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Thermodynamic Insights into Polymorphism-Driven Lithium-Ion Storage in Monoelemental 2D Materials

Kabiraj, A and Bhattacharyya, AJ and Mahapatra, S (2021) Thermodynamic Insights into Polymorphism-Driven Lithium-Ion Storage in Monoelemental 2D Materials. In: Journal of Physical Chemistry Letters, 12 (4). pp. 1220-1227.

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Official URL: https://dx.doi.org/10.1021/acs.jpclett.0c03642


Monoelemental two-dimensional materials (borophene, silicene, etc.) are exciting candidates for electrodes in lithium-ion batteries because of their ultralight molar mass. However, these materials' lithium-ion binding mechanism can be complex as the inherited polymorphism may induce phase changes during the charge-discharge cycles. Here, we combine genetic-algorithm-based bottom-up and stochastic top-down structure searching techniques to conduct thermodynamic scrutiny of the lithiated compounds of 2D allotropes of four elements: B, Al, Si, and P. Our first-principles-based high-throughput computations unveil polymorphism-driven lithium-ion binding process and other nonidealities (e.g., bond cleavage, adsorbent phase change, and electroplating), which lacks mention in earlier works. While monolayer B (2479 mAh/g), Al (993 mAh/g), and Si (954 mAh/g) have been demonstrated here as excellent candidates for Li-ion storage, P falls short of the expectation. Our well-designed computational framework, which always searches for lithiated structures at global minima, provides convincing thermodynamical insights and realistic reversible specific-capacity values. This will expectedly open up future experimental efforts to design monoelemental two-dimensional material-based anodes with specific polymorphic structures. © 2021 American Chemical Society.

Item Type: Journal Article
Publication: Journal of Physical Chemistry Letters
Publisher: American Chemical Society
Additional Information: The copyright of this article belongs to American Chemical Society
Keywords: Aluminum alloys; Electrodes; Genetic algorithms; Ions; Monolayers; Polymorphism; Silicon; Stochastic systems, Charge-discharge cycle; Computational framework; First principles; Lithium ion storages; Polymorphic structure; Reversible specific capacity; Searching techniques; Two-dimensional materials, Lithium-ion batteries
Department/Centre: Division of Chemical Sciences > Solid State & Structural Chemistry Unit
Division of Electrical Sciences > Electronic Systems Engineering (Formerly Centre for Electronic Design & Technology)
Date Deposited: 05 Mar 2021 08:53
Last Modified: 05 Mar 2021 08:53
URI: http://eprints.iisc.ac.in/id/eprint/68114

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