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Utilizing silicon as an anode material for Li-ion batteries has been the subject of many studies. However, due to the huge volume change of silicon during lithiation, the electrochemical performance of silicon is poor. Here, we have investigated a novel yet simple approach to synthesize nanostructured silicon/graphite composites with a carbon coating and engineered voids. High-energy ball mill is employed to convert micrometer-sized silicon and graphite to nanostructured silicon/graphite composite building blocks, while a thin carbon coating is applied to encapsulate these composite agglomerates, followed by partial etching of silicon to create engineered voids inside the composite agglomerates. The batteries made with this tailored nanostructure exhibit improved electrochemical performance over the counterparts made with silicon nanoparticles and exhibited a specific capacity of ~1800 mA h g-1 discharge capacity at the first cycle, 580 mA h g-1 after 40 cycles, and 350 mA h g-1 after 300 cycles. This study has established a novel method scalable at industry environment and capable of producing low cost Si anodes and clearly shown that the cycle stability of the tailored nanostructure improves with increasing engineered voids in the range we have investigated.
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Silicon Microreactor as a Fast Charge, Long Cycle Life Anode with High Initial Coulombic Efficiency Synthesized via a Scalable Method
Applications of silicon as a high-performance anode material has been impeded by its low intrinsic conductivity and huge volume expansion (> 300%) during lithiation. To address these problems, nano-Si particles along with conductive coatings and engineered voids are often employed, but this results in high cost anodes. Here, we report a scalable synthesis method that can realize high specific capacity (~800 mAh g-1), ultrafast charge/discharge (at 8 A g-1 Si) and high initial Coulombic efficiency (~90%) with long cycle life (1000 cycles) at the same time. To achieve 1000 cycle stability, micron-sized Si particles are subjected to high-energy ball milling to create nanostructured Si building blocks with nano-channel shaped voids encapsulated inside a nitrogen (N)-doped carbon shell (termed as Si micro-reactor). The nano-channel voids inside a Si micro-reactor not only offer the space to accommodate the volume expansion of Si, but also provide fast pathways for Li ion diffusion into the center of the nanostructured Si core and thus ultrafast charge/discharge capability. The porous N-doped carbon shell helps to improve the conductivity while allowing fast Li ion transport and confining the volume expansion within the Si micro-reactor. Submicron-sized Si micro-reactors with limited specific surface area (35 m2 g-1) afford sufficient electrode/electrolyte interfacial area for fast lithiation/delithiation, leading to the specific capacity ranging from ~800 to 420 mAh g-1 under ultrafast charging conditions (8 A g-1), but not too much interfacial area for surface side reactions and thus high initial coulombic efficiency (~90%). Since Si micro-reactors with superior electrochemical properties are synthesized via an industrially scalable and eco-friendly method, they have the potential for practical applications in the future.
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- PAR ID:
- 10253020
- Date Published:
- Journal Name:
- ACS applied energy materials
- Volume:
- 4
- Issue:
- 5
- ISSN:
- 2574-0962
- Page Range / eLocation ID:
- 4744 – 4757
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/https://doi.org/10.1021/acsaem.1c00351
