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Surface modifications and growth of titanium dioxide for photo-electrochemical water splitting

机译:用于光电化学水分解的二氧化钛的表面改性和生长

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摘要

This study investigates photo-anodes based on titanium dioxide (TiO2) that can be used to produce hydrogen by the photo-electrochemical decomposition of water. udTiO2 is a wide band gap semiconductor that absorbs only the UV region of the solar spectrum. Sensitization of TiO2 to visible light by the addition of gold nanoparticles (AuNPs) was studied. AuNPs sustain localized surface plasmon resonance (LSPR) that results in the absorption of light at the resonant energy. The evidence for water splitting by Au-TiO2 systems is discussed critically. Fabrication of arrays of AuNPs was done by; annealing sputtered gold thin films, micellar nanolithography, and nano-sphere lithography. The optical characteristics and photo-electrochemical ‘water splitting’ performance of AuNP coated rutile (110) electrodes were determined. Nb-doped crystals coated in AuNPs of ca. 20 nm exhibited a small photocurrent that was not present with the bare rutile electrode. Reduced un-doped rutile (110) with AuNPs did not exhibit the ‘plasmonic photocurrent’. Some Nb-doped electrodes did not exhibit an effect. Batches of Nb-doped and reduced rutile were examined using voltammetry and impedance spectroscopy and it was found that the ‘inactive’ Nb-doped TiO2 was partially reduced. udThin films of TiO2 were fabricated by pulsed laser deposition (PLD) onto amorphous and single crystal substrates. The effect of growth conditions on the phase and orientation of the film were studied, and procedures to grow anatase films oriented with (100), (001), and (101) were developed. The temperature and heating regime of TiO2 films fused silica affected the orientation of film growing. Nb doping of the films also affected the temperature of the anatase-rutile phase transition and the orientation of the films, acting to stabilize anatase at higher temperatures. Surprisingly, highly doped films were found to be non-conductive. The importance of the oxygen partial pressure in producing conductive films for use as electrodes is discussed.
机译:这项研究研究了基于二氧化钛(TiO2)的光阳极,该光阳极可用于通过水的光电化学分解产生氢气。 udTiO2是一种宽带隙半导体,仅吸收太阳光谱的紫外线区域。研究了通过添加金纳米颗粒(AuNPs)将TiO2增至可见光。 AuNP维持局部表面等离振子共振(LSPR),导致共振能量吸收光。关键讨论了Au-TiO2系统进行水分解的证据。 AuNP阵列的制造是通过:退火溅射金薄膜,胶束纳米光刻和纳米球光刻。确定了AuNP包覆的金红石(110)电极的光学特性和光电化学“水分解”性能。大约在AuNPs中包覆的Nb掺杂晶体。 20 nm的光电流很小,而金红石裸露电极则不存在。用AuNPs还原的未掺杂金红石(110)不会表现出“等离子体光电流”。一些掺Nb的电极没有显示效果。使用伏安法和阻抗光谱法检查了一批掺Nb和还原的金红石,发现“非活性” Nb掺杂的TiO2被部分还原了。通过在非晶和单晶衬底上脉冲激光沉积(PLD)制备TiO2薄膜。研究了生长条件对薄膜相和取向的影响,并开发了以(100),(001)和(101)取向的锐钛矿薄膜生长方法。 TiO2熔融石英薄膜的温度和加热方式影响了薄膜生长的方向。薄膜的Nb掺杂也会影响锐钛矿-金红石相变的温度和薄膜的取向,从而在更高的温度下稳定锐钛矿。令人惊讶地,发现高掺杂的膜是不导电的。讨论了氧分压在生产用作电极的导电膜中的重要性。

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    Alexander John Callum;

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