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A novel open–framework spheniscidite photocatalyst with excellent visible light photocatalytic activity: Silver sensitization effect and DFT study
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2017-10-31 , DOI: 10.1016/j.apcatb.2017.10.070
Dandan Tang , Jun Li , Gaoke Zhang

We report a novel silver modified spheniscidite (SPH–Ag) visible light responsive photocatalyst with open–framework structure. The SPH–Ag photocatalyst was firstly synthesized by one step hydrothermal method. Meanwhile, the contribution of silver sensitization to the visible light photocatalytic property of SPH–Ag was confirmed by characterization results and DFT calculation. Ag+ is demonstrated to enter into the spheniscidite cavities and replace one NH4+ per unit cell without destroying the structure. Noteworthy, compared to SPH, the pure phase SPH–Ag catalyst equipped with larger specific surface area, broader visible light response region, stronger oxidizing ability and lower recombination rate of electrons and holes. Meanwhile, the valence electrons are rearranged and the unoccupied Ag 5 s orbital hybridizes with Fe 3d and O 2p orbitals at valance band, which greatly improves the SPH–Ag’s ability of gaining electrons and the separation of photo generated charge carriers. As expected, the SPH–Ag catalyst exhibited enhanced photocatalytic activity for ARG degradation under visible light irradiation, which is mainly attributed to the generation of h+ and O2 species. Furthermore, its photocatalytic property was highly maintained as well as its structure and surface chemical properties after five recycles. This work may provide insight into the design of new–type Ag–based photocatalysts and their photocatalytic mechanism.



中文翻译:

具有优异可见光光催化活性的新型开放骨架的绿闪石光催化剂:银敏化作用和DFT研究

我们报告了一种新型的银修饰的钠长石(SPH–Ag)可见光响应型光催化剂,具有开放式骨架结构。SPH-Ag光催化剂首先通过一步水热法合成。同时,表征结果和DFT计算证实了银敏化对SPH-Ag可见光光催化性能的贡献。已证明,Ag +会进入亚硒酸钠腔并取代一种NH 4 +每个单元格,而不会破坏结构。值得注意的是,与SPH相比,纯相SPH-Ag催化剂具有更大的比表面积,更宽的可见光响应区域,更强的氧化能力以及更低的电子和空穴复合率。同时,价电子重新排列,未占据的Ag 5 s轨道在价带上与Fe 3d和O 2p轨道杂化,这大大提高了SPH-Ag的电子获取能力和光生载流子的分离。正如所料,SPH-银催化剂表现出增强的对ARG降解的光催化活性的可见光照射,这主要归因于h的生成下+ö 2 -物种。此外,经过五次循环后,其光催化性能以及结构和表面化学性能得以高度保持。这项工作可能会为新型的基于Ag的光催化剂的设计及其光催化机理提供见解。

更新日期:2017-10-31
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