氫氣為一種理想潔淨的能源載體，使用生質乙醇製氫，可以使二氧化碳成為一封閉的碳循環，而達到近乎零碳排放的目標。本實驗室先前研究顯示利用模板法合成之銅鎳觸媒中的CuNi-NiO界面有利乙醇蒸氣重組反應，可在溫和條件下催化乙醇重組獲得高氫氣產率，為了提高CuNi- NiO界面在H2中的穩定性，並開發簡易實用的觸媒製備方法。本研究以不同比例La、Gd摻雜NiO作為載體製作觸媒，期望藉由提升NiO還原溫度以維持活性界面，研究中並改變不同前處理條件進行比較討論。
研究結果顯示摻雜15%La觸媒於P-2(250℃, 30min)半還原條件下可使觸媒還原程度接近50%，且CuNi合金和NiO晶粒較小，能產生較穩定且活性較好的CuNi-NiO界面，在反應溫度350℃時，在本研究的操作下可使EtOH幾乎完全轉化，含碳產物含有約20％CH4、15％CO、60％的CO2，H2的產率為3.8。比較不同摻雜金屬與其含量，摻雜La觸媒有優於摻雜Gd觸媒之反應速率，提高摻雜金屬含量會使反應活化能提高，對反應乙醇蒸氣重組有較好的改善。
Cu/La15-NiO-P2觸媒在325℃持溫10小時可以保持穩定反應活性，得知反應後觸媒仍具有NiO結構，顯示可以穩定維持ESR反應活性，在10小時內仍可產生穩定的H2；說明Cu/La15-NiO觸媒中，摻雜金屬的NiO可以促使CuNi-NiO活性界面在較溫和反應條件下穩定存在。

關鍵字: 銅鎳觸媒、前處理、蒸氣重組、金屬氧化物界面

Hydrogen is an ideal clean carrier. Zero carbon emissions can be achieved by using, hydrogen from the reforming of bio-ethanol. In our previous study CuNi-NiO interface in a (Cu-NiO) catalyst prepared by hard-template method can have good activity in ethanol steam reforming reaction(ESR), obtaining high hydrogen yield at mildle conditions. This study intends to improve the stability of CuNi-NiO interface and to prepare workable catalyst preparation method for industal application. In this study dope La and Gd in NiO as support for Cu, expecting the acticity interface can be stabilized by an increase in the NiO reduction temperature.
The results show that Cu/La15-NiO after P-2 pretreatment (250 ℃, 30min) have a degree of reduction of around 50% and good ESR activity. The CuNi alloy and NiO particle size are smaller than other catalysts, which can result in more CuNi-NiO interface. At 350℃, EtOH is nearly completely converted with C-products including 20% CH4, 15% CO and 60% CO2 and a H2 yield of 3.8. Comparing with different type and amount of dopant, the La-doped catalysts have better reaction performance than the Gd-doped catalysts.
The stability test of Cu/La15-NiO-P2 catalyst at 325℃ for 10 hours, indicate stable ESR activity the same H2 yield, the spent catalyst still contain NiO structure, indicating that the metal–doped Cu/La15-NiO catalyst can maintain stable CuNi-NiO interface under the ESR condition.

Keywords: Copper-nickel catalysts, pretreatment, steam reforming, metal oxide interface.

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