Towards a molecular understanding of deactivation issues in methane reforming catalysts

这项研究方案汇集了表面化学、多相催化、固态化学、红外光谱、拉曼光谱和非弹性中子散射光谱方面的专家，以确定负责维持甲烷重整催化剂氢产率的关键因素。Ormerod已经制备了一些甲烷重整催化剂，并对其进行了部分表征，这些催化剂在氢气选择性和操作寿命方面表现出了广泛的性能。虽然标准配方显示出预期的催化剂失活特性，但一些改进的催化剂表现出极好的氢选择性，可以在更长的时间内保持，即观察到最小的失活。研究小组提出了一个工作计划，通过该计划，研究小组将从机理上理解为什么“好的”催化剂倾向于高氢选择性，并避免导致表面寡聚物种形成并最终导致催化剂失活的碳沉积过程。这项多学科和多机构的研究建议与英国化学工业的能源需求直接相关，而且还针对科学基础的关键领域，如最近Whiteside的报告和EPSRC的研究优先事项和机会文件所强调的那样。

This research proposal brings together a grouping of specialists in surface chemistry, heterogeneous catalysis, solid state chemistry, infrared spectroscopy, Raman spectroscopy and inelastic neutron scattering spectroscopy to identify the critical factors responsible for maintaining hydrogen yields in methane reforming catalysts. Ormerod has already prepared, and partially characterised, a number of methane reforming catalysts that display a wide range of performance, in terms of hydrogen selectivity and operational lifetime. Whereas the standard formulations display the expected catalyst deactivation characteristics, some of the modified catalysts exhibit excellent hydrogen selectivity that can be maintained over extended periods of time, i.e. minimal deactivation is observed. A workplan is presented whereby the research team will develop a mechanistic understanding of why the 'good' catalysts favour high hydrogen selectivity and avoid the carbon laydown processes, that lead to the formation of surface oligermic species and, ultimately, catalyst deactivation. This multi-disciplinary and multi-institutional research proposal has direct connections to energy requirements of the UK chemical industry and, moreover, targets key areas of the science base as highlighted in the recent Whiteside's report and the EPSRC's Research Priorities and Opportunities document.