- 學位論文
鉬基多孔性觸媒應用於溼式合成氣重組反應
Application of Porous Mo-Based Catalyst for Wet Restructuring Reaction of Syngas
摘要
為因應我國能源自給困難，本研究期使能利用國內有機及生質廢棄物，以合成氣重組之方式將之轉製為生質燃料，同時亦可解決環境污染之問題。 本研究中使用漿態反應器，於高溫高壓之環境中進行溼式合成氣重組反應，並添加微米級之ZSM5-PW (with no Mo)、1MoS2/ZSM5-PW (with 5.2 wt.% Mo)及4MoS2/ZSM5-PW (with 16.0 wt.% Mo)觸媒進行溼式觸媒催化合成氣重組反應(wet catalytic syngas restructuring reaction, WCSR)。研究結果顯示於溼式反應器中進行無觸媒之合成氣重組反應(wet syngas restructuring reaction, WSR)，即有提高醇類產物選擇性之效果。研究中探討觸媒鉬含量對合成氣重組反應之影響，結果顯示提高觸媒之鉬含量可顯著提升一氧化碳(CO)之轉化效率。另外亦對反應之操作參數進行探討，包括反應溫度(T)、時間(t)，進氣中H2與CO之mole比(H2/CO mole ratio, MH/C)，以及H2及CO之進氣總壓(初始壓力, PC/H,0)。結果顯示，操作參數之改變中T過高將導致高碳數醇類(丙醇、丁醇)選擇性下降。t過長則將導致有機化合物之比生產速率(specific production rates, SPR)降低。而隨進氣之不同，對產物之選擇性也有一定之影響，其中降低MH/C (如降至0.6)可使高碳數醇類之選擇性增加，有效使醇類之碳鏈加長。提高反應之PC/H,0可提升所有非CO2含碳化合物之SPR，並使高碳數醇類之選擇性上升，可避免如T升高使較高碳數之醇類分解之問題。
並列摘要
In order to reduce the stress of energy demand in Taiwan, utilizing the refuse resulted from biomass to produce bio-energy has been considered as one of the good alternatives available. It can be firstly gasified to generate synthesis gas, and then converted to liquid fuel by the technology called syngas restructuring reaction. Besides above advantage for energy application, using waste as the feedstock also offers a solution for reducing the environmental burden in dealing with garbage. In this study, the experiments of wet syngas restructuring reaction (WSR) were operated at high temperature (T) and pressure (P) in a slurry reactor. For enhancing the reaction, micron catalysts named ZSM5-PW (with no Mo), 1MoS2/ZSM5-PW (with 5.2 wt.% Mo) and 4MoS2/ZSM5-PW (with 16.0 wt.% Mo) were used to proceed the wet catalytic syngas restructuring reaction (WCSR). The sole WSR without catalyst, already exhibits higher selectivities (S) for high-carbon-containing alcohols (or higher alcohols) than for low-carbon-containing alcohols (or lower alcohols). The effect of Mo content of catalyst (MMo) on the CO conversion (XCO) via WCSR is significantly positive. Furthermore, the influences of other key parameters such as the reaction temperature, reaction time (t), and H2/CO mole ratio (MH/C) and initial total pressure (PC/H,0) of the feed of synthesis gas were also examined. The results show that the selectivities of higher alcohols decrease if T is too high. The specific production rates (SPRs) of organic compounds decrease with the increase of t. At a proper low MH/C of 0.6, the selectivities of higher alcohols are elevated, favoring the production of higher alcohols. A higher PC/H,0 of H2 and CO can raise up the SPRs of non-CO2 carbon-containing compounds, and increase the selectivities of higher alcohols avoiding the decomposition of higher alcohols at higher T.