游文岳Yi-An Wang王翊安2025-11-142025-11-142025https://scholars.lib.ntu.edu.tw/handle/123456789/733688https://ntu.primo.exlibrisgroup.com/permalink/886NTU_INST/14poklj/alma991039401169604786獎項：傅斯年獎；指導教授：游文岳In this research project, I synthesized palladium-supported manganese dioxide catalysts (Pd/MnO2) and applied them to the deNOx reaction for the removal of the harmful gas nitric oxide (NO). The catalysts were prepared using the hydrothermal method by adjusting the precursor ratio, hydrothermal temperature, and reaction time to obtain four different crystalline structures of MnO2 supports (α-, β-, γ-, and δ-MnO2). Palladium was subsequently deposited onto these supports via the deposition-precipitation method to obtain Pd/MnO2 catalysts. The Pd/MnO2 catalysts were then applied to the selective catalytic reduction of NO with hydrogen (H2-SCR). Under these conditions, it was found that hydrogen was not selectively reducing NO to nitrogen (N2) but instead preferentially reacted with oxygen to form H2O. Therefore, the reaction conditions were modified to an oxygen-free environment to facilitate the conversion of NO to ammonia (NH3). Hydrogen temperature-programmed reduction (H2-TPR) and hydrogen temperature-programmed desorption (H2-TPD) analyses revealed that the introduction of palladium nanoparticles significantly enhanced the hydrogen adsorption capacity of the catalyst surface, which contributed to an improved NO conversion efficiency and its reduction to NH3, a product of high economic value. Additionally, the structure of the MnO2 support had a significant impact on catalytic activity, with Pd/β-MnO2 exhibiting the highest NO conversion and NH3 selectivity. The NO pulse experiment further suggested that this superior performance was associated with the relatively high NO adsorption capacity of β-MnO2.本研究製備鈀金屬二氧化錳擔體觸媒(Pd/MnO2)並應用於有害氣體一氧化氮(NO)的脫硝(deNOx)反應。我以水熱法(hydrothermal method)作為合成方法，藉由調整前驅物比例、水熱溫度及時間，製備四種不同晶型結構的二氧化錳擔體(α、β、γ以及δ-MnO2)，接著以沉積沉澱法(deposition-precipitation method)擔載鈀金屬製得Pd/MnO2觸媒。本研究將Pd/MnO2應用於NO的氫氣選擇性催化還原(H2-SCR)反應，發現在此條件下，氫氣無法選擇性將NO還原為氮氣，而是傾向直接與氧氣反應並生成H2O。因此，我調整反應條件成無氧環境，期望能將NO轉化為氨氣。氫氣程序升溫還原(H2-TPR)及程序升溫脫附(H2-TPD)結果得知，擔載金屬鈀顆粒後，觸媒表面的吸氫量顯著提升，有助於提升NO的轉化能力並將其還原為高經濟價值的NH3。此外，擔體結構也對催化活性有著顯著的影響，其中以Pd/β-MnO2表現出最佳的NO轉化率以及氨氣選擇率，由NO脈衝鑑定結果推測與β-MnO2有相對高的NO吸附反應量有關。NO removalPd/MnO2Pulse surface reactionMetal-Support interaction脫硝反應鈀/二氧化錳脈衝式表面反應金屬-載體交互作用thesis