低一氧化碳選擇率、高熱穩定性的金、鈰修飾銅鋅觸媒甲醇-過氧化氫蒸氣重組之研究

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研究生：	林昭男 Lin, Chao-Nan.
論文名稱：	低一氧化碳選擇率、高熱穩定性的金、鈰修飾銅鋅觸媒甲醇-過氧化氫蒸氣重組之研究 Low CO Selectivity and High Thermal Durability of Copper Zinc Catalyst with Gold and Cerium Promoters in the Hydrogen Peroxide-Oxidative Steam Reforming of Methanol
指導教授：	黃鈺軫 Huang, Yuh-Jeen
口試委員:	葉君棣 Yeh, Chuin-Tih 汪成斌 Wang, Chen-Bin
學位類別：	碩士 Master
系所名稱：	原子科學院 - 生醫工程與環境科學系 Department of Biomedical Engineering and Environmental Sciences
論文出版年：	2018
畢業學年度：	106
語文別：	英文
論文頁數：	114
中文關鍵詞：	金、鈰、雙氧水-甲醇蒸氣氧化重組、低CO選擇率、熱穩定性
外文關鍵詞：	gold, cerium, H2O2-OSRM, low CO selectivity, thermal durability
相關次數：	點閱：1 下載：0
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本研究以共沉澱法製備不同比例的鈰 (Ce = 10、20、30wt%) 修飾銅鋅複合型觸媒，並以三種不同的甲醇重組反應測試其活性、選擇性及穩定性，分別為甲醇部分氧化(POM)、甲醇水蒸氣重組(SRM)和雙氧水系統的甲醇蒸氣氧化重組(H2O2-OSRM)反應，接著經由一些觸媒鑑定 (XRD、ICP-MS、H2-TPR、N2O吸附、BET) 探討添加後物理特性的改變。鈰的添加在SRM及OSRM中不僅能有效降低一氧化碳的選擇率(>275°C，降低30-50%)，還能改善銅鋅觸媒熱穩定性不佳(失活常數: 0.528 → 0.273 hr-1(SRM)，0.542 → 0.230 hr-1(H2O2-OSRM))的問題。
雖然CCe10Z有效抑制了一氧化碳的產生，並增強了穩定性，但同時也造成活性的損失，為了能增加反應活性，本研究進一步以沉積沉澱法，添加不同比例的金(Au = 0.5、1、3、5wt%)修飾銅鈰鋅複合觸媒，並以TEM、XRD觀察金的顆粒大小。研究結果發現，金的顆粒大小會隨著添加比例而逐漸變大，反應最佳的觸媒是Au1CCe10Z，在275°C時， H2O2-OSRM中甲醇轉換率達97% 、一氧化碳選擇率達2.6%、氫氣產率達160 mmole*s-1kg-1，H2O2-OSRM和SRM同為液體進樣系統，能有效改善燃料電池體積較大的問題，在反應測試中，H2O2-OSRM系統因含有氧氣，因此甲醇轉換率相較於SRM系統提升了12%，此為H2O2-OSRM系統的一大優勢。

In this study, copper-zinc complex with different amounts of cerium (Ce = 10, 20, 30wt%) were prepared by the coprecipitation method. In activity, selectivity and thermal durability were tested by methanol reforming reactions including partial oxidation of methanol (POM), steam reforming of methanol (SRM) and hydrogen peroxide-oxidative steam reforming of methanol (H2O2-OSRM) reactions. Their physicochemical properties were characterized by XRD, ICP-MS, H2-TPR, BET and N2O chemisorption. The experimental results show that addition of cerium not only reduced the selectivity of carbon monoxide (> 275°C, reduce 30-50%) but also improved the poor thermal stability of copper-zinc catalyst in SRM (deactivation constant: 0.528 → 0.273 hr-1) and H2O2-OSRM reaction (deactivation constant: 0.542 → 0.230 hr-1).
Although CCe10Z effectively reduced the selectivity of carbon monoxide and enhanced their thermal durability, but loss the reforming reactivity. To increase the reactivity, CCe10Z with various amounts of gold (Au = 0.5, 1, 3, 5 wt%) were synthesized by deposition precipitation method. The Au particle sizes were characterized by XRD and TEM. The optimize performance of catalyst is Au1CCe10Z which achieves 97% methanol conversion, 160 mmole*s-1kg-1 H2 yield, and 2.6% CO selectivity. H2O2-OSRM and SRM were liquid injection system which could reduce the volume of fuel cell. In the reaction test, H2O2-OSRM system performed 12% improvement in methanol conversion over SRM system due to the oxygen contained which was a major benefit in the H2O2-OSRM system.

Abstract    IV
摘要    V
謝誌    VI
Category    VII
Chapter 1. Motivation and approaches    1
Chapter 2. Background and introduction    3
2-1 Use of energy    3
2-2 Fuel cell    4
2-3 Advantages and applications of fuel cells    7
2-4 Proton exchange membrane fuel cells (PEMFCs)    10
2-5 Hydrogen storage    12
2-6 Production of hydrogen from methanol    17
2-7 Paper review of producing hydrogen from methanol reforming    22
2-7-1. Catalysts for methanol reforming    22
2-7-2. CuZn- based catalyst    24
2-7-3. Promoter of Ce    25
2-7-4. Promoter of Au    27
Chapter 3. Experimental Section    30
3-1 Chemicals and solutions    30
3-2 Catalyst preparation method    32
3-2-1. Cu/ZnO (CZ)    32
3-2-2. Cu/CexZnO (CCexZ)    33
3-2-3. AuxCu/Ce10ZnO    34
3-3 Inductively coupled plasma-mass spectrometry (ICP-Mass)    36
3-4 Vacuum system and nitrogen physical adsorption    37
3-5 Transmission electron microscopy (TEM)    40
3-6 Powder X-ray diffractometer (XRD)    41
3-7 Hydrogen Temperature programmed reduction (H2-TPR)    42
3-8 N2O Chemisorption    43
3-9 In-situ diffuse reflectance infrared fourier transform spectroscopy    45
3-10 Catalytic activity    46
Chapter 4. The relationship between cerium content and copper zinc catalyst in the methanol reforming process    49
4-1 CZ-based catalysts with cerium    49
4-2 Composition and Cu dispersion of catalysts    50
4-3 X-ray powder diffraction    51
4-4 Hydrogen temperature programmed reduction(H2-TPR)    53
4-5 Catalytic activity test of partial oxidation of methanol reaction    55
4-5-1. In-situ DRIFT investigation    58
4-6 Catalytic activity test of steam reforming of methanol reaction    60
4-7 Catalytic activity test of oxidative steam reforming of methanol reaction    62
Chapter 5. The relationship between gold content and CCe10Z catalyst in the methanol reforming process    65
5-1 CCe10Z-based catalysts with gold    65
5-2 Metallic composition and Cu dispersion of catalysts    65
5-3 X-ray powder diffraction    67
5-4 Transmission Electrons Microscopy    69
5-5 Hydrogen temperature programmed reduction (H2-TPR)    71
5-6 Catalytic activity test    73
5-6-1. Partial oxidation of methanol reaction    73
5-6-2. Steam reforming of methanol reaction    76
5-6-3. Oxidative steam reforming of methanol reaction    80
5-7 Thermal durability test of methanol reforming reaction    83
Chapter 6. Conclusions    94
Reference    96

                                

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