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標題: 超高溫水氣轉化反應觸媒與膜反應器合成氣產氫之實驗探討
Experimental Study on Ultrahigh Temperature Water-gas Shift Catalysts and Membrane Reactors for Hydrogen Production from Syngas
作者: 林筵翔
Lin, Yen-Hsiang
關鍵字: 超高溫;ultrahigh temperature;水氣轉化反應;CO轉化率;鈀銀合金;膜反應器;water-gas shift (WGS) reaction;CO conversion;Pd-Ag alloy;membrane reactor
出版社: 機械工程學系所
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本研究第一部分為開發適用於超高溫水氣轉化反應之觸媒,藉由改變觸媒的成分、促進劑的摻雜比例以進行觸媒性能測試。實驗於超高溫(750-850℃)環境中操作,透過改變不同的進料水碳莫耳比與長時間的操作以得知觸媒的一氧化碳轉化效果、氫氣產量與熱穩定性。在WGS觸媒研究首先製備2.5wt% Pt/Al2O3觸媒進行測試做為比較基準,藉由改變促進劑CeO2的添加比例、Ni金屬觸媒的摻雜與調整貴金屬Pt的含量以觀察觸媒性能。實驗結果以2.5wt%Pt-2.5wt% Ni/5wt%CeO2/Al2O3觸媒進行WGS反應在操作溫度750℃、反應時間24~36小時及進料水碳莫耳比S/C = 5時有最佳的CO轉化率平均為76.5%,且經過36小時測試後並沒有活性下降問題,展現了良好的穩定性。將白金含量降低至0.5wt%

本研究亦嘗試以無電鍍法於多孔不銹鋼基材上製備緻密性的鈀銀合金薄膜並應用於WGS反應。在無電鍍薄膜實驗前將以沸石(zeolite)及合成凝膠(synthesis gel)對基材進行改質以縮減孔徑。實驗利用薄膜反應器通入氫氮混合氣觀察薄膜在不同操作壓力與溫度下對於氫氣之滲透係數,期許未來可將膜反應器整合於高溫水氣轉化反應系統中。

In this study, catalyst for water-gas shift (WGS) reaction operated at ultrahigh temperatures (750~850℃) was prepared and tested. The catalyst was prepared by using the Al2O3 as support and varying the amounts of noble metal (Pt), Transition metal (Ni), and promoter (CeO2). The catalyst performance was characterized by measuring the CO conversion, H2 yield, and the thermal stability for the WGS reaction. Using the performance of 2.5wt%Pt/ Al2O3 catalyst as the comparison basis, it was found that the 2.5wt%Pt-2.5wt%Ni/5wt%CeO2/Al2O3 catalyst has the best performance among all the catalysts prepared in this study. Using this catalyst with reaction temperature of 750℃ and carbon to steam ratio of 5, CO conversion of 76.5% can be reached and thermal stability can be maintained in 36 hours operation.

The membrane reactor for carrying out the WGS reaction was also prepared in this study by coating the Pd-Ag alloy membrane on the porous stainless steel tube. The zeolite and synthesis gel was used to reduce the pore size of the porous support before the electroless plating for the membrane coating. Using H2/N2 mixture for the pre-test, the hydrogen permeation at different pressure and temperature can be observed. It is expected that the prepared membrane reactor could be used in the future WGS experiments.
其他識別: U0005-2308201316580600
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