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BULLETIN OF MATERIALS SCIENCE · 2022 ·Vol. 45 ·期 2 ·1-12 · IF 1.878

Preparation of myoglobin-imprinted polymer with a new sulphoxide monomer on the surface of foam-graphene/nano Au via eATRP

Han Zhen,Zhou Yuxi,Yang Yifei,Sun Yu,Wang Yuping,Wang Yifan,Sun Yue

Molecular-imprinted polymers (MIPs) are generally considered as substituents for natural antibodies. MIPs synthesis needs to select appropriate functional monomers. Because of its strong interaction with the template, antibody–antigen complexes can be formed before polymerization. In this paper, myoglobin (Mb)-imprinted polymers with a new sulphoxide monomer (2-(methylsulphonyl) ethyl acrylate, MSEA) as functional monomers were successfully prepared via electrochemically mediated atom transfer radical polymerization (eATRP). At the same time, to solve the problems of low selectivity and large template size limitations, the Mb-imprinted polymers were prepared on the surface of Au electrode decorated with three-dimensional foam graphene (FG) and nano Au (nAu). Cyclic voltammetry, electrochemical impedance spectroscopy, scanning electron microscope and X-ray photoelectron spectroscopy were used to characterize the Au electrode modified with Mb-imprinted polymer (Au/FG/nAu/MIP MSEA ). The prepared Au/FG/nAu/MIP MSEA electrode was used as an electrochemical sensor to detect Mb. The results of experiments showed that the proposed biosensor had good selectivity, reproducibility, repeatability and stability. The linear response range was from 1.0 × 10 −12 to 1.0 × 10 −1 mg·l −1 , and the detection limit was 1.21 × 10 −13 mg·l −1 ( S/N  = 3). Compared with other methods for detecting Mb, the sensor had a wider detection range and lower detection limit.

研究领域: 材料科学 · 电化学 · 分析化学 · 纳米技术 · 生物传感器
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Surfaces and Interfaces · 2017 · IF 0

A effective approach for surface modification of polymer membrane via SI-eATRP in an electrochemical cell with a three electrode system

Jiayu Wu,Haiming Song,Dan Li,Weifeng Zhao,Weijie Zhang,Long Kang,Fen Ran,Changsheng Zhao

In this study, an environmentally friendly approach for surface modification of polymer membrane was reported, which named surface-initiated electrochemically mediated atom transfer radical polymerization (SI-eATRP). It was triggered after diffusion of a CuI/L activator generated at a working electrode. The introduction of electrochemically mediation can control the polymerization of monomers by a one-electron reduction of an initially added air-stable CuII salt. The reaction was carried out in an electrochemical cell with a three-electrode system at low temperature. Using this technique, hydrophilic polymer brushes of poly(N-vinylpyrrolidone) were grafted onto PES membrane surface. The effects of reaction conditions like polymerization time, monomer concentration, initiator amount, and different monomer on the polymerizations of monomer were investigated in detail. Based on these data, we concluded that the polymerization on polymer membrane surface could be controlled by mediating the reaction condition. Moreover, the precisely controlled polymerization may allow it to serve as excellent model systems for polymer membrane modification, in general, to illustrate the role of electrochemically mediating on the polymerization approach. And the water contact angle of the modified membrane decreased from 89° to 72°. The APTT of the modified membrane increased from 46   s to 81   s. Those results indicated that the surface modification by grafting PVP brushes provided practical application for the PES membranes with high surface properties.

研究领域: 材料科学 · 表面化学 · 生物医学工程
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LANGMUIR · 2016 · IF 3.993

Antifouling Zwitterionic Coating via Electrochemically Mediated Atom Transfer Radical Polymerization on Enzyme-Based Glucose Sensors for Long-Time Stability in 37 °C Serum

Yichuan Hu,Bo Liang,Lu Fang,Guanglong Ma,Guang Yang,Qin Zhu,Shengfu Chen,Xuesong Ye

In this study, a versatile fabrication method for coating enzyme-based biosensors with ultrathin antifouling zwitterionic polymer films to meet the challenge of the long-time stability of sensors in vivo was developed. Electrochemically mediated atom transfer radical polymerization (eATRP) was applied to polymerize zwitterionic sulfobetaine methacrylate monomers on the rough enzyme-absorbed electrode surfaces; meanwhile, a refined overall bromination was developed to improve the coverage of polymers on the biosensor surfaces and to maintain the enzyme activity simultaneously for the first time. X-ray photoelectron spectroscopy and atomic force microscopy were used to characterize the properties of the polymer layers. The antifouling performance and long-time stability in 37 °C undiluted bovine serum in vitro were evaluated. The results showed that the polymer brush coatings diminished over 99% nonspecific protein adsorption and that the sensitivity of the evaluated sensor was maintained at 94% after 15 days. The overall sensitivity deviation of 7% was nearly 50% lower than that of the polyurethane-coated ones and also much smaller than the current commercially available glucose biosensors. The results suggested that this highly controllable electrodeposition procedure could be a promising method to develop implantable biosensors with long-time stability.

研究领域: 生物传感器 · 聚合物化学 · 材料科学 · 分析化学
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Materials Science & Engineering C-Materials for Biological Applications · 2018 · IF 5.08

A new approach for membrane modification based on electrochemically mediated living polymerization and self-assembly of N-tert-butyl amide- and β-cyclodextrin-involved macromolecules for blood purification

Fen Ran,Jiayu Wu,Xiaoqin Niu,Dan Li,Chuanxiong Nie,Rui Wang,Weifeng Zhao,Weijie Zhang,Yuhong Chen,Changsheng Zhao

We report a convenient, highly efficient, and universal approach for blood-compatible modification of polymer membrane based on the SI-eATRP, RAFT, and self-assembly of N - tert -butyl amide and β -cyclodextrin existed in macromolecules chains. The functional membrane surfaces with any polymer chains of hydrophilic, ionic polymer, and polysaccharide segments, for example, the copolymers of N -vinyl pyrrolidone, sodium p -styrenesulfonate hydrate, and glucose allyl amide, are easily designed and fabricated; and the thickness of polymer brushes are efficiently controlled by polymerization conditions like monomer concentration and initiator amount. As a key bio-plastic, the modified polyethersulfone membrane shows suppressed platelet adhesion, significant decreases in thrombin-antithrombin generation, and the complement activations on C3a and C5a levels compared with pristine polyethersulfone membrane; while the platelet activation (PF4) decreased. Due to the similar groups as heparin-like structure, the modified membrane effectively prolonged the activated partial thromboplastin time, thrombin time, and prothrombin time. The water contact angle of the modified membrane decreases from 89.2 to 22.3°, and the cytocompatibility of the modified membranes largely enhanced. It could be concluded that the new approach could be widely used for polymer membrane modification, and the mimic heparin-like surface seems to be a promising structure to improve the biocompatibility for blood purification application.

研究领域: 材料科学 · 聚合物化学 · 生物医学工程
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ANALYTICAL CHEMISTRY · 2024 · IF 6.7

Site-Directed Electrochemical Grafting for Amplified Detection of Antibody Pharmaceuticals

Jianwen Wan,Yiyan Tian,Di Wu,Zhuojun Ye,Songmin Chen,Qiong Hu,Mengge Wang,Junpeng Lv,Wenhui Xu,Xiyao Zhang,Dongxue Han,Li Niu

Antibody pharmaceuticals have become the most popular immunotherapeutic drugs and are often administered with low serum drug dosages. Hence, the development of a highly sensitive method for the quantitative assay of antibody levels is of great importance to individualized therapy. On the basis of the dual signal amplification by the glycan-initiated site-directed electrochemical grafting of polymer chains (glyGPC), we report herein a novel strategy for the amplified electrochemical detection of antibody pharmaceuticals. The target of interest was affinity captured by a DNA aptamer ligand, and then the glycans of antibody pharmaceuticals were decorated with the alkyl halide initiators (AHIs) via boronate cross-linking, followed by the electrochemical grafting of the ferrocenyl polymer chains from the glycans of antibody pharmaceuticals through the electrochemically controlled atom transfer radical polymerization (eATRP). As the glycans can be decorated with multiple AHIs and the grafted polymer chains are composed of tens to hundreds of electroactive tags, the glyGPC-based strategy permits the dually amplified electrochemical detection of antibody pharmaceuticals. In the presence of trastuzumab (Herceptin) as the target, the glyGPC-based strategy achieved a detection limit of 71.5 pg/mL. Moreover, the developed method is highly selective, and the results of the quantitative assay of trastuzumab levels in human serum are satisfactory. Owing to its uncomplicated operation and cost-effectiveness, the glyGPC-based strategy shows great promise in the amplified electrochemical detection of antibody pharmaceuticals.

CAS / MDL: 7791-03-9 14282-91-8
研究领域: 分析化学 · 电化学 · 药学 · 生物技术
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