Long-term Cyclability of Substoichiometric Silicon Nitride Thin Film Anodes for Li-ion Batteries

Ulvestad, Asbjørn; Andersen, Hanne Flåten; Mæhlen, Jan Petter; Prytz, Øystein; Kirkengen, Martin

doi:10.1038/s41598-017-13699-0

Cited by 24 publications

(22 citation statements)

References 54 publications

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“…32 have reported that 200 nm and 500 nm SiN 0.92 thin films exhibited first cycle reversible capacities of approximately 1,500 mAh/g and 1,000 mAh/g, and retained capacities of 1,300 mAh/g and 700 mAh/g after 100 cycles, respectively. Similar thin films of a-SiN 0.89 have also been found to exhibit a comparable reversible capacity of more than 1250 mAh/g 33 over 2400 cycles. In these works, silicon nitride is assumed to function as a conversion material, forming active silicon and an inactive nitride matrix component 31 – 33 .…”

Section: Introductionmentioning

confidence: 78%

“…Similar thin films of a-SiN 0.89 have also been found to exhibit a comparable reversible capacity of more than 1250 mAh/g 33 over 2400 cycles. In these works, silicon nitride is assumed to function as a conversion material, forming active silicon and an inactive nitride matrix component 31 – 33 . The exact nature of the matrix has not yet been determined, but it has been suggested to consist of Si 3 N 4 and/or Li 3 N 30 , 31 , or a ternary lithium silicon nitride, e.g.…”

Section: Introductionmentioning

confidence: 78%

“…Some electrodes were also subjected to rate testing with current rates increasing from C/4 to 16C, doubling the rate by every 5 cycles. The C-rates for these experiments were estimated from the compositions by linear interpolation between 1,200 mAh/g for SiN 0.89 33 and 3,579 mAh/g for Si, as described in the supplementary information. When compared to the charge capacity obtained in the experiments during the initial formation cycles, these estimates were found to be satisfactory.…”

Section: Methodsmentioning

confidence: 99%

“…The exact nature of the matrix has not yet been determined, but it has been suggested to consist of Si 3 N 4 and/or Li 3 N 30 , 31 , or a ternary lithium silicon nitride, e.g. Li 2 SiN 2 32 , 33 . The following reaction schematically describes the general processes of conversion of SiN x and subsequent cycling: Similarly as for the silicon sub-oxides, the expected function of the matrix is primarily to buffer the volume change of the active silicon domains during lithiation and delithiation, while providing necessary lithium ion conductivity for lithium to reach these domains.…”

Section: Introductionmentioning

confidence: 99%

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Substoichiometric Silicon Nitride – An Anode Material for Li-ion Batteries Promising High Stability and High Capacity

Ulvestad

Andersen

Jensen

et al. 2018

Sci Rep

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Silicon is often regarded as a likely candidate to replace graphite as the main active anode material in next-generation lithium ion batteries; however, a number of problems impacting its cycle stability have limited its commercial relevance. One approach to solving these issues involves the use of convertible silicon sub-oxides. In this work we have investigated amorphous silicon sub-nitride as an alternative convertible silicon compound by comparing the electrochemical performance of a-SiNx thin films with compositions ranging from pure Si to SiN0.89. We have found that increasing the nitrogen content gradually reduces the reversible capacity of the material, but also drastically increases its cycling stability, e.g. 40 nm a-SiN0.79 thin films exhibited a stable capacity of more than 1,500 mAh/g for 2,000 cycles. Consequently, by controlling the nitrogen content, this material has the exceptional ability to be tuned to satisfy a large range of different requirements for capacity and stability.

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Section: Introductionmentioning

confidence: 78%

Section: Introductionmentioning

confidence: 78%

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Substoichiometric Silicon Nitride – An Anode Material for Li-ion Batteries Promising High Stability and High Capacity

Ulvestad

Andersen

Jensen

et al. 2018

Sci Rep

Self Cite

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“…Silicon nitride films are useful in microelectronics applications [1] such as oxidation masks, protection and passivation barrier layers, gate dielectrics and interlevel insulations due their remarkable hardness, high thermal stability, chemical inertness and excellent insulation capabilities [2]. These films also play important role in optoelectronic applications such as antireflection coatings and optimization of optical performance of devices due to its capability of providing the refractive index variation from silicon oxide like (~1.46) to stochiometric silicon nitride (~2.0) and by providing transparency in ultraviolet (250nm) to infrared (9µm) regions of optical spectrum [3].…”

Section: Introductionmentioning

confidence: 99%

Effect on Silicon Nitride thin Films Properties at Various Powers of RF Magnetron Sputtering

Mustafa¹,

Majeed²,

Iqbal³

2018

IJET

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Silicon nitride thin films have numerous applications in microelectronics and optoelectronics fields due to their unique properties. In this work, silicon nitride thin films were produced using radio frequency (R.F.) magnetron sputtering technique at various sputtering powers. The prepared thin films were characterized with XRD, FE-SEM, FTIR, surface profiler, AFM and spectral reflectance techniques for structure, surface morphology, chemical bonding information, growth rate, surface roughness and optical properties. The results showed that silicon nitride thin films were amorphous in nature. The films were smooth and densely packed with no voids or cracks at the surface. FTIR characterization informed about Si-N bonding existence which confirmed the formation of silicon nitride films. The sputtering power showed the impetus effect on growth rate, surface roughness and optical properties of produced films.

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Active Buffer Matrix in Nanoparticle‐Based Silicon‐Rich Silicon Nitride Anodes Enables High Stability and Fast Charging of Lithium‐Ion Batteries

Kilian

Wankmiller

Sybrecht

et al. 2022

Adv Materials Inter

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first and foremost are defined by both anode and cathode material properties.Silicon is considered the most attractive high-capacity anode material for the next generation of LIBs, showing a low working potential and a high theoretical storage capacity of 3579 mAh g −1 . [1,2] Additional advantages include better rate performance compared to graphite, [3,4] high natural abundance, and low cost. [5][6][7] In spite of these clear advantages, the implementation of silicon-based anodes has not yet been accomplished, mainly due to two major challenges: the continuous solid electrolyte interphase (SEI) growth and the pulverization of the anode material. These challenges have their origin in the high capacity of Si and the alloying reaction with Li that inevitably leads to huge volume expansion of up to 300% in a fully lithiated state. [8] The volume changes during charging and discharging lead to mechanical instability of the anode, noticeable by severe cracking and eventually a loss of electrical contact of active material. [9,10] Thus, silicon-based electrodes show rapid degradation and failure after only a few cycles, while the application of nanomaterials, such as nanowires, nanoparticles, or thin films, have been shown to circumvent distinct mechanical failure. [11][12][13][14] Whereas nanostructures mitigate challenges related to, for example, fracturing and pulverization, they do promote irreversible capacity losses and capacity fading associated with excessive SEI build-up during cycling, owing to their usually A very promising way to improve the stability of silicon in lithium-ion battery (LIB) anodes is the use of nanostructured silicon-rich silicon nitride (SiN x ), known as a conversion-type anode material. To investigate the conversion mechanism in this material in detail, SiN 0.5 nanoparticles are synthesized and examined as LIB anodes using a combination of ex situ X-ray photoelectron spectroscopy and solid-state 7 Li MAS NMR measurements. During the initial cycle, the conversion of SiN 0.5 nanoparticles results in the formation of lithium silicides and a buffer matrix consisting of different lithium nitridosilicates and lithium nitride. These phases can be reversibly lithiated and contribute to the total reversible capacity of the silicon nitride active material. The structure of the material after conversion is best described by an amorphous solid solution. Further, it is shown that silicon-rich silicon nitrides possess improved rate capability because of the higher ionic conductivity of the buffer matrix compared to pure silicon, and very fine dispersion of silicon clusters throughout the buffer matrix. Thus, unlike most conversion materials, the silicon-rich silicon nitride exhibits an additional intrinsic active functionality of the buffer matrix that goes far beyond the mere reduction of electrolyte contact area and volume expansion.

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Long-term Cyclability of Substoichiometric Silicon Nitride Thin Film Anodes for Li-ion Batteries

Cited by 24 publications

References 54 publications

Substoichiometric Silicon Nitride – An Anode Material for Li-ion Batteries Promising High Stability and High Capacity

Substoichiometric Silicon Nitride – An Anode Material for Li-ion Batteries Promising High Stability and High Capacity

Effect on Silicon Nitride thin Films Properties at Various Powers of RF Magnetron Sputtering

Active Buffer Matrix in Nanoparticle‐Based Silicon‐Rich Silicon Nitride Anodes Enables High Stability and Fast Charging of Lithium‐Ion Batteries

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