以鋯有機金屬氣凝膠模板合成氧化鎳/鋯鈰氧氣凝膠應用於二氧化碳/氫氣甲烷化反應

溫室氣體為現今全球暖化的元凶之一，二氧化碳又佔最大多數，因此若能藉由二氧化碳捕捉並再利用，不只能減少溫室氣體，減緩全球暖化，且能轉化成具有經濟價值之產物，加以利用。近年來，科技的進步，人類大量活動，使得石化燃料日益匱乏，成為一大問題。二氧化碳氫氣甲烷化反應為一種常見的二氧化碳再利用的方式之一，甲烷為重要的燃料，因此其反應不只能減緩溫室氣體的排放，更能產甲烷解決眼下的能源危機。為了使二氧化碳氫氣甲烷化反應能夠有效的產甲烷，在反應中加入觸媒，降低反應所需之能量，減少能量之消耗。金屬有機骨架為良好氣體儲存之材料，藉由良好儲存及高比表面積等特性並加上氣凝膠中孔洞之性質，能夠幫助較大分子的吸附或運輸。以UiO-66(Zr)為模板提供微孔及高比表面積，為了增加鹼性位點，添加鈰增加二氧化碳的吸附能力。添加活性金屬鎳，以利氫氣之吸附，提高其反應效能。本研究透過不同檢測證明成功製備以鋯有機金屬氣凝膠模板合成氧化鎳/鋯鈰氧氣凝膠，進行二氧化碳甲烷反應，對於不同反應參數進行探討，針對不同載體之莫耳比例、不同活性金屬之莫耳比例、不同氣體流量以及不同溫度對甲烷化反應之影響。氧化鎳/鋯鈰氧氣凝膠中，鋯鈰鎳的莫耳比在3/7/9，反應溫度為300°C，反應流量為氮氣5 ml/min、氫氣4 ml/min以及二氧化碳1ml/min，有最佳的二氧化碳轉化率74.5%，甲烷選擇比皆維持100%，長時間穩定與重複利用皆維持在一定的穩定性，因此材料對於二氧化碳氫氣甲烷化反應可以增加反應效能。

關鍵字

甲烷化反應；氫化反應；金屬氧化催化劑；金屬有機氣凝膠；鋯鈰氧氣凝膠附載氧化鎳

並列摘要

Greenhouse gases are one of the main culprits of global warming, and carbon dioxide accounts for the most. Therefore, if carbon dioxide can be captured and reused, it will not only reduce greenhouse gases and slow down global warming, but also can be transformed into products with economic value. In recent years, large number of human activities have made fossil fuels increasingly run out, which has become a major problem. Carbon dioxide methanation reactions is one of the common ways to reuse carbon dioxide. The metal-organic framework is a material for good gas storage combined with the macropore in the aerogel, it can help the transportation of larger molecules. UiO-66 (Zr) is used as a template to provide micropores and high specific surface area. In order to increase basic sites, cerium is added to increase the carbon dioxide adsorption capacity. Add active metal nickel to facilitate the adsorption of hydrogen and improve its reaction efficiency. This study proved through different tests to successfully synthesis of NiO/zirconium-cerium oxide aerogel using zirconium metal-organic aerogel templates for carbon dioxide Methanation reactions. In the NiO/zirconium-cerium oxide aerogel the molar ratio of zirconium/cerium/nickel is 3/7/9, the reaction temperature is 300°C, and the reaction flow ratio of N2/H2/CO2 is 5/4/1, the best carbon dioxide conversion rate is 74.5%, methane selection can be maintained at 100%, long-term stability and reuse are maintained, so the material can increase the reaction efficiency for the carbon dioxide hydrogen methanation reaction.

並列關鍵字

Methanation ； Oxide catalysis ； Metal organic aerogel ； NiO/Zirconium-Cerium oxide aerogel

參考文獻

1. Younas, Muhammad, Leong Loong Kong, Mohammed J. K. Bashir, Humayun Nadeem, Areeb Shehzad, and Sumathi Sethupathi, Recent Advancements, Fundamental Challenges, and Opportunities in Catalytic Methanation of CO2. Energy Fuels, 2016. 30(11): p. 8815-8831.