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研究生:蕭偉利
研究生(外文):Hsiao, Wei Li
論文名稱:混合物實驗設計法配製高分子電解質與特性分析
論文名稱(外文):The Polymer Electrolytes are Prepared by the Mixture Design Method and Analyse the Properties
指導教授:杜景順
指導教授(外文):Jing-Shan DO
學位類別:碩士
校院名稱:東海大學
系所名稱:化學工程學系
學門:工程學門
學類:化學工程學類
論文種類:學術論文
論文出版年:1997
畢業學年度:85
語文別:中文
論文頁數:1
中文關鍵詞:高分子電解質電解質混合物實驗設計法
外文關鍵詞:SPEpolymer electrolytemixture design
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摘 要

本論文首先利用混合物實驗設計法探討PEO-LiCF3SO3-Tetraglyme
和PEO-LiCF3SO3-Tetraglycol兩系統之最佳導電度組合。利用Zeolite
和g-Al2O3添加至高分子電解質系統中,討論其對高分子電解質性質之
影響,最後將製備之高分子電解質組裝成Li / SPE / MnO2電池,探討
其放電特性。在混合物實驗設計法中改變PEO-LiCF3SO3-Tetraglyme和
PEO-LiCF3SO3-Tetraglycol高分子電解質之成分比例,實驗結果顯示,
當電解質組成範圍為15-67% (wt) PEO、10-20% LiCF3SO3及34-83%
Tetraglyme與10-77% PEO、10-20% LiCF3SO3及21-88% Tetraglycol
可得最佳導電度。22.0PEO / 19.0LiCF3SO3 / 59.0Tetraglyme與20.0
PEO / 17.0LiCF3SO3 / 63.0Tetraglycol(wt%)高分子電解質膜有較
佳的室溫導電度,分別為8.23×10-5S / cm及7.37×10-5S / cm。另外
,添加Zeolite和g-Al2O3於高分子電解質中,可增加電解質之機械性質
,且可增加導電度。

由線性掃描伏安法分析製備之高分子電解質之氧化分解電位,其分
解電位介於4.8V~5.4V之間。此外,添加Zeolite有增加氧化分解電位的
能力。

分析製備之高分子電解質鋰離子傳遞係數發現,在PEO-LiCF3SO3-
Tetraglyme系統中,當22.0PEO / 19.0LiCF3SO3 / 59.0Tetraglyme +
Zeolite(Zeolite / (PEO+LiCF3SO3 + Tetraglyme)=0.2)之下,在
55℃具有最大之tLi+,其值為0.27;而PEO-LiCF3SO3-Tetraglycol系統
中,當20.0PEO / 17.0LiCF3SO3 / 63.0Tetraglycol + Zeolite
(Zeolite / (PEO+LiCF3SO3 + Tetraglycol)=0.2)時,55℃下之最大
tLi+則為0.26。傳遞係數tLi+值會隨導電度的增加而增加,亦會隨著溫
度升高而逐漸增加。

利用循環伏安法分析鋰離子的沈積反應,由實驗結果發現鋰離子的
沈積反應為完全不可逆之行為。由此分析中可求得鋰離子在22.0PEO /
19.0LiCF3SO3 / 59.0Tetraglyme + g-Al2O3(g-Al2O3 / (PEO+LiCF3SO3
+ Tetraglyme)=0.1)與20.0PEO / 17.0LiCF3SO3 / 63.0Tetraglycol +
g-Al2O3(g-Al2O3 / (PEO+LiCF3SO3 + Tetraglycol)=0.2)高分子電解
質中的擴散係數分別為1.89×10-8cm2 / s與1.66×10-8cm2 / s。並求得
兩系統中之ana與k0之關係式,分別為ana=3.17×10-2及
k0 =2.10×10-5 exp (-1.07 E0*)與ana=3.05×10-2及
k0 =1.77×10-5 exp (-1.03 E0*)。

將製備所得之高分子電解質組裝成Li / SPE / MnO2一次電池,發現
仍須在高於55℃之環境下才會有較高的放電電容量,且其放電速率應該
小於0.382 mA / cm2。在自放電現象方面,添加Zeolite和g-A2O3於高分
子電解質中,發現能抑制自放電現象,當添加Zeolite和g-A2O3至PEO-
LiCF3SO3-Tetraglycol系統中,可使自放電率由6.2%減少為5.1%與5.3
% 。在55℃時以20.0PEO / 17.0LiCF3SO3 / 63.0Tetraglycol +
Zeolite (Zeolite / (PEO + LiCF3SO3 + Tetraglycol)=0.2)組
裝成電池,具 有最佳的放電電容量,其值為2.10 mAh。
Abstract

The maximum coductivity compositions of PEO-LiCF3SO3-Tetraglyme
and PEO-LiCF3SO3-Tetraglycol were studied in this thesis by
using the mixture design method. Zeolite and g-Al2O3
were added to modify the solid polymer electrolytes(
SPE). Using prepared SPE, the discharge
characteristics of Li / SPE / MnO2 was also studied.
The maximum conductivity composition intervals of two SPE
systems were experimentally found as 15-67% (wt) PEO
、10-20% LiCF3SO3 and 34-83% Tetraglyme for PEO-LiCF3
SO3-Tetraglyme as were as 10-77% PEO 、10-20% LiCF3SO3
and 21-88% Tetraglycol for PEO-LiCF3SO3-Tetraglycol. The
experimental also indicated that the maximum conductivities of
PEO-LiCF3SO3-Tetraglyme and PEO-LiCF3SO3-Tetraglycol were
8.23×10-5S / cm and 7.37×10-5S / cm, respectively, and its
compostions were 22.0PEO / 19.0LiCF3SO3 / 59.0Tetraglyme and
20.0 PEO / 17.0LiCF3SO3 / 63.0Tetraglycol(wt%)at room
temperature. In addition, the mechainical
characteristics and conductivity increased when
Zeolite and g-Al2O3 were added to SPE.
The decomposition voltages of the polymer electrolytes were
obtained by the linear sweep voltammetry in the rang of 4.8V ~
5.4V. The decomposition voltages of SPE increased as
Zeolite added. The experimental results
revealed that the maximum Li+ transfer numbers(tLi+)
for the systems of PEO-LiCF3SO3-Tetraglyme,
22.0PEO / 19.0LiCF3SO3 / 59.0Tetraglyme + Zeolite(Zeolite /
(PEO+LiCF3SO3 + Tetraglyme)=0.2)and PEO-LiCF3SO3-Tetraglycol,
20.0PEO / 17.0LiCF3SO3 / 63.0Tetraglycol + Zeolite(Zeolite /
(PEO+LiCF3SO3 + Tetraglycol)=0.2)were 0.27 and 0.26,
respectively, at 55℃. The Lithium ion transport number
increased with increasing conductivity and temperature.

The total irreverisible reaction was found in the deposition of
Li+ at stainless steel by the results of cyclic voltammetry.
Using cyclic voltammetry, the diffusion coefficient
of Li+ in the 22.0PEO / 19.0LiCF3SO3 /
59.0Tetraglyme + g-Al2O3(g-Al2O3 / (PEO+LiCF3
SO3 + Tetraglyme)=0.1) and 20.0PEO / 17.0LiCF3SO3 /
63.0Tetraglycol + g-Al2O3(g-Al2O3 / (PEO+LiCF3SO3 +
Tetraglycol)=0.2) were obtained as 1.89×10-8cm2 / s and
1.66×10-8cm2 / s, respectively. The parameter of ana were
also evaluated as 3.17×10-2 and 3.05×10-2, and the
relationships of k0 were obtained as 2.10×10-5 exp (-1.07 E0*)
and 1.77×10-5 exp (-1.03 E0*).

The better discharge capacity of Li / SPE / MnO2 was found when
the operating temperature was larger than 55℃, and the
discharge current density less than 0.382 mA / cm2. The
results indicated that Zeolite and g-Al2O3 can inhibit
the self-discharge of Li / SPE / MnO2. Comparison
with PEO - LiCF3SO3 - Tetraglycol with no additive, the
self-discharge fraction decreased from 6.2% to 5.1% and 5.3%,
respectively, when Zeolite and g-Al2O3 were added to modify this
SPE. When 20.0PEO / 17.0LiCF3SO3 / 63.0Tetraglycol +
Zeolite (Zeolite / (PEO + LiCF3SO3 + Tetraglycol)=0.2)
was used to prepare Li / SPE / MnO2, the maximum
discharge capacity was found as 2.10 mAh at 55℃.
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