First-Principles Calculation of Synergistic (N, P)-Codoping Effects on the Visible-Light Photocatalytic Activity of Anatase TiO2
First-Principles Calculation of Synergistic (N, P)-Codoping Effects on the Visible-Light Photocatalytic Activity of Anatase TiO2
复制标题
DOI：
10.1021/jp100802r
复制
发表时间：
2010-06
影响因子：
3.7
通讯作者：
R. Long;Niall J. English
中科院分区：
文献类型：
--
作者：
R. Long;Niall J. English
用第一性原理密度泛函理论计算了N和/或P掺杂的体相和锐钛矿相Ti02(101)表面的能量和电子性质。对于体相系统，在低浓度下，(N，P)共掺杂的锐钛矿型TiO2光催化剂的禁带宽度并不比单独掺N的锐钛矿型TiO2光催化剂的窄。随着P/N浓度比的增加，禁带宽度变窄更加明显。对于(N，P)共掺表面体系，当N和P同时作为替代掺杂时，禁带宽度略有变窄。然而，当N和P吸附在表面时，即使在低掺杂浓度下，带隙也显著变窄。计算的能量结果支持这样的观点，即在N掺杂的块体TiO2中掺入P并不能促进N的进一步引入，而与单一的N或P单掺杂相比，N和P可以更容易地在原始的锐钛矿相(101)表面掺杂。这些结果为近期实验观察到的不同光催化效率提供了合理的解释。
The energetic and electronic properties of N- and/or P-doped bulk and anatase TiO2 (101) surfaces have been calculated based on first-principles density functional theory. For the bulk system, (N, P)-codoping of anatase TiO2 does not narrow the band gap much more than that of single N-doped anatase TiO2 at low concentration. An increasing P/N concentration ratio leads to more significant band-gap narrowing. For (N, P)-codoped surface systems, the band gap is narrowed slightly when both N and P act as substitutional dopants. However, upon N and P adsorption on the surface, the band gap narrows significantly even at low dopant concentrations. The calculated energy results support the viewpoint that incorporation of P into N-doped bulk TiO2 cannot promote further N introduction, whereas N and P can be doped on the pristine anatase (101) surface more easily vis-a-vis single N- or P-monodoping. These results provide a reasonable explanation for recent experimental observations of different photocatalytic effic...