在铁基金属有机框架上直接将甲转化为乙烯和乙烯
Yujie Ma1, Xue Han1,2, Shaojun Xu3
1Department of Chemistry, University of Manchester, Manchester M13 9PL, U.K.
Journal of the American Chemical Society
|September 18, 2023
概括
本研究表明,在环境条件下使用非热等离子体和金属有机框架 (MFM-300(Fe)) 将甲直接转化为有价值的乙烯和乙烯. 这一突破提供了高效的天然气利用和综合产品分离.
科学领域:
- 催化和材料科学
- 化学工程
- 可持续的化学
背景情况:
- 直接将甲 (CH4) 转化为更高的碳化合物,如乙烯 (C2H4) 和乙烯 (C2H2),对于天然气的价值化至关重要.
- 传统方法需要严苛的条件 (高温/高压) 并面临产品分离的挑战.
- 在温和条件下开发高效的催化剂和甲转化工艺是非常理想的.
研究的目的:
- 使用非热等离子体将甲直接转化为乙烯和乙烯.
- 在环境条件下研究金属有机框架材料MFM-300的催化性能.
- 开发一种用于甲转化和产品分离的综合系统.
主要方法:
- 在环境温度 (25 °C) 和压力 (1 atm) 的流量条件下使用的非热等离子体.
- 使用MFM-300 ((Fe) 作为甲转化催化剂.
- 应用现场光谱技术 (中子衍射,INS,NMR,EPR,DRIFTS) 和建模以阐明反应机制.
- 开发了一种连锁固定系统,用于在线分离产品.
主要成果:
- 在乙烯和乙烯形成方面获得高选择性 (96%),时间产量为334μmolgcat-1h-1.
- 在10%的甲转化时,对C2+碳化合物具有超过98%的选择性,时间产量超过2056μmolgcat-1h-1.
- 确定了MFM-300中的Fe-O (H) -Fe位点,这些位点对于通过Fe-O (CH3) -Fe添加物进行甲激活和中间稳定至关重要.
- 通过在线将乙烯和乙烯从未反应的甲中分离,成功实现了甲转化.
结论:
- 与MFM-300 ((Fe) 结合的非热等离子使甲在环境条件下能够有效地直接转化为有价值的C2碳化合物.
- 这项研究为甲转化设定了新的基准,超过了以前的记录.
- 综合转换和分离系统为天然气利用的实际应用铺平了道路.
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