In situ Blue titania via band shape engineering for exceptional solar H2 production in rutile TiO2
In situ Blue titania via band shape engineering for exceptional solar H2 production in rutile TiO2
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DOI：
10.1016/j.apcatb.2021.120380
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发表时间：
2021-06-03
影响因子：
22.1
通讯作者：
Ide, Yusuke
中科院分区：
文献类型：
--
作者：
Doustkhah, Esmail;Assadi, M. Hussein N.;Ide, Yusuke
设计一种基于TiO 2的优良太阳能光催化剂，而不需要外部助催化剂，如Pt，尽管其在可再生能源生产方面具有特殊的潜力，但仍然没有解决。在这里，我们报告了一个国家的最先进的太阳能驱动的光催化Cl掺杂的金红石二氧化钛，在纳米片形态与（110）方面，在没有任何外部助催化剂的情况下，从水裂解H-2生产。通过简单的稀盐酸处理和在方便的温度下加热，通过层状钛酸盐的相互转化容易地合成Cl掺杂的金红石型TiO 2纳米片。我们表明，工程的带状可以导致持久的光生Ti 3+，随后可以作为原位助催化剂在金红石型TiO 2。根据我们的密度泛函计算，Cl掺杂剂在改善TiO 2的能带形状方面具有关键作用，即，显著降低了光生电子和空穴的有效质量，尤其是与氧空位的影响相比时。因此，由较轻的载流子引起的增强的载流子迁移率光生大量的延长的Ti 3+物质，其原位增强光催化活性（即，原位蓝二氧化钛）。我们的研究结果表明，尽管已经针对缩小二氧化钛的带隙相当大的努力，带形工程提供了一个更容易和强大的解决方案，为二氧化钛。
Designing an excellent solar photocatalyst based on TiO2 without an external cocatalyst such as Pt remains unresolved despite its exceptional potential for renewable energy production. Here, we report a state-of-the-art solar-driven photocatalytic Cl-doped rutile TiO2, in nanosheet morphology with (110) facets, for H-2 production from water splitting in the absence of any external cocatalyst. The Cl-doped rutile TiO2 nanosheets are easily synthesised via a layered titanate's interconversion through a simple dilute HCl treatment and thermal heating at a convenient temperature. We demonstrate that engineering the band shape can result in long-lasting photogenerated Ti3+, which subsequently can act as an in situ cocatalyst in rutile TiO2. According to our density functional calculations, the Cl dopant has a pivotal role in improving the band shape of TiO2, i.e., significantly reducing the effective mass of the photogenerated electrons and holes, especially when compared to the effect of oxygen vacancy. Consequently, the boosted carrier mobility, resulting from lighter carriers, photogenerates a significant number of prolonged Ti3+ species that enhance photocatalytic activity in situ (i.e., in situ blue titania). Our results show that despite the considerable efforts that have been directed towards narrowing TiO2's band gap, band shape engineering offers a more facile and robust solution for photocatalysis.