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Enhanced molecular oxygen activation of Ni2+-doped BiO2-x nanosheets under UV, visible and near-infrared irradiation: Mechanism and DFT study
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2018-04-12 , DOI: 10.1016/j.apcatb.2018.04.016
Jun Li , Jia Wang , Gaoke Zhang , Yuan Li , Kai Wang

Although molecular oxygen activation plays a significant role in photocatalytic process for pollutants removal, it is still challenging to activate molecular oxygen into superoxide radical (O2) by photocatalysts under near-infrared (NIR) light irradiation. Herein, we successfully synthesized Ni2+-doped BiO2-x nanosheets, which could efficiently achieve the molecular oxygen activation into O2 under ultraviolet (UV), visible and NIR irradiation. Meanwhile, we found the doping Ni2+ facilitated the formation of BiO2-x nanosheets. More importantly, the contribution of doping Ni2+ on full spectrum molecular oxygen activation over Ni2+-doped BiO2-x was further confirmed by experiments and density functional theory (DFT) study. The introduction of Ni2+ into BiO2-x structure resulted in the formation of a new doping energy level band between the valence band (VB) and conduction band (CB) of Ni2+-doped BiO2-x, which contributed to the faster separation of carriers and highly efficient full spectrum driven molecular oxygen activation under UV, visible and NIR irradiation, especially with the irradiation of NIR light as compared to BiO2-x. In addition, the doping Ni2+ promoted the optical absorption property of BiO2-x with narrowing band gap and the up-shift position of VB and CB. As expected, the Ni2+-doped BiO2-x nanosheets exhibited enhanced photocatalytic activity for rhodamine B (RhB) degradation under UV, visible and NIR irradiation than pure BiO2-x nanosheets. The photocatalyst still revealed high photocatalytic activity even after five cycles. Finally, a possible photocatalytic mechanism of the degradation processes by Ni2+-doped BiO2-x was proposed. This work not only confirmed Ni2+ doping could promote the formation of BiO2-x nanosheets and enhance their full spectrum driven molecular oxygen activation ability, but also presented an in-depth understanding on the mechanism of full spectrum driven molecular oxygen activation.



中文翻译:

紫外,可见光和近红外辐射下Ni 2+掺杂的BiO 2-x纳米片增强的分子氧活化作用:机理和DFT研究

虽然分子氧活化在污染物去除光催化过程一个显著的作用,它仍然是具有挑战性的激活分子氧超氧自由基(ö 2 - )通过近红外(NIR)光照射下光催化剂。在此,我们成功地合成的Ni 2+掺杂BIO 2-X纳米片,这可能有效地实现分子氧活化为ö 2 -下的紫外线(UV),可见光和NIR照射。同时,我们发现掺杂的Ni 2+促进了BiO 2-x纳米片的形成。更重要的是,掺杂Ni 2+的贡献实验和密度泛函理论(DFT)的研究进一步证实了分子光谱对氧原子在Ni 2+掺杂的BiO 2-x上的活化的影响。引进的Ni 2+为生物2-X结构导致的价带(VB)和Ni的导带(CB)之间形成了新的掺杂能级带2+掺杂BIO 2-X ,这有助于与BiO 2-x相比,在UV,可见光和NIR辐照下,尤其是在NIR光辐照下,载流子的分离速度更快,并且高效的全光谱驱动分子氧活化。另外,掺杂Ni 2+通过窄带隙和VB和CB的上移位置,促进了BiO 2-x的光吸收性能。如所预期的,与纯BiO 2-x纳米片相比,Ni 2+掺杂的BiO 2-x纳米片在紫外,可见光和NIR照射下对罗丹明B(RhB)降解表现出增强的光催化活性。即使经过五个循环,光催化剂仍然显示出高的光催化活性。最后,提出了一种可能的光催化机理,即Ni 2+掺杂的BiO 2-x的降解过程。这项工作不仅证实了Ni 2+的掺杂可以促进BiO 2-x的形成 纳米片并增强了其全光谱驱动的分子氧活化能力,但也对全光谱驱动的分子氧活化的机理提出了深入的认识。

更新日期:2018-04-12
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