钱继东,郭远来,王星浩,牟小辉,杨志禄,熊开琴,黄楠,涂秋芬.基于贻贝灵感和点击化学构建的高效抗菌涂层[J].表面技术,2023,52(5):257-267.
QIAN Ji-dong,GUO Yuan-lai,WANG Xing-hao,MOU Xiao-hui,YANG Zhi-lu,XIONG Kai-qin,HUANG Nan,TU Qiu-fen.#$NPMussel-inspired and Click Chemistry Engineered Surface Strategies for Constructing Efficient Antibacterial Coating[J].Surface Technology,2023,52(5):257-267 |
| 基于贻贝灵感和点击化学构建的高效抗菌涂层 |
| #$NPMussel-inspired and Click Chemistry Engineered Surface Strategies for Constructing Efficient Antibacterial Coating |
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| DOI：10.16490/j.cnki.issn.1001-3660.2023.05.025 |
| 中文关键词: 表面改性 贻贝灵感化学 点击反应 抗菌肽 血液接触器械 |
| 英文关键词:surface modification mussel-inspired chemistry click reaction antibacterial peptide blood contact devices |
| 基金项目:国家自然科学基金(82072072);南方医科大学附属东莞医院高层次人才支持与发展计划(K202102);四川省国际科技创新合作项目(2021YFH0056) |
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| Author | Institution |
| QIAN Ji-dong | Key Laboratory of Advanced Technology of Materials of Education Ministry, School of Materials Science and Engineering, Southwestern Jiaotong University, Chengdu 610031, China |
| GUO Yuan-lai | Key Laboratory of Advanced Technology of Materials of Education Ministry, School of Materials Science and Engineering, Southwestern Jiaotong University, Chengdu 610031, China |
| WANG Xing-hao | Key Laboratory of Advanced Technology of Materials of Education Ministry, School of Materials Science and Engineering, Southwestern Jiaotong University, Chengdu 610031, China |
| MOU Xiao-hui | Key Laboratory of Advanced Technology of Materials of Education Ministry, School of Materials Science and Engineering, Southwestern Jiaotong University, Chengdu 610031, China |
| YANG Zhi-lu | Key Laboratory of Advanced Technology of Materials of Education Ministry, School of Materials Science and Engineering, Southwestern Jiaotong University, Chengdu 610031, China;Dongguan People's Hospital, Affiliated Dongguan Hospital, Southern Medical University, Guangdong Dongguan 523059, China |
| XIONG Kai-qin | Key Laboratory of Advanced Technology of Materials of Education Ministry, School of Materials Science and Engineering, Southwestern Jiaotong University, Chengdu 610031, China;State Key Laboratory of Molecular Engineering of Polymers, Fudan University, Shanghai 200438, China |
| HUANG Nan | Key Laboratory of Advanced Technology of Materials of Education Ministry, School of Materials Science and Engineering, Southwestern Jiaotong University, Chengdu 610031, China |
| TU Qiu-fen | Key Laboratory of Advanced Technology of Materials of Education Ministry, School of Materials Science and Engineering, Southwestern Jiaotong University, Chengdu 610031, China |
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| 中文摘要: |
| 目的 通过对材料表面进行改性，形成一层具有抗菌肽(ABP)分子的涂层，使得材料具有高效抗菌的功能。方法 利用多巴胺(DA)邻苯二酚结构的黏附能力以及己二胺(HD)的多胺化学结构，将DA与HD按照一定的配比混合，通过简单的一步分子自组装，在材料表面构建多巴胺-己二胺(DA/HD)基底涂层。通过DA/HD涂层表面丰富的氨基与叠氮化的NHS(NHS-N3)发生酰胺反应，从而在DA/HD涂层表面引入叠氮基团，得到N3涂层。再通过点击反应在N3涂层表面接枝ABP，得到ABP涂层。通过在多种不同材质表面制备DA/HD涂层与进行氨基量密度测定，对DA/HD涂层的广谱适用性进行分析。利用水接触角测量仪(WCA)、傅里叶变换红外仪(FTIR)、X射线光电子能谱仪(XPS)、耗散型石英晶体微天平(QCM-D)以及椭圆偏振光谱仪等，对涂层亲疏水性、成分及结构等进行检测分析。通过细菌试验检测以及与多种已报道抗菌涂层的抗菌率进行综合比较来评价ABP涂层的抗菌性能。结果 在多种不同材质表面都能成功制备DA/HD涂层，且具有较高的氨基量密度，表明DA/HD涂层具有广谱的适用性。通过WCA、FTIR、XPS、QCM-D以及椭圆偏振光谱仪的检测结果，证实了基于DA/HD基底涂层的ABP涂层制备成功且接枝量高达352.7 ng/cm2。表面抗菌试验以及与多种抗菌涂层的抗菌率比较结果表明，ABP涂层对大肠杆菌和表皮葡萄球菌都具有高效的抗菌率，且抗菌率分别高达(89.0±9.9)%和(97.3±1.7)%。结论 DA/HD涂层具有广谱的适用性。对基底表面进行改性后，成功在其表面形成一层具有高效抗菌功能的ABP涂层。该涂层与细菌直接接触，能够破坏菌膜，对革兰氏阴性菌和阳性菌具有高效的抑制作用。 |
| 英文摘要: |
| It is an advanced surface modification technology that can provide the highly effective antibacterial properties to the substrate material surfaces of the blood contact devices without altering the physical properties of the substrate material by constructing a coating with antibacterial peptide (ABP) molecules on the surface of substrate material. Current substrates for blood contact devices have poor antibacterial properties and are at risk of local or systemic infection after use. In this paper, we investigated the highly effective antibacterial properties of ABP coatings based on mussel-inspired and click chemistry constructs. As a substrate material for the study, 316L stainless steel was prepared as a disc of 1 cm diameter and 2 mm thickness, smoothed and polished with sandpaper and cleaned with anhydrous ethanol and distilled water, and finally the samples were dried. Firstly, the samples were immersed in Tris-base buffer (10 mM, pH=8.5) containing dopamine (1 mg/mL) and hexanediamine (2.44 mg/mL) at 25 ℃ for 24 hours. The material with deposits on the surface was then washed by ultrasonication with distilled water and dried under nitrogen to obtain a dopamine-hexanediamine (DA/HD) base coating. Then, the dried DA/HD coated samples were immersed in a PBS buffer solution of NHS-N3 (1 mg/mL) and submerged for 24 hours at 25 ℃. The material was then ultrasonically washed with distilled water and removed and dried with nitrogen to obtain the azidized DA/HD coating (N3 coating). Finally, the N3 coating was immersed in a PBS buffered solution of DBCO-ABP (1 mg/mL) for 24 hours at 25 ℃. The material was then washed ultrasonically with distilled water and removed and dried with nitrogen to obtain the ABP coating. Broad-spectrum applicability of DA/HD coatings was analyzed by preparing DA/HD coatings on a variety of different material surfaces and performing amine groups density measurements. The thickness of the coating was calculated through Cauchy model analysis with an ellipsometric polarisation spectrometer (M-2000V). The hydrophile of the material was determined with a water contact angle goniometer (DSA 100). The structural composition of the coating was analyzed with Fourier infrared absorption spectroscopy (Nicolet 5700) and X-ray photoelectron spectroscopy (K-Alpha). The number of ABP molecules grafted on the surface of the N3 coating was quantified in real time with a dissipative quartz crystal microbalance (Q-sense). The surface morphology of the specimens was observed with a scanning electron microscope (JSM-6390). Finally, the antimicrobial performance of ABP coatings was evaluated by antimicrobial experiments of E. coil and S. epidermidis and comparison of antimicrobial rates of various antimicrobial coatings. Dopamine (DA), which contained an adhesion-capable catechol structure, and hexanediamine (HD), which had a polyamine chemical structure, were mixed in a certain ratio to construct a DA/HD substrate coating on the surface of the material in a simple one-step molecular self-assembly. The N3 coating was obtained by introducing azide group on the surface of the DA/HD coating through the amide reaction between the abundant amino groups on the surface of the DA/HD coating and the azidized NHS (NHS-N3). The ABP coating was obtained by grafting ABP on the surface of the N3 coating by click reaction. The successful preparation of DA/HD coatings with a high amine groups density on a wide range of different material surfaces demonstrated the broad spectrum applicability of DA/HD coatings. The results of WCA, FTIR, XPS, QCM-D and ellipsometric polarisation spectroscopy confirmed that ABP coatings based on DA/HD substrate coatings were successfully prepared, the ABP graft on the ABP coating was as high as 352.7 ng/cm2. The results of surface antibacterial experiments and comparison of antimicrobial rates of various antimicrobial coatings showed that the ABP coating was highly effective against both E. coli and S. epidermidis with antibacterial rates of (89.0±9.9)% and (97.3±1.7)% respectively. The DA/HD coating has a broad spectrum of applicability. ABP coatings with highly effective antibacterial properties is successfully prepared on the surface of the substrate after modification. The coating is in direct contact with bacteria and is able to provide highly effective inhibition of Gram-negative and positive bacteria by disrupting the bacterial film. |
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