中孔洞矽化合物及碳材之合成、鑑定 及其在染料吸附暨鋰離子電池負極應用;Synthesis and Characterizations of Ordered Mesoporous Silica and Carbon Materials and Their Applications as Adsorbents for Dye Adsorption and Anode Materials for Lithium Ion Batteries

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題名:	中孔洞矽化合物及碳材之合成、鑑定及其在染料吸附暨鋰離子電池負極應用;Synthesis and Characterizations of Ordered Mesoporous Silica and Carbon Materials and Their Applications as Adsorbents for Dye Adsorption and Anode Materials for Lithium Ion Batteries
作者:	王梓樺;Wang,Tzu-hua
貢獻者:	化學學系
關鍵詞:	中孔洞矽材;中孔洞碳材;染料吸附;鋰離子電池;碳負極;硬碳;mesoporous silica;mesoporous carbon;dye adsorption;lithium ion battery;carbon anode;hard carbon
日期:	2014-07-21
上傳時間:	2014-10-15 14:37:13 (UTC+8)
出版者:	國立中央大學
摘要:	本研究主要是利用非離子型介面活性劑Brij-76與TEOS (Tetraethyl orthosilicate) 、CES (Carboxyethylsilanetriol sodium salt) 做為共同矽源，一步合成出具有羧酸官能基的規則p6mm對稱中孔洞矽材簡稱為BCT-x系列，並且探討羧酸其官能基在不同pH值環境下對於一維鏈狀結構的小分子亞甲基藍吸附能力的影響。以及利用奈米模鑄法合成 p6mm 及 Ia d 對稱性的規則中孔洞碳材，比較合成出的碳材其孔洞結構性質差異及產生的影響，藉此探討不同結構的規則中孔碳材作為負極材料時，其結構的差異性對於電池的充放電次數，導電度，可容納的鋰離子數目，電容量的差異等等，並且作為吸附劑時，染料分子在其中的吸附情形．以及其p6mm 及 Ia d 對稱的孔道結構對於一維鏈狀結構的小分子亞甲基藍吸附能力的影響．在鋰離子電池的負極應用中，則探討p6mm 及 Ia d 對稱性的規則中孔洞碳材在不同比例下 (碳材:導電碳黑:PVDF=8:1:1、7:2:1) 的電性表現，以及孔洞結構對於電容量的影響，結果發現在表面積、碳材層間距、雜質、導電度都相同的情況下，Ia d孔洞碳材表現出相當出色的電容量，並且在多次充放電之後維持著相當傑出的表現，尤其在活物：碳黑：PVDF比例7:2:1的樣品表現，在60次充放電之後仍舊維持在550mAh/g的水準，幾乎為石墨理論電容量的兩倍．對於吸附小分子結構的亞甲基藍，發現碳材不管是p6mm 還是 Ia d孔道結構，大致上隨著其材料的表面積愈大，吸附量就愈大，且由 Langmuir 及 Freundlich 等溫吸附模型的分析，屬於Langmuir單層吸附。另外，藉由 pseudo-first-order 及 pseudo-second-order 動力學模型的分析，發現碳材對其吸附模式較適合用 pseudo-second-order 動力學模型來描述。　　在中孔洞矽材BCT-x系列則發現在較高pH值下時，含羧酸官能基的樣品染料吸附比較符合 Langmuir 所假設的單層吸附模式，當pH值較低時吸附量只和表面積相關，所以證明孔洞表面積在不含羧酸官能基時為影響其吸附此小分子染料的主要因素。並且在pH =9時，含羧酸官能基30%的BCT-30%樣品其單位表面積的吸附量為不含羧酸官能基樣品BCT-0%的兩倍。並且不論在任何pH值下其吸附模式皆適用 pseudo-second-order 的動力學模型來進行描述。 ;Periodic mesoporous organosilicas (PMOs) have attracted great scientific interest since 1990s due to their applications in various fields. The thesis is mainly focused on two types of mesoporous materials. The first type is carboxylic acid functionalized mesoporous silicas with hexagonal structures (p6mm symmatry) and they were synthesized by using simple one-pot synthesis route. The other type is ordered mesoporous carbon (OMC) materials with cubic structures (Ia d symmatry). The mesoporous carbon materials were synthesized by nanocasting method. Both the mesoporous materials were used as adsorbents for the adsorption of dye. The main purpose of this work is to compare the dye adsorption ability when different amounts of carboxylic groups are incorporated into mesoporous silicas, and to investigate whether the electrostatic attraction dominates the adsorption process or not in the solution with different pH values. Moreover, the dynamics model and thermodynamics model during adsorption were analyzed. Rechargeable lithium-ion battery (LIB) is one of the most promising batteries which is currently used in many portable electronic devices and electric vehicles due to its high energy density, long cycle life, and low toxicity. In recent years, there are some applications of mesoporous carbons as anode materials for lithium ion batteries because of their high specific capacity. In the present work, ordered mesoporous carbons CMK-3 and CMK-8 were characterized for their use as anode materials in lithium ion batteries. A comparative study of their performances was carried out to evaluate the role of their morphologies and structures in electrochemical behavior. The first cycle discharge capacity of 964 and 1983 mAh g-1 were obtained for CMK-3 and CMK-8, respectively. The synthesized materials have great prospect to be used in commercial batteries.
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