钼基催化剂MoS2结构和尺寸调控及其对耐硫甲烷化性能的影响

本项目研究目标是对钼基催化剂中的MoS2结构和尺寸进行调控，探讨耐硫甲烷化催化剂的活性位并确定钼基催化剂构效关系。拟通过改变非负载型催化剂的制备条件获得不同形貌和尺寸的MoS2（如多晶型、纳米管型）催化剂，采用加入其它助剂和柱撑法调变MoS2的层状结构和尺寸，对不同结构和尺寸的硫化钼用于耐硫甲烷化的性能进行系统研究,结合甲烷化性能测试结果探讨耐硫甲烷化活性位及其构效关系，为负载型钼基催化剂的制备提供有益的指导。将研究催化剂中活性组分与载体间相互作用对MoS2晶型与结构的影响，系统探讨不同载体如Al2O3、ZrO2、CeO2及复合载体如CeO2-Al2O3负载的钼基催化剂中钼物种的晶粒大小、分布及结构与载体的关系，获得MoO3分散度、MoS2结构和尺寸对耐硫甲烷化反应性能的影响规律。将催化剂制备和甲烷化性能相关联，为设计合成高活性、高稳定性的钼基耐硫甲烷化催化剂提供基础。

The research objective of the project is to investigate the effect of MoS2 structure and size regulation on sulfur-resistant methanation performance, to explore the active site for sulfur-resistant methanation and to determine the structure-activity relationship on molybdenum-based catalysts. For unsupported catalyst, the catalysts with different MoS2 morphologies (such as polycrystalline and nanotubes) can be obtained by changing the catalyst preparation conditions. The MoS2 layered nanocomposites structure was modified by adding other additives or using the Pillared method to achieve intercalation between layers of S-S. The effect of different shape, structure and composition of molybdenum disulfide on the performance of sulfur-resistant methanation will be explored systematically. Based on methanation performance and discussion about the effect of MoS2 shape and composition on methanation performance, the structure-activity relationship of the catalyst for sulfur-resistant methanation was further investigated, which can provide useful guidance for the preparation of supported Mo-based catalysts. Different oxide supports such as Al2O3, ZrO2, CeO2 and composite supports like CeO2-Al2O3 will be used to prepare Mo-based catalysts to study the effect of the interaction between support and molybdenum species on methanation performance. Detailed studies lie in the effect of support on MoO3 dispersion, MoS2 crystalline form and structure, etc. Evaluation of these catalysts for sulfur-resistant methanation performance will be done. Associating catalyst preparation and the methanation performance will provide a basis for design and synthesis of molybdenum-based sulfur-resistant methanation catalyst with high activity and high stability.