• 作者： Li, Kuo-Tseng; Wang, Shen-Zen
• 中文摘要： 本論文利用錳觸媒於一高壓批式反應器中催化苯胺之氧羰基化反應以合成胺苯基甲酸乙酯,探討之項目包括錳觸媒之種類,觸媒之濃度,一氧化碳分壓,反應時間及溫度,氧氣分壓,及促進劑等因素對此觸媒催化性能之影響。我們發現溴離子對於此錳系觸媒系統是必需之成分,而且Mn(CO)/sub 5/Br是催化苯胺氧羰基化反應之真正活性物質,對於此Mn(CO)/sub 5/Br催化之羰基化反應我們提出一反應機構。由實驗得到之反應速率數據顯示此反應對苯胺為一次反應級數,而對氧氣為0.85次反應級數。由此對苯胺為一次反應級數的實驗結果可推知在所提出之反應機構中,苯胺和Mn(CO)/sub 5/Br間之反應為速率決定步驟。
• 英文摘要： The oxidative carbonylation of aniline to ethyl N- phenylcarbamate was studied in a high pressure batch reactor using manganese-based catalysts. The effects of manganese compounds, catalyst loading, carbon monoxide pressure, reaction time and temperature, oxygen pressure, and promoters on the catalyst performance were investigated. It was found that bromide ion was the required component for the manganese-based catalyst system and Mn(CO)/sub 5/Br was the real active species for the oxidative carbonylation of aniline. A catalytic cycle was proposed for the Mn(CO)/sub 5/Br-catalyzed reaction. The experimental reaction rate data was first-order with respect to aniline and 0.85- order with respect to oxygen. The first-order dependence on aniline suggests that the reaction between Mn(CO)/sub 5/Br and aniline is the rate-olimiting step in the proposed mechanism.
• 中文關鍵字： 合成; 催化; 錳; 胺苯基甲酸乙酯; 批式反應器
• 英文關鍵字： Synthesis; Catalysis; Manganese; Ethyl N-Phenylcarbamate; Batch Reactor