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| 研究生： |
容美蘭 Meilani - Kurniawati Wibowo |
|---|---|
| 論文名稱： |
A Computational Study of Sulfone-based Solvents for High-Voltage Li-ion Battery A Computational Study of Sulfone-based Solvents for High-Voltage Li-ion Battery |
| 指導教授： |
江志強
Jyh-Chiang Jiang |
| 口試委員: |
魏金明
Ching-Ming Wei 何嘉仁 Jia-Jen Ho |
| 學位類別： |
碩士 Master |
| 系所名稱： |
工程學院 - 化學工程系 Department of Chemical Engineering |
| 論文出版年： | 2013 |
| 畢業學年度： | 101 |
| 語文別： | 英文 |
| 論文頁數： | 57 |
| 中文關鍵詞： | sulfone-based solvents 、high oxidation potential 、high-voltage Li-ion battery |
| 外文關鍵詞： | sulfone-based solvents, high oxidation potential, high-voltage Li-ion battery |
| 相關次數： | 點閱：177 下載：0 |
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The high-voltage cathode materials in Li-ion battery need to be matched with high-oxidation potential of electrolyte system. Therefore, the search of high-voltage electrolyte has become a high priority. This study is to propose new sulfone-based solvent molecules; 3-((difluoroboryl)sulfonyl)propanenitrile (DSPN), 3-((difluoroboryl)- sulfonyl)propane (DSP), and 1-difluoroboryl-2-((methyl)sulfonyl) ethane (DMSE) with high oxidation potential. With the aid of quantum chemistry calculation using Moller Plesset perturbation theory, we calculate the electrochemical properties, oxidative and reductive decomposition of these sulfone-based solvents. On the basis of our calculation, we found that the oxidation potentials of these sulfone-based solvents are higher than those of the organic carbonate-based solvents. These sulfone-based solvents show high oxidative stability due to the high energy is needed to form the radical cation. Whereas it is easy to further decompose with lower energy barrier after the formation of radical cation. The primary products from the oxidative decomposition are BF2+, SO2, SO, CH2CH2CN radical, OCH2CH2CH3 radical, CH2CH2CH3 radical, [CH3SO2]+ and CH2BF2 radical. On the other hand, these sulfone-based solvents are easy to be reduced and form the thermodynamically favourable radical anion, which is difficult to decompose since the energy barrier of the decomposition reaction is relative high. Therefore these sulfone-based solvents have no tendency to form the SEI on the anode surface. The primary products of reductive decomposition are BF2 radical, SO2, [CH2CH2CH3]-, [CH2CH2CH3]-, and [CH3SO2CH2CH2]-.
The high-voltage cathode materials in Li-ion battery need to be matched with high-oxidation potential of electrolyte system. Therefore, the search of high-voltage electrolyte has become a high priority. This study is to propose new sulfone-based solvent molecules; 3-((difluoroboryl)sulfonyl)propanenitrile (DSPN), 3-((difluoroboryl)- sulfonyl)propane (DSP), and 1-difluoroboryl-2-((methyl)sulfonyl) ethane (DMSE) with high oxidation potential. With the aid of quantum chemistry calculation using Moller Plesset perturbation theory, we calculate the electrochemical properties, oxidative and reductive decomposition of these sulfone-based solvents. On the basis of our calculation, we found that the oxidation potentials of these sulfone-based solvents are higher than those of the organic carbonate-based solvents. These sulfone-based solvents show high oxidative stability due to the high energy is needed to form the radical cation. Whereas it is easy to further decompose with lower energy barrier after the formation of radical cation. The primary products from the oxidative decomposition are BF2+, SO2, SO, CH2CH2CN radical, OCH2CH2CH3 radical, CH2CH2CH3 radical, [CH3SO2]+ and CH2BF2 radical. On the other hand, these sulfone-based solvents are easy to be reduced and form the thermodynamically favourable radical anion, which is difficult to decompose since the energy barrier of the decomposition reaction is relative high. Therefore these sulfone-based solvents have no tendency to form the SEI on the anode surface. The primary products of reductive decomposition are BF2 radical, SO2, [CH2CH2CH3]-, [CH2CH2CH3]-, and [CH3SO2CH2CH2]-.
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