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동함유 제올라이트상에서 일산화탄소의 산화반응

Carbon Monoxide Oxidation on Copper Zeolites

HWAHAK KONGHAK, April 1989, 27(2), 130-137(8), NONE
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Abstract

이온 교환 및 담지에 의해 제조한 동함유 제올라이트 촉매상에서 일산화탄소의 산화반응을 실시하였다. 수소형 모더나이트(HM)와 이를 열처리 및 염화암모늄 용액으로 이온 교환을 반복 실시하여 부분적으로 탈알루미늄됨 모던나이트(HM#), 그리고 HY를 질산구리 용액으로 이온 교환하여 동의 함량을 달리하는 이온 교환 촉매를 얻었다. 또한 HY, HM#, 및 HZSM-5에 1wt%의 동 및 백금을 담지시켜 이들과 이온 교환 촉매의 활성을 비교하였다. 일산환탄소의 산화반응에 대한 이온 교환 촉매의 활성을 동의 함량에 따라 증가하였으며 또 동의 원자가 상태가 Cu(II)<Cu(I)<Cu(0)의 순으로 증가하였다. 또한 이온 교환 촉매의 활성은 제올라이트 구조내의 실리카-알루미나 비에 의해서도 영향을 받는 것으로 생각된다. 즉, 부분적인 탈알루미늄에 의해 실리카-알루미나 비가 커진 CuHM#가 가장 큰 활성을 보였다. 동이 담지된 촉매는 같은 양의 동이 이온교환된 촉매보다 더 큰 활성을 보였다. 또한 담지 촉매에서도 이온 교환 촉매와 마찬가지로 구조내의 실리카-알루미나의 비가 증가함에 따라 활성은 증가하였다. 또한 Cu(0)의 경우 환원으로 인해 생성된 금속 동이 제올라이트 결정 표면에 편재하게 되어 활성을 증가시키기 때문으로 생각된다.
The oxidation of carbon monoxide was carried out on the copper zeolites prepared by ion exchange and impregnation. Hydrogen mordenite(HM), partially dealuminated mordenite(HM#) obtained by repeating thermal treatment as well as ammonium ion-exchange and HY were ion-exchanged in cupric nitrate solution to get the copper zeolites having various level of copper content. HY, HM#, and HZSM-5 were impregnated with copper or platinum in 1wt% and the activities of these impregnated catalysts were compared with those of ion-exchanged ones. The activities of ion-exchanged catalysts for the oxidation of carbon monoxide increased with an increase in the copper containing level of the catalysts, but decreased with an increase in the valence state of the copper[i.e., Cu(0)>Cu(I)>Cu(II). It is considered that the activity of ion-exchanged catalysts is affected by the sillica-alumina ratio of the zeolite structure. Par-tially dealuminated copper mordenite showed highest activity among the catalysts. The impregnated catalyst was more active than the ion-exchanged one at the same level of copper content. The activity of impregnated catalyst was more active than the ion-exchanged one at the same level of copper content. The activity of impregnated catalysts also in-creased as their silica-alumina ratio of the structure increased as the same as the ino-exchanged catalysts. The higher activity for Cu(0) could be also explained by the increase of copper concentration on the surface of zeolite.

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