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Manipulating spin polarization of titanium dioxide for efficient photocatalysis.
Nature Communications ( IF 14.7 ) Pub Date : 2020-01-21 , DOI: 10.1038/s41467-020-14333-w
Lun Pan 1, 2 , Minhua Ai 1, 2 , Chenyu Huang 1 , Li Yin 3 , Xiang Liu 3 , Rongrong Zhang 1, 2 , Songbo Wang 1, 4 , Zheng Jiang 5, 6 , Xiangwen Zhang 1, 2 , Ji-Jun Zou 1, 2 , Wenbo Mi 3
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Photocatalysis has been regarded as a promising strategy for hydrogen production and high-value-added chemicals synthesis, in which the activity of photocatalyst depends significantly on their electronic structures, however the effect of electron spin polarization has been rarely considered. Here we report a controllable method to manipulate its electron spin polarization by tuning the concentration of Ti vacancies. The characterizations confirm the emergence of spatial spin polarization among Ti-defected TiO2, which promotes the efficiency of charge separation and surface reaction via the parallel alignment of electron spin orientation. Specifically, Ti0.936O2, possessing intensive spin polarization, performs 20-fold increased photocatalytic hydrogen evolution and 8-fold increased phenol photodegradation rates, compared with stoichiometric TiO2. Notably, we further observed the positive effect of external magnetic fields on photocatalytic activity of spin-polarized TiO2, attributed to the enhanced electron-spin parallel alignment. This work may create the opportunity for tailoring the spin-dependent electronic structures in metal oxides.

中文翻译:

操纵二氧化钛的自旋极化以进行有效的光催化。

光催化被认为是制氢和高附加值化学合成的一种有前途的策略,其中光催化剂的活性在很大程度上取决于其电子结构,但是很少考虑电子自旋极化的影响。在这里,我们报告了一种可控制的方法,通过调节Ti空位的浓度来控制其电子自旋极化。这些特征证实了钛偏转的TiO2中出现了空间自旋极化,这通过电子自旋取向的平行排列提高了电荷分离和表面反应的效率。具体地说,与化学计量的TiO2相比,具有强烈的自旋极化作用的Ti0.936O2的光催化氢释放量增加了20倍,苯酚的光降解速率增加了8倍。值得注意的是,我们进一步观察到外部磁场对自旋极化TiO2的光催化活性的积极影响,这归因于增强的电子自旋平行排列。这项工作可能会为在金属氧化物中定制自旋相关的电子结构创造机会。
更新日期:2020-01-22
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