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Received July 31, 2014
Accepted August 31, 2014
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Ni/Al2O3 촉매를 사용한 에틸렌글리콜의 수증기 개질 반응: 촉매 제조 방법과 환원온도의 영향
Steam Reforming of Ethylene Glycol over Ni/Al2O3 Catalysts: Effect of the Preparation Method and Reduction Temperature
아주대학교 에너지시스템학과, 화학공학과, 443-749 경기도 수원시 영통구 월드컵로 206
Department of Chemical Engineering and Department of Energy Systems Research, Ajou University, 206 World cup-ro, Yeongtong-gu, Suwon 443-749, Korea
edpark@ajou.ac.kr
Korean Chemical Engineering Research, June 2015, 53(3), 372-381(10), 10.9713/kcer.2015.53.3.372 Epub 2 June 2015
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Abstract
본 연구에서는 Ni/Al2O3 촉매를 사용한 에틸렌글리콜의 수증기 개질반응에서 제조 방법에 따른 영향을 알아보았다. 촉매들은 건식 함침법, 습식 함침법 그리고 공침법을 사용하여 제조하였다. 공침법을 사용하여 촉매 제조시 침전제를 KOH, K2CO3, NH4OH를 각각 사용하여 침전제에 따른 영향 또한 알아보았다. 제조한 촉매들은 질소 물리흡착, 유도결합 플라즈마 질량분석법(ICP-AES), X선 회절법(XRD), 수소 승온 환원법(TPR), 수소 화학흡착, 승온 산화법(TPO), 주사전자현미경(SEM), 열분석법(TGA)을 사용하여 촉매의 물리화학적인 특성을 분석하였다. 773 K에서 환원한 촉매의 경우 KOH 혹은 K2CO3를 침전제로 사용하여 공침법으로 제조한 촉매가 가장 높은 활성을 보였다. 촉매 제조 방법은 Ni의 입자크기, Ni 산화물의 환원도, 반응에서의 활성과 안정성, 반응 중 탄소 침적의 형태 등에 영향을 끼치는 것을 확인할 수 있었다. KOH를 침전제로 사용하여 공침법으로 제조한 촉매의 경우 환원온도를 773~1173 K까지 증가시켰을 때, Ni 입자크기의 증가에도 불구하고 Ni 산화물의 환원도가 증가하므로 반응활성이 증가하는 것으로 나타났다.
The effect of preparation method on the catalytic activities of the Ni/Al2O3 catalysts on steam reforming of ethylene glycol was investigated. The catalysts were prepared with various preparation methods such as an incipient wetness impregnation, wet impregnation, and coprecipitation method. In the case of coprecipitation method, various precipitants such as KOH, K2CO3, and NH4OH were compared. The prepared catalysts were characterized by using N2 physisorption, inductively coupled plasma-atomic emission spectroscopy, X-ray diffraction, temperatureprogrammed reduction, pulsed H2 chemisorption, temperature-programmed oxidation, scanning electron microscopy, and thermogravimetric analysis. Among the catalysts reduced at 773 K, the Ni/Al2O3 catalyst prepared by a coprecipitation with KOH or K2CO3 as precipitants showed the best catalytic performance. The preparation method affected the particle size of Ni, reducibility of nickel oxides, catalytic performance (activity and stability), and types of coke formed during the reaction. The Ni/Al2O3 catalyst prepared by a coprecipitation with KOH showed the increasing catalytic activity with an increase in the reduction temperature from 773 to 1173 K because of an increase in the reduction degree of Ni oxide species even though the particle size of Ni increased with increasing reduction temperature.
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