The photocatalytic property for water splitting and the structural stability of CuMgM layered double hydroxides (M = Al, Cr, Fe, Ce)
The photocatalytic property for water splitting and the structural stability of CuMgM layered double hydroxides (M = Al, Cr, Fe, Ce)
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DOI：
10.1016/j.clay.2015.06.023
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发表时间：
2015-09
影响因子：
5.6
通讯作者：
Shengjie Xia;Lianyang Zhang;Xiaobo Zhou;G. Pan;Z. Ni
中科院分区：
文献类型：
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作者：
Shengjie Xia;Lianyang Zhang;Xiaobo Zhou;G. Pan;Z. Ni
本文成功合成了四种具有良好晶体结构的CuMgM层状双氢氧化物（LDHs，M = Al，Cr，Fe，Ce）。研究了这些LDH材料在可见光下光催化还原水分解的活性。实验结果表明，与其他CuMgM-LDHs相比，具有最窄带隙和最大表面积的CuMgCr-LDHs在可见光下具有最高的产氢效率。 CuMgCr-LDHs催化产氢的产率为452.9 μmol/g h，效率非常高。此外，通过周期密度泛函理论（DFT）计算分析了CuMgM-LDHs的电子能带结构，这与UV-vis实验结果非常吻合。此外，通过密度泛函理论（DFT）分析几何参数、电子排列、电荷布居、氢键和结合能，研究了不同M3+对CuMgM-LDHs结构和稳定性的影响。理论计算结果表明，LDH材料的结构稳定性依次为CuMgAl>CuMgCe>CuMgFe>CuMgCr，而实验结果表明4种材料的光催化活性依次为CuMgCr>CuMgFe>CuMgCe>CuMgAl。
In this paper, four types of CuMgM layered double hydroxides (LDHs, M = Al, Cr, Fe, Ce) with good crystal structures were successfully synthesized. The activity of those LDH materials for photocatalytic reduction of water splitting under visible light was investigated. The experimental results showed that CuMgCr-LDHs with the narrowest band gap and the largest surface areas behave with the highest efficiency for hydrogen production under visible light than the other CuMgM-LDHs. The yield for hydrogen production catalyzed by CuMgCr-LDHs was 452.9 μmol/g h, which was very highly efficient. Furthermore, the electronic band structure of CuMgM-LDHs was analyzed by periodic density functional theory (DFT) calculation, which is in good agreement with the experimental result from UV–vis. In addition, the influence of the different M3 +on the structures and stability of the CuMgM-LDHs was also investigated by analyzing the geometric parameters, electronic arrangement, charge populations, and hydrogen-bonding and binding energies by density functional theory (DFT) analysis. The theoretical calculation results showed that the structural stability of LDH materials followed the order of CuMgAl > CuMgCe > CuMgFe > CuMgCr, while the experimental results indicated that the photocatalytic activity of the four materials followed the order of CuMgCr > CuMgFe > CuMgCe > CuMgAl.