固体核磁共振技术研究甲烷活化和转化的反应机理

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	固体核磁共振技术研究甲烷活化和转化的反应机理
Alternative Title	Mechanistic Investigation on the Activation and Conversion of Methane by Solid-State NMR
	吴剑峰
Subtype	博士
Thesis Advisor	王为
	2014-05-25
Degree Grantor	兰州大学
Place of Conferral	兰州
Degree Name	博士
Keyword	固体核磁甲烷 Zn/H‒ ZSM-5分子筛反应机理
Abstract	甲烷作为天然气的主要成份，具有储量大，价格低廉的优势。研究表明锌修饰的分子筛对甲烷的共转化反应具有很高的催化活性。为此，我们首先分离了甲烷在锌修饰的H-ZSM-5分子筛上活化生成的三种表面物种：锌甲基物种、锌甲氧基物种和甲酸锌盐物种。然后，我们研究了它们的反应活性。我们在Zn/H-ZSM-5分子筛上研究了甲烷分别和二甲醚、溴和二氧化碳的活化和转化机理。我们在Zn/H-ZSM-5分子筛上首次发现的结果有：（1）甲烷和二甲醚能够共转化为甲基取代的苯。（2）甲烷在溴存在的条件下，能够在室温下活化生成锌甲氧基物种。在673 K下，锌甲氧基物种进一步转化生成一溴甲烷。（3）甲烷和二氧化碳能够选择性的共转化为乙酸。我们在Zn/H-ZSM-5分子筛上研究了甲烷和二氧化碳直接转化为乙酸的催化效果。在673 K和不同反应压力下，乙酸的选择性均保持很高（> 96.73%）。
Other Abstract	Methane, the primary component of natural gas, is one of the most abundant and low-cost feed stocks available. The research showed that the zinc-modified zeolites have high activity towards the co-conversion of methane. Hence, we isolate these three surface species after methane activation on zinc-modified H-ZSM-5 zeolite: zinc methyl species, zinc methoxy species, and surface formate species. Then, we studied their reactivity. We investigate the activation and conversion of methane with DME, Br2, and carbon dioxide, respectively, on Zn/H-ZSM-5 zeolite. On Zn/H-ZSM-5 zeolite, we found for the first time that: (1) methane and DME could co-conversion into methyl substituted benzenes. (2) In the presence of Br2, methane could be activated to generate zinc methoxy species at room temperature. At 673 K, zinc methoxy species could transform into methyl bromide. (3) Methane and carbon dioxide could selectively co-conversion into acetic acid. We investigate the catalytic effect of the direct conversion of methane and carbon dioxide on Zn/H-ZSM-5 zeolite. The selectivity of acetic acid keeps high (> 96.73%) at 673 K with different reaction pressure.
URL	查看原文
Language	中文
Document Type	学位论文
Identifier	https://ir.lzu.edu.cn/handle/262010/237721
Collection	化学化工学院
Recommended Citation GB/T 7714	吴剑峰. 固体核磁共振技术研究甲烷活化和转化的反应机理[D]. 兰州. 兰州大学,2014.

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