Aqueous-Phase Partial Oxidation of Methane over Pd-Fe/ZSM-5 with O2 in the presence of H2
산소와 수소 존재 하에 Pd-Fe/ZSM-5를 사용하여 생성시킨 과산화수소를 이용한 메탄의 액상산화 반응
- 주제(키워드) hydrogen peroxide , methanol , partial oxidation of methane , Pd-Fe/ZSM-5 , stability
- 주제(DDC) 621.042
- 발행기관 아주대학교 일반대학원
- 지도교수 박은덕
- 발행년도 2024
- 학위수여년월 2024. 2
- 학위명 석사
- 학과 및 전공 일반대학원 에너지시스템학과
- 실제URI http://www.dcollection.net/handler/ajou/000000033479
- 본문언어 한국어
- 저작권 아주대학교 논문은 저작권에 의해 보호받습니다.
초록/요약
Methane is a major component in natural gas, shale gas, coalbed gas, biogas, and gas hydrates, which are available in abundance. Additionally, it is used as a chemical feedstock via syngas (a mixture of CO and H2) in an energy-intensive process. Such commercial application requires the use of large-scale manufacturing plants. Thus, there is a demand for a process that enables the direct conversion of methane under mild reaction conditions. Partial oxidation of methane to methane oxygenates with molecular oxygen is an ideal route for the direct methane conversion technique as it is thermodynamically favorable even at low reaction temperatures. In the pursuit of this objective, numerous oxidizing agents have been employed in the reaction. However, except for oxygen, many of these oxidants are often regarded as economically impractical. A catalytic system that oxidizes methane to methane oxygenates using H2O2 generated in-situ could be of the solutions. In this study, we have developed a one-body catalyst composed of Pd-Fe/ZSM-5, containing a low concentration of palladium, for the selective aqueous-phase oxidation of methane in the presence of H2 and O2. The palladium metal component facilitated the synthesis of H2O2, which then reacted with methane over the nearby iron species located within the zeolite pores. Remarkably, 0.28%Pd-0.56%Fe/ZSM-5 displayed excellent productivity of c.a. 30 mmol kgcat-1 h-1 and methane oxygenates selectivity of 70% in a continuous flow reactor. *Keyword: hydrogen peroxide, methanol, partial oxidation of methane, Pd-Fe/ZSM-5, stability.
more목차
Chapter I. Introduction 1
1.1. Background 1
1.2. Partial oxidation of methane to methane oxygenates 4
1.3. Liquid-phase partial oxidation of methane with H2O2 synthesized under in-situ condition 8
Chapter II. Experimental 15
2.1. Preparation of catalysts 15
2.2. Partial oxidation of methane 15
2.3. Characterization of catalysts 16
Chapter III. Results and Discussion 18
3.1. Partial oxidation of methane over Pd-Fe/ZSM-5 in the presence of O2 and H2 18
3.2. Characterization 35
Chapter IV. Conclusion 48
국문 초록 49
References 50
