Department of Chemistry, University of Southampton, Southampton, SO17 1BJ, UK.
Dalton Trans. 2018 Aug 7;47(31):10536-10543. doi: 10.1039/c7dt04694d.
In this paper we report on a novel chemical vapour deposition approach to the formation and control of composition of mixed anion materials, as applied to titanium oxynitride thin films. The method used is the aerosol assisted chemical vapour deposition (AACVD) of a mixture of single source precursors. To explore the titanium-oxygen-nitrogen system the single source precursors selected were tetrakis(dimethylamido) titanium and titanium tetraisopropoxide which individually are precursors to thin films of titanium nitride and titanium dioxide respectively. However, by combining these precursors in specific ratios in a series of AACVD reactions at 400 °C, we are able to deposit thin films of titanium oxynitride with three different structure types and a wide range of compositions. Using this precursor system we can observe films of nitrogen doped anatase, with 25% anion doping of nitrogen; a new composition of pseudobrookite titanium oxynitride with a composition of Ti3O3.5N1.5, identified as being a UV photocatalyst; and rock-salt titanium oxynitride in the range TiO0.41N0.59 to TiO0.05N0.95. The films were characterised using GIXRD, WDX and UV-vis spectroscopy, and in the case of the pseudobrookite films, assessed for photocatalytic activity. This work shows that a so-called dual single-source CVD approach is an effective method for the deposition of ternary mixed anion ceramic films through simple control of the ratio of the precursors, while keeping all other experimental parameters constant.
本文报道了一种新颖的化学气相沉积方法,用于形成和控制混合阴离子材料的组成,应用于钛氧氮化物薄膜。所采用的方法是气溶胶辅助化学气相沉积(AACVD)的混合物单源前体。为了探索钛-氧-氮体系,选择的单源前体是四(二甲基氨基)钛和钛四异丙醇盐,它们分别是氮化钛和二氧化钛薄膜的前体。然而,通过在 400°C 的一系列 AACVD 反应中以特定比例组合这些前体,我们能够沉积具有三种不同结构类型和广泛组成的钛氧氮化物薄膜。使用这种前体系统,我们可以观察到氮掺杂锐钛矿的薄膜,氮的阴离子掺杂率为 25%;一种新的组成的赝钙钛矿钛氧氮化物,组成比为 Ti3O3.5N1.5,被鉴定为紫外线光催化剂;以及在 TiO0.41N0.59 到 TiO0.05N0.95 范围内的岩盐钛氧氮化物。使用 GIXRD、WDX 和紫外可见光谱对薄膜进行了表征,对于赝钙钛矿薄膜,还评估了其光催化活性。这项工作表明,所谓的双单源 CVD 方法是通过简单控制前体的比例,同时保持所有其他实验参数不变,沉积三元混合阴离子陶瓷薄膜的有效方法。