Journal of the Korean Industrial and Engineering Chemistry, Vol.11, No.5, 473-478, August, 2000
나노화학적 접근에 의한 제올라이트 촉매 응용연구
Nano-Chemical Approach in Zeolite Catalysis
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초록
제올라이트 촉매응용 연구에 대해 나노화학적 접근으로 고찰해 보았다. 이 연구에서는 H2와 O2로부터 직접적으로 H2O2를 합성하는데 시용되는 불균일성촉매를, Y 제올라이트에 Pb 나노입자와 2-ethylantraquinone를 함께 포접화하여 만들었다. 이 촉매를 사용할 경우 H2O2의 생성량은 미세 세공에 포접된 2-ethylantraquinone의 도움에 의해 상승적으로 증가되었다. 또한 bicatalyst를 사용하면 H2와 O2를 이용하여 벤젠으로부터 직접적으로 페놀을 만드는 반응이 쉽게 수행되었다. Pd-Y 촉매를 2-ethylantraquinone로 변형시키면 페놀을 만드는 반응 과정중의 내부적인 H2O2 생성으로 인하여 반응성이 괄목하게 증가되었고 또한 Ti-이나 V-MCM-41를 포함하는 bicatalyst에 Cl-를 첨가하면 페놀의 생성량이 크게 증가였다. 마지막으로 다른 두 방법으로 제조하여 Pd 치환된 BEA 제올라이트 촉매를 이용하여 과량의 산소하에서 메탄으로 NO의 SCR를 연구하였다. 이때 유기물질이 존재하는 경우에 제올라이트 세공의 외부자리에 선택적으로 P얘종을 만들 수 있었으며, 이것이 낮은 온도에서도 SCR 효율성을 높이는데 기여하는 것으로 생각되었다.
Nano-chemical approach in zelite catalysis was investigated. In this study, heterogeneous catalysts for direct produciton of H2O2 from H2 and O2 were designed by the encapsulation of 2-ethylantraquinone together with Pd nano-species on Y zeolite. Such catalysts can produce H2O2 from H2 and O2 in aqueous solution and its production is synergistically enhanced with the aid of the encapsulated 2-ethylantraquinone in faujasite pores. The direct hydroxylation of benzen with H2 and O2 was performed under mild reaction condition by the bicatalyst system with considerable activity. The modification of Pd-Y with 2-ethylantraquinone significantly improved the activity via in-situ generation of H2o2 during hydroxylation in collaboration with redox zeolite. Moreover, remarkable increase in yield of phenol was achieved upon addition of Cl- in the reaction mixture over the bicatalyst containing Ti- or V-MCM-41. The SCR of NO with methane in excess oxygen was carried out over Pd-exchanged BEA zeolites prepared by two different methods: with or without organic template. The Pd-exchange on BEA in the presence of organic compound was an efficient way of introducing PdO species selectively onto the external site of zeolite pore, which seemed to be responsible for the enhanced SCR activity at lower temperature.
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