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Stability Enhancement by Hydrophobic Anchoring and a Cross-Linked Structure of a Phospholipid Copolymer Film for Medical Devices
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2024-07-22 , DOI: 10.1021/acsami.4c07752 Kazuto Uchida 1 , Tsukuru Masuda 1 , Shintaro Hara 1, 2 , Youichi Matsuo 1 , Yuwei Liu 3 , Hiroyuki Aoki 3, 4 , Yoshihiko Asano 5 , Kazuki Miyata 5, 6 , Takeshi Fukuma 5, 6 , Toshiya Ono 7 , Takashi Isoyama 7, 8 , Madoka Takai 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2024-07-22 , DOI: 10.1021/acsami.4c07752 Kazuto Uchida 1 , Tsukuru Masuda 1 , Shintaro Hara 1, 2 , Youichi Matsuo 1 , Yuwei Liu 3 , Hiroyuki Aoki 3, 4 , Yoshihiko Asano 5 , Kazuki Miyata 5, 6 , Takeshi Fukuma 5, 6 , Toshiya Ono 7 , Takashi Isoyama 7, 8 , Madoka Takai 1
Affiliation
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Surface modification using zwitterionic 2-methacryloyloxyethylphosphorylcholine (MPC) polymers is one of the most reasonable ways to prepare medical devices that can suppress undesired biological reactions such as blood coagulation. Usable MPC polymers are hydrophilic and water soluble, and their surface modification strategy involves exploiting the copolymer structures by adding physical or chemical bonding moieties. In this study, we developed copolymers composed of MPC, hydrophobic anchoring moiety, and chemical cross-linking unit to clarify the role of hydrophobic interactions in achieving biocompatible and long-term stable coatings. The four kinds of MPC copolymers with cross-linking units, such as 3-methacryloxypropyl trimethoxysilane (MPTMSi), and four different hydrophobic anchoring moieties, such as 3-(methacryloyloxy)propyltris(trimethylsiloxy)silane (MPTSSi) named as PMMMSi, n-butyl methacrylate (BMA) as PMBSi, 2-ethylhexyl methacrylate (EHMA) as PMESi, and lauryl methacrylate as PMLSi, were synthesized and coated on polydimethylsiloxane, polypropylene (PP), and polymethyl pentene. These copolymers were uniformly coated on the substrate materials PP and poly(methyl pentene) (PMP), to achieve hydrophilic and electrically neutral coatings. The results of the antibiofouling test showed that PMBSi repelled the adsorption of fluorescence-labeled bovine serum albumin the most, whereas PMLSi repelled it the least. Notably, all four copolymers suppressed platelet adhesion similarly. The variations in protein adsorption quantities among the four copolymer coatings were attributed to their distinct swelling behaviors in aqueous environments. Further investigations, including 3D scanning force microscopy and neutron reflectivity measurements, revealed that the PMLSi coating exhibited a higher water intake under aqueous conditions in comparison to the other coatings. Consequently, all copolymer coatings effectively prevented the invasion of platelets but the proteins penetrated the PMLSi network. Subsequently, the dynamic stability required to induce shear stress was evaluated using a circulation system. The results demonstrated that the PMMMSi and PMLSi coatings on PMP and PP exhibited exceptional platelet repellency and maintained high stability during circulation. This study highlights the potential of hydrophobic moieties to improve hemocompatibility and stability, offering potential applications in medical devices.
中文翻译：
用于医疗器械的磷脂共聚物薄膜的疏水锚定和交联结构增强稳定性
使用两性离子2-甲基丙烯酰氧基乙基磷酰胆碱（MPC）聚合物进行表面改性是制备可抑制凝血等不良生物反应的医疗器械的最合理方法之一。可用的 MPC 聚合物是亲水性和水溶性的，其表面改性策略包括通过添加物理或化学键合部分来利用共聚物结构。在这项研究中，我们开发了由MPC、疏水锚定部分和化学交联单元组成的共聚物，以阐明疏水相互作用在实现生物相容性和长期稳定涂层中的作用。四种具有交联单元的MPC共聚物，如3-甲基丙烯酰氧基丙基三甲氧基硅烷(MPTMSi)，和四种不同的疏水锚定部分，如命名为PMMMSi的3-(甲基丙烯酰氧基)丙基三(三甲基硅氧基)硅烷(MPTSSi)， n -合成了甲基丙烯酸丁酯（BMA）作为PMBSi、甲基丙烯酸2-乙基己酯（EHMA）作为PMESi、甲基丙烯酸月桂酯作为PMLSi，并涂覆在聚二甲基硅氧烷、聚丙烯（PP）和聚甲基戊烯上。将这些共聚物均匀涂覆在基材PP和聚甲基戊烯（PMP）上，获得亲水性和电中性的涂层。抗生物污损试验结果表明，PMBSi对荧光标记牛血清白蛋白的吸附排斥力最强，而PMLSi对荧光标记牛血清白蛋白的吸附排斥力最弱。值得注意的是，所有四种共聚物都类似地抑制血小板粘附。四种共聚物涂层之间蛋白质吸附量的变化归因于它们在水环境中不同的溶胀行为。 包括 3D 扫描力显微镜和中子反射率测量在内的进一步研究表明，与其他涂层相比，PMLSi 涂层在含水条件下表现出更高的吸水量。因此，所有共聚物涂层都有效地阻止了血小板的侵入，但蛋白质却穿透了 PMLSi 网络。随后，使用循环系统评估引起剪切应力所需的动态稳定性。结果表明，PMP 和 PP 上的 PMMMSi 和 PMLSi 涂层表现出优异的血小板排斥性，并在循环过程中保持高稳定性。这项研究强调了疏水部分改善血液相容性和稳定性的潜力，为医疗器械提供了潜在的应用。
更新日期：2024-07-22
中文翻译：
用于医疗器械的磷脂共聚物薄膜的疏水锚定和交联结构增强稳定性
使用两性离子2-甲基丙烯酰氧基乙基磷酰胆碱（MPC）聚合物进行表面改性是制备可抑制凝血等不良生物反应的医疗器械的最合理方法之一。可用的 MPC 聚合物是亲水性和水溶性的，其表面改性策略包括通过添加物理或化学键合部分来利用共聚物结构。在这项研究中，我们开发了由MPC、疏水锚定部分和化学交联单元组成的共聚物，以阐明疏水相互作用在实现生物相容性和长期稳定涂层中的作用。四种具有交联单元的MPC共聚物，如3-甲基丙烯酰氧基丙基三甲氧基硅烷(MPTMSi)，和四种不同的疏水锚定部分，如命名为PMMMSi的3-(甲基丙烯酰氧基)丙基三(三甲基硅氧基)硅烷(MPTSSi)， n -合成了甲基丙烯酸丁酯（BMA）作为PMBSi、甲基丙烯酸2-乙基己酯（EHMA）作为PMESi、甲基丙烯酸月桂酯作为PMLSi，并涂覆在聚二甲基硅氧烷、聚丙烯（PP）和聚甲基戊烯上。将这些共聚物均匀涂覆在基材PP和聚甲基戊烯（PMP）上，获得亲水性和电中性的涂层。抗生物污损试验结果表明，PMBSi对荧光标记牛血清白蛋白的吸附排斥力最强，而PMLSi对荧光标记牛血清白蛋白的吸附排斥力最弱。值得注意的是，所有四种共聚物都类似地抑制血小板粘附。四种共聚物涂层之间蛋白质吸附量的变化归因于它们在水环境中不同的溶胀行为。 包括 3D 扫描力显微镜和中子反射率测量在内的进一步研究表明，与其他涂层相比，PMLSi 涂层在含水条件下表现出更高的吸水量。因此，所有共聚物涂层都有效地阻止了血小板的侵入，但蛋白质却穿透了 PMLSi 网络。随后，使用循环系统评估引起剪切应力所需的动态稳定性。结果表明，PMP 和 PP 上的 PMMMSi 和 PMLSi 涂层表现出优异的血小板排斥性，并在循环过程中保持高稳定性。这项研究强调了疏水部分改善血液相容性和稳定性的潜力，为医疗器械提供了潜在的应用。
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