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相较于快速热蒸发物理气相沉积(PVD),等离子体增强化学气相沉积(PE-CVD)可提高生物相容性 SiOx 薄膜在植入氧化铝陶瓷上的水解稳定性。

Plasma-Enhanced Chemical Vapor Deposition (PE-CVD) yields better Hydrolytical Stability of Biocompatible SiOx Thin Films on Implant Alumina Ceramics compared to Rapid Thermal Evaporation Physical Vapor Deposition (PVD).

机构信息

Department of Dental Materials and Biomaterials Research, RWTH Aachen University Hospital , Pauwelsstrasse 30, 52074 Aachen, Germany.

Technical and Macromolecular Chemistry, University of Paderborn , Warburger Strasse 100, 33098 Paderborn, Germany.

出版信息

ACS Appl Mater Interfaces. 2016 Jul 20;8(28):17805-16. doi: 10.1021/acsami.6b04421. Epub 2016 Jul 7.

Abstract

Densely sintered aluminum oxide (α-Al2O3) is chemically and biologically inert. To improve the interaction with biomolecules and cells, its surface has to be modified prior to use in biomedical applications. In this study, we compared two deposition techniques for adhesion promoting SiOx films to facilitate the coupling of stable organosilane monolayers on monolithic α-alumina; physical vapor deposition (PVD) by thermal evaporation and plasma enhanced chemical vapor deposition (PE-CVD). We also investigated the influence of etching on the formation of silanol surface groups using hydrogen peroxide and sulfuric acid solutions. The film characteristics, that is, surface morphology and surface chemistry, as well as the film stability and its adhesion properties under accelerated aging conditions were characterized by means of X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectroscopy (EDX), scanning electron microscopy (SEM), inductively coupled plasma-optical emission spectroscopy (ICP-OES), and tensile strength tests. Differences in surface functionalization were investigated via two model organosilanes as well as the cell-cytotoxicity and viability on murine fibroblasts and human mesenchymal stromal cells (hMSC). We found that both SiOx interfaces did not affect the cell viability of both cell types. No significant differences between both films with regard to their interfacial tensile strength were detected, although failure mode analyses revealed a higher interfacial stability of the PE-CVD films compared to the PVD films. Twenty-eight day exposure to simulated body fluid (SBF) at 37 °C revealed a partial delamination of the thermally deposited PVD films whereas the PE-CVD films stayed largely intact. SiOx layers deposited by both PVD and PE-CVD may thus serve as viable adhesion-promoters for subsequent organosilane coupling agent binding to α-alumina. However, PE-CVD appears to be favorable for long-term direct film exposure to aqueous solutions.

摘要

高密度烧结氧化铝(α-Al2O3)在化学和生物学上是惰性的。为了提高与生物分子和细胞的相互作用,在将其用于生物医学应用之前,必须对其表面进行改性。在这项研究中,我们比较了两种沉积技术,用于在整体α-氧化铝上促进 SiOx 薄膜的粘附,以促进稳定的有机硅烷单层的偶联;热蒸发的物理气相沉积(PVD)和等离子体增强化学气相沉积(PECVD)。我们还研究了使用过氧化氢和硫酸溶液对蚀刻对形成硅醇表面基团的影响。通过 X 射线光电子能谱(XPS)、能量色散 X 射线光谱(EDX)、扫描电子显微镜(SEM)、电感耦合等离子体-发射光谱(ICP-OES)和拉伸强度测试,对薄膜特性(即表面形貌和表面化学)以及在加速老化条件下的薄膜稳定性和粘附性能进行了表征。通过两种模型有机硅烷以及对鼠成纤维细胞和人间充质干细胞(hMSC)的细胞毒性和活力,研究了表面功能化的差异。我们发现两种 SiOx 界面均不会影响两种细胞类型的细胞活力。尽管失效模式分析表明 PE-CVD 薄膜的界面稳定性高于 PVD 薄膜,但在两种薄膜之间未检测到界面拉伸强度的显着差异。在 37°C 的模拟体液(SBF)中暴露 28 天,导致热沉积 PVD 薄膜的部分分层,而 PE-CVD 薄膜基本保持完整。因此,通过 PVD 和 PE-CVD 沉积的 SiOx 层可以作为后续有机硅烷偶联剂与α-氧化铝结合的可行粘附促进剂。然而,PE-CVD 似乎有利于长期直接暴露于水溶液中的薄膜。

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