以電化學雙電池模組促進分解氮氧化物與二氧化硫之實際應用性研究

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研究生：	李承晉 Lee, Cheng Chin
論文名稱：	以電化學雙電池模組促進分解氮氧化物與二氧化硫之實際應用性研究 A study of practical applications of promoted decomposition of nitrogen oxide and sulfur dioxide via a module of electrochemical double-cell
指導教授：	黃大仁 Huang, Ta Jen
口試委員:	葉君棣呂世源汪上曉竇維平
學位類別：	博士 Doctor
系所名稱：	工學院 - 化學工程學系 Department of Chemical Engineering
論文出版年：	2015
畢業學年度：	103
語文別：	中文
論文頁數：	116
中文關鍵詞：	電化學雙電池、電觸媒蜂巢、觸媒、氮氧化物、二氧化硫
外文關鍵詞：	electrochemical double cell, electro-catalytic honeycomb, catalyst, nitrogen oxide, sulfur dioxide
相關次數：	點閱：2 下載：0
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引擎的技術不斷的進步，燃燒效率增加，產生更多氮氧化物廢氣，以及工廠廢氣中大量排放的二氧化硫廢氣，按照現有商業化技術皆沒有辦法完美的處理此兩樣化合物。而目前已經出現電催化處理氮氧化物之技術，且在相關理論與實驗皆以取得很大的成果，且利用電催化技術發展出來的陶瓷支撐電化學雙電池具有可以處理氮氧化物和硫氧化物的兩種功能，惟平板陶瓷材料無法大面積且大量的生產，且耗費材料成本巨大，因此，本研究之主要目的首先為利用陽極來當作支撐體，對於陽極支撐型電化學雙電池進行一系列活性測試，進而發展出電化學雙電池模組，參考製程至蜂巢觸媒轉化器，進行真實廢氣的催化效果測試。
在電化學雙電池板實驗中，再次證實確實有二氧化硫和氮氧化物的處理效果，對於二氧化硫在不同氧濃度與溫度下的分解做出一系列結果，另外也將其規模擴大(scale-up)到蜂巢製程，發現其觸媒的單位面積反應速率可能會因為紊流(turbulent flow)而比平板效果更佳，另外呈現了在不同系統下的電觸媒蜂巢處理效果，其效果在不同的系統下都有選擇性觸媒還原的數十倍反應速率，證明其應用於業界的潛力。

Because of the progress of technique of engine,there are more and more exhaust gas ,like NOx and SO2,discharged into the atmosphere.
According to existing commercial technologies are no perfect way to deal with this different harmful compounds.Our group have developed the promoted nitrogen oxides decomposition technology since several years age and we made great achievements theoretically and experimentally.
The use of electro-catalytic technology developed ceramic supported electrochemical double cell can handle nitrogen oxides and sulfur oxides at the same time.This study show that we can take advantage of the anode supported electrochemical double cell to treat NOx and SO2 greatly.
Then,we scale up the double cell into electro-catalytic honeycomb(ECH) and use ECH to treat the exhaust gas of boiler and diesel engine.The result of the experiment show that the reaction rate of ECH can reach several times of reaction rate of SCR.This result demonstrate the potential to be applied to the industry.

摘 要    II
Abstract    III
第一章 緒 論    1
第二章 文獻回顧    5
2-1. 氮氧化物的生成    5
2-2 氮氧化物排放與處理    7
2-2-1三相觸媒(three-way catalysts)還原氮氧化物    9
2-2-2選擇性觸媒還原法(selective catalytic reduction, SCR)    11
2-2-3氮氧化物儲存還原法( NOx  Storage Reduction,NSR )    13
2-3氮氧化物直接分解    15
2-3-1電化學還原法    15
2-3-2 SOFC處理NOx (SOFC-DeNOx)    17
2-3-3金屬氧化物催化分解氮氧化物    21
2-3-4氮氧化物於電觸媒陰極直接分解    25
2-4二氧化硫廢氣處理    34
2-4-1二氧化硫處理技術    34
2-4-2二氧化硫直接分解    38
2-5蜂巢狀觸媒結構(honeycomb)    41
2-5-1前言    41
2-5-2電解質的材料與燒結    42
第三章 研究構想    46
第四章 實驗方法與步驟    49
4-1. 實驗藥品    49
4-2. 粉體合成    52
4-2-1. NiO/YSZ陽極粉體合成    52
4-2-2 La0.6Sr0.4CoO3-δ (LSC)合成    52
4-3. 塗佈漿料合成    53
4-3-1. 平板用電解質漿料    53
4-3-2. 蜂巢電解質漿料    53
4-3-3. 平板用 GDC漿料    54
4-3-4. 蜂巢用 GDC漿料    55

4-5. 電觸媒蜂巢製作    61
4-5-1. 蜂巢陽極    61
4-5-2. 蜂巢電解質層製程    62
4-5-3. GDC層塗佈與燒結製程    63
4-5-4. 陰極層製程    65
4-5-5. 蜂巢還原與封裝製程    66
4-6. 實驗廢氣取樣系統    67
4-7. 實驗流程    70
第五章 實驗結果與討論    71
5-1. 電化學雙電池板(Electrochemical Double Cell plates,EDP)    71
5-1-1. 鑭鍶鈷(LSC)為EDP陰極材料行脫硝反應    72
5-1-2. 不同實驗參數對LSC-EDP的影響    74
5-2. 電化學雙電池板直接分解二氧化硫    85
5-2-1. 鑭鍶錳(LSM)為EDP陰極材料行脫硫反應    85
5-2-2. 不同實驗參數對LSM-EDP的影響    86
5-3. 電觸媒蜂巢ECH測試結果    95
5-3-1. 柴油引擎燃燒廢氣系統    95
5-3-2. 鍋爐燃燒廢氣系統    102
第六章  結 論    110
參 考 文 獻    113

                                

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