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Insights into the Electrocatalytic Behavior of Defect-Centered Reduced Titania (TiO1.23)
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2018-01-17 00:00:00 , DOI: 10.1021/acs.jpcc.7b10754 Jayashree Swaminathan 1 , Subbiah Ravichandran 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2018-01-17 00:00:00 , DOI: 10.1021/acs.jpcc.7b10754 Jayashree Swaminathan 1 , Subbiah Ravichandran 1
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As an attempt to explore the instantaneous changes that occur in titania during the cathodization process, herein we employ electron paramagnetic resonance (EPR) operando spectroscopy throughout the cathodization. This in-situ probing facilitates an experimentally verifiable clue about the underlying active sites in the highly active catalyst (TiO1.23) resulting from the cathodization. Furthermore, this study correlates the evolution of cathodization-driven defects and the resultant polaronic motion with hydrogen evolution reaction (HER). The defect richness and structural diversity in the reduced titania attribute ‘magic effects’ on its charge carrier dynamics and activity. Also, the enhanced electrocatalytic activity of TiO1.23 is explained in terms of its orbital reconstruction, electronic and structural modifications. Moreover, work function measurements reveal shifting of Fermi level toward the conduction band by defect-mediated Urbach tail and bound excitonic emissions, in line with the findings based on EPR spectroscopy. The observed phenomenon in TiO1.23 is further validated by its high (negative) surface charge, enhanced hydrophilicity and surface roughness compared with native TiO2. Therefore, these studies are earmarked for deep insight into the electronic structure modification of titania during the cathodization process and also provide a better understanding of the HER process that occurred in TiO1.23.
中文翻译：
缺陷为中心的还原二氧化钛（TiO 1.23）的电催化行为的见解
为了探索在阴极化过程中二氧化钛中发生的瞬时变化，我们在整个阴极化过程中采用电子顺磁共振（EPR）操作光谱。这种原位探测有助于从阴极上获得关于高活性催化剂（TiO 1.23）中潜在活性位点的实验可验证线索。此外，本研究将阴极驱动缺陷的演化以及由此产生的极化运动与氢演化反应（HER）相关联。还原的二氧化钛中的缺陷丰富度和结构多样性为其电荷载流子动力学和活性赋予了“魔术效应”。另外，TiO 1.23的增强的电催化活性根据其轨道重建，电子和结构修改来解释。而且，功函数测量揭示了缺陷介导的Urbach尾巴和束缚的激子发射使费米能级向导带移动，这与基于EPR光谱学的发现一致。与天然TiO 2相比，其高（负）表面电荷，增强的亲水性和表面粗糙度进一步证实了在TiO 1.23中观察到的现象。因此，这些研究专用于深入研究氧化过程中二氧化钛的电子结构修饰，还可以更好地了解TiO 1.23中发生的HER过程。
更新日期：2018-01-17
中文翻译：
缺陷为中心的还原二氧化钛（TiO 1.23）的电催化行为的见解
为了探索在阴极化过程中二氧化钛中发生的瞬时变化，我们在整个阴极化过程中采用电子顺磁共振（EPR）操作光谱。这种原位探测有助于从阴极上获得关于高活性催化剂（TiO 1.23）中潜在活性位点的实验可验证线索。此外，本研究将阴极驱动缺陷的演化以及由此产生的极化运动与氢演化反应（HER）相关联。还原的二氧化钛中的缺陷丰富度和结构多样性为其电荷载流子动力学和活性赋予了“魔术效应”。另外，TiO 1.23的增强的电催化活性根据其轨道重建，电子和结构修改来解释。而且，功函数测量揭示了缺陷介导的Urbach尾巴和束缚的激子发射使费米能级向导带移动，这与基于EPR光谱学的发现一致。与天然TiO 2相比，其高（负）表面电荷，增强的亲水性和表面粗糙度进一步证实了在TiO 1.23中观察到的现象。因此，这些研究专用于深入研究氧化过程中二氧化钛的电子结构修饰，还可以更好地了解TiO 1.23中发生的HER过程。
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