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A Close Look at the Structure of the TiO2-APTESInterface in Hybrid Nanomaterials and Its DegradationPathway: An Experimental and Theoretical Study

机译：仔细观察TiO2-APTES的结构杂化纳米材料的界面及其降解途径：实验和理论研究

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摘要

The surface functionalization of TiO2-based materials with alkylsilanes is attractive in several cutting-edge applications, such as photovoltaics, sensors, and nanocarriers for the controlled release of bioactive molecules. (3-Aminopropyl)triethoxysilane (APTES) is able to self-assemble to form monolayers on TiO2 surfaces, but its adsorption geometry and solar-induced photodegradation pathways are not well understood. We here employ advanced experimental (XPS, NEXAFS, AFM, HR-TEM, and FT-IR) and theoretical (plane-wave DFT) tools to investigate the preferential interaction mode of APTES on anatase TiO2. We demonstrate that monomeric APTES chemisorption should proceed through covalent Si–O–Ti bonds. Although dimerization of the silane through Si–O–Si bonds is possible, further polymerization on the surface is scarcely probable. Terminal amino groups are expected to be partially involved in strong charge-assisted hydrogen bonds with surface hydroxyl groups of TiO2, resulting in a reduced propensity to react with other species. Solar-induced mineralization proceeds through preferential cleavageof the alkyl groups, leading to the rapid loss of the terminal NH2 moieties, whereas the Si-bearing head of APTES undergoesslower oxidation and remains bound to the surface. The suitabilityof employing the silane as a linker with other chemical species isdiscussed in the context of controlled degradation of APTES monolayersfor drug release and surface patterning.
机译：具有烷基硅烷的TiO2基材料的表面功能化在一些前沿应用中具有吸引力，例如光伏，传感器和用于控制释放生物活性分子的纳米载体。 （3-氨基丙基）三乙氧基硅烷（APTES）能够自组装以在TiO2表面上形成单层，但是其吸附几何形状和太阳光诱导的光降解途径尚不十分清楚。我们在这里采用高级实验（XPS，NEXAFS，AFM，HR-TEM和FT-IR）和理论（平面波DFT）工具研究APTES与锐钛矿型TiO2的优先相互作用模式。我们证明单体APTES化学吸附应通过共价Si-O-Ti键进行。尽管通过Si–O–Si键使硅烷二聚化是可能的，但几乎不可能在表面进一步聚合。预计末端氨基会部分参与与TiO2表面羟基的强电荷辅助氢键，从而降低与其他物种发生反应的倾向。太阳诱发的矿化作用通过优先分裂而进行烷基，导致末端NH2部分快速丢失，而APTES的含硅头经历较慢的氧化作用并保持结合在表面上。适用性使用硅烷作为与其他化学物种的连接基的方法是在APTES单层受控降解的背景下讨论用于药物释放和表面图案化。

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