Boosting Conversion of the Si-O Bond by Introducing Fe in Carbon-Coated SiO for Superior Lithium Storage.

ACS Appl Mater Interfaces

Key Laboratory of Eco-Functional Polymer Materials of the Ministry of Education, College of Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou 730070, Gansu, China.

Published: July 2024

SiO-based anodes are of great promise for lithium-ion batteries due to their low working potential and high specific capacity. However, several issues involving large volume expansion during the lithiation process, low intrinsic conductivity, and unsatisfactory initial Coulombic efficiency (ICE) hinder their practical application. Here, an Fe-SiO@C composite with significantly improved lithium-storage performance was successfully synthesized by combining Fe modification with a carbon coating strategy. The results of both experiments and density functional theory calculations confirm that the Fe modification not only effectively achieves uniform carbon coating but also weakens the bonding energy of the Si-O bond and boosts reversible lithiation/delithiation reactions, resulting in great improvement in the electrical conductivity, ICE, and reversible specific capacity of the as-obtained Fe-SiO@C. Together with the coated carbon, the in situ-generated conductive Fe-based intermediates also ensure the electrical contact of active components, relieve the volume expansion, and maintain the structural integrity of the electrode during cycling. And the Fe-SiO@C ( ≈ 1.5) electrode can deliver a high-rate capacity of 354 mA h g at 2.0 A g and long-term cycling stability (552.4 mA h g at 0.5 A g even after 500 cycles). The findings here provide a facile modification strategy to improve the electrochemical lithium-storage performance of SiO-based anodes.

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Source
http://dx.doi.org/10.1021/acsami.4c08687DOI Listing

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