Wang Fang, Cao Yuehan, Wei Shiqian, Zhou Ying
State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu, 610500, China.
The Center of New Energy Materials and Technology, School of Materials Science and Engineering, Southwest Petroleum University, Chengdu, 610500, China.
J Mol Model. 2017 Jan;23(1):23. doi: 10.1007/s00894-016-3198-3. Epub 2017 Jan 7.
We have provided a straightforward route to screen a series of metal-free doped bulk h-BN as potential visible-light photocatalysts via the first-principle computations. Various nonmetal dopants are considered including Si, P, C, S, Cl, O, and F atoms according to increasing electronegativity. The results show that the introduction of nonmetals leads to small lattice distortions but significant modifications of band structures, electron transition paths and chemical bonding interactions. Generally, all doped h-BN except Si doping have an active response to the visible-light, and dopants with higher electronegativity can significantly narrow the band gaps, which could induce easier optical transition under visible-light excitation. Based on the electronic structures and absorption spectra, three different mechanisms of enhanced visible-light response for the doping effect are proposed. It is expected that F, Cl, and S-doped h-BN could be used as potential efficient visible-light driven photocatalysts. This study could aid in the design of novel efficient h-BN photocatalysts. Graphical Abstract The mechanisms of the enhanced visible-light response of metal-free doped bulk h-BN.
我们通过第一性原理计算提供了一条直接的途径，来筛选一系列无金属掺杂的块状h-BN作为潜在的可见光光催化剂。根据电负性的增加，考虑了各种非金属掺杂剂，包括Si、P、C、S、Cl、O和F原子。结果表明，非金属的引入会导致小的晶格畸变，但会显著改变能带结构、电子跃迁路径和化学键相互作用。一般来说，除了Si掺杂外，所有掺杂的h-BN对可见光都有活性响应，电负性较高的掺杂剂可以显著缩小带隙，这可能会在可见光激发下诱导更容易的光学跃迁。基于电子结构和吸收光谱，提出了三种不同的掺杂效应增强可见光响应的机制。预计F、Cl和S掺杂的h-BN可以用作潜在的高效可见光驱动光催化剂。这项研究有助于新型高效h-BN光催化剂的设计。图形摘要 无金属掺杂块状h-BN增强可见光响应的机制。
