A Strategy of Enhancing the Photoactivity of g-C3N4 via Doping of Nonmetal Elements: A First-Principles Study
A Strategy of Enhancing the Photoactivity of g-C3N4 via Doping of Nonmetal Elements: A First-Principles Study
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通过非金属元素掺杂增强 g-C3N4 光活性的策略：第一性原理研究
DOI：
10.1021/jp308334x
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发表时间：
2012-11-08
影响因子：
3.7
通讯作者：
Zhu, Yongfa
中科院分区：
文献类型：
--
作者：
Ma, Xinguo;Lv, Yanhui;Zhu, Yongfa
介绍了一种通过掺杂非金属(硫或磷)杂质来改善g-C3N4光电化学性能的有效结构掺杂方法。本文建立了具有不同掺杂位置的g-C3N4体系的代位和间隙掺杂模型，并用第一性原理密度泛函理论分别计算了它们的掺杂生成能和电子性质，研究了它们的稳定性和可见光活性。我们的结果表明，S原子优先取代g-C3N4的边N原子，而P原子优先位于g-C3N4的面内空位。此外，还证明了非金属杂质的掺杂减小了g-C3N4的能隙，从而提高了对可见光的吸收。掺杂使HOMO和LUMO的轮廓分布更加分散，有利于载流子迁移率的提高，而非共面的HOMO和LUMO有利于提高载流子迁移率。
An effective structural doping approach has been described to modify the photoelectrochemical properties of g-C3N4 by doping with nonmetal (sulfur or phosphorus) impurities. Here, the substitutional and interstitial doped models of g-C3N4 systems were constructed with different doped sites, and then their dopant formation energies and electronic properties were performed to study the stability and visible-light photoactivity using first-principles density functional theory, respectively. Our results have identified that an S atom preferentially substitutes for the edge N atom of g-C3N4; however, a P atom preferentially situates the interstitial sites of in-planar of g-C3N4. Furthermore, it is demonstrated that the doping with nonmetal impurities reduces the energy gap to enhance the visible-light absorption of g-C3N4. The increased dispersion of the contour distribution of the HOMO and LUMO brought by doping facilitates the enhancement of the carrier mobility, while the noncoplanar HOMO and LUMO favor the...