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  • 學位論文

自供熱低溫微流道泡棉床甲醇重組器

Autothermal microchannel-foam methanol reformer for hydrogen production at low temperature

指導教授 : 沈家傑

摘要


本實驗旨在建立OSRM反應自供熱低溫銅泡棉微流道甲醇重組器(Microchannel foam reactor,MFR),盼將高活性Cu35Pd2Ce20Zn43及商購ICI 33-5催化劑,藉由催化劑洗積技術將其附著在銅泡棉的表面,以進行自供熱甲醇氧化水蒸氣重組反應 (oxidative steam reforming of mehtnaol, OSRM)。光學及電子顯微照片表示催化劑洗積於銅泡棉表面,洗積層在銅泡棉表面的厚度介於32-80 μm。在WHSV = 60 h-1、S/C = 1.3及O/C = 0.35條件,GC實驗結果顯示,兩者催化劑之MFR均可自供熱進行OSRM反應,MFR- Cu35Pd2Ce20Zn43催化床溫度可維持在240-350℃,甲醇轉化率為90 %及產氫率為1.5;但MFR-ICI 33-5催化床溫度僅在210℃,甲醇轉化率為82 %及產氫率為1.7。前者MFR反應催化床溫度較高應歸咎於Pd催化,使得上游易進行POM,放熱程度劇烈及伴隨燒氫所致。此外,配合溫度感測器監控MFR的催化床溫度分佈量測發現在MFR- Cu35Pd2Ce20Zn43催化床在上、中及下游溫度變化分別為350℃ 、 250 ℃ 及 240 ℃,催化床溫度分佈優於MCR,表示傳統PBR之催化床熱點及其銅燒結可有效被抑制。MFR- Cu35Pd2Ce20Zn43的產氫量(乾式)為1150 mL/min,約可提供188 W之理論電量輸出。

並列摘要


This study is to develop autothermal methanol reformers for hydrogen production in a microchannel-foam reactor (MFR)。 The high activity Cu35Pd2Ce20Zn43 and commercial ICI 33-5 (CuZnAl) catalysts washcoated on the surface of Cu foams were used to carry out an oxidative steam reforming of methanol (OSRM)。Electron micrographs indicate that the thickness of the catalyst layer coated ranges from 32-80 μm. In the conditions of WHSV = 60 h-1, S/C = 1.3 and O/C = 0.35,both Cu35Pd2Ce20Zn43 and ICI 33-5 MCFs demonstrated to have an ability to run autothermal OSRM. In the autothermal reforming temperatures (Ta) from 240 to 350 °C in a MFR-Cu35Pd2Ce20Zn43, the measured methanol conversion and hydrogen yield were 90% and 1.5,respectively。 On the other hand,Ta in a MFR-ICI 33-5 was 210 °C, and measured methanol conversion and hydrogen yield were 82 % and 1.7,respectively。 The observed highly Ta is ascribed to the occurrence of exothermic partial oxidative methanol (POM) over Pd-promoted catalyst in the beginning of OSRM stream in MFR。causing to hydrogen combustion to lose hydrogen yield rate。 In addition, the thermalcouplers inserted into a MFR-Cu35Pd2Ce20Zn43 showed that the beginning,middle end temperature were 350 °C,250 °C and 240 °C,respectively。The distribution of reforming temperature in MFR was more uniform than that in other microchannel reactor,indicating hot-spot and the sinter of Cu active sites encountered usually in packed-bed reactors can be eliminated effectively。Hydrogen rate (dry in reformate) produced in MFR-Cu35Pd2Ce20Zn43 was approximately of 1150 mL/min,which provides a theoretical power output of 188 W。

參考文獻


[20] 簡調源, “微流道泡棉甲醇蒸氣重組反應器之研究” 元智大學
[3] K. Faungnawakij, R. Kikuchi, K. Eguchi, “Thermodynamic
evaluation of methanol steam reforming for hydrogen
production,” J. Power Sources, 161 (2006) 87-94.
(1999) 31-49.

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