Low-Oxidized Siloxene Nanosheets with High Capacity, Capacity Retention, and Rate Capability in Lithium-Based Batteries

Arnot, David J.; Li, Wenzao; Bock, David C.; Stackhouse, Chavis A.; Tong, Xiao; Head, Ashley R.; Takeuchi, Esther S.; Takeuchi, Kenneth J.; Yan, Shan; Wang, Lei; Marschilok, Amy C.

doi:10.1002/admi.202102238

Title: Low-Oxidized Siloxene Nanosheets with High Capacity, Capacity Retention, and Rate Capability in Lithium-Based Batteries

Journal Article · 23 March 2022 · Advanced Materials Interfaces

DOI: https://doi.org/10.1002/admi.202102238 · OSTI ID:1896877

Arnot, David J. ^[1]; Li, Wenzao ^[1]; Bock, David C. ^[2]; Stackhouse, Chavis A. ^[2]; Tong, Xiao ^[3]; Head, Ashley R. ^[3];

^[2];

^[2]; Yan, Shan ^[1]; Wang, Lei ^[2];

^[2]

Stony Brook Univ., NY (United States)
Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Abstract The mechanical degradation experienced by Si electrodes during Li (de)alloying reactions can potentially be mitigated by using Si‐based materials with layered 2D geometries. Such materials are expected to exhibit favorable mechanical properties and be capable of buffering the volume change associated with (de)lithitation. In this work, 2D siloxene nanosheets are synthesized using a facile topotactic reaction followed by ultrasonication as an exfoliation step. Detailed structural and chemical characterization via electron microscopy, X‐ray photoelectron spectroscopy (XPS), and Raman spectroscopy is conducted, revealing a low‐oxidized siloxene nanosheet material with only 15% surface Si‐oxide. The obtained siloxene nanosheets are tested as Li‐ion negative electrodes in lithium‐based electrochemical cells. The cells exhibit high rate capability with a capacity of 935 mAh g ^–1 at 3200 mA g ^–1 and ≈99.5% coulombic efficiency. The inclusion of fluoroethylene carbonate (FEC) in the electrolyte improves capacity retention over 200 cycles from 13% to 77% at 1000 mA g ^–1 . This behavior is attributed to the FEC decomposition forming a solid electrolyte interphase (SEI) with higher ion conductivity and robust LiF/Li _x PO _y F _z content, as characterized via XPS Raman spectroscopy.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2M)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE

Grant/Contract Number:: SC0012704; EE0009184; SC0012673

OSTI ID:: 1896877

Alternate ID(s):: OSTI ID: 1856443

Report Number(s):: BNL-223662-2022-JAAM

Journal Information:: Advanced Materials Interfaces, Vol. 9, Issue 17; ISSN 2196-7350

Publisher:: Wiley-VCHCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Low-Oxidized Siloxene Nanosheets with High Capacity, Capacity Retention, and Rate Capability in Lithium-Based Batteries

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