Defect-Mediated Crystallization of the Particulate TiO2 Photocatalyst Grown by Atomic Layer Deposition

IF 3.3 3区 化学 Q2 CHEMISTRY, PHYSICAL
Bela D. Bhuskute, Harri Ali-Löytty, Jesse Saari, Arto Hiltunen, Tero-Petri Ruoko, Turkka Salminen, Mika Valden
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Abstract

Nanopowders or films of pure and mixed oxides in nanoparticulate form have gained specific interest due to their applicability in functionalizing high-surface-area substrates. Among various other applications, our presented work primarily focuses on the behavior of TiO2 as a photocatalyst deposited by atomic layer deposition (ALD) on a quartz particle. The photocatalytic activity of TiO2 on quartz particles grown by ALD was studied in terms of ALD growth temperature and post-treatment heating rate. Amorphous TiO2 thin films (30 nm) were grown from tetrakis(dimethylamido)titanium (TDMAT) at 100 and 200 °C on quartz particles (0.35–3.5 μm) and crystallized using oxidative heat treatment at 500 °C with variable heating rates. The growth temperature was found to affect the TiO2 defect structure: TiO2 grown at 200 °C is black due to Ti3+ defects, whereas the film grown at 100 °C is white but contains some traces of the TDMAT ALD precursor. During the oxidative heat treatment, precursor traces desorbed and Ti3+ defects were oxidized. ALD TiO2 grown at 100 °C crystallized as anatase, whereas the rutile-to-anatase ratio of 200 °C grown TiO2 increased with the heating rate. The hydrogen production rate of mixed-phase TiO2 was found to outperform that of anatase TiO2.

Abstract Image

原子层沉积法生长TiO2颗粒光催化剂的缺陷介导结晶
纳米颗粒形式的纯氧化物和混合氧化物的纳米粉末或薄膜由于其在功能化高表面积基底方面的适用性而获得了特别的兴趣。在各种其他应用中,我们提出的工作主要集中在二氧化钛作为光催化剂的行为,通过原子层沉积(ALD)沉积在石英颗粒上。从ALD生长温度和后处理升温速率两方面研究了TiO2在ALD生长石英颗粒上的光催化活性。以四(二甲酰胺)钛(TDMAT)为原料,在100℃和200℃的温度下在石英颗粒(0.35 ~ 3.5 μm)上生长出30 nm的无定形TiO2薄膜,并在500℃、变升温速率下进行氧化热处理结晶。发现生长温度对TiO2缺陷结构有影响:在200℃下生长的TiO2由于Ti3+缺陷呈黑色,而在100℃下生长的TiO2薄膜为白色,但含有少量的TDMAT ALD前体。在氧化热处理过程中,前驱体被解吸,Ti3+缺陷被氧化。在100℃下生长的ALD TiO2结晶为锐钛矿,而在200℃下生长的TiO2金红石与锐钛矿的比值随着升温速率的增加而增加。混合相TiO2的产氢速率优于锐钛矿型TiO2。
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来源期刊
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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