초록

· 생체모방계인 Gif 산화계에서 반응속도를 증가시키기 위하여 리간드의 연구를 시도하였으며 picolinic acid를 포함하여 여러종류의 리간드를 개발하였다.· Fe-Pd 산화계를 개발하여 균일계를 불균일계로 발전시켰으며 촉매의 수명을 연장시켰다.· 제올라이트를 담체나 촉매로 사용하여 형상선택성을 갖는 불균일계의 반응계를 개발하였다.· 공업화의 기초연구를 수행하여 상기 산화계를 10배규모반응기에서 수행하였을 경우 촉매의 활성등은 재현성을 보여주었으며 공정상 발생할 수 있는 문제점을 점검 해결하고자 하였다.

Abstract ▼

The selective oxidation of hydrocarbons under mild conditions (room temperature, atmospheric pressure) is an industrially important subject, which is presently operated at high pressure and high temperature. Since the discovery of biological Cp-450 model system, this research has become a stimulatin

The selective oxidation of hydrocarbons under mild conditions (room temperature, atmospheric pressure) is an industrially important subject, which is presently operated at high pressure and high temperature. Since the discovery of biological Cp-450 model system, this research has become a stimulating research area. In this report, the oxidation of cyclohexane under mild conditions have been developed with slightly modified Gif system and cyclohexanone and cyclohexanol are selectively produced. The ligand effect was investigated to increase the oxygen activity. Picolinic acid, pyridine having carboxyl group on ortho position, showed the best reactivity in our experimental conditions. From the results of the investigation of the role of carboxyl group on ortho position of pyridine new mechanism was suggested. For practical use, we found out simple and effsctive catalyst systems such as Fe-Pd and Fe-Zeolites system. This was an heterogeneous system and therefore, separation of the catalyst form reaction mixture and products from solvent were simpler. The active component was found to be Fe₂O₃ and was deactivated to Fe₃O₄ after several usage, however, these catalysts can be recycled by simple drying at 120 ℃. Zeolites were selected and dealuminated to use as supports of Fe₂O₃Especially, dealuminated zeolite (Si/Al=20) showed increased conversion upto 8%. We also found optimum temperature was at 30-35 ℃. Scale-up test was performed with 10 times expanded reactor and all the catalysts showed similar activity with that conducted at small scale.

목차 Contents

• 제 1 장 서 론...15
• 제 2 장 국내외 기술개발현황...17
• 제 3 장 연구개발수행 내용 및 결과...22
• 제 3-1 장 분석장비...22
• 제 3-2 장 균일계촉매 산화반응...24
• 제 1 절 서론...24
• 제 2 절 실험...26
• 제 3 절 결과 및 고찰...27
• 제 4 절 결론...39
• 제 3-3 장 Fe-Pd 촉매계...40
• 제 1 절 서론...40
• 제 2 절 실험...40
• 제 3 절 결과 및 고찰...41
• 제 4 절 결론...62
• 제 3-4 장 제올라이트촉매계...63
• 제 1 절 서론...63
• 제 2 절 실험...63
• 제 3 절 결과 및 고찰...90
• 제 4 절 결론...101
• 제 3-5 장 확대반응기에서의 연구...102
• 제 1 절 서론...102
• 제 2 절 실험...102
• 제 3 절 결과 및 고찰...103
• 제 4 절 결론...116
• 제 4 장 연구개발목표 달성도 및 대외기여도...117
• 제 5 장 연구개발결과의 활용계획...119
• 제 6 장 참고문헌...120