純氧燃燒與碳捕捉封存被視為兼顧產能與低汙染排放之潛力燃燒技術之一，若結合具碳中和特性之生質料於能源系統(產電/熱)，亦可逐漸降載對化石燃料的高度依賴與達成負碳排之目標。有別於傳統空氣燃燒，純氧燃燒時需將部分煙道氣體迴流至燃燒室用以控制爐溫，可分為乾迴流(O2/CO2)與濕迴流(O2/H2O/CO2)。其中濕迴流模式下的生質料燃燒過程極為複雜，牽涉許多異相與氣相反應及燃燒現象仍待釐清。因此，本研究選用木顆粒作為代表燃料，探討在不同溫度與氣體氛圍中的點燃與燃燒機制。首先透過成份分析、熱重分析、恆溫裂解產氣等實驗進行燃料基礎受熱特性探討，並建置一套新型單顆料錠燃燒系統，量測木顆粒在均溫強制對流環境(空氣、乾/濕迴流純氧燃燒)下之影像、質量、顆粒溫度與尾氣變化。最後利用反應動力學搭配化學反應機制模擬氣態揮發份(C0-C3碳氫燃料)的自動點燃特性。
熱重分析結果顯示，木顆粒在空氣下的質量流失溫度區間主要在240–400°C與400–520°C，異相點燃發生在293°C，整體活化能約介於108.8–184.8 (kJ/mol)。然而，在空氣環境下之燃燒特性指數(Dv, Di, Db與S index)顯示與21–30%之純氧環境(O2/CO2)相當。單顆木顆粒(0.5 g)在恆溫下的燃燒實驗發現當環境氣流溫度Ts ≥ 550°C時有明顯的氣態火焰點燃，且在Ts = 650°C時機制發生了轉變，這是由於快速脫揮發導致氧氣在受熱初期無法擴散至焦炭表面，因此氣相點燃率先發生。尾氣分析呈現焦炭燃燒階段具有較高的CO排放，揮發份燃燒時氣態燃料則傾向轉為CO2。基於不同起始溫度與氣體環境，歸納了熱裂解、異相氧化、氣相氧化與異相氣化反應，並確立了焦炭與氣態火焰之點燃溫度區間，可作為生質料在熱化學轉換應用時之操作參考。
在Ts = 550°C與Re = 450之純氧對流環境下，氣態火焰穩駐燃燒發生在氧氣濃度需大於21%。而隨著H2O取代CO2，顆粒燃燒溫度與重量流失速率均明顯提升。當Oxy-21%時，若以H2O取代20%的CO2，反應時間ti,char、ti,flame、tchar與ttotal分別縮短7.89%、6.02%、17.98%與16.05%，這是由於H2O相較於CO2具有較高的熱擴散係數(約2.1倍)，且O2在H2O中的質量擴散能力也較高(約1.61倍)，因此促進整體反應速率的提升。此外，發現tflame大幅度地上升約266%，此為H2O增進了焦炭氣化反應並轉移部份燃料至可燃性氣體的緣故。最後歸納在純氧環境(15–33% O2搭配0–50% H2O)下的正規化焦炭燃燒時間關係式為[O2]-1.616[H2O]-0.232，顯示氣體與焦炭的反應速率依序為char-O2 > char-H2O > char-CO2。此外，木顆粒在27%O2/73%CO2及21%O2/50%H2O/29%CO2環境下的總燃燒時間顯示與空氣燃燒相當。
數值模擬結果顯示除了CO之外，大多數C0-C3燃料可在450–550°C空氣中引燃，與實驗觀測到的揮發分火焰點燃溫度區間相似。在550°C純氧環境中，點燃時間隨著O2與H2O濃度的提升而降低。在Oxy-21%環境下且H2O逐漸取代CO2時，可發現OH與H自由基濃度明顯提升，且主導最大熱釋率的反應步驟顯示逐漸由R3(H2+OH↔H+H2O)與R91(CH3+O↔CH2O+H)轉移至R35(CO+OH↔CO2+H)與R6(H+OH+M↔H2O+M)。點燃時間的靈敏度分析則顯示R98 (CH3+HO2↔CH3O+OH)、R156 (CH2O+HO2↔HCO+H2O2)與R46 (CH4+HO2↔CH3+H2O2)為主導步驟。最後，關於H2O在純氧對流環境下取代CO2時促進生質料的氣相引燃現象，本研究提出以流體停滯時間(tflow)與化學反應時間(tchem)之關係式加以描述。添加水氣會導致燃料脫揮發速率與氣相化學反應速率提升，降低tchem，使達姆科勒數(Damköhler number)的上升速率高於在O2/CO2環境下，率先達臨界值而發生火焰引燃。本研究提供了對生質料點燃和燃燒基本原理的探討，可作為未來將生質料應用在濕迴流純氧燃燒系統之參考。

Oxy-fuel combustion is a promising strategy for carbon capture and storage (CCS). The transition from burning fossil fuels to carbon-neutral biomass enables negative CO2 emissions with CCS. Nowadays, numerous studies have compared coal combustion in O2/CO2 with air. However, due to the complexity of the thermal behaviors in ignition and char conversion stages, the combustion of biomass pellets in wet flue gas recirculation scenario remains unclear and there is scarce literature. In this study, the ignition and combustion mechanism of a single wood pellet in air and oxy-atmospheres over wide temperature ranges has been investigated and implemented by several experimental approaches, such as TG-FTIR analysis, packed-bed pyrolysis, and a novel single-particle combustion under isothermal convective heating. In addition, kinetic modeling was carried out by CHEMKIN simulation to identify the autoignition characteristics of volatile fuels.
The results showed that wood primarily decomposed between 240–520°C, and the heterogeneous ignition was found to occur at 293°C as the hemicellulose component in wood could initiate the exothermic reaction at a low temperature. The rate of char combustion highly depends on oxygen diffusion. The combustibility index revealed that wood combustion in the air is similar in the range of oxy 21–30%. Regarding pellet combustion in an isothermal hot air stream, a unique heterogeneous-induced homogeneous combustion phenomenon was observed at stream temperature Ts ≥ 350°C. In addition, the ignition mechanism shifted to homogeneous mode at 650°C because of the interplay of devolatilization and O2 diffusion near the fuel surface. It was also observed that char combustion favored the production of CO, and volatiles burning tended to convert fuel into CO2. Based on the temperature and gas surroundings, a reaction scheme including pyrolysis, heterogeneous oxidation, homogeneous oxidation, and heterogeneous gasification of wood pellets was identified.
According to oxy-fuel combustion under 550°C and Re = 450 conditions, the stabilized volatile flame around the wood pellet appeared when O2 ≥ 21%. With H2O partially replacing 20% of CO2 at oxy-21%, the ignition delay time of char (ti,char) and flame (ti,flame), char combustion duration (tchar), and total combustion time (ttotal) reduced 7.89%, 6.02%, 17.98%, and 16.05% was found, respectively. It is attributing that H2O possesses a higher thermal diffusivity (2.1 times) and O2 mass diffusivity (1.61 times) than CO2, which promotes combustion. In particular, volatile flame burning duration (tflame) significantly elevated 266% due to char-H2O gasification reaction shifting carbon to flammable fuels to sustain the flame. The obtained correlation equation of normalized char combustion time was varied by [O2]-1.616[H2O]-0.232 relation in O2/H2O/CO2 atmospheres under 15–33% O2 and 0–50% H2O combination, demonstrating that reaction rates follow char-O2 > char-H2O > char-CO2. Furthermore, ttotal of wood combustion under 27%O2/73%CO2 and 21%O2/50%H2O/29%CO2 condition was found comparable with that in air.
The simulations showed that radicals (OH, H) were enhanced with steam addition in oxy-combustion, leading to a shorter ignition time. The dominant reactions for heat release rate were gradually shifted from (R3) H2+OH↔H+H2O and (R91) CH3+O↔CH2O+H to (R35) CO+OH↔CO2+H and (R33) H+OH+M↔H2O+M with steam addition. In summary, an overall conceptual Damköhler number (Da = tflow/tchem) evolution in the gas-phase region was proposed based on the competition of chemical time (tchem) and flow residence time (tflow) to illustrate the faster ignition of H2O substitute CO2 in oxy-combustion. The growth of additional volatiles by char-H2O gasification and chemical reaction rate enhancement resulted in a faster increase of Da number from zero to reach a critical value for flame ignition. This study provides insight into biomass ignition and combustion fundamentals, which is beneficial to its application in industrial oxy-combustion systems.

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