Anchoring and Catalytic Performance of Co@C<sub>2</sub>N Monolayer for Rechargeable Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> Batteries: A First-Principles Calculations

Se<i><sub>x</sub></i>S<i><sub>y</sub></i> composite cathode materials, which offer superior theoretical capacity compared to pure selenium and improved electrochemical properties relative to pure sulfur, have aroused considerable interest in recent dec...

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Main Authors: Xiaojing Li, Yingbo Zhang, Chenchen Liu, Shuwei Tang
Format: Article
Language:English
Published: MDPI AG 2024-11-01
Series:Molecules
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Online Access:https://www.mdpi.com/1420-3049/29/22/5264
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author Xiaojing Li
Yingbo Zhang
Chenchen Liu
Shuwei Tang
author_facet Xiaojing Li
Yingbo Zhang
Chenchen Liu
Shuwei Tang
author_sort Xiaojing Li
collection DOAJ
description Se<i><sub>x</sub></i>S<i><sub>y</sub></i> composite cathode materials, which offer superior theoretical capacity compared to pure selenium and improved electrochemical properties relative to pure sulfur, have aroused considerable interest in recent decades on account of their applications in electric vehicles and energy storage grids. In the current work, the feasibility of a Co@C<sub>2</sub>N monolayer as a promising host candidate for the cathode material of Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> batteries has been evaluated using first-principles calculations, and particular efforts have been devoted to underscoring the anchoring mechanism and catalytic performance of the Co@C<sub>2</sub>N monolayer. The pronounced synergistic effects of Co-S and Li-N bonds lead to increased anchoring performance for Li<sub>2</sub>Se<i><sub>x</sub></i>S<i><sub>y</sub></i>/Se<i><sub>x</sub></i>S<i><sub>y</sub></i> clusters on the surface of Co@C<sub>2</sub>N monolayer, which effectively inhibit the shuttle effect. The charge density difference and Mulliken charge analysis underscores a substantial charge transfer from the Li<sub>2</sub>Se<i><sub>x</sub></i>S<i><sub>y</sub></i> and Se<i><sub>x</sub></i>S<i><sub>y</sub></i> clusters to the Co@C<sub>2</sub>N monolayer, which indicates a noticeable chemical interaction between them. Further electronic property calculations show that the Co@C<sub>2</sub>N monolayer can improve the electrical conductivity of cathode materials for Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> batteries by maintaining semi-metallic characteristics after anchoring of Li<sub>2</sub>Se<i><sub>x</sub></i>S<i><sub>y</sub></i>/Se<i><sub>x</sub></i>S<i><sub>y</sub></i> clusters. Additionally, the catalytic performance of the Co@C<sub>2</sub>N monolayer is evaluated in terms of the reduction pathway of Se<sub>8</sub> and the decomposition energy barrier of the Li<sub>2</sub>SeS cluster, which highlights the catalytic role of the Co@C<sub>2</sub>N monolayer in the formation and decomposition of the Li<sub>2</sub>SeS cluster during the cycle processes. Overall, the Co@C<sub>2</sub>N monolayer emerges as a promising host material and catalyst for Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> batteries with remarkable anchoring and catalytic performance.
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spelling doaj-art-ba7eb580d5b641ebb19afb99bc5e6ef92025-08-20T02:04:55ZengMDPI AGMolecules1420-30492024-11-012922526410.3390/molecules29225264Anchoring and Catalytic Performance of Co@C<sub>2</sub>N Monolayer for Rechargeable Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> Batteries: A First-Principles CalculationsXiaojing Li0Yingbo Zhang1Chenchen Liu2Shuwei Tang3Department of Automotive Engineering, Hebei Petroleum University of Technology, Chengde 067000, ChinaDepartment of Automotive Engineering, Hebei Petroleum University of Technology, Chengde 067000, ChinaCollege of Materials Science and Engineering, Liaoning Technical University, Fuxin 123000, ChinaCollege of Materials Science and Engineering, Liaoning Technical University, Fuxin 123000, ChinaSe<i><sub>x</sub></i>S<i><sub>y</sub></i> composite cathode materials, which offer superior theoretical capacity compared to pure selenium and improved electrochemical properties relative to pure sulfur, have aroused considerable interest in recent decades on account of their applications in electric vehicles and energy storage grids. In the current work, the feasibility of a Co@C<sub>2</sub>N monolayer as a promising host candidate for the cathode material of Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> batteries has been evaluated using first-principles calculations, and particular efforts have been devoted to underscoring the anchoring mechanism and catalytic performance of the Co@C<sub>2</sub>N monolayer. The pronounced synergistic effects of Co-S and Li-N bonds lead to increased anchoring performance for Li<sub>2</sub>Se<i><sub>x</sub></i>S<i><sub>y</sub></i>/Se<i><sub>x</sub></i>S<i><sub>y</sub></i> clusters on the surface of Co@C<sub>2</sub>N monolayer, which effectively inhibit the shuttle effect. The charge density difference and Mulliken charge analysis underscores a substantial charge transfer from the Li<sub>2</sub>Se<i><sub>x</sub></i>S<i><sub>y</sub></i> and Se<i><sub>x</sub></i>S<i><sub>y</sub></i> clusters to the Co@C<sub>2</sub>N monolayer, which indicates a noticeable chemical interaction between them. Further electronic property calculations show that the Co@C<sub>2</sub>N monolayer can improve the electrical conductivity of cathode materials for Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> batteries by maintaining semi-metallic characteristics after anchoring of Li<sub>2</sub>Se<i><sub>x</sub></i>S<i><sub>y</sub></i>/Se<i><sub>x</sub></i>S<i><sub>y</sub></i> clusters. Additionally, the catalytic performance of the Co@C<sub>2</sub>N monolayer is evaluated in terms of the reduction pathway of Se<sub>8</sub> and the decomposition energy barrier of the Li<sub>2</sub>SeS cluster, which highlights the catalytic role of the Co@C<sub>2</sub>N monolayer in the formation and decomposition of the Li<sub>2</sub>SeS cluster during the cycle processes. Overall, the Co@C<sub>2</sub>N monolayer emerges as a promising host material and catalyst for Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> batteries with remarkable anchoring and catalytic performance.https://www.mdpi.com/1420-3049/29/22/5264Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> batteriesCo@C<sub>2</sub>N monolayershuttle effectLi<sub>2</sub>Se<i><sub>x</sub></i>S<i><sub>y</sub></i>/Se<i><sub>x</sub></i>S<i><sub>y</sub></i>first-principles calculations
spellingShingle Xiaojing Li
Yingbo Zhang
Chenchen Liu
Shuwei Tang
Anchoring and Catalytic Performance of Co@C<sub>2</sub>N Monolayer for Rechargeable Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> Batteries: A First-Principles Calculations
Molecules
Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> batteries
Co@C<sub>2</sub>N monolayer
shuttle effect
Li<sub>2</sub>Se<i><sub>x</sub></i>S<i><sub>y</sub></i>/Se<i><sub>x</sub></i>S<i><sub>y</sub></i>
first-principles calculations
title Anchoring and Catalytic Performance of Co@C<sub>2</sub>N Monolayer for Rechargeable Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> Batteries: A First-Principles Calculations
title_full Anchoring and Catalytic Performance of Co@C<sub>2</sub>N Monolayer for Rechargeable Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> Batteries: A First-Principles Calculations
title_fullStr Anchoring and Catalytic Performance of Co@C<sub>2</sub>N Monolayer for Rechargeable Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> Batteries: A First-Principles Calculations
title_full_unstemmed Anchoring and Catalytic Performance of Co@C<sub>2</sub>N Monolayer for Rechargeable Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> Batteries: A First-Principles Calculations
title_short Anchoring and Catalytic Performance of Co@C<sub>2</sub>N Monolayer for Rechargeable Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> Batteries: A First-Principles Calculations
title_sort anchoring and catalytic performance of co c sub 2 sub n monolayer for rechargeable li se i sub x sub i s i sub y sub i batteries a first principles calculations
topic Li-Se<i><sub>x</sub></i>S<i><sub>y</sub></i> batteries
Co@C<sub>2</sub>N monolayer
shuttle effect
Li<sub>2</sub>Se<i><sub>x</sub></i>S<i><sub>y</sub></i>/Se<i><sub>x</sub></i>S<i><sub>y</sub></i>
first-principles calculations
url https://www.mdpi.com/1420-3049/29/22/5264
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