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Continuous Partial Oxidation of Methane into Methanol over Cu-mordenite

초록/요약

The direct conversion of methane into methanol is an ideal, auspicious process; however, its application remains challenging. Herein, a systematic study was carried out on the continuous gas-phase oxidation of methane into methanol with steam in the absence and presence of O2 over Cu-mordenite (Cu-MOR) with various Cu loadings. The methanol productivity was found to depend on the Cu/Al ratio and selecting the optimum Cu/Al ratio was crucial in maximizing methanol productivity. Methanol productivity increased with the O2 concentration up to a certain point, after which methanol selectivity decreased. The stability of the catalyst improved with increasing Cu/Al ratio. Methanol selectivity was found to be 100% under anaerobic conditions, indicating the effectiveness of steam in activating methane and preventing further oxidation of the methoxy group. However, under aerobic conditions, methanol selectivity decreased due to the oxidation of the methoxy group by O2. The developed catalysts achieved stable methanol production rates, and the dominant Cu species changed with the Cu/Al ratio. Overall, the results suggest that optimizing the Cu/Al ratio and carefully controlling the O2 concentration in the feed can improve the conversion of methane into methanol using Cu-MOR catalysts.

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목차

CHAPTER 1 INTRODUCTION 1
1.1 Background 1
1.2 Homogeneous catalytic methane oxidation technology 7
1.3 Heterogenous catalytic methane oxidation technology 9
1.3.1 Molybdenum-based Catalysts 9
1.3.2 Vanadium-based Catalysts 11
1.3.3 Iron-based catalysts 13
1.3.4 Copper-based catalysts 15
CHAPTER 2 EXPERIMENTAL 19
2.1 Material 19
2.2 Preparation of catalyst 20
2.3 Characterization of catalyst 21
2.4 Catalytic activity evaluation 22
CHAPTER 3 RESULTS AND DISCUSSION 24
3.1 Catalyst Characterization 24
3.2 Continuous conversion of methane into methanol with steam under anaerobic conditions 37
3.3 Continuous conversion of methane into methanol with steam under aerobic conditions 40
3.4 The stability of catalyst 49
3.5 The study of post-reaction characterization and catalytic performance analysis of Cu-MOR. 53
3.6 Reaction activation energy and catalytic activity comparison of Cu-MOR 63
CHAPTER 4 CONCLUSION 71
REFERENCES 72

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