Silicon-based Anode Materials and Application to High Performance Li-ion Batteries

Liu,  Hongbin

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シリコン系負極材料の合成、キャラクタリゼーション及び高性能リチウムイオン電池への応用

https://doi.org/10.18997/00008672

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sei_k_414.pdf (6.9 MB)

アイテムタイプ

学位論文 = Thesis or Dissertation(1)

公開日

2022-01-04

資源タイプ

資源タイプ識別子

http://purl.org/coar/resource_type/c_db06

資源タイプ

doctoral thesis

タイトル

Silicon-based Anode Materials and Application to High Performance Li-ion Batteries

言語

タイトル

シリコン系負極材料の合成、キャラクタリゼーション及び高性能リチウムイオン電池への応用

言語

eng

著者

Liu, Hongbin

抄録

内容記述タイプ

Abstract

内容記述

Lithium-ion batteries have been widely used due to their significant advantages such as high energy density, good cycle stability, environmental protection, and wide working range. As an important part of lithium-ion batteries, the development of high-energy-density electrode materials has important research significance. Silicon anode has great potential to replace the graphite as the anode material in the next generation of lithium-ion batteries, due to its high theoretical capacity of 4200 mAh g-1 as fully intercalated with lithium. However, the volume expansion and poor conductivity of the silicon materials during the lithiation-delithiation cycles largely restricts the practical application of silicon-based anodes. In this thesis, three materials that can effectively adapt to the volume expansion of silicon-based anodes and improved stability are described. As we expected, when the materials are used as the anode of the lithium ion batteries, the materials exhibit excellent electrochemical performance and superior lithium storage performance. In chapter 1, the history and background of the development of lithium-ion batteries, as well as the recent development status are first introduced. By analyzing the reaction principle and composition of lithium-ion batteries, traditional commercial anode materials are less able to bear the urgent needs, so anode materials with high specific capacity are indispensable. A great deal of research then focused on silicon-based material, which with a specific capacity ten times that of graphite. Based on the principle of silicon embedded with lithium, the structure can adapt to volume expansion and improve the electrical conductivity of the material, which is an important step to advance the lithium ion battery. Silicon-based composites combine silicon with other materials with better flexibility and electrical conductivity, retaining high capacity, while improving the mechanical strength and electrical conductivity of the composites. In the actual test, the silicon-based materials also show superior electrochemical performance. In chapter 2, silicon materials with a thin hollow structure to accommodate the expansion and maintain the electrochemical stability of lithium ion batteries was constructed. Hollow silicon nanotubes （HSiNTs） were synthesized on carbon cloth by reducing silicon oxide and corroding zinc oxide nanorods templates. The resulting HSiNTs/CC was directly used as the anode of lithium-ion batteries without any binders or conductive additives, exhibiting superior Li-battery performance with large reversible capacity, excellent cyclic performance, and good rate capability. A reversible capacity of 1420 mAh g-1 was achieved at a current density of 100 mA g-1. After 100 cycles, the fabricated LIBs retained 93.7% of the initial capacity. Even when the current density was increased to 1000 mA g-1, the LIBs had a capacity of 871 mAh g-1 and retained 89.7% of the initial capacity after 80 cycles. The results demonstrate that thin hollow structures are well-suited to accommodate the volume expansion of silicon and improve the stability of the HSiNTs/CC anode during the lithiation-delithiation cycles. In chapter 3, surface engineering strategy is adopted to develop the ultra-stable silicon/carbon anode for lithium-ion batteries. Deposited thin silicon on carbon substrate （DTSi/CC） was synthesized, and directly used as the anode without any binders or conductive additives. Electrochemical measurements indicated that fabricated LIBs achieved a reversible capacity of 1457 mAh g-1 and retained 70.9% of the initial capacity at a current density of 100 mA g-1 after 100 cycles. Even when the current density was increased to 1000 mA g-1, the LIBs boasted a capacity of 1037 mAh g-1 and 76.8% capacity retention after 500 cycles. The results demonstrated that thin layer structures with plenty of buffer space well suit to accommodate the volume expansion of silicon anode and improve the stability during cycles. In chapter 4, a creative and effective strategy for synthesizing composite materials of hydrothermal self-assembled silicon nanosphere and two-dimensional material Cu2MoS4 （Cu2MoS4/SiNS） was elaborated. The porous silicon dispersed on a two-dimensional material Cu2MoS4/SiNS can effectively release the volume expansion and mechanical stress generated, serving the two-dimensional layered structure that can provide a fast channel for ion transmission. As expected, when used as the anode of lithium-ion battery, the Cu2MoS4/SiNS material exhibits an enhanced specific capacity and excellent stability. At the current density of 100 mA g-1, it boasted a delightful discharge specific capacity of 1920 mAh g-1, and even can receive the capacity of 1330 mAh g-1 when the current density increases to 1.0 A g-1 after 100 cycles. When further increased the current density to 2.0 A g-1 to test the fast charging performance of the Cu2MoS4/SiNS material, we got exciting results that the specific capacity of 1170 mAh g-1 and 88.7% capacity retention can still be maintained after 500 cycles. Finally, the general conclusions and generalizations of this thesis on design and synthesis of materials are given, and the application prospects of silicon-based materials on lithium-ion batteries are predicted. In general, these three kinds of silicon-based composites shown excellent electrochemical performance and stability of lithium storage after thoughtful design synthesis. The ultra-stable performance and superior capacity of the materials obtained by the straightforward synthesis route provide the potential direction for the construction of high-performance lithium-ion batteries.

内容記述タイプ

TableOfContents

内容記述

1 Introduction||2 Hollow-Structure Engineering of Silicon-Carbon Anode for Ultra-Stable Lithium-ion||3 Surface engineering sinking silicon as anode to improve LIB stability and capacity||4 Self-assembled silicon combined with two-dimensional materials to improve electrode stability

備考

内容記述タイプ

Other

内容記述

九州工業大学博士学位論文学位記番号：生工博甲第414号学位授与年月日：令和3年9月24日

キーワード

主題Scheme

Other

主題

Silicon-based material

キーワード

主題Scheme

Other

主題

LIB anode

キーワード

主題Scheme

Other

主題

Energy

キーワード

主題Scheme

Other

主題

Stability

キーワード

主題Scheme

Other

主題

Straightforward synthesis

アドバイザー

馬, 廷麗

学位授与番号

甲第414号

学位名

博士（工学）

学位授与年月日

2021-09-24

学位授与機関

学位授与機関識別子Scheme

kakenhi

学位授与機関識別子

17104

学位授与機関名

九州工業大学

学位授与年度

内容記述タイプ

Other

内容記述

令和3年度

出版タイプ

VoR

出版タイプResource

http://purl.org/coar/version/c_970fb48d4fbd8a85

アクセス権

open access

アクセス権URI

http://purl.org/coar/access_right/c_abf2

ID登録

10.18997/00008672

ID登録タイプ

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シリコン系負極材料の合成、キャラクタリゼーション及び高性能リチウムイオン電池への応用

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