Li-Ions Transport Promoting and Highly Stable Solid–Electrolyte Interface on Si in Multilayer Si/C through Thickness Control

Zhao, Yi; Wang, Jun; He, Qiang; Shi, Juan; Zhang, Zhiya; Men, Xuehu; Yan, Dingshun; Wang, Huazhi

doi:10.1021/acsnano.9b00670

Cited by 45 publications

(37 citation statements)

References 58 publications

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“…According to our results, the transportation of Li ions in the TiO 2 /C electrodes is dominated by the diffusion process. The evaluation method is the same as that used in our previous work 42 and will not be elaborated here. The relevant data are shown in Figures S5 and S6.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Boosting Lithium-Ion Transport Kinetics by Increasing the Local Lithium-Ion Concentration Gradient in Composite Anodes of Lithium-Ion Batteries

Sun

et al. 2021

ACS Appl. Mater. Interfaces

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Constructing composite electrodes is considered to be a feasible way to realize high-specific-capacity Li-ion batteries. The core–double-shell-structured Si@C@TiO2 would be an ideal design for such batteries, considering that carbon (C) can buffer the volume change and TiO2 can constrain the structural deformation of Si. Although the electrochemical performance of the shells themselves is relatively clear, the complexity of the multishell heterointerface always results in an ambiguous understanding about the influence of the heterointerface on the electrochemical properties of the core material. In this work, a multilayer film model that can simplify and simultaneously expand the area of the heterointerface is used to study the heterointerfacial behavior. First, a multilayer film TiO2/C with different numbers of TiO2/C heterointerfaces is studied. It shows that the electrochemical performance is enhanced apparently by increasing the number of TiO2/C heterointerfaces. On the one hand, the TiO2/C heterointerface exhibits a strong lithium-ion storage capacity. On the other hand, the TiO2/C heterointerface appears to effectively promote the local Li-ion concentration gradient and thus boost the Li-ion transport kinetics. Then, TiO2/C is combined with Si to construct a composite anode Si/C/TiO2. An obvious advantage of TiO2/C over single TiO2 and C is observed. The utilization rate of Si is greatly improved in the first cycle and reaches up to 98% in Si/C/TiO2. The results suggest that the electrochemical performance of Si can be greatly manipulated by the heterointerface between the multishells.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Boosting Lithium-Ion Transport Kinetics by Increasing the Local Lithium-Ion Concentration Gradient in Composite Anodes of Lithium-Ion Batteries

Sun

et al. 2021

ACS Appl. Mater. Interfaces

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“…Further exploring to increase the mass loading is highly necessary for practical applications. In addition, compared with the film electrodes, such as those with thicknesses in several hundred nanometer level, [19d,35] the present electrode has a thickness of ≈4 μm. It is hopeful that the present electrode is expected to be developed in the application of some of the film electrode areas after further modifications of the electrochemical properties.…”

Section: Resultsmentioning

confidence: 98%

A Unique Structural Highly Compacted Binder‐Free Silicon‐Based Anode with High Electronic Conductivity for High‐Performance Lithium‐Ion Batteries

Dong

Gu³

et al. 2021

Small Structures

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Herein, a unique structural Si‐based anode with high electronic conductivity, high compact density, and with no traditional organic binder is put forward. By adding a few amounts of Sn to the Si anode material, followed by carbonization of the organic binder after the general anode preparation and subsequently hot pressing, Sn melts and squeezes during hot pressing, bonding strongly the Si particles, and an interlayer of Cu3Si/Cu3Sn is in situ formed at the interface of the Si‐based active materials and the Cu current collector, resulting in a metallurgical bonding between them. The organic binder‐derived carbon coats on the Si particles, coupling with the squeezed Sn and the Cu3Si/Cu3Sn interlayer, and a highly electron conductive skeleton is formed. The skeleton also offers a highly stable structural integrity of the electrode during cycling. With an optimization of the hot‐pressing pressure, the Si‐based anode shows superior cycling stability and rate performance. As the active materials are almost compacted to half of its initial thickness, the electrode has potential for high volumetric capacity. The fabrication method is new for Si‐based anodes of high compact density. The work provides new insights into the development of advanced silicon‐based anodes for lithium‐ion batteries.

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“…It is conspicuous that the impedance increases dramatically from the 40th to 100th cycle, while the capacity decade is much less obvious. This phenomenon may ascribe to a competition between electrode activation and capacity fade. , One the one hand, the activation reaction may continually conduct after the 40th cycle and maintain the capacity enhancement. One the other hand, due to the limited ability of building blocks, the volume expansion and contraction are inevitable, which make the SEI fractured and reconstituted, followed by the loss of the electrolyte and capacity as well as the increased impedance.…”

Section: Results and Discussionmentioning

confidence: 99%

Interface Engineering of Silicon/Carbon Thin-Film Anodes for High-Rate Lithium-Ion Batteries

Tong

Wang

Fang

et al. 2020

ACS Appl. Mater. Interfaces

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Silicon is one of the most promising alternative active materials for next-generation lithium-ion battery (LIB) applications due to its advantage of high specific capacity. However, the enormous volume variations during lithiation/delithiation still remain to be an obstacle to commercialization. In this work, binder-free pure silicon and silicon/carbon (Si/C) multilayer thin-film electrodes, prepared by scalable one-step magnetron sputtering, are systematically investigated by an interlayer strategy. Herein, we present a rationally structural modification by an amorphous carbon film to enhance the electrical conductivity, mechanical integrity, and electrochemical performance of Si film-based LIBs. Therefore, to maintain the consistency of the direct-contact layer with the electrolyte and current collection, symmetrical Si/C/Si and Si/C/Si/C/Si/C/Si electrodes are deliberately designed to study the influence of embedded carbon. An anode with a carbon content of 10.38 wt % yields an initial discharge specific capacity of 1888.74 mAh g–1 and a capacity retention of 96.82% (1243.56 mAh g–1) after 150 cycles at a high current density of 4000 mA g–1. It also shows that the best rate capability remains 96.0% of the initial capacity in the 70th cycle. At last, three mechanisms are proposed for an in-depth understanding of the interface effect. This work offers a new perspective scheme toward Si/C-based LIBs with a capability of high rate and high energy density.

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Li-Ions Transport Promoting and Highly Stable Solid–Electrolyte Interface on Si in Multilayer Si/C through Thickness Control

Cited by 45 publications

References 58 publications

Boosting Lithium-Ion Transport Kinetics by Increasing the Local Lithium-Ion Concentration Gradient in Composite Anodes of Lithium-Ion Batteries

Boosting Lithium-Ion Transport Kinetics by Increasing the Local Lithium-Ion Concentration Gradient in Composite Anodes of Lithium-Ion Batteries

A Unique Structural Highly Compacted Binder‐Free Silicon‐Based Anode with High Electronic Conductivity for High‐Performance Lithium‐Ion Batteries

Interface Engineering of Silicon/Carbon Thin-Film Anodes for High-Rate Lithium-Ion Batteries

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