Surface Properties of Battery Materials Elucidated Using Scanning Electrochemical Microscopy: The Case of Type I Silicon Clathrate

Tsvetan Tarnev; Patrick Wilde; Andrew Dopilka; Wolfgang Schuhmann; Candace K. Chan; Edgar Ventosa

doi:10.1002/celc.201901688

Surface Properties of Battery Materials Elucidated Using Scanning Electrochemical Microscopy: The Case of Type I Silicon Clathrate

Tsvetan Tarnev, Patrick Wilde, Andrew Dopilka, Wolfgang Schuhmann, Candace K. Chan, Edgar Ventosa

Engineering, Ira A. Fulton Schools of (IAFSE)

Research output: Contribution to journal › Article › peer-review

16 Scopus citations

Abstract

Silicon clathrates have attracted interest as potential anodes for lithium-ion batteries with unique framework structures. However, very little is known about the surface reactivity and solid electrolyte interphase (SEI) properties of clathrates. In this study, operando scanning electrochemical microscopy (SECM) is used to investigate the effect of pre-treatment on the formation dynamics and intrinsic properties of the SEI in electrodes prepared from type I Ba₈Al₁₆Si₃₀ silicon clathrates. Although X-ray photoelectron spectroscopy (XPS) analysis does not reveal large changes in SEI composition, it is found through SECM measurements that ball-milling combined with chemical acid/base etching of the clathrates lead to a more stable and rapidly formed SEI as compared to purely ball-milled samples, resulting in enhanced coulombic efficiency.

Original language	English (US)
Pages (from-to)	665-671
Number of pages	7
Journal	ChemElectroChem
Volume	7
Issue number	3
DOIs	https://doi.org/10.1002/celc.201901688
State	Published - Feb 3 2020

Keywords

battery material
lithium-ion batteries
operando SECM
silicon clathrate
solid electrolyte interphase

ASJC Scopus subject areas

Catalysis
Electrochemistry

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10.1002/celc.201901688

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title = "Surface Properties of Battery Materials Elucidated Using Scanning Electrochemical Microscopy: The Case of Type I Silicon Clathrate",

abstract = "Silicon clathrates have attracted interest as potential anodes for lithium-ion batteries with unique framework structures. However, very little is known about the surface reactivity and solid electrolyte interphase (SEI) properties of clathrates. In this study, operando scanning electrochemical microscopy (SECM) is used to investigate the effect of pre-treatment on the formation dynamics and intrinsic properties of the SEI in electrodes prepared from type I Ba8Al16Si30 silicon clathrates. Although X-ray photoelectron spectroscopy (XPS) analysis does not reveal large changes in SEI composition, it is found through SECM measurements that ball-milling combined with chemical acid/base etching of the clathrates lead to a more stable and rapidly formed SEI as compared to purely ball-milled samples, resulting in enhanced coulombic efficiency.",

keywords = "battery material, lithium-ion batteries, operando SECM, silicon clathrate, solid electrolyte interphase",

author = "Tsvetan Tarnev and Patrick Wilde and Andrew Dopilka and Wolfgang Schuhmann and Chan, {Candace K.} and Edgar Ventosa",

note = "Funding Information: P.W. is grateful to the Association of the Chemical Industry e.V. (VCI) for funding of his Ph.D fellowship. A.D. and C.K.C. acknowledge support from the U.S. National Science Foundation under awards DMR-1206795 and DMR-1710017, an ASU Fulton Schools of Engineering Dean's Fellowship, and Alexander von Humboldt Foundation Research Fellowship. W.S. is grateful to the Deutsche Forschungsgemeinschaft (DFG) under Germany's Excellence Strategy (EXC-2033 – 390677874) for financial support. The authors also acknowledge the use of characterization equipment within the Eyring Materials Center at ASU. The authors thank R. Zhao and S. Bobev for assistance with synthesizing the clathrate materials. Publisher Copyright: {\textcopyright} 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim",

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AU - Wilde, Patrick

AU - Dopilka, Andrew

AU - Schuhmann, Wolfgang

AU - Chan, Candace K.

AU - Ventosa, Edgar

N1 - Funding Information: P.W. is grateful to the Association of the Chemical Industry e.V. (VCI) for funding of his Ph.D fellowship. A.D. and C.K.C. acknowledge support from the U.S. National Science Foundation under awards DMR-1206795 and DMR-1710017, an ASU Fulton Schools of Engineering Dean's Fellowship, and Alexander von Humboldt Foundation Research Fellowship. W.S. is grateful to the Deutsche Forschungsgemeinschaft (DFG) under Germany's Excellence Strategy (EXC-2033 – 390677874) for financial support. The authors also acknowledge the use of characterization equipment within the Eyring Materials Center at ASU. The authors thank R. Zhao and S. Bobev for assistance with synthesizing the clathrate materials. Publisher Copyright: © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

PY - 2020/2/3

Y1 - 2020/2/3

N2 - Silicon clathrates have attracted interest as potential anodes for lithium-ion batteries with unique framework structures. However, very little is known about the surface reactivity and solid electrolyte interphase (SEI) properties of clathrates. In this study, operando scanning electrochemical microscopy (SECM) is used to investigate the effect of pre-treatment on the formation dynamics and intrinsic properties of the SEI in electrodes prepared from type I Ba8Al16Si30 silicon clathrates. Although X-ray photoelectron spectroscopy (XPS) analysis does not reveal large changes in SEI composition, it is found through SECM measurements that ball-milling combined with chemical acid/base etching of the clathrates lead to a more stable and rapidly formed SEI as compared to purely ball-milled samples, resulting in enhanced coulombic efficiency.

AB - Silicon clathrates have attracted interest as potential anodes for lithium-ion batteries with unique framework structures. However, very little is known about the surface reactivity and solid electrolyte interphase (SEI) properties of clathrates. In this study, operando scanning electrochemical microscopy (SECM) is used to investigate the effect of pre-treatment on the formation dynamics and intrinsic properties of the SEI in electrodes prepared from type I Ba8Al16Si30 silicon clathrates. Although X-ray photoelectron spectroscopy (XPS) analysis does not reveal large changes in SEI composition, it is found through SECM measurements that ball-milling combined with chemical acid/base etching of the clathrates lead to a more stable and rapidly formed SEI as compared to purely ball-milled samples, resulting in enhanced coulombic efficiency.

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Surface Properties of Battery Materials Elucidated Using Scanning Electrochemical Microscopy: The Case of Type I Silicon Clathrate

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