Designing double-layered Si and Si/LATP nanocomposite anode for high-voltage aqueous lithium-ion batteries

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Designing double‑layered Si and Si/LATP nanocomposite anode for high‑voltage aqueous lithium‑ion batteries Anjali Paravannoor1 · Deepthi Panoth1 · Pattathil Praveen2 Received: 3 May 2020 / Accepted: 25 September 2020 © Springer Nature Switzerland AG 2020

Abstract A novel anode design is demonstrated with Si nanostructures with double-layered protection for an aqueous rechargeable Li-ion Battery (ARLIB). Si nanoparticle-embedded LATP (lithium aluminum titanium phosphate; ­Li1.3Al0.3Ti1.7(PO4)3), as well as LATP-PVDF polymer nanocomposites, is used as the protective layers. The unique anode structure is expected to be useful in overcoming the cathodic challenges and subsequent gas evolution reactions, thus widening the operating voltage of an ARLIB up to 3.5 V. The layered anodes exhibited discharge capacities of 2630 mAh ­g−1 at 0.1 C as half cells in 2 M ­Li2SO4 aqueous solution as the electrolyte. They are also coupled with ­LiFePO4 cathode, and the full cells demonstrate a discharge capacity of 123 mAh g ­ −1 with the calculated energy density values of 138 Wh k­ g−1 which is comparable with the conventional organic electrolyte-based LIBs. They can cycle 500 times with capacity retention of more than 75%. Hence, the conclusions from the present study project a promising anode design for ARLIBs, with high capacities and long cycling stabilities. Keywords  Li-ion battery · Aqueous electrolyte · Silicon anode · Layered anode · LATP

1 Introduction Li-ion batteries are one of the most widely accepted technologies of choice when it comes to energy storage devices, especially for portable electronic applications [1–3]. Researches try to explore various possibilities of anode and cathode materials and electrolyte formulations to enhance the durability and energy efficiency of the system [4, 5]. However, the technology is often questioned for its safety as there are incidents involving high-profile explosions and these concerns hinder their applications in large-scale purposes, especially in electric vehicles and hybrid electric vehicles as they require large-format LIBs (> 30 Ah) [6]. One of the major challenges associated with the safe scaling up of conventional LIBs is the highly

flammable organic electrolyte formulations that fuel the chemical combustion initiated by high energy electrode materials like Li metal which in turn would lead to thermal runaways [7, 8]. Since the energy density of the LIBs is not to be compromised, the obvious solution to address the associated disadvantages is to replace the highly inflammable organic electrolytes which project safety concerns also of their own [9]. One of the most suitable replacements for the carbonate ester-based conventional organic electrolytes is water which possesses additional advantages of its high values of dipole moment (1.8546 Debye), acceptor, and donor numbers (AN = 54.8, DN = 18) and dielectric constant (ε =  78 at 25 °C). The factor that hinders the use of aqueous electrolytes in LIBs is the low electrochemical stability

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