Comparison of electrochemical characteristics of thin-film batteries with a composite anode Si@O@Al and lithium metal formed by in situ method

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This study compares the electrochemical characteristics of solid-state thin-film lithium-ion batteries with two different structures: Ti/Anode/LiPON/LiCoO2/Ti (with an anode) and Ti/LiPON/LiCoO2/Ti (anode-free). Si@O@Al composite anode with thicknesses of 154 and 15 nm, as well as pre-lithiated LixSi@O@Al composite with a thickness of 192 nm, were used as anodes. In anode-free batteries, the lithium anode was formed by the in situ method. Batteries with 154 nm Si@O@Al and LixSi@O@Al anodes have good cyclability due to their moderate volume change during lithium-ion insertion/extraction and reliable adhesion to the LiPON solid electrolyte. These batteries are promising in terms of high energy density due to the lithium anode formation in situ, although they have poor cycling performance due to peeling off the upper current collector. The introducing of a Si@O@Al thin film with a thickness of ~15 nm between the LiPON and the current collector allows maintaining the high energy density that is inherent in batteries with lithium anodes, while also improving their cyclability.

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作者简介

S. Kurbatov

RUDN University

编辑信件的主要联系方式.
Email: kurbatov-93@bk.ru
俄罗斯联邦, 6 Miklukho-Maklaya St, Moscow, 117198

L. Mazaletsky

P.G. Demidov Yaroslavl State University

Email: kurbatov-93@bk.ru
俄罗斯联邦, 14 Sovetskaya str., Yaroslavl, 150003

A. Mironenko

P.G. Demidov Yaroslavl State University

Email: kurbatov-93@bk.ru
俄罗斯联邦, 14 Sovetskaya str., Yaroslavl, 150003

V. Naumov

P.G. Demidov Yaroslavl State University

Email: kurbatov-93@bk.ru
俄罗斯联邦, 14 Sovetskaya str., Yaroslavl, 150003

A. Rudy

P.G. Demidov Yaroslavl State University

Email: rudy@uniyar.ac.ru
俄罗斯联邦, 14 Sovetskaya str., Yaroslavl, 150003

A. Skundin

A.N. Frumkin Institute of Physical Chemistry and Electrochemistry of RAS

Email: kurbatov-93@bk.ru
俄罗斯联邦, Moscow

D. Pukhov

Valiev Institute of Physics and Technology of Russian Academy of Sciences

Email: kurbatov-93@bk.ru

Yaroslavl branch

俄罗斯联邦, Yaroslavl

M. Smirnova

P.G. Demidov Yaroslavl State University

Email: kurbatov-93@bk.ru
俄罗斯联邦, 14 Sovetskaya str., Yaroslavl, 150003

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2. Fig. 1. (a) – substrate with batteries after applying LiPON, (b) – mask for applying the anode layer with an additional screen, (c) – substrate after applying the anode layer (in this case Si@O@Al).

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3. Fig. 2. SEM images of a transverse cleavage of TTLIA: (a) – with a 154 nm thick Si@O@Al anode, (b) – a sample with a 15 nm thick Si@O@Al anode, (c) – with a lithiated LixSi@O@Al anode and (d) – “anodeless” sample.

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4. Fig. 3. Raman spectrum of the LCO cathode layer deposited on a substrate with a Ti(200 nm)/SiO2 (900 nm)/Si structure.

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5. Fig. 4. Comparison of discharge curves of anodic and “anodeless” TTLIA. Designations in the figure: 1 – Si@O@Al (154 nm)/LiPON (500 nm)/LCO (490 nm), 2 – Si@O@Al (15 nm)/LiPON (518 nm)/LCO (474 ​​nm), 3 – LixSi@O@Al (192 nm)/LiPON (513 nm)/LCO (672 nm) and 4 – “anodeless” TTLIA with the structure (in situ Li)/LiPON(571 nm)/LCO(733 nm). The current density is 32 μA/cm2, the potential window is 1.5 V – 3.8 for TTLIA with Si@O@Al-154 nm and LixSi@O@Al anodes, 3.0 – 4.0 V for “anodeless” and Si@O@Al-15 nm.

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6. Fig. 5. CVA of TTLIA samples with different anodes. The numbering in the figure corresponds to the samples with anodes: 1 – Si@O@Al-154 nm, 2 – Si@O@Al-15 nm, 3 – LixSi@O@Al and 4 – “anodeless”. The potential scan rate is 0.5 mV/s, the cycling limits are 1.5 V-4.2 for TTLIA with Si@O@Al-154, Si@O@Al-15 nm anodes and the “anodeless” sample, 1.0-4.1 V for the LixSi@O@Al sample.

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7. Fig. 6. Dependence of the discharge capacity on the cycle number. The numbering in the figure corresponds to the samples with anodes: 1 – Si@O@Al-154 nm, 2 – Si@O@Al-15 nm, 3 – LixSi@O@Al and 4 – “anodeless”. The charge-discharge current density is 32 μA/cm2. For the samples with the Si@O@Al-154 nm and LixSi@O@Al anodes, a potential window of 1.5 – 3.8 V was used, for the “anodeless” sample and with the thin Si@O@Al-15 nm anode – a window of 3.0 – 4.0 V.

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8. Fig. 7. SEM images of the transverse cleavage of the “anodeless” TTLIA after cycling.

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