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Vol. 16 (2024)

Boosted Lithium-Ion Transport Kinetics in n-Type Siloxene Anodes Enabled by Selective Nucleophilic Substitution of Phosphorus

https://doi.org/10.1007/s40820-024-01428-y
Se In Kim
School of Civil, Environmental and Architectural Engineering, Korea University, 02841 Seoul, South Korea
Woong‑Ju Kim
School of Civil, Environmental and Architectural Engineering, Korea University, 02841 Seoul, South Korea
Jin Gu Kang
Nanophotonics Research Center, Korea Institute of Science and Technology, 02792 Seoul, South Korea
Dong‑Wan Kim
School of Civil, Environmental and Architectural Engineering, Korea University, 02841 Seoul, South Korea

Corresponding Author: Dong‑Wan Kim

dwkim1@korea.ac.kr

Nano-Micro Letters, Vol. 16 (2024), Article Number: 219

Abstract

Doped two-dimensional (2D) materials hold significant promise for advancing many technologies, such as microelectronics, optoelectronics, and energy storage. Herein, n-type 2D oxidized Si nanosheets, namely n-type siloxene (n-SX), are employed as Li-ion battery anodes. Via thermal evaporation of sodium hypophosphite at 275 °C, P atoms are effectively incorporated into siloxene (SX) without compromising its 2D layered morphology and unique Kautsky-type crystal structure. Further, selective nucleophilic substitution occurs, with only Si atoms being replaced by P atoms in the O3≡Si–H tetrahedra. The resulting n-SX possesses two delocalized electrons arising from the presence of two electron donor types: (i) P atoms residing in Si sites and (ii) H vacancies. The doping concentrations are varied by controlling the amount of precursors or their mean free paths. Even at 2000 mA g−1, the n-SX electrode with the optimized doping concentration (6.7 × 1019 atoms cm−3) delivers a capacity of 594 mAh g−1 with a 73% capacity retention after 500 cycles. These improvements originate from the enhanced kinetics of charge transport processes, including electronic conduction, charge transfer, and solid-state diffusion. The approach proposed herein offers an unprecedented route for engineering SX anodes to boost Li-ion storage.


Highlights:
1 Extrinsic doping is proposed as a novel route to enhance the intrinsic properties of the two-dimensional oxidized Si nanosheet (namely, siloxene) anode for Li-ion batteries.
2 Fabrication of P-doped n-type siloxene is revealed to be possible through selective nucleophilic substitution of Si atoms in siloxene with P atoms.
3 Due to boosted charge transport kinetics, n-type siloxene (6.7 × 1019 P atoms cm-3) exhibits the excellent storage performance (594 mAh g-1 after 500 cycles) even at 2000 mA g-1.

Keywords

Li-ion battery Two-dimensional N-type siloxene Doping mechanism Kinetics
Kim, Se In, Woong‑Ju Kim, Jin Gu Kang, and Dong‑Wan Kim. 2024. “Boosted Lithium-Ion Transport Kinetics in N-Type Siloxene Anodes Enabled by Selective Nucleophilic Substitution of Phosphorus”. Nano-Micro Letters 16 (June):219. https://doi.org/10.1007/s40820-024-01428-y.
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