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Low-temperature plasmas have seen increasing use for synthesizing high-quality, mono-disperse nanoparticles (NPs). Recent work has highlighted that an important process in NP growth in plasmas is particle trapping—small, negatively charged nanoparticles become trapped by the positive electrostatic potential in the plasma, even if only momentarily charged. In this article, results are discussed from a computational investigation into how pulsing the power applied to an inductively coupled plasma (ICP) reactor may be used for controlling the size of NPs synthesized in the plasma. The model system is an ICP at 1 Torr to grow silicon NPs from an Ar/SiH 4 gas mixture. This system was simulated using a two-dimensional plasma hydrodynamics model coupled to a three-dimensional kinetic NP growth and trajectory tracking model. The effects of pulse frequency and pulse duty cycle are discussed. We identified separate regimes of pulsing where particles become trapped for one pulsed cycle, a few cycles, and many cycles—each having noticeable effects on particle size distributions. For the same average power, pulsing can produce a stronger trapping potential for particles when compared to continuous wave power, potentially increasing particle mono-dispersity. Pulsing may also offer a larger degree of control over particle size for the same average power. Experimental confirmation of predicted trends is discussed.
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Controlled growth of silicon particles via plasma pulsing and their application as battery material
Abstract The use of silicon nanoparticles for lithium-ion batteries requires a precise control over both their average size and their size distribution. Particles larger than the generally accepted critical size of 150 nm fail during lithiation because of excessive swelling, while very small particles (<10 nm) inevitably lead to a poor first cycle coulombic efficiency because of their excessive specific surface area. Both mechanisms induce irreversible capacity losses and are detrimental to the anode functionality. In this manuscript we describe a novel approach for enhanced growth of nanoparticles to ∼20 nm using low-temperature flow-through plasma reactors via pulsing. Pulsing of the RF power leads to a significant increase in the average particle size, all while maintaining the particles well below the critical size for stable operation in a lithium-ion battery anode. A zero-dimensional aerosol plasma model is developed to provide insights into the dynamics of particle agglomeration and growth in the pulsed plasma reactor. The accelerated growth correlates with the shape of the particle size distribution in the afterglow, which is in turn controlled by parameters such as metastable density, gas and electron temperature. The accelerated agglomeration in each afterglow phase is followed by rapid sintering of the agglomerates into single-crystal particles in the following plasma-on phase. This study highlights the potential of non-thermal plasma reactors for the synthesis of functional nanomaterials, while also underscoring the need for better characterization of their fundamental parameters in transient regimes.
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- Award ID(s):
- 1940952
- PAR ID:
- 10322698
- Date Published:
- Journal Name:
- Journal of Physics D: Applied Physics
- Volume:
- 55
- Issue:
- 9
- ISSN:
- 0022-3727
- 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/10.1088/1361-6463/ac3867
