Rui Yang, Xiao-Huan Lv, Ke-Xin Hou, Xing-Qiang Shi, Jiang-Long Wang
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引用次数: 0
Abstract
The graphene/MoS2 heterostructures (Gr/MoS2) exhibit excellent performance for ion batteries, such as superior stability and cyclicity for ion battery storage, and have great potentials for other applications. Lithium (Li) adsorption on/in Gr/MoS2 heterostructures exhibits advanced properties and interesting phenomena, as well as the phase engineering of MoS2. However, unified understanding for the different adsorption behaviors remains lacking, although fully understanding to the adsorption behaviors is of vital importance for their applications. In the current work, the Li adsorptions on the Gr surface of Gr/dT(H)-MoS2 heterostructures are systematically analyzed based on density functional theory calculations, and highlight the differences between Gr/H-MoS2 and Gr/dT-MoS2 for Li adsorption. To fully understand the adsorption behaviors, we perform detailed analyses from four interrelated aspects: 1) Electrostatic interactions from detailed Bader charge analysis, 2) charge density difference Δρ(z), 3) energy-level alignment between Li and the band edges of Gr, dT-, and H-MoS2, and 4) the resulted interface dipoles. We find that partial electrons in Li can pass through Gr to H-MoS2 and the origin is attributed to the weak electronic-shielding of Gr (even weaker than H-MoS2). All of the above extended analysis not only enables us to understand the abnormal adsorption of Li on the Gr surface of Gr/dT(H)-MoS2 heterostructures, but also helps guide the selection of ion battery materials. Moreover, we extend the discussion of Li adsorption to other alkali metal atoms with smaller work functions (such as: Na and K). Our work not only provides understanding to the abnormal adsorption of Li on the Gr surface of Gr/dT(H)-MoS2 heterostructures, but also helps guide the selection of ion battery materials. So, the insights from this study are important for their related applications. This paper reveals and explains an interesting abnormal adsorption phenomenon of lithium on van der Waals heterostructures of graphene and different phases of MoS2.The conclusion and insights from this work is not limited to Li (applicable at least to Na and K, also), and hence our work is helpful for establishing the surface-adsorption mechanisms of ion batteries.
期刊介绍:
Surface Science is devoted to elucidating the fundamental aspects of chemistry and physics occurring at a wide range of surfaces and interfaces and to disseminating this knowledge fast. The journal welcomes a broad spectrum of topics, including but not limited to:
• model systems (e.g. in Ultra High Vacuum) under well-controlled reactive conditions
• nanoscale science and engineering, including manipulation of matter at the atomic/molecular scale and assembly phenomena
• reactivity of surfaces as related to various applied areas including heterogeneous catalysis, chemistry at electrified interfaces, and semiconductors functionalization
• phenomena at interfaces relevant to energy storage and conversion, and fuels production and utilization
• surface reactivity for environmental protection and pollution remediation
• interactions at surfaces of soft matter, including polymers and biomaterials.
Both experimental and theoretical work, including modeling, is within the scope of the journal. Work published in Surface Science reaches a wide readership, from chemistry and physics to biology and materials science and engineering, providing an excellent forum for cross-fertilization of ideas and broad dissemination of scientific discoveries.