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Clean Technology, Vol.21, No.3, 200-206, September, 2015
Ce 첨가에 따른 저온수성가스전이반응용 Cu/Zn 촉매의 활성 연구
Enhanced Catalytic Activity of Cu/Zn Catalyst by Ce Addition for Low Temperature Water Gas Shift Reaction
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초록
산화세륨의 첨가가 수성가스전이반응 효율에 미치는 영향을 조사하기 위해서, Cu-ZnO-CeO2촉매를 공침법을 사용하여 제조하였다. 일련의 Cu-ZnO-CeO2 촉매는 Cu 함량(50 wt%)을을 고정시키고 산화세륨(CeO2 기준으로, 0, 5, 10, 20, 30, 40 wt%)의 함량을 조절하면서 제조되었고 이를 이용하여 GHSV 95,541 h-1의 기체 유량범위, 200~400 ℃의 온도범위에서 수성가스전이반응 촉매활성이 측정되었다. 또한, BET, SEM, XRD, H2-TPR, XPS 분석을 통하여 촉매특성이 분석되었다. CeO2가 첨가된 촉매는 구리 분산도와 결합에너지 같은 촉매특성의 다양한 변화를 나타내었다. 10wt%의 CeO2가 최적의 첨가량으로 판단되며 이때 촉매는 가장 낮은 온도에서 환원이 일어났으며 반응에서 가장 높은 촉매 활성을 보였다. 또한 CeO2가 첨가된 촉매는 CeO2가 첨가되지 않는 촉매와 비교하여 높은 온도영역에서 활성이 향상되었다. 따라서, 최적 조성의 CeO2첨가는 높은 구리 분산도, 낮은 결합에너지, 구리 금속의 응집 방지를 유도하여 높은 촉매활성을 유도하였다.
In order to investigate the effect of cerium oxide addition, Cu-ZnO-CeO2 catalysts were prepared using co-precipitation method for water gas shift (WGS) reaction. A series of Cu-ZnO-CeO2 catalyst with fixed Cu Content (50 wt%, calculated as CuO) and a given ceria content (e.g., 0, 5, 10, 20, 30, 40 wt%, calculated as CeO2) were tested for catalytic activity at a GHSV of 95,541 h-1, and a temperature range of 200 to 400 ℃. Cu-ZnO-CeO2 catalysts were characterized by using BET, SEM, XRD, H2-TPR, and XPS analysis. Varying composition of Cu-ZnO-CeO2 catlysts led the difference characteristics such as Cu dispersion, and binding energy. The optimum 10 wt% doping of cerium facilitated catalyst reduction at lower temperature and improved the catalyst performance greatly in terms of CO conversion. Cerium oxide added catalyst showed enhanced activities at higher temperature when it compared with the catalyst without cerium oxide. Consequently, ceria addition of optimal composition leads to enhanced catalytic activity which is attributed to enhanced Cu dispersion, lower binding energy, and hindered Cu metal agglomeration.
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