Li Zhenzi, Wang Shijie, Xie Ying, Yang Wutao, Tao Bing, Lu Jing, Wu Jiaxing, Qu Yang, Zhou Wei
Shandong Provincial Key Laboratory of Molecular Engineering, School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, People's Republic of China.
School of Chemistry and Materials Science, Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, Heilongjiang University, Harbin 150080, People's Republic of China.
J Colloid Interface Sci. 2021 Aug 15;596:12-21. doi: 10.1016/j.jcis.2021.03.116. Epub 2021 Mar 24.
Low charge separation efficiency of semiconductor materials is the main obstacle for high-performance photocatalyst. Herein, we report surface defects engineered uniform mesoporous TiO nanospheres (DMTNSs) through surfactant-mediated self-assembly solvothermal approach combined with hydrogenation strategy to promote charge separation. The surface defects induced charge imbalance result in the formation of built-in field, which can promote photogenerated charge separation efficiently and be confirmed by experimental and density functional theory (DFT) calculations. Under AM 1.5G irradiation, the photocatalytic hydrogen evolution of DMTNSs is 3.34 mmol h g, almost 3.5 times higher than that of pristine non-defective TiO nanospheres (0.97 mmol h g), due to the engineered surface defects narrowing the bandgap (3.01 eV) and inducing charge imbalance to boost spatial charge separation and extend visible-light response. The defect induced charge imbalance strategy opens a new valuable perspective for fabricating other high-efficient oxide photocatalysts.
半导体材料的低电荷分离效率是高性能光催化剂的主要障碍。在此，我们报告了通过表面活性剂介导的自组装溶剂热法结合氢化策略来设计表面缺陷的均匀介孔TiO纳米球（DMTNSs），以促进电荷分离。表面缺陷引起的电荷不平衡导致形成内建电场，这可以有效地促进光生电荷分离，并通过实验和密度泛函理论（DFT）计算得到证实。在AM 1.5G光照下，DMTNSs的光催化析氢量为3.34 mmol h g，几乎是原始无缺陷TiO纳米球（0.97 mmol h g）的3.5倍，这是由于设计的表面缺陷使带隙变窄（3.01 eV）并引起电荷不平衡，从而促进空间电荷分离并扩展可见光响应。缺陷诱导的电荷不平衡策略为制备其他高效氧化物光催化剂开辟了一个新的有价值的视角。
