Dual-Size Silicon Nanocrystal-Embedded SiO<sub><i>x</i></sub> Nanocomposite as a High-Capacity Lithium Storage Material

Park, Eunjun; Yoo, Hyundong; Lee, Jae Woo; Park, Min; Kim, Young Jun; Kim, Hansu

doi:10.1021/acsnano.5b03166

Cited by 109 publications

(78 citation statements)

References 31 publications

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“…Despite the significantly improved cyclability based on these structural designs, the industry has instead adopted the silicon monoxide phase (SiO x , x ≈ 1) as the first Si-based commercial anode material (FIG. 2c), because these materials can be produced in massive quantities in both gas-phase 42,43 and solution-based 44 processes, and are also available at a reasonable price (approximately US$100 per kg versus $10-20 per kg of graphite) and with reliable quality. However, SiO x is used in a blended form with graphite, but its content is typically less than 5 wt%, which reflects the infancy of Si anode technology.…”

Section: Near-term Technologiesmentioning

confidence: 99%

Promise and reality of post-lithium-ion batteries with high energy densities

2016

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What characteristics define a good rechargeable battery? Although properties such as rate capability, cost, cycle life and temperature tolerance must be taken into consideration in any evaluation of a rechargeable battery 1,2 , it is the improvement in energy density that has primarily driven the overall technological progress over the past 150 years -from lead-acid cells in the 1850s, nickelcadmium cells in the 1890s and nickel metal hydride cells in the 1960s to, finally, lithium-ion batteries (LIBs) in the present day.In the current era of LIBs, there is an ever-growing demand for even higher energy densities to power mobile IT devices with increased power consumption and to extend the driving range of electric vehicles. The growth of the global electric vehicle market has been slower than initially predicted about 5 years ago 3 , which reflects the challenge that the battery industry faces: customers react very sensitively to the driving range (and thus the energy density) and price of electric vehicles. Because the energy density of a rechargeable battery is determined mainly by the specific capacities and operating voltages of the anode and the cathode, active materials have been the main focus of research in recent years. Other cell components, including separators, binders, outer cases and, to some extent, the major components of the electrolyte solution (that is, solvent and salt), have little room for further improvement. In other words, a dramatic increase in the energy density requires new redox chemistries between charge-carrier ions and host materials beyond the conventional 'intercalation' mechanisms 4 . Intercalationbased materials have a relatively small number of crystallographic sites for storing charge-carrier ions, leading to limited energy densities. For this reason, the electrodes that operate on the basis of distinct solid-state reactions, such as alloying and conversion, or that use gas-phase reactants have encountered growing interest owing to the likelihood that they will surpass the energy densities of intercalation-based electrodes.New chemistries for charge-carrier ion storage serve as the basis for 'beyond intercalation' or so-called postLIBs 5-7 . The systems governed by these new chemistries offer higher theoretical energy densities, and this benefit is usually translated to, at least, the initial cycles in experimental testing. It is becoming increasingly evident that the short lifetime is a serious problem of post-LIB systems. Indeed, the main technological challenge associated with these systems is overcoming their inferior reversibility. The main factors responsible for the low reversibility are instabilities during the phase transition of active materials and/or uncontrolled reactions at the electrode/electrolyte interface 8 ; this implies that the electrode structures and electrolyte solutions should be developed and optimized as integrated systems to enable the realization of post-LIBs.In this Review, we discuss a wide range of promising post-LIBs, focusing on their advant...

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Section: Near-term Technologiesmentioning

confidence: 99%

Promise and reality of post-lithium-ion batteries with high energy densities

2016

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“…403 mA h −1 g −1 ). Once the granular structure of the Si/SiOC NP composite was formed, the initial reversible capacity increased to around 1000 mA h −1 g −1 , attributable to the expanded voltage plateau around 0.4 V caused by dealloying of the Li x Si phase . Furthermore, a large hysteresis was observed for the Si/SiOC composite electrodes, in that approximately one‐fifth of the capacity could only be extracted over 2 V, as seen for porous SiOC materials…”

Section: Resultsmentioning

confidence: 99%

“…Once the granulars tructure of the Si/SiOC NP composite was formed, the initial reversible capacity increased to around1 000 mA h À1 g À1 ,a ttributable to the expanded voltage plateau around0 .4 Vc aused by dealloying of the Li x Si phase. [19] Furthermore, al arge hysteresis was observed for the Si/SiOC composite electrodes, in that approximately one-fifth of the capacity could only be extracted over 2V ,a ss een for porousSiOC materials. [20] The cyclingp erformanceso fS i/SiOC composites are shown in Figure 3c,d.Cells were firstly activated over 2c ycles at 50 mA g À1 and then cycled at 500 mA g À1 .T he bare SiOC anode showedn oo bvious capacity loss at 500 mA g À1 ,a nd a reversible capacity of about 200 mA h À1 g À1 was maintained over 500 cycles, regardless of as light capacity increase (ca.…”

Section: Resultsmentioning

confidence: 99%

A Nanostructured Si/SiOC Composite Anode with Volume‐Change‐Buffering Microstructure for Lithium‐Ion Batteries

Cheng

et al. 2019

Chemistry A European J

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Si/SiOC composites are promising high‐capacity anode materials for lithium‐ion batteries since the SiOC matrix can effectively buffer the volumetric change of Si during cycling. However, a structure of Si nanoparticles (NPs) enwrapped by a continuous SiOC phase typically shows poor cyclic stability and low charge/discharge rate due to structure failure of bulk SiOC shells derived from carbon‐rich organosilicon. To address this issue, in this work, an Si/SiOC nanocomposite with volume‐change‐buffering microstructure, in which Si NPs are uniformly dispersed in a matrix of SiOC nanospheres, has been synthesized. Our results show that the space between Si and SiOC NPs can accommodate the large volume change of Si during cycling and facilitate infiltration of the electrolyte. The nanostructured SiOC skeleton serves as both a mechanically robust buffer to alleviate the intrinsic expansion of Si and an effective electron conductor. The Si/SiOC NP composite displays significantly increased capacity and cyclic stability compared with pure SiOC, and delivers reversible capacities of around 800 mA h−1 g−1 at a current density of 100 mA g−1 (approximately 100 % capacity retention after 100 cycles) and around 600 mA h−1 g−1 at 500 mA g−1 (capacity retention about 80 % after 500 cycles).

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“…6 To gain further higher performance with nanostructures, tremendous efforts have been conducted for accommodating the volume expansion by Si-active/inactive material composites. [6][7][8][9][10][11][12] For example, Si surface coating with carbonized materials and polymers [13][14][15][16][17][18][19][20][21] for the integration of pulverized Si particles, the use of a new type of binder, 22 development of a hollow Si architecture, 23 peculiar design of Si composite structures, 24,25 and development of a processing method 7,26 are adopted to improve the cycle life, capacity retention, and Coulombic efficiency. Many experimental and theoretical studies on mechanical properties have been focused on mainly for the lithiation process on Si.…”

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confidence: 99%

Theoretical prediction of fracture conditions for delithiation in silicon anode of lithium ion battery

Cho

Lee

et al. 2017

APL Materials

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Structural instability such as fractures of a silicon anode in a lithium ion battery, intrinsically induced by the large variation of the ratio, Li/Si, upon lithiation and delithiation, limits its potential for commercial use. Here, we study mechanical properties during delithiation in lithiated silicon particles to identify the conditions under which fracture is preventing during delithiation in terms of Li contents and silicon particle sizes. We employed the first principles calculation within the density functional framework combined with the continuum based calculation for the macroscopic mechanical properties. The theoretical limit for the largest crystalline silicon particle size that can prevent fractures upon complete delithiation is ∼0.6 μm at the lithium flux per unit surface area of 5.657 × 10−2 s−1 nm out of amorphous Li3.75Si, much larger than the critical fracture size (0.15 μm) that occurs during the first lithiation of crystalline Si. Furthermore, fractures during delithiation are nearly unaffected by the silicon particle size for a residual lithium fraction larger than x ∼ 2.1 in amorphous LixSi.

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Dual-Size Silicon Nanocrystal-Embedded SiO_x Nanocomposite as a High-Capacity Lithium Storage Material

Cited by 109 publications

References 31 publications

Promise and reality of post-lithium-ion batteries with high energy densities

Promise and reality of post-lithium-ion batteries with high energy densities

A Nanostructured Si/SiOC Composite Anode with Volume‐Change‐Buffering Microstructure for Lithium‐Ion Batteries

Theoretical prediction of fracture conditions for delithiation in silicon anode of lithium ion battery

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Dual-Size Silicon Nanocrystal-Embedded SiOx Nanocomposite as a High-Capacity Lithium Storage Material

Cited by 109 publications

References 31 publications

Promise and reality of post-lithium-ion batteries with high energy densities

Promise and reality of post-lithium-ion batteries with high energy densities

A Nanostructured Si/SiOC Composite Anode with Volume‐Change‐Buffering Microstructure for Lithium‐Ion Batteries

Theoretical prediction of fracture conditions for delithiation in silicon anode of lithium ion battery

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Dual-Size Silicon Nanocrystal-Embedded SiO_x Nanocomposite as a High-Capacity Lithium Storage Material