本研究從三個方向提升鐵氧磁體程序（ferrite process, FP）的價值：首先是藉由FP污泥資源化生產觸媒以扭轉FP成本較高的劣勢；其次是發展延長反應式鐵氧磁體程序（extended reaction ferrite process, ERFP）及淘洗程序以增進FP的效能；第三是整合Fenton氧化法作為FP的前處理程序以解決螯合劑影響FP的困擾。
在測試了六種以FP製作的鐵氧磁體觸媒（MxFe(3-x)O4 , M = Cu, Zn, Mn, Ni, Cr, Fe）後發現：Cu/Fe莫耳比為 1/2.5 的銅鐵氧磁體觸媒（Cu-ferrite catalyst）只需要140℃的反應溫度就能夠在空間速度為 6000 hr-1 的條件下，把入口濃度4000 ppm的CO完全轉化為CO2 。而且即使O2 濃度減少至只剩1 %，鐵氧磁體觸媒的催化性能仍不受影響，顯示其對於氧化反應有極佳的發展潛力。
另一方面，為了利用FP發展一套可以處理大多數重金屬廢液的程序，吾人配製了極端複雜的模擬廢液，其中包含十種常見的重金屬：Cd、Pb、Cu、Cr、Zn、Ag、Hg、Ni、Sn、Mn濃度各為0.002 M。實驗數據指出雖然傳統的FP無法完整處理此種廢液，但應用ERFP可以處理至滿足法規要求。ERFP延長段的FeSO4加藥方式以間歇式優於連續式，最佳的操作參數在初始段為：pH= 9、FeSO4加藥量= 0.2 mol/L、溫度= 90 oC、空氣供應量= 3 L/min/L、反應時間= 40 min；在延長段為：間歇式投藥，每5 min一次，每公升廢液投入10 mL 1M-FeSO4 溶液、pH= 9、溫度= 90 oC、空氣供應量= 3 L/min/L、反應時間= 80min。淘洗程序可適度節省ERFP的費用並進一步確保污泥品質能符合毒性特性溶出程序（toxicity characteristic leaching procedure ,TCLP）之標準，建議在pH 2.88至4之間操作，淘洗時間為6小時。
實驗結果亦確認了先使用Fenton氧化法分解去除螯合劑再以FP處理重金屬，可完全解決螯合劑干擾的問題。Fenton/ ERFP串聯程序中Fenton氧化法去除EDTA最佳的條件組合如下： pH= 2、亞鐵離子初始濃度[Fe2+]0 = 1×10-2 M 、過氧化氫添加速率= 5×10-4 mol/min/L，此反應可在10 min內完成。
最後，基於研究的心得歸納出應用FP及輔助方法處理重金屬廢液的實施策略，並且實際處理多種實場廢液都獲得令人滿意的成效。

This work increased the value of ferrite process (FP) in three directions: firstly, changed the inferiority of FP on cost by transforming the FP sludge into a catalyst; secondly, used ERFP and elutriation to promote the performance of FP; thirdly, developed Fenton oxidation as a pretreatment step for avoiding the interference from chelating agents.
Six ferrite catalysts (MxFe(3-x)O4, M = Cu, Zn, Mn, Ni, Cr or Fe) formed from FP were tested. Experimental results indicate that the Cu-ferrite catalyst with a Cu/Fe ratio of 1/2.5 can completely convert CO to CO2 at an inlet CO concentration of 4000 ppm and a space velocity of 6000 hr-1 were held at 140℃. The catalytic performance of Cu-ferrite did not reduce even when the concentration of O2 was just 1%. This work proves that the ferrite catalysts have good potential for catalyzing oxidation.
For developing FP for effectively treating almost all heavy metal waste liquid, hence an extremely difficult treating target- simulated waste liquid was designed. It contains ten heavy metals - Cd, Pb, Cu, Cr, Zn, Ag, Hg, Ni, Sn and Mn, each at a concentration of 0.002 M. Although conventional FP could not be used to treat the simulated waste liquid completely, the enhanced FP, i.e. ERFP, could be used to satisfy regulatory limits. FeSO4 can be added in the extended stage of ERFP intermittently rather than continuously. The optimum operating parameters in the initial stage are pH = 9 , FeSO4 dosage = 0.2 mol/L, temperature = 90 oC, air supply rate = 3 L/min/L and reaction time = 40 min; in the extended stage, they are intermittent dosing, adding 10 mL 1M-FeSO4 solution per liter waste liquid every 5 min, pH = 9, temperature = 90 oC, air supply rate = 3 L/min/L and reaction time = 80min. Elutriation was conducted to reduce the cost of ERFP and ensure that the sludge met Toxicity Characteristic Leaching Procedure (TCLP) standards. An operating pH from 2.88 to 4 and an elutriation time of 6 h were recommended.
Used Fenton oxidation to decompose chelating agent in waste liquid and then treated heavy metal by FP, this research showed that under proper operational conditions Fenton/ ERFP could completely solve the chelating agent interference problem. The best condition for decreasing EDTA using the Fenton method was: pH = 2, ferrous ion initial concentration [Fe2+]0 = 1×10-2M, hydrogen peroxide addition rate = 5×10-4 mol/min/L and reaction time = 10 min.
Lastly, a lot of real waste liquids were treated satisfactorily by applying the results of this study.

摘要…………………………………………………………………………I
Abstract………………………………………………………………….. III
目錄…………………………………………………………………..……V
圖目錄……………………………………………………………………XI
表目錄……………………………………..……………………………XIII
第一章序論……………………………………………………………... 1-1
1-1 研究緣起……………………...…………………………………... 1-1
1-2 研究目的及架構…………………………………………..………1-4
1-2-1 鐵氧磁體污泥資源化產製觸媒….............................................. 1-4
1-2-2 鐵氧磁體程序的改良………………………………………...…1-5
1-2-3 整合Fenton氧化法作為鐵氧磁體程序的前處理方法………..1-5

第二章文獻回顧……………………………………………...……..….. 2-1
2-1 重金屬廢液之定義及傳統的處理程序………………..……….... 2-1
2-1-1 重金屬廢水/廢液……………………………………………..…2-1
2-1-2 重金屬廢液的傳統處理程序…………………………….…..... 2-3
2-2 鐵氧磁體程序之理論與相關研究…………………………….…. 2-4
2-2-1 鐵氧磁體程序…………………….…………...…………….…..2-4
2-2-2 鐵氧磁體的基本性質……………....……………………….…. 2-9
2-2-3 鐵氧磁體的合成方法………………………..……………….. 2-14
2-2-4 鐵氧磁體程序之影響因子………………………………...…. 2-16
2-3 鐵氧磁體觸媒與觸媒焚化技術…………..……………….……. 2-19
2-3-1 鐵氧磁體觸媒之相關研究………………….……………….. 2-19
2-3-2 觸媒焚化技術…………………………………………...……. 2-21
2-3-3 轉化一氧化碳為二氧化碳……………………………….……2-23
2-4 EDTA之基本特性及相關研究……………………………..….. 2-26
2-4-1 EDTA之基本特性……………………………………..…….. 2-26
2-4-2 EDTA之應用概況………………………………………...….. 2-29
2-4-3 處理EDTA之相關研究…………………………………….…. 2-30
2-5 Fenton氧化法…………………………………………….……... 2-31
2-5-1 Fenton氧化原理與應用………………………………………. 2-31
第三章鐵氧磁體污泥資源化產製觸媒………………………………... 3-1
3-1 研究方法………………………………..……………………...…. 3-1
3-1-1 鐵氧磁體觸媒之合成……………………...……………………3-1
3-1-1-1 FP反應設備………………………………………………….. 3-1
3-1-1-2 觸媒合成之程序及條件……………………….…………..... 3-3
3-1-2 觸媒反應設備………………………………………..…………3-5
3-1-2-1 觸媒反應器………………………………………………...... 3-5
3-1-2-2 氣體成分分析……………………………………….……..... 3-5
3-1-3 實驗規劃……… ………………………………………..………3-7
3-1-3-1 活性金屬篩選………………..……………………………..... 3-7
3-1-3-2 M/Fe對催化效果的影響……………….………………….…3-7
3-1-3-3 O2濃度對催化效果的影響……………………………..……. 3-7
3-1-3-4 CO2濃度對催化效果的影響…………………………………3-8
3-1-3-5 溼度對催化效果的影響……………………………………... 3-8
3-1-3-6 觸媒表面性質分析………………………………………….. 3-8
3-1-3-7 鐵氧磁體粒徑分布………………………………….………. 3-9
3-2 結果與討論…………………………………………...…………. 3-10
3-2-1 活性中心金屬種類的選擇……………………………..…….. 3-10
3-2-2 M/Fe對催化效果的影響………………………………………3-12
3-2-3 O2濃度對催化效果的影響…………………………………... 3-15
3-2-4 CO2濃度對催化效果的影響………………………………..... 3-21
3-2-5 溼度對催化效果的影響…………………………………..….. 3-23
3-2-6 觸媒表面性質分析………………………………………….... 3-23
3-2-7 鐵氧磁體粒徑分布…………………………..……………….. 3-25
3-2-8 應用FP 衍生ferrite catalyst的潛力………………………… 3-26
第四章鐵氧磁體程序的改良………………………………….……….. 4-1
4-1 研究方法……………………………………………………….…. 4-1
4-1-1 混雜性重金屬模擬廢液的配製……………………………….. 4-1
4-1-2 分析方法……………………………………………………….. 4-3
4-1-3 反應設備……………………………………………………….. 4-4
4-1-4 以傳統式FP處理混雜性重金屬廢液………………….………4-5
4-1-5 以ERFP處理混雜性重金屬廢液………………………………4-7
4-1-6 以淘洗法處理污泥…………………………………………….. 4-9
4-2 結果與討論………………………………………………..……. 4-10
4-2-1 以傳統式FP處理混雜性重金屬廢液…………………………4-10
4-2-2 以ERFP處理混雜性重金屬廢液……………………….……4-18
4-2-3 以淘洗法處理FP污泥……………………………..…………4-23
4-2-4 綜合討論…………………………………………………..….. 4-27
第五章整合Fenton氧化法作為鐵氧磁體程序的前處理方法……….. 5-1
5-1 研究方法…………………………………………………….……5-1
5-1-1 Fenton 氧化法分解 EDTA……………………………….……5-1
5-1-1-1 反應設備………………………………………………….….. 5-1
5-1-1-2 以Fenton 氧化法分解 EDTA實驗操作………………….…5-4
5-1-1-3 pH值對Fenton氧化法去除EDTA的影響…………………5-5
5-1-1-4 Fe2+添加量對Fenton氧化法去除EDTA的影響……………5-6
5-1-1-5 H2O2添加量對Fenton氧化法去除EDTA的影響……….…5-6
5-1-2 以Fenton / FP串聯處理含EDTA之重金屬廢液………..….. 5-6
5-1-2-1 模擬廢液的配製……………………..…………..…………... 5-6
5-1-2-2 Fenton氧化法反應條件…………………………………….. 5-7
5-1-2-3 FP反應條件………………………………………..…………5-7
5-1-2-4 TCLP實驗方法………………………………………………5-8
5-1-2-5 溶液中重金屬分析前處理………………………………….. 5-8
5-2 結果與討論 ……………………………………………………... 5-9
5-2-1 pH值對Fenton氧化法處理EDTA之影響………………….... 5-9
5-2-2 亞鐵離子添加量對處理效果之影響……………………….…. 5-9
5-2-3 過氧化氫添加量對處理效果之影響……………………….... 5-12
5-2-4 以Fenton / FP 處理含EDTA 及重金屬之廢水……………..5-14
第六章以鐵氧磁體程序與輔助方法處理實場廢液的實施策略……... 6-1
6-1 FP與輔助技術的實施策略…………………………………….…6-1
6-1-1 前處理的實施策略……………………….…………………..…6-1
6-1-2 FP及污泥處理方案的實施策略………………………………..6-4
6-2 以FP與輔助技術處理實場廢液………………………………... 6-6
6-2-1 以FP處理印刷電路板業蝕刻銅廢液並製作觸媒……………6-6
6-2-2 以FP和ERFP結合淘洗處理重金屬實驗室廢液……………6-8
6-2-2-1 實驗室廢液的特性…………………………………………... 6-8
6-2-2-2 以FP結合淘洗處理重金屬實驗室廢液………………….…6-9
6-2-3 以Fenton/FP串聯處理金屬表面處理廠廢液……………..…6-12
第七章結論與建議………………………………………….......……... 7-1
7-1 鐵氧磁體污泥資源化產製觸媒之研究成果……………………. 7-1
7-2 FP程序的改良之研究成果……………………………………….7-3
7-3 整合Fenton氧化法作為FP的前處理方法之研究成果………...7-4
7-4 展望與建議………………………………………………………. 7-5
參考文獻…………………………………………………………….…參-1
附錄：口試委員意見答覆及處理………………………………………附-1

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