Computational study on the half-metallicity in transition metal-oxide-incorporated 2D g-C3N4 nanosheets
Computational study on the half-metallicity in transition metal-oxide-incorporated 2D g-C3N4 nanosheets
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过渡金属氧化物掺入的二维 g-C3N4 纳米片半金属性的计算研究
DOI：
10.1007/s11467-018-0754-6
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发表时间：
2018
影响因子：
7.5
通讯作者：
Hu Zhen-Peng
中科院分区：
文献类型：
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作者：
Gao Qian;Wang Hui-Li;Zhang Li-Fu;Hu Shuang-Lin;Hu Zhen-Peng
在本研究中，我们基于第一性原理计算，系统地研究了过渡金属氧化物掺杂的二维g-C3N4纳米薄片(标记为C3N4-Tm-O，Tm=Sc-Mn)的电磁性质。结果表明，在所有体系中，TM-O都与g-C3N4纳米片紧密结合。我们发现，二维C3N4-Tm-O骨架在Tm=Sc，Ti，V，Cr时是铁磁性的，而在Tm=Mn时是反铁磁性的。所有的铁磁系统都表现出半金属性质。此外，基于海森堡模型的蒙特卡罗模拟表明，C3N4-Tm-O(Tm=Sc，Ti，V，Cr)骨架的居里温度(TC)分别为169K、68K、203K和190K。基于Bader电荷分析，我们发现费米能区的半金属性可以部分归因于Tm原子向g-C3N4纳米片的电子转移。此外，我们还发现，对于2Dg-C3N4纳米薄片，不仅电子，而且空穴都可以诱导半金属性，这可能有助于理解石墨化氮化碳的半金属性的起源。
In this study, based on the first-principles calculations, we systematically investigated the electronic and magnetic properties of the transition metal–oxide-incorporated 2D g-C3N4nanosheet (labeled C3N4–TM–O, TM = Sc–Mn). The results suggest that the TM–O binds to g-C3N4nanosheets strongly for all systems. We found that the 2D C3N4–TM–O framework is ferromagnetic for TM = Sc, Ti, V, Cr, while it is antiferromagnetic for TM = Mn. All the ferromagnetic systems exhibit the half-metallic property. Furthermore, Monte Carlo simulations based on the Heisenberg model suggest that the Curie temperatures (Tc) of the C3N4–TM–O (TM = Sc, Ti, V, Cr) framework are 169 K, 68 K, 203 K, and 190 K, respectively. Based on Bader charge analysis, we found that the origin of the half-metallicity at Fermi energy can be partially attributed to the transfer of electrons from TM atoms to the g-C3N4nanosheet. In addition, we found that not only electrons but also holes can induce half-metallicity for 2D g-C3N4nanosheets, which may help to understand the origin of half-metallicity for graphitic carbon nitride.