Synergy of Epoxy Chemical Tethers and Defect‐Free Graphene in Enabling Stable Lithium Cycling of Silicon Nanoparticles

Liu, Wei; Li, Hongju; Jin, Jialun; Wang, Yizhe; Zhang, Zheng; Chen, Zidong; Wang, Qin; Chen, Yungui; Paek, Eunsu; Mitlin, David

doi:10.1002/anie.201906612

Title: Synergy of Epoxy Chemical Tethers and Defect‐Free Graphene in Enabling Stable Lithium Cycling of Silicon Nanoparticles

Journal Article · 26 September 2019 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.201906612 · OSTI ID:1603182

^[1]; Li, Hongju ^[1]; Jin, Jialun ^[1]; Wang, Yizhe ^[1]; Zhang, Zheng ^[2]; Chen, Zidong ^[2]; Wang, Qin ^[2]; Chen, Yungui ^[1]; Paek, Eunsu ^[3];

^[4]

Institute of New-Energy and Low-Carbon Technology (INELT) Sichuan University Chengdu Sichuan 610065 China, Engineering Research Center of Alternative Energy Materials &, Devices Ministry of Education Sichuan University Chengdu Sichuan 610065 China
Institute of New-Energy and Low-Carbon Technology (INELT) Sichuan University Chengdu Sichuan 610065 China
Chemical &, Biomolecular Engineering Clarkson University Potsdam NY 13699 USA
Walker Department of Mechanical Engineering The University of Texas at Austin Austin Texas 78712-1591 USA

Abstract We report a new approach for nanosilicon–graphene hybrids with uniquely stable solid electrolyte interphase. Expanded graphite is gently exfoliated creating “defect‐free” graphene that is non‐catalytic towards electrolyte decomposition, simultaneously introducing high mass loading (48 wt. %) Si nanoparticles. Silane surface treatment creates epoxy chemical tethers, mechanically binding nano‐Si to CMC binder through epoxy ring‐opening reaction while stabilizing the Si surface chemistry. Epoxy‐tethered silicon pristine–graphene hybrid “E‐Si‐pG” exhibits state‐of‐the‐art performance in full battery opposing commercial mass loading (12 mg cm ⁻² ) LiCoO ₂ (LCO) cathode. At 0.4 C, with areal capacity of 1.62 mAh cm ⁻² and energy of 437 Wh kg ⁻¹ , achieving 1.32 mAh cm ⁻² , 340.4 Wh kg ⁻¹ at 1 C. After 150 cycles, it retains 1.25 mAh cm ⁻² , 306.5 Wh kg ⁻¹ . Sputter‐down XPS demonstrates survival of surface C‐Si‐O‐Si groups in E‐Si‐pG after repeated cycling. The discovered synergy between support defects, chemical‐mechanical stabilization of Si surfaces, and SEI‐related failure may become key LIB anode design rule.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0018074

OSTI ID:: 1603182

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 46 Vol. 58; ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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