1D/2D C3N4/Graphene Composite as a Preferred Anode Material for Lithium Ion Batteries: Importance of Heterostructure Design via DFT Computation
1D/2D C3N4/Graphene Composite as a Preferred Anode Material for Lithium Ion Batteries: Importance of Heterostructure Design via DFT Computation
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DOI：
10.1021/acsami.0c04900
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发表时间：
2020-06-10
影响因子：
9.5
通讯作者：
Hankel, Marlies
中科院分区：
文献类型：
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作者：
Adekoya, David;Zhang, Shanqing;Hankel, Marlies
石墨烯通常通过形成石墨烯基异质结构来改善可充电电池中电极材料的电化学性能。二维石墨氮化碳（C3N4）是石墨烯的类似物，通常用于形成1D/2D和2D/2D C3N4/石墨烯异质结构。然而，缺乏对这些异质结构中的异质界面及其如何影响其电化学性能的理论理解。在这项工作中，我们研究了 1D/2D 和 2D/2D C3N4/石墨烯异质结构的异质界面以及不同尺寸如何影响异质结构的锂离子电池性能。我们的密度泛函理论（DFT）研究表明，2D/2D C3N4/石墨烯异质结构中常见的C-N键断裂问题不会出现在1D/2D异质结构中。此外，与 C3N4/石墨烯的 2D/2D 异质结构相比，1D/2D 异质结构表现出优异的电导率。 1D/2D C3N4/石墨烯异质结构还具有高理论容量和快速电荷转移。这些结果表明异质结构的性能受到界面处材料尺寸的影响。这些关于异质结构电极材料尺寸与其电化学性能之间关系的发现将推动可充电电池先进电极材料的设计。
Graphene is commonly used to improve the electrochemical performance of electrode materials in rechargeable batteries by forming graphene-based heterostructures. Two-dimensional graphitic carbon nitride (C3N4) is an analogue of graphene, and it is often used to form 1D/2D and 2D/2D C3N4/graphene heterostructures. However, a theoretical understanding of the heterointerface in these heterostructures and how this affects their electrochemical performance is lacking. In this work we study the heterointerface of 1D/2D and 2D/2D C3N4/graphene heterostructures and how the different dimensions influence the lithium ion battery performance of the heterostructure. Our density functional theory (DFT) study showed that the common problem of C-N bond breakage experienced in 2D/2D C3N4/graphene heterostructure does not occur in the 1D/2D heterostructure. Furthermore, the 1D/2D heterostructure showed superior conductivity in comparison to that of the 2D/2D heterostructure of C3N4/graphene. The 1D/2D C3N4/graphene heterostructure also recorded a high theoretical capacity and rapid charge transfer. These results suggest that the properties of a heterostructure are influenced by the dimension of materials at the interface. These discoveries on the relationship between material dimension in heterostructure electrodes and their electrochemical performance will motivate the design of advanced electrode materials for rechargeable batteries.