MBAA) in a stainless capillary column. The prepared monolithic column showed good permeability, high extraction selectivity and capacity. The column-to-column reproducibility was satisfactory and the enrichment factors were 17–243 for four monoamine neurotransmitters. Parameters that influence the online extraction efficiency, including pH of sample solution, flow rate of extraction and desorption, extraction volume and desorption volume were investigated. Under the optimized conditions, the developed method exhibited low limit of detection (0.06–0.80   μg/L), good linearity (with R 2 between 0.9979 and 0.9993). The recoveries in urine samples were 81.0–105.5% for four monoamine neurotransmitters with intra- and inter-day RSDs of 2.1–8.2% and 3.7–10.6%, respectively. The online analytical method was sensitive, accurate, selective, reliable and applicable to analysis of trace monoamine neurotransmitters in human urine sample.

研究领域: 分析化学 · 医学诊断 · 神经科学
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JOURNAL OF THE SCIENCE OF FOOD AND AGRICULTURE · 2016 ·Vol. 97 ·期 8 ·2426-2435 · IF 2.076

Immune-affinity monolithic array with chemiluminescent detection for mycotoxins in barley

Li Li,Liru Xia,Yongfu Zhao,Min Wang,Xizhi Jiang

BACKGROUND Mycotoxins are produced by fungi as secondary metabolites. They often multi-contaminate food and feed commodities posing a health risk to humans and animals. Fast and easy multiplex screening could be thought as a useful tool for detection of multi-contaminated food and feed commodities. RESULTS A highly sensitive immune-affinity monolithic arrays for detecting the mycotoxins zearalenone, deoxynivalenol, T-2 toxin, HT-2 toxin, aflatoxins, ochratoxin A, and fumonisin B 1 were fabricated using UV induced co-polymerisation. The mycotoxin antibodies firstly reacted with functional monomer to form antibody/functional monomer bio-conjugates. Subsequently, the antibody/functional monomer bio-conjugates co-polymerised with cross-linker to form mycotoxins immune-affinity arrays. With optimal fabrication conditions, all mycotoxin immune-affinity monolithic arrays exhibited a linear response spanning three orders of magnitude. And the immune-affinity monolithic array has a low detection limit and has a good uniformity (intra-assay CV, and inter-assay CV both <8%). CONCLUSION The fabricated mycotoxin immune-affinity monolithic arrays were proved as a sensitive, stable and economical tool in real food samples detection. Moreover, the mycotoxin immune-affinity monolithic arrays would be able to minimise manipulation steps: add samples and enzyme labelled mycotoxins, and detect CL signals. © 2016 Society of Chemical Industry

研究领域: 食品科学 · 分析化学 · 免疫学
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JOURNAL OF CHROMATOGRAPHY A · 2021 · IF 4.759

Online specific recognition of mycotoxins using aptamer-grafted ionic affinity monolith with mixed-mode mechanism

Jinxin Chi,Dandan Zhu,Yiqiong Chen,Guihua Huang,Xucong Lin

Herein, a facile and practical aptamer-grafted ionic affinity monolith with mixed-mode mechanism was explored as a versatile platform for online specific recognition of polar and non-polar mycotoxins. The mixed-mode mechanism including molecular affinity adsorption (between aptamers and targets), hydrophilic interaction and ionic interaction (between stationary phase and targets) were adopted and provided a better flexibility in adjusting separation selectivity to reduce nonspecific adsorption with respect to the single mode. Preparation and characterization of aptamer-based affinity monoliths were investigated, The characterization of pore size distribution, Brunauer-Emmett-Teller (BET) surface area and the specificity and cross-reaction were also evaluated. As a result, the hydrophilic nature and negative charge on affinity monolith were obtained. Multiple interactions including aptamer affinity binding, hydrophilic interaction (HI) and ion exchange (IE) could be adopted for online selective extraction. Specific recognitions of polar ochratoxin A (OTA), non-polar zearalenone (ZEN) and aflatoxin B1 (AFB1) was fulfilled with LODs as 0.03, 0.05 and 0.05 μg/L, respectively. Applied to real cereals, good recoveries of the fortified OTA, AFB1 and ZEN were achieved as 92.6 ± 1.3% ~ 95.6 ± 1.3% (n=3), 93.9 ± 2.3% ~ 98.2 ± 3.4% (n=3) and 92.7 ± 2.0% ~ 96.9 ± 3.5% (n=3) in corn, wheat and rice, respectively. The results displayed that Apt-MCs with hydrophilic and ionic interaction mixed-mode mechanism were efficient enough and competent for the online recognition of mycotoxins in cereals.

研究领域: 分析化学 · 食品科学 · 毒理学
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TALANTA · 2019 · IF 4.916

Preparation and evaluation of highly hydrophilic aptamer-based hybrid affinity monolith for on-column specific discrimination of ochratoxin A

Yiqiong Chen,Xinyue Ding,Dandan Zhu,Xucong Lin,Zenghong Xie

Nonspecific adsorption is a challenge of specific recognition on aptamer-based affinity monoliths. Here, a novel highly hydrophilic polyhedral oligomeric silsesquioxane (POSS)-containing aptamer-based hybrid-silica affinity monolith with a good recognition nature was prepared and used for specific discrimination of ochratoxin A (OTA). A homogeneous polymerization mixture consisted of POSS chemicals, hydrophilic monomers and aptamer solution was directly polymerized via the “one-pot” method. Preparation and characterization of the resultant affinity monolith were studied in detail. A highly hydrophilic nature was obtained and the typical hydrophilic interaction liquid chromatography (HILIC) was observed when acetonitrile (ACN) content in mobile phase was 25%, which reached the highest hydrophilicity of POSS-based hybrid monoliths. By using OTA as model analyte, the nonspecific adsorption was effectively suppressed. The recovery of the analogue ochratoxin B (OTB) was only about 0.1% even if the content of OTB was 50 times more than OTA, which was much better than other POSS-containing monoliths and polar siloxane-based hybrid monoliths. Applied to beer samples, the adsorption of background materials was drastically resisted, and efficient recognition of OTA was obtained with the recoveries of 94.9–99.8%. Much less disturbance was observed than that occurred in hydrophobic POSS-based affinity monolith. It lights an attractive implement with high hydrophilicity and specificity for online selective recognition of OTA.

研究领域: 分析化学 · 食品科学 · 材料科学
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ANALYTICA CHIMICA ACTA · 2023 · IF 6.2

Tetrapeptide-based mimotope affinity monolith for the enrichment and analysis of anti-HER2 antibody and antibody-drug conjugate

Chendi Zhu,Hai Han,Zhiwei Chen,Yuan Shen,Qiaoxuan Zhang,Cai Bao,Jia-Huan Qu,Qiqin Wang,Zhengjin Jiang

Selective enrichment and analysis of therapeutic antibodies in biological fluids are crucial for the development of biopharmaceuticals. Recently, peptide-based affinity chromatography has exhibited fascinating prospects for antibody enrichment due to the high affinity and specificity of small peptides. However, the post-modification approach of peptide ligands on the material surface is complicated and time-consuming. In this study, a methacrylate modified tetrapeptide ( m -EDPW) was firstly demonstrated as the affinity ligand of trastuzumab ( K d  = 1.91 ± 1.81 μM). Next, the m -EDPW based affinity monolith was prepared using a facile one-step polymerization method, which could overcome the drawbacks of traditional post-modification preparation strategies. Based on the monolith as described above, a simple enrichment approach was developed under the optimal washing and elution conditions. Based on the excellent properties, such as high porosity (53.09%), weak electrostatic interaction and suitable affinity (1.00 ± 2.14 μM for anti-HER2 ADC), this novel monolith exhibited good specificity and recovery for antibodies (91.6% for trastuzumab, 98.37% for anti-HER2 ADC), and low nonspecific adsorption for human serum albumin (DBC 10%  = 0.5 mg/g polymer). Particularly, this material was successfully applied to enrich trastuzumab and its related antibody-drug conjugate (ADC) from different cell culture medias. The dynamic tracking analysis of ADC in the critical quality attributes (e.g., charge variants, drug to antibody ratio and subunit conjugation ratio) was also achieved by combining the enrichment approach, capillary electrophoresis or reversed phase liquid chromatography . In summary, the exploited peptide-based mimotope affinity materials showed a great potential for the application in biopharmaceutical analysis.

研究领域: 生物技术 · 药学 · 分析化学 · 生物化学
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