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Unfolding the Impact of H2-Reduction Treatment in Enhancing the Photocatalytic Activity of Rutile TiO2 Based on Photocarriers Dynamics
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2023-05-24 , DOI: 10.1021/acs.jpcc.3c00855
Junie Jhon M. Vequizo 1 , Kosaku Kato 2 , Fumiaki Amano 3 , Akira Yamakata 2
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2023-05-24 , DOI: 10.1021/acs.jpcc.3c00855
Junie Jhon M. Vequizo 1 , Kosaku Kato 2 , Fumiaki Amano 3 , Akira Yamakata 2
Affiliation
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In the pursuit of efficient titania photocatalysts for water splitting, several strategies have been employed. One of these is reduction of titania (TiO2) via treatment under hydrogen atmosphere, a promising technique to improve the photocatalytic performance. It has been proposed that electron injection induced by reduction on TiO2 demonstrated an improved photocatalytic activity. However, the dynamical processes involving the photogenerated charge carriers in reduced TiO2 have not been fully explored and understood yet. In this work, we employ time-resolved absorption spectroscopy (TAS) and photoluminescence (PL) measurements to unravel the impact of H2 reduction treatment on the photocarriers in rutile TiO2 (R-TiO2). TAS results revealed that the photoexcited electrons are preferentially filling the shallower trap states of reduced R-TiO2, with the lowest energy limit of ∼0.25 eV below the conduction band minimum, much shallower than that of nonreduced R-TiO2 (∼0.62 eV). Furthermore, these favorable effects of H2-reduction resulted in notable increase of long-lived shallow-trapped electrons, substantially extending the lifetimes of electrons and holes. PL measurements strongly support the positive impact of H2 reduction treatment: the NIR emission (∼850 nm) is largely quenched, indicating that the radiative recombination of deep trapped electrons and holes is significantly reduced. The combined PL and TAS results shed light on the impact of H2 reduction on R-TiO2, and this strategy can be potentially useful for further development of other photocatalytic materials.
中文翻译：
基于光载流子动力学揭示 H2 还原处理对增强金红石 TiO2 光催化活性的影响
在寻求用于水分解的高效二氧化钛光催化剂的过程中，已经采用了几种策略。其中之一是通过在氢气氛下处理来还原二氧化钛 (TiO 2 )，这是一种提高光催化性能的有前途的技术。有人提出，通过在 TiO 2上还原诱导的电子注入证明了改进的光催化活性。然而，涉及还原 TiO 2中光生载流子的动力学过程尚未得到充分探索和理解。在这项工作中，我们采用时间分辨吸收光谱 (TAS) 和光致发光 (PL) 测量来揭示 H 2的影响金红石TiO 2 (R-TiO 2 )中光载流子的还原处理。TAS 结果表明，光激发电子优先填充还原 R-TiO 2的较浅陷阱态，最低能量极限低于导带最小值 ~0.25 eV，比未还原 R-TiO 2浅得多（~0.62 eV ). 此外，H 2还原的这些有利影响导致长寿命浅层俘获电子显着增加，大大延长了电子和空穴的寿命。PL 测量强烈支持 H 2的积极影响还原处理：近红外发射（~850 nm）大部分被淬灭，表明深捕获电子和空穴的辐射复合显着减少。PL 和 TAS 的组合结果揭示了 H 2还原对 R-TiO 2的影响，并且该策略可能对进一步开发其他光催化材料有用。
更新日期：2023-05-24
中文翻译：
基于光载流子动力学揭示 H2 还原处理对增强金红石 TiO2 光催化活性的影响
在寻求用于水分解的高效二氧化钛光催化剂的过程中，已经采用了几种策略。其中之一是通过在氢气氛下处理来还原二氧化钛 (TiO 2 )，这是一种提高光催化性能的有前途的技术。有人提出，通过在 TiO 2上还原诱导的电子注入证明了改进的光催化活性。然而，涉及还原 TiO 2中光生载流子的动力学过程尚未得到充分探索和理解。在这项工作中，我们采用时间分辨吸收光谱 (TAS) 和光致发光 (PL) 测量来揭示 H 2的影响金红石TiO 2 (R-TiO 2 )中光载流子的还原处理。TAS 结果表明，光激发电子优先填充还原 R-TiO 2的较浅陷阱态，最低能量极限低于导带最小值 ~0.25 eV，比未还原 R-TiO 2浅得多（~0.62 eV ). 此外，H 2还原的这些有利影响导致长寿命浅层俘获电子显着增加，大大延长了电子和空穴的寿命。PL 测量强烈支持 H 2的积极影响还原处理：近红外发射（~850 nm）大部分被淬灭，表明深捕获电子和空穴的辐射复合显着减少。PL 和 TAS 的组合结果揭示了 H 2还原对 R-TiO 2的影响，并且该策略可能对进一步开发其他光催化材料有用。
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