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首页> 外文期刊>Chemistry: A European journal >Epoxide opening versus silica condensation during sol-gel hybrid biomaterial synthesis
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Epoxide opening versus silica condensation during sol-gel hybrid biomaterial synthesis

机译：溶胶-凝胶杂化生物材料合成过程中的环氧开放与二氧化硅缩合

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Hybrid organicinorganic solids represent an important class of engineering materials, usually prepared by solgel processes by cross-reaction between organic and inorganic precursors. The choice of the two components and control of the reaction conditions (especially pH value) allow the synthesis of hybrid materials with novel properties and functionalities. 3- Glycidoxypropyltrimethoxysilane (GPTMS) is one of the most commonly used organic silanes for hybrid-material fabrication. Herein, the reactivity of GPTMS in water at different pH values (pH 211) was deeply investigated for the first time by solution-state multinuclear NMR spectroscopic and mass spectrometric analysis. The extent of the different and competing reactions that take place as a function of the pH value was elucidated. The NMR spectroscopic and mass spectrometric data clearly indicate that the pH value determines the kinetics of epoxide hydrolysis versus silicon condensation. Under slighly acidic conditions, the epoxy-ring hydrolysis is kinetically more favourable than the formation of the silica network. In contrast, under basic conditions, silicon condensation is the main reaction that takes place. Full characterisation of the formed intermediates was carried out by using NMR spectroscopic and mass spectrometric analysis. These results indicate that strict control of the pH values allows tuning of the reactivity of the organic and inorganic moities, thus laying the foundations for the design and synthesis of solgel hybrid biomaterials with tuneable properties.
机译：杂化有机无机固体代表了一类重要的工程材料，通常通过溶胶凝胶法通过有机和无机前体之间的交叉反应制备。两种组分的选择和反应条件（特别是pH值）的控制允许合成具有新颖特性和功能的杂化材料。 3-环氧丙氧基丙基三甲氧基硅烷（GPTMS）是混合材料制造中最常用的有机硅烷之一。本文中，首次通过溶液态多核NMR光谱和质谱分析对GPTMS在不同pH值（pH 211）下的反应性进行了深入研究。阐明了不同反应和竞争反应随pH值变化的程度。 NMR光谱和质谱数据清楚地表明，pH值决定了环氧水解相对于硅缩合的动力学。在弱酸性条件下，环氧环水解在动力学上比二氧化硅网络的形成更为有利。相反，在基本条件下，硅缩合是发生的主要反应。通过使用NMR光谱和质谱分析对形成的中间体进行全面表征。这些结果表明，严格控制pH值可以调节有机和无机部分的反应性，从而为具有可调节特性的solgel混合生物材料的设计和合成奠定了基础。

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