S和Al掺杂单层g-C3N4电子结构与光学性质的第一性原理研究

doi:10.11896/cldb.21100044

材料导报

2023, Vol. 37

Issue (9): 21100044-6 https://doi.org/10.11896/cldb.21100044

无机非金属及其复合材料

S和Al掺杂单层g-C₃N₄电子结构与光学性质的第一性原理研究

刘晨曦¹, 庞国旺¹, 潘多桥¹, 史蕾倩¹, 张丽丽^1,*, 雷博程^1,*, 赵旭才¹, 黄以能^1,2

1 伊犁师范大学物理科学与技术学院,新疆凝聚态相变与微结构实验室,新疆伊宁 835000
2 南京大学物理学院,固体微结构物理国家重点实验室,南京 210093

First-principles Study on Electronic Structure and Optical Properties of S and Al Doped Monolayer g-C₃N₄

LIU Chenxi¹, PANG Guowang¹, PAN Duoqiao¹, SHI Leiqian¹, ZHANG Lili^1,*, LEI Bocheng^1,*, ZHAO Xucai¹, HUANG Yineng^1,2

1 Xinjiang Laboratory of Phase Transitions and Microstructures in Condensed Matter, College of Physical Science and Technology, Yili Normal University, Yining 835000, Xinjiang, China
2 National Laboratory of Solid State Microstructures, School of Physics, Nanjing University, Nanjing 210093, China

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摘要 g-C₃N₄是一种典型的聚合物半导体材料,在可见光下就能完成对半导体要求较高的光催化反应。采用基于密度泛函理论的第一性原理平面波超软赝势方法研究了单层g-C₃N₄、S单掺g-C₃N₄、Al单掺g-C₃N₄和S-Al共掺g-C₃N₄的形成能、电子结构及光学性质。结果表明:S掺杂空隙I位置、Al掺杂N2位置时,杂质原子最易掺入g-C₃N₄体系。与单层g-C₃N₄相比,掺杂后的体系均发生了晶格畸变以及红移现象,拓展了体系的光吸收范围,可推测出S、Al掺杂能够提高g-C₃N₄体系的光催化性。其中,S-Al共掺杂体系的光催化性是最优的,原因是共掺杂体系的分子轨道有较强的离域性,有利于提高载流子的迁移率,并且共掺杂能使单掺杂引入的深能级变浅,减少杂质能级上的复合中心。因此,本工作提出的S-Al共掺杂可作为提高g-C₃N₄光催化活性的一种有效手段。

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	刘晨曦
	庞国旺
	潘多桥
	史蕾倩
	张丽丽
	雷博程
	赵旭才
	黄以能

关键词: 掺杂石墨相氮化碳电子结构光学性质第一性原理

Abstract: The g-C₃N₄ is a typical polymer semiconductor material, which can complete the photocatalytic reaction with high requirements for semiconductors under visible light. The electronic structures and optical properties of monolayer g-C₃N₄, S doped g-C₃N₄, Al doped g-C₃N₄, and S-Al doped g-C₃N₄ systems were investigated using plane-wave density functional theory with ultra-soft pseudopotentials. The results showed that the impurity atoms are most likely to be doped into g-C₃N₄ system at the position of S doped gap I and Al doped N2. Compared with the monola-yer g-C₃N₄, the doped systems have lattice distortion and redshift phenomenon, which expands the light absorption range of the system. It can be inferred that S, Al doped can improve the photocatalytic performance of the g-C₃N₄ system. The photocatalytic performance of the S-Al co-doped system is the best, because the molecular orbital of the co-doped system have strong delocalization, which is beneficial to improve the mobility of carriers. And it can make the deep energy level introduced by single doping shallow, and reduce the appearance of recombination center on the impurity energy level. Therefore, S-Al co-doped system can be used as an effective means to improve the photocatalytic activity of g-C₃N₄.

Key words: doped graphite phase carbon nitride electronic structure optical property first-principle

出版日期: 2023-05-10 发布日期: 2023-05-04

ZTFLH:

O643.36

基金资助: 新疆维吾尔自治区重点实验室开放课题(2021D04015);新疆维吾尔自治区高校科技计划项目(XJEDU2021Y044);伊犁师范大学博士启动基金(2021YSBS009);自治区研究生创新项目(XJ2021G323)

通讯作者: *张丽丽,于2020年获得南京大学博士学位,现为伊犁师范大学物理科学与技术学院副教授,主要从事玻璃化转变机制、金属氧化物电子结构的计算机模拟研究,已在Scientific Reports、International Journal of Modern Physics B、European Physical Journal E、Journal of Molecular Modeling、OPTIK等期刊上发表论文80余篇。suyi2046@sina.com
雷博程,2019年毕业于伊犁师范大学,获得理学硕士学位。现为伊犁师范大学物理科学与技术学院讲师,目前从事金属氧化物磁性及光催化性能领域的研究,发表论文10余篇。lbc0428@sina.com

作者简介: 刘晨曦,2019年6月毕业于伊犁师范大学,获得理学学士学位。现为伊犁师范大学物理科学与技术学院硕士研究生,在张丽丽副教授的指导下进行研究。目前主要从事氧化物半导体、二维材料及异质结光催化及磁性等领域的研究。

引用本文:

刘晨曦, 庞国旺, 潘多桥, 史蕾倩, 张丽丽, 雷博程, 赵旭才, 黄以能. S和Al掺杂单层g-C₃N₄电子结构与光学性质的第一性原理研究[J]. 材料导报, 2023, 37(9): 21100044-6.
LIU Chenxi, PANG Guowang, PAN Duoqiao, SHI Leiqian, ZHANG Lili, LEI Bocheng, ZHAO Xucai, HUANG Yineng. First-principles Study on Electronic Structure and Optical Properties of S and Al Doped Monolayer g-C₃N₄. Materials Reports, 2023, 37(9): 21100044-6.

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http://www.mater-rep.com/CN/10.11896/cldb.21100044 或 http://www.mater-rep.com/CN/Y2023/V37/I9/21100044

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