Flash Heat Treatment Constructing Organic-Inorganic Hybrid Layer for High-Performance Silicon Anode

Haoyu Hu; Tonghui Cai; Junbin Wang; Jixian Cao; Wei Xing

doi:10.54097/rhymn859

Authors

Haoyu Hu
Tonghui Cai
Junbin Wang
Jixian Cao
Wei Xing

DOI:

https://doi.org/10.54097/rhymn859

Keywords:

Lithium-ion batteries, silicon anode, organic-inorganic hybrid layer.

Abstract

The commercialization of silicon (Si) anodes has long faced critical challenges of severe volume expansion and poor conductivity. While traditional surface coating strategies can mitigate these issues, rigid carbon coatings exhibit poor stress tolerance, and flexible organic polymers with polymer networks lack sufficient electron/ion conductivity. This study developed a novel flash heat treatment strategy. By subjecting polypyrrole (PPy)-coated nano-silicon (nmSi) to short-duration high-temperature treatment, we achieved partial carbonization of the PPy shell, resulting in a core-shell silicon material (nmSi@PCHS) featuring a unique organic polymer/inorganic carbon (PPy/C) hybrid layer. After optimizing treatment time, nmSi@PCHS-5 demonstrated optimal electrochemical performance: exceptional long-term cycling stability (1000 mAh/g after 500 cycles) and superior rate capability (1200 mAh/g at 5 A/g). The performance enhancement stems from the synergistic effect of the C/PPy hybrid shell: the carbon component significantly improves electrical conductivity and lithium-ion transport, while the retained PPy network provides inherent elasticity and toughness, effectively buffering silicon volume changes and maintaining structural integrity during cycling. This work demonstrates that flash heat treatment can create multifunctional hybrid interfacial layers that effectively optimize conductivity and mechanical resilience in synergy, offering unique insights for developing high-performance silicon-based anodes.

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References

[1] Yu Z, Rudnicki P E, Zhang Z, et al. Rational solvent molecule tuning for high-performance lithium metal battery electrolytes[J]. Nature Energy, 2022, 7(1): 94-106.

[2] Xue W, Huang M, Li Y, et al. Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte[J]. Nature Energy, 2021, 6(5): 495-505.

[3] Choi J W, Aurbach D. Promise and reality of post-lithium-ion batteries with high energy densities[J]. Nature Reviews Materials, 2016, 1(4): 16013.

[4] Rahman M A, Song G, Bhatt A I, et al. Nanostructured Silicon Anodes for High‐Performance Lithium‐Ion Batteries[J]. Advanced Functional Materials, 2015, 26(5): 647-678.

[5] Yu R, Pan Y, Jiang Y, et al. Regulating Lithium Transfer Pathway to Avoid Capacity Fading of Nano Si Through Sub‐Nano Scale Interfused SiOx/C Coating[J]. Advanced Materials, 2023, 35(49).

[6] He Y, Jiang L, Chen T, et al. Progressive growth of the solid–electrolyte interphase towards the Si anode interior causes capacity fading[J]. Nature Nanotechnology, 2021, 16(10): 1113-1120.

[7] Liu D, Cao G. Engineering nanostructured electrodes and fabrication of film electrodes for efficient lithium-ion intercalation[J]. Energy & Environmental Science, 2010, 3(9).

[8] Tan D H S, Chen Y-T, Yang H, et al. Carbon-free high-loading silicon anodes enabled by sulfide solid electrolytes[J]. Science, 2021, 373(6562): 1494-1499.

[9] Wang F, Chen G, Zhang N, et al. Engineering of carbon and other protective coating layers for stabilizing silicon anode materials[J]. Carbon Energy, 2019, 1(2): 219-245.

[10] Li H, Wan Z, Wu T, et al. Modified polyacrylonitrile cross-linked with carboxymethyl cellulose constructing a hydrogen bonding network for high-performance silicon anodes[J]. Inorganic Chemistry Frontiers, 2023, 10(23): 7073-7081.

[11] Wang W, Wang Y, Huang W, et al. In Situ Developed Si@Polymethyl Methacrylate Capsule as a Li-Ion Battery Anode with High-Rate and Long Cycle-Life[J]. ACS Applied Materials & Interfaces, 2021, 13(5): 6919-6929.

[12] Schnabel M, Harvey S P, Arca E, et al. Surface SiO2 Thickness Controls Uniform-to-Localized Transition in Lithiation of Silicon Anodes for Lithium-Ion Batteries[J]. ACS Applied Materials & Interfaces, 2020, 12(24): 27017-27028.

[13] Li N, Yi Z, Lin N, et al. An Al2O3 coating layer on mesoporous Si nanospheres for stable solid electrolyte interphase and high-rate capacity for lithium-ion batteries[J]. Nanoscale, 2019, 11(36): 16781-16787.

[14] Ma Q, Xie H, Qu J, et al. Tailoring the Polymer-Derived Carbon Encapsulated Silicon Nanoparticles for High-Performance Lithium-Ion Battery Anodes[J]. ACS Applied Energy Materials, 2019, 3(1): 268-278.

[15] Luo W, Chen X, Xia Y, et al. Surface and Interface Engineering of Silicon‐Based Anode Materials for Lithium‐Ion Batteries[J]. Advanced Energy Materials, 2017, 7(24).

[16] Li L, Du B, Yang Y, et al. Ionic/Electronic Dual‐Conductor Coating Layer Fabrication Enabling High‐Performance Silicon Anode[J]. Small Structures, 2022, 4(2).

[17] Liu S, Liu B, Yu Z, et al. Rapid Release of Silicon by Ultrafast Joule Heating Generates Mechanically Stable Shell–Shell Si/C Anodes with Dominant Inward Deformation[J]. ACS Nano, 2024, 18(26): 17326-17338.