Korean Chemical Engineering Research

The Korean Institute of Chemical Engineers (한국화학공학회)
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Study on Preparation of Methyl N-Phenyl Carbamate by Oxidative Carbonylation of Aniline and Methanol

아닐린과 메탄올의 산화 카르보닐화에 의한 Methyl N-phenyl carbamate 제조 연구

  • Roh, Jong-Seon (Department of Chemical & Biological Engineering, Korea University Seoul Campus) ;
  • Lee, Kwan-Young (Department of Chemical & Biological Engineering, Korea University Seoul Campus) ;
  • Kim, Tae-Soon (Invironment & Resource Research Center, Korea Research Institute of Chemical Technology (KRICT)) ;
  • Chang, Tae-Seon (Invironment & Resource Research Center, Korea Research Institute of Chemical Technology (KRICT)) ;
  • Yoon, Byung-Tae (Invironment & Resource Research Center, Korea Research Institute of Chemical Technology (KRICT)) ;
  • Kim, Seong-Bo (Invironment & Resource Research Center, Korea Research Institute of Chemical Technology (KRICT))
  • 노종선 (고려대학교 화공생명공학과) ;
  • 이관영 (고려대학교 화공생명공학과) ;
  • 김태순 (한국화학연구원 온실가스자원화연구그룹) ;
  • 장태선 (한국화학연구원 온실가스자원화연구그룹) ;
  • 윤병태 (한국화학연구원 온실가스자원화연구그룹) ;
  • 김성보 (한국화학연구원 온실가스자원화연구그룹)
  • Received : 2017.04.24
  • Accepted : 2017.08.18
  • Published : 2018.02.01
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Abstract

The production of methyl N-phenyl carbamate by an oxidative carbonylation method of aniline and methanol is of great interest as an environmentally friendly process that can replace the monomer production process of a polymer produce using conventional phosgene. In this study, heterogeneous catalysts were prepared by using Y-zeolite, $SiO_2$, $Al_2O_3$ as support, and oxidative carbonylation continuous operation from aniline and methanol was attempted using the prepared heterogeneous catalyst. Batch reactor was used to determine the support, and various reaction conditions such as reaction temperature, reaction pressure, and effect of promoter were established using palladium catalyst. A reaction kinetics study was conducted under optimum reaction conditions. The basic data for carbamate process development were obtained by performing continuous operation for a long time under established reaction condition.

아닐린과메탄올의산화 카르보닐화방법에의한 Methyl N-phenyl carbamate 제조는 기존의포스겐을사용하는폴리머의 단량체 생산공정을 대체할 수 있는 환경 친화적인 공정으로 많은 관심을 가지고 있다. 본 연구에서는 담지체로 Y-zeolite, $SiO_2$, $Al_2O_3$를 사용하여 불균일화 촉매를 제조하였고, 제조 된 불균일화 촉매를 이용하여 아닐린과 메탄올로부터 산화카르보닐화 연속운전을 시도하였다. 회분식반응기를 이용하여 담지체를 결정하였으며, 담지된 palladium 촉매를 이용하여 조촉매의 영향과 반응온도, 반응압력 등 여러 반응최적조건을 확립하였다. 최적의 반응조건 MPC의 수율은 98.6% 였으며, 반응속도론적 연구를 수행하였다. 각 반응온도의 반응속도상수로부터 얻어진 활성화 에너지는 각각 E=82.38 kJ/mol, E=66.20 kJ/mol 이었다. 또한 확립된 반응조건에서 장시간 연속운전을 수행하여 카바메이트 공정 개발을 위한 기초자료를 구하였다.

Keywords

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