Size and Surface Effects of Silicon Nanocrystals in Graphene Aerogel Composite Anodes for Lithium Ion Batteries

Aghajamali, Maryam; Xie, Hezhen; Javadi, Morteza; Kalisvaart, W. Peter; Buriak, Jillian M.; Veinot, Jonathan G. C.

doi:10.1021/acs.chemmater.8b03198

Cited by 58 publications

(32 citation statements)

References 60 publications

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“…Silicon has been intensively studied as a Li-ion battery (LIB) anode material because of its high theoretical storage capacity of ~3600 mAh/g 1,2 . It also has one of the highest theoretical reversible capacities for sodium-ion battery (SIB) anodes (954 mAh/g), corresponding to a one-to-one ratio of sodium to silicon (NaSi).…”

Section: Introductionmentioning

confidence: 99%

Sb–Si Alloys and Multilayers for Sodium-Ion Battery Anodes

Kalisvaart

Olsen

Luber

et al. 2019

ACS Appl. Energy Mater.

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Silicon has a theoretical sodium-storage capacity of 954 mAh/g, which even exceeds that of tin (847 mAh/g). However, this capacity has never been reached in practice. Antimony is one of the best-performing Na-storage materials in terms of both capacity and cycling stability. By combining silicon and antimony, either by cosputtering or depositing multilayers with bilayer thickness down to 2 nm, we can achieve capacities exceeding even the theoretical capacity of Sb (660 mAh/g). Minor addition of silicon, 7 at. % or 7 wt % (25 at. %), increases the measured reversible capacity from 625 mAh/g for pure Sb to 663 and 680 mAh/g, respectively. All Sb-rich (>50 at. %) compositions show improved cycling stability over elemental Sb. Si 0.07 Sb 0.93 reached a maximum capacity of 663 mAh/g after 140 cycles and showed negligible capacity degradation up to 200 cycles. The fully sodiated state in cosputtered films evolves from single-phase amorphous to a mixture of a Sb-rich and Si-rich sodiated phases as cycling progresses, when the Si content is between 75 and 50 at. %. The typical desodiation signature of c-Na 3 Sb is observed only after 100 cycles or more. Careful examination of the voltage profiles of multilayers shows that they initially tend toward intermixing between the Si and Sb layers, contrary to expectations based on the phase diagram. When the Si and Sb layer thickness is decreased to 2 nm, the multilayer and cosputtered film behave almost identically. A general direction for finding promising multicomponent sodium-ion battery (SIB) alloy anodes is proposed.

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Section: Introductionmentioning

confidence: 99%

Sb–Si Alloys and Multilayers for Sodium-Ion Battery Anodes

Kalisvaart

Olsen

Luber

et al. 2019

ACS Appl. Energy Mater.

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“…Batteries, owing to their high energy density and ability to supply a constant source of electrical power, dominate the worlds of portable electronics and electric vehicles. This is especially true for lithium-ion type batteries (LIBs) [154]. Supercapacitors, on the other hand, are ideal for short-term energy needs due to their extremely quick and high efficiency charging capabilities, while also being able to operate for a virtually unlimited number of charge-discharge cycles [155,156].…”

Section: Applicationsmentioning

confidence: 99%

Nanomaterials in Advanced, High-Performance Aerogel Composites: A Review

et al. 2019

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Aerogels are one of the most interesting materials of the 21st century owing to their high porosity, low density, and large available surface area. Historically, aerogels have been used for highly efficient insulation and niche applications, such as interstellar particle capture. Recently, aerogels have made their way into the composite universe. By coupling nanomaterial with a variety of matrix materials, lightweight, high-performance composite aerogels have been developed for applications ranging from lithium-ion batteries to tissue engineering materials. In this paper, the current status of aerogel composites based on nanomaterials is reviewed and their application in environmental remediation, energy storage, controlled drug delivery, tissue engineering, and biosensing are discussed.

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“…All electrodes exhibit two broad peaks during lithiation and delithiation at the second cycle, typical of amorphous silicon. 46,47 After 18 cycles, the electrode with only elemental Si on Cu shows a sharp delithiation peak at ca. 0.42 V vs Li, indicating the formation of c-Li3.75Si at the end of the lithiation step (Figure 5a); the lack of formation of the c-Li3.75Si phase during the first 18 cycles may be attributed to stress resulting from the substrate-silicon interface.…”

Section: Electrode Preparation and Battery Assemblymentioning

confidence: 99%

Adhesion and Surface Layers on Silicon Anodes Suppress Formation of c-Li3.75Si and Solid Electrolyte Interphase

Xie

Sayed

Kalisvaart

et al. 2019

Preprint

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<div>The formation of c-Li3.75Si is known to be detrimental to silicon anodes in lithium-ion batteries. To suppress the formation of this crystalline phase and improve the electrochemical performance of Sibased anodes, three approaches were amalgamated: addition of a nickel adhesion sublayer, alloying of the silicon with titanium, and the addition of either carbon or TiO2 as a capping layer. The silicon-based films were analyzed by a suite of methods, including scanning electron microscopy (SEM) and a variety of electrochemical methods, as well as X-ray photoelectron spectroscopy (XPS) to provide insights into the composition of the resulting solid electrolyte interphase (SEI). A nickel adhesion layer decreased the extent of delamination of the silicon from the underlying copper substrate, compared to Si deposited directly on Cu, which resulted in less capacity loss. Alloying of silicon with titanium (85% silicon, 15% titanium) further increased the stability. Finally, capping these multilayer electrodes with either a thin 10 nm layer of carbon or TiO2 resulted in the best electrode behavior, and lowest cumulative relative irreversible capacity. TiO2 is slightly more effective in enhancing the capacity retention, most likely due to differences in the resulting solid electrolyte interphase (SEI). The combination of an adhesion layer, alloying, and surface coatings shows a cumulative suppression of the formation of c-Li3.75Si and SEI, resulting in the greatest improvement of capacity retention when all three are incorporated together. However, these strategies appear to only delay the onset of the c-Li3.75Si phase; eventually, the c-Li3.75Si phase will form, and at that point, the rate of capacity degradation of all the electrodes becomes similar.</div>

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Size and Surface Effects of Silicon Nanocrystals in Graphene Aerogel Composite Anodes for Lithium Ion Batteries

Cited by 58 publications

References 60 publications

Sb–Si Alloys and Multilayers for Sodium-Ion Battery Anodes

Sb–Si Alloys and Multilayers for Sodium-Ion Battery Anodes

Nanomaterials in Advanced, High-Performance Aerogel Composites: A Review

Adhesion and Surface Layers on Silicon Anodes Suppress Formation of c-Li3.75Si and Solid Electrolyte Interphase

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