Korean Chemical Engineering Research

The Korean Institute of Chemical Engineers (한국화학공학회)
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Regeneration of TS-1 Catalyst During Phenol Hydroxylation(Calcination temperature dependence)

페놀의 수산화 반응에 사용한 TS-1 촉매의 효과적인 재생 방법(소성 온도 의존성)

  • 권송이 (한국화학연구원 그린화학연구단) ;
  • 윤성훈 (한국화학연구원 그린화학연구단) ;
  • 엄경섭 (선경워텍(주)) ;
  • 이재욱 (서강대학교 화공생명공학과) ;
  • 이철위 (한국화학연구원 그린화학연구단)
  • Received : 2010.05.06
  • Accepted : 2010.06.08
  • Published : 2010.12.31
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Abstract

In this study, calcination temperature dependence of TS-1 catalyst was investigated in the hydroxylation of phenol with hydrogen peroxide during the regeneration of catalyst. Catalyst was regenerated 5 times by calcining at $550^{\circ}C$ and $700^{\circ}C$, respectively. When the catalyst was regenerated at $550^{\circ}C$ after 5th regeneration phenol conversion was decreased from 22.9% to 15.1% and at $700^{\circ}C$ after 5th regeneration phenol conversion was decreased from 22.9% to 18.8%. For formation ratio of catechol/hydroquinone was increased from 1.28 to 1.45 after 5th regeneration at $550^{\circ}C$, and from 1.28 to 1.20 after 5th regeneration at $700^{\circ}C$. The main reasons for deactivation of the catalyst were suggested by analyzing chemical/physical properties with XRD, UV-vis spectra, $N_2$ adsorption/desorption and TGA, and evaluating the catalytic activity such as phenol conversion and product selectivity.

본 연구에서는 과산화수소수에 의한 페놀의 수산화 반응에서 사용한 TS-1 촉매를 효과적으로 재사용할 때, 소성 온도가 촉매의 특성에 미치는 영향에 대해서 연구하였다. TS-1 촉매를 5회 재생시켜 반복 사용하였는데, 매회 마다 $550^{\circ}C$ 및 $700^{\circ}C$에서 각각 소성하였다. Fresh한 촉매의 페놀 전환율은 22.9%이었는데, $550^{\circ}C$에서 소성한 촉매에서는 5회 재 생하였을 때 15.1%로 감소하였고, $700^{\circ}C$에서 소성한 촉매는 5회 재생하였을 때 18.8%로 감소하였다. 그리고 카테콜/하이드로퀴논의 생성비가 $550^{\circ}C$에서 5회 재생 후에는 1.45, $700^{\circ}C$에서 5회 재생 후에는 1.2가 되었다. 소성 온도에 따른 재생 전 후 촉매에 대한 XRD, UV-vis spectra, $N_2$ 흡착/탈착 시험, TGA 등과 같은 특성 분석 및 촉매 성능(페놀 전환율 및 생성물의 선택도)을 비교함으로써 촉매의 비활성화 원인을 예측하였다.

Keywords

References

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