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Journal ArticleDOI

Micro-sized Si-C Composite with Interconnected Nanoscale Building Blocks as High-Performance Anodes for Practical Application in Lithium-Ion Batteries

TLDR
In this paper, a Si-C nanocomposites (e.g., nanowires, nanotubes, or nanoparticles) has been used to improve the capacity and cycling stability of high-energy-density lithium-ion batteries.
Abstract
The emerging markets of electric vehicles (EV) and plug-in hybrid electric vehicles (PHEV) generate a tremendous demand for low-cost lithium-ion batteries (LIBs) with high energy and power densities and long cycling life. [ 1–4 ] The development of such LIBs requires development of low cost, high energy-density cathode and anode materials. Conventional anode materials in commercial LIBs are primarily synthetic graphite-based materials with a capacity of ∼ 370 mAh/g. [ 5 ] Improvements in anode performance, particularly in anode capacity, are essential to achieving high energy densities in LIBs for EV and PHEV applications. Silicon has been intensively pursued as the most promising anode material for high-energy-density LIBs because of its high specifi c capacity ( > 3500 mAh/g) and abundance. [ 6 ] Despite its high capacity, Si suffers from fast capacity fading caused by its large volume change ( > 300%) during lithiation/delithiation and the serious issues stemming from this volume change, e.g., unstable solid electrolyte interphase (SEI) and disintegration (cracking and crumbling) of the electrode structure. [ 7 , 8 ] The development of Si-C nanocomposites (e.g., nanowires, nanotubes, or nanoparticles) has been widely studied. [ 9–18 ] These nanocomposites proved to be an effective method of improving capacity and cycling stability, since nano-sized Si can alleviate fracture during volume changes and the contact between Si and carbon can maintain electrical contact and improve conductivity of the nanocomposites. However, practical application of nano-sized Si materials in LIBs is diffi cult. First, achieving a high tap density is important for fabrication of high-energy LIBs for EVs and PHEVs, because it offers a high volumetric energy density. Unfortunately, the tap density of nano-sized materials is generally low, which in turn holds down their volumetric capacity. [ 19 ] Furthermore, preparation of nano-sized Si either requires chemical/physical vapor deposition or involves complicated processes, leading to costly, low-yield synthesis that is diffi cult to scale up to practical levels. [ 20–22 ] To date, the abundance of Si has not been fully capitalized upon due to lack

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Citations
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Journal ArticleDOI

Ionothermal Synthesis of Crystalline Nanoporous Silicon and Its Use as Anode Materials in Lithium-Ion Batteries.

TL;DR: This work reports a facile, high-yield, and scalable approach to prepare nanoporous silicon, in which commercial magnesium silicide reacted with the acidic ionic liquid at 100 °C and ambient pressure.
Journal ArticleDOI

Computational modeling of electro-chemo-mechanics of high-capacity composite electrodes in Li-ion batteries

TL;DR: In this paper, a microstructurally resolved porous composite electrode model is proposed to capture the rate-dependent, coupled electro-chemo-mechanical behavior of high-capacity composite electrodes that agree well with experimental results.
Journal ArticleDOI

Gallic acid-assisted synthesis of nitrogen-doped carbon microspheres as efficient bifunctional materials for oxygen reduction and volumetric lithium storage

TL;DR: In this paper, N-doped carbon microspheres (NCM) were prepared using low-cost chitosan as a nitrogen and carbon source by a simple one-step solvothermal method with the assistance of gallic acid as a molecular nucleating agent.

Understanding the structure-property-performance relationship of silicon negative electrodes

Jiazhi Hu
Abstract: OF DISSERTATION UNDERSTANDING THE STRUCTURE-PROPERTY-PERFORMANCE RELATIONSHIP OF SILICON NEGATIVE ELECTRODES Rechargeable lithium ion batteries (LIBs) have long been used to power not only portable devices, e.g., mobile phones and laptops, but also large scale systems, e.g., electrical grid and electric vehicles. To meet the ever increasing demand for renewable energy storage, tremendous efforts have been devoted to improving the energy/power density of LIBs. Known for its high theoretical capacity (4200 mAh/g), silicon has been considered as one of the most promising negative electrode materials for high-energydensity LIBs. However, diffusion-induced stresses can cause fracture and, consequently, rapid degradation in the electrochemical performance of Si-based negative electrodes. To mitigate the detrimental effects of the large volume change, several strategies have been proposed. This dissertation focuses on two promising approaches to make high performance and durable Si electrodes for high capacity LIBs. First, the effect of polymeric binders on the performance of Si-based electrodes is investigated. By studying two types of polymeric binders, polyvinylidene fluoride (PVDF) and sodium alginate (SA) using peel tests, SEM, XPS, and FTIR, I show that the high cohesive strength at the binder-silicon interface is responsible for the superior cell performance of the Si electrodes with SA as a binder. Hydrogen bonds formed between SA and Si is the main reason for the high cohesive strength since neither PVDF nor SA bonds covalently with Si. Second, the fabrication of high performance Si/polyacrylonitrile (PAN) composite electrode via oxidative pyrolysis is investigated. We show that high performance Si/polyacrylonitrile (PAN) composite negative electrodes can be fabricated by a robust heat treatment in air at a temperature between 250 and 400oC. Using Raman, SEM, XPS, TEM, TGA, and nanoindention, we established that oxidation, dehydration, aromatization, and intermolecular crosslinking take place in PAN during the heat treatment, resulting in a stable cyclized structure which functions as both a binder and a conductive agent in the Si/PAN composite electrodes. With a Si mass loading of 1 mg/cm2, a discharge capacity of ~1600 mAh/g at the 100th cycle is observed in the 400oC treated Si/PAN composite electrode when cycled at a rate of C/3. These studies on the structure-property-performance relations of Si based negative electrode may benefit the LIB community by providing (1) a guide for the design and optimization of binder materials for Si electrodes and (2) a facile method of synthesizing Si-based composite negative electrodes that can potentially be applied to other Si/polymer systems for further increasing the power/energy density and lower the cost of LIBs for electric vehicle applications and beyond.
Journal ArticleDOI

Facile Fabrication of Si-Embedded Amorphous Carbon@Graphitic Carbon Composite Microspheres via Spray Drying as High-performance Lithium-Ion Battery Anodes

TL;DR: In this article , a spray-dried composite microsphere consisting of Si nanopowders, dextrin, and iron salt is transformed to uniquely structured Si/[email protected] microspheres via one-step carbonization followed by acid etching.
References
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Journal ArticleDOI

Building better batteries

TL;DR: Researchers must find a sustainable way of providing the power their modern lifestyles demand to ensure the continued existence of clean energy sources.
Journal ArticleDOI

Nanostructured materials for advanced energy conversion and storage devices

TL;DR: This review describes some recent developments in the discovery of nanoelectrolytes and nanoeLECTrodes for lithium batteries, fuel cells and supercapacitors and the advantages and disadvantages of the nanoscale in materials design for such devices.
Journal ArticleDOI

High-performance lithium battery anodes using silicon nanowires

TL;DR: The theoretical charge capacity for silicon nanowire battery electrodes is achieved and maintained a discharge capacity close to 75% of this maximum, with little fading during cycling.
Journal ArticleDOI

Lithium Batteries and Cathode Materials

TL;DR: This paper will describe lithium batteries in more detail, building an overall foundation for the papers that follow which describe specific components in some depth and usually with an emphasis on the materials behavior.
Journal ArticleDOI

Battery materials for ultrafast charging and discharging

TL;DR: It is shown that batteries which obtain high energy density by storing charge in the bulk of a material can also achieve ultrahigh discharge rates, comparable to those of supercapacitors.
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