微介孔复合分子筛限域的单分散Fe(Mo)催化体系无氧直接转化甲烷制乙烯

The efficient utilization of gaseous hydrocarbon resources (i.e., methane) has restricted the development of China's energy industry. The vast reserves of the resource will be converted into high-value fuels and chemicals (especially olefins), which has sparked the interest of researchers worldwide and spurred unprecedented investment. This is also an important step to improve China's energy structure. The proposal aims to fabricate a novel catalyst with single-atom Fe(Mo) center confined in a micro-mesoporous zeolite channel, which enables the direct non-oxidative conversion of methane without coke deposition and the channel-shape-selective methane to ethylene and hydrogen with high selectivity. Via a series of in situ techniques and DFT calculations, we will further explore and reveal the stucture of active sites, chain-growth mechanism of products and rate-determined steps in the direct conversion of methane to ethylene over a catalyst with single-atom Fe(Mo)center confined in a micro-mesoporous zeolite channel. Furthermore, we will recognize and understand the effect of shape selectivity of zeolite channel on the rational conversion of methane to ethylene with high selectivity. The proposal will provide reliable experimental evidence and theoretical guidance for the novel process of direct non-oxidative methane to ethylene and hydrogen. This will further enrich and develop the theoretical basis of direct non-oxidative conversion of methane to ethylene, and promote the practical chemical utilization of natural gas and shale gas.

高效利用气态碳氢资源（甲烷）已成为制约我国能源工业发展的重要环节，将这种丰富的资源转化为燃料和高附加值的化学品（特别是低碳烯烃）重新激起了世界范围的兴趣，同时也是改善我国能源结构的重要步骤。本项目旨在构建结构新颖的分子筛孔道限域单分散Fe（Mo）中心催化体系，高效的实现甲烷无氧零积炭活化转化和孔道择形定向合成乙烯的过程。并辅以先进原位表征技术和DFT理论计算工具，深入探讨和揭示微介孔复合分子筛孔道限域的单分散Fe（Mo）中心催化体系在甲烷无氧直接制乙烯和氢气过程中的活性位结构、产物链增长机制和速控步骤；同时认识和理解分子筛孔道对甲烷定向合成乙烯的择形效应。本项目将为新型甲烷无氧直接制乙烯和氢气过程提供可靠的实验依据和理论指导，丰富和发展甲烷无氧直接转化的理论基础，推动天然气和页岩气化工利用的实用化发展。

气态碳氢资源（甲烷）转化为燃料和高附加值的化学品（特别是低碳烯烃）重新激起了世界范围的兴趣，同时也是改善我国能源结构的重要步骤。我们成功构建结构新颖的分子筛孔道限域单分散Fe（Mo）中心催化体系，实现了甲烷无氧零积炭活化转化和孔道择形定向合成乙烯的过程。并辅以先进原位表征技术，深入探讨和揭示微介孔复合分子筛孔道限域的单分散Fe（Mo）中心催化体系在甲烷无氧直接制乙烯和氢气过程中的活性位结构、产物链增长机制和速控步骤；同时认识和理解分子筛孔道对甲烷定向合成乙烯的择形效应。本项目将为新型甲烷无氧直接制乙烯和氢气过程提供可靠的实验依据和理论指导，丰富和发展甲烷无氧直接转化的理论基础，推动天然气和页岩气化工利用的实用化发展。