化學迴路程序具有多種優勢，例如減少燃料中氮元素氧化所產生之NOx以及提高二氧化碳在廢氣中的濃度。而化學迴路釋氧程序是一種在高溫下以載氧體產生之氧氣燃燒固體廢棄物的新興技術。本研究利用熱重分析儀（TGA）分析載氧體的鐵錳重量比、粒徑大小及鍛燒溫度對反應性和循環性的影響，在Fe2O3和Mn2O3以重量比3：1混合，並篩選粒徑大小為2毫米的顆粒以900 ℃之空氣環境中鍛燒2小時之條件製備時，鐵錳載氧體具有較佳的效能，其中，摻入氧化錳是改善循環性的關鍵。以X光繞射儀（XRD）、掃描電子顯微鏡（SEM）和能量分散式光譜儀（EDS）分析反應過程中鐵錳載氧體的晶體結構與表面形態之變化。檢測結果顯示反應前之鐵錳載氧體由Fe2O3和FeMnO3組成，表面多有利於增進質傳的細小分支與不規則孔洞，而隨著還原程度增加，晶體結構逐漸轉變成Fe與MnO且表面有些微的燒結現象發生。以TGA紀錄瞬時之重量變化與氣固反應模型計算，鐵錳載氧體以氫氣還原符合一階孔擴散反應機制，經線性回歸得表觀活化能為17.06 kJ/mole。進行化學迴路燃燒程序前，探討了三聚氰胺甲醛樹脂（MF resin）為主成分之廢棄塑膠製品和以廢棄木造建材與漂流木製成之垃圾衍生燃料（RDF）在不同升溫速率之熱裂解行為並計算在各轉化率下之活化能，結果顯示提高升溫速率對熱裂解速率有顯著的正面效果，但也會使DTG之峰值延後，並以Flynn-Wall-Ozawa模型預測兩燃料之轉化率較為適合。本研究以固定床反應器進行化學迴路燃燒程序實驗，研究鐵錳載氧體與燃料之重量比和反應溫度對煙氣組成的影響。以煙氣組成分析儀紀錄瞬時的煙氣濃度變化，結果顯示提高載氧體與燃料之重量比和反應溫度都可以促進燃燒效率。本研究對鐵錳載氧體的合成比例、鐵錳載氧體的還原模型、MF resin與RDF之熱裂解行為與各轉化率下之活化能以及化學迴路燃燒MF resin與RDF之操作參數對煙氣組成的影響。

Chemical looping process (CLP) has exceptional performance such as reducing NOx production due to oxidation of fuel-N and increasing CO2 concentration in exhaust gases. Chemical looping with oxygen uncoupling (CLOU) is one of CLP technology that could burn the solid waste with gaseous oxygen at elevated temperature. In this study, the reactivity and recyclability of iron-manganese oxygen carriers in various compositions, particle sizes, and calcination temperatures were evaluated by thermogravimetric analyzer. Considering the reactivity and recyclability, oxygen carriers containing 75 % iron oxide in particle size 2.00 mm calcined at 900 ℃ is suitable for CLOU process. The presence of manganese oxide is the key to enhances the recyclability of oxygen carriers. The crystal structure and surface morphology of oxygen carriers before and after the reaction was analyzed by X-ray diffraction (XRD), scanning electron microscope (SEM), and energy-dispersive X-ray spectroscopy (EDS), respectively. XRD patterns showed the composition of fresh oxygen carriers was mixed by Fe2O3 and FeMnO3 then reduced to Fe and MnO gradually. The surface of fresh oxygen carriers showed small branches and irregular pores which were beneficial to the mass transfer, however, the sintering phenomenon happened was observed in SEM images after the reaction. The reduction kinetics was discussed under hydrogen atmosphere and proposed based on the gas-solid model. The regression analysis showed that reduction of oxygen carriers could be modeled by first order pore diffusion model and the apparent activation energy is 17.06 kJ/mole. This work involved two types of solid fuels used in CLOU process. One is the waste plastic made out of melamine-formaldehyde (MF) resin which is a thermosetting polymer and the other is refuse derived fuel (RDF) mainly made from agricultural and forestry residues, wood waste.
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