Citation: Zhang Rui, Jian Wei, Yang Zhao-Di, Bai Fu-Quan. Insights into the photocatalytic mechanism of the C₄N/MoS₂ heterostructure: A first-principle study[J]. Chinese Chemical Letters, ;2020, 31(9): 2319-2324. doi: 10.1016/j.cclet.2020.04.055 shu

Insights into the photocatalytic mechanism of the C₄N/MoS₂ heterostructure: A first-principle study

Zhang Rui ^a ,
Jian Wei ^b ,
Yang Zhao-Di ^a,*, ,
Bai Fu-Quan ^b,c,*,

a.
College of Chemical and Environmental Engineering, Harbin University of Science and Technology, Harbin 150080, China
b.
Laboratory of Theoretical and Computational Chemistry, Institute of Theoretical Chemistry and College of Chemistry, Jilin University, Changchun 130023, China
c.
Beijing National Laboratory for Molecular Sciences(BNLMS), Beijing 100190, China

^**

yangzhaodi@163.com

baifq@jlu.edu.cn

Received Date: 26 March 2020
Revised Date: 25 April 2020
Accepted Date: 28 April 2020
Available Online: 4 May 2020

Figures(4)

Constructing heterostructures by combining COFs and TMD is a new strategy to design efficient photocatalysts for CO₂ reduction reaction (CO₂RR) due to their good stability, tunable band gaps and efficient charge separation. Based on the synthesis of completely novel C₄N-COF in our previous reported work, a new C₄N/MoS₂ heterostructure was constructed and then the related structural, electronic and optical properties were also studied using first principle calculations. The interlayer coupling effect and charge transfer between the C₄N and MoS₂ layer are systematically illuminated. The reduced band gap of the C₄N/MoS₂ heterostructure is beneficial to absorb more visible light. For the formation of type-Ⅱ band alignment, a built-in electric field appears which separates the photogenerated electrons and holes into different layers efficiently and produces redox active sites. The band alignment of the heterostructure ensures its photocatalytic activities of the whole CO₂ reduction reaction. Furthermore, the charge density difference and charge carrier mobility confirm the existence of the built-in electric field at the interface of the C₄N/MoS₂ heterostructure directly. Finally, the high optical absorption indicates it is an efficient visible light harvesting photocatalyst. Therefore, this work could provide strong insights into the internal mechanism and high photocatalytic activity of the C₄N/MoS₂ heterostructure and offer guiding of designing and synthesizing COF/TMD heterostructure photocatalysts.
- First-principles calculations,
- C₄N/MoS₂ heterostructure,
- Electronic structure,
- Built-in electric field,
- Charge separation,
- Photocatalyst
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Insights into the photocatalytic mechanism of the C₄N/MoS₂ heterostructure: A first-principle study