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二氧化碳還原生產甲醇之光觸媒及其製程
專利名稱 二氧化碳還原生產甲醇之光觸媒及其製程
申請日 (校編號) 2006/06/08  (095020TW)
專利證書號 I317301 中華民國
專利權人 國立中央大學
發明人 陳郁文、魏聰揚、潘姵彣


技術摘要:
本發明係一種承載於四氧化銦鉭之鎳觸媒之製備方法,及一種承載於銦鉭氧化物之鎳觸媒由光激發下將溶於水之二氧化碳於低於80℃下反應生成甲醇之製程,其中氧化鎳/四氧化銦鉭觸媒之製法為分別以銦和鉭的氧化物為起始物質,均勻混合上述兩種物質,經研磨後,在900至1400℃之間煆燒2至24小時,得到四氧化銦鉭。將四氧化銦鉭放置於容器中,再加入硝酸鎳的水溶液,並以水浴加熱趕走多餘的水分後,在300至500℃間煆燒1至10小時,氧化鎳/四氧化銦鉭之重量比介於0.3%至1%之間,然後用氫氣於300至600℃間還原1至10小時,再用氧氣於150至300℃間氧化1至5小時,以使光觸媒表面同時具有金屬鎳與氧化鎳,其中四氧化銦鉭為微米級顆粒直徑,其顆粒直徑在1微米至3微米之間,且其為結晶型態。本發明亦包括在室溫至80℃間以上述觸媒進行二氧化碳還原反應的製程,二氧化碳還原反應製程係在一反應器中進行,以水及二氧化碳為原料,反應溫度在10至80℃之間,所使用的觸媒為銦鉭系列的觸媒,所使用的光源為一般太陽光或可見光或紫外光。 This invention declares the preparation of indium-tantalum photocatalysts for carbon dioxide reduction to produce methanol using indium-tantalum-supported micro nickel catalysts. Indium-tantalum was synthesized by a solid-state reaction method. The pre-dried In2O3, Ta2O5with purity of 99.99% were used as starting materials. The stoichiometric amounts of precursors were mixed and reacted in an aluminum crucible in air at 900-1400℃ for 2-24 h. In order to obtain high photocatalytic activity, it is essential to load a metal or metal oxide on the surface of photocatalyst as electron acceptors. We tested loading NiOxon surface of the catalyst. The nickel was loaded on surface of the catalysts powders from aqueous Ni(NO3)2solution. The Ni-loaded photocatalysts were calcined at 300-500℃ for 1-10 h in air, then prepared by H2(200 Torr) reduction at 300-600℃ for 1-10 h and subsequent O2(100 Torr) oxidation at 150-300℃ for 1-5 h. The double-layered structure of metallic Ni and NiO was formed on the surface of photocatalyst by this reduction-oxidation procedure. The content of Ni-loaded is controlled at weight percent between 0.3 and 1. The particle size of indium-tantalum photocatalysts is less than 3 μm. Nickel species is in metallic state. Photocatalytic reactions were carried out in a closed gas circulation system. A 0.14 g powder sample was suspended in 50 ml 0.2 M potassium hydrogen carbonate aqueous solution bubbling with carbon dioxide using a Pyrex glass cell (75 ml). A 500W halogen lamp was placed onto the down face of the Pyrex glass cell. The temperature of reduction of carbon dioxide is controlled between 10℃ and 80℃. NiO-loaded In TaO4showed a high photocatalytic activity for carbon dioxide reduction into methanol in a stoichiometric amount under visible irradiation.

解決的問題或達成的功效:
創新未曾揭示之方法,先以固態反應法製備四氧化銦鉭,以初濕含浸法製備鎳觸媒,經由精確控制製備過程,所得到之觸媒在室溫至50℃之間,於飽和二氧化碳之碳酸氫鉀液體中能成功的產生甲醇。

應用領域:
製備含有銦鉭的微米光觸媒,其顆粒直徑在微米範圍,能帶間隙為2.7 eV,而且氧化銦鉭係以結晶型態存在,此光觸媒對於可見光的二氧化碳還原為甲醇之反應,具有高的活性。

適用產品:
觸媒

IPC:
B01J-023/755(2006.01);B01J-037/00(2006.01);C07C-029/15(2006.01);C07C-031/04(2006.01)

Claim 1:
1.一種承載於四氧化銦鉭之鎳觸媒的製造方法,其包括以銦的氧化物為起始物質;以鉭的氧化物為起始物質;混合上述兩種物質,並研磨之,在900至1400℃間煆燒2至24小時,得到四氧化銦鉭;將四氧化銦鉭置於容器中,再加入硝酸鎳水溶液,並以水浴加熱法趕走多餘的水分後,於300至500℃間加熱1至10小時,使氧化鎳之重量為全部觸媒重量的0.3 %至1 %之間;之後在300至600℃間以氫氣還原1至10小時,再用氧氣或空氣於室溫至150至300℃間氧化1至5小時。

聯繫方式
聯絡人:研發處智權技轉組 與我連絡
電話:03-4227151 #27076、27077 網址:http://www.caic.ncu.edu.tw/
地 址: 32001桃園市中壢區中大路300號
 
                 
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