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Structure and performance of zeolite supported Pd for complete methane oxidation
Catalysis Today ( IF 5.3 ) Pub Date : 2020-12-28 , DOI: 10.1016/j.cattod.2020.11.026
Ida Friberg , Adam H. Clark , Phuoc Hoang Ho , Nadezda Sadokhina , Glen J. Smales , Jungwon Woo , Xavier Auvray , Davide Ferri , Maarten Nachtegaal , Oliver Kröcher , Louise Olsson

The influence of zeolite support materials and their impact on CH4 oxidation activity was studied utilizing Pd supported on H-beta and H-SSZ-13. A correlation between CH4 oxidation activity, Si/Al ratio (SAR), the type of zeolite framework, reduction-oxidation behaviour, and Pd species present was found by combining catalytic activity measurements with a variety of characterization methods (operando XAS, NH3-TPD, SAXS, STEM and NaCl titration). Operando XAS analysis indicated that catalysts with high CH4 oxidation activity experienced rapid transitions between metallic- and oxidized-Pd states when switching between rich and lean conditions. This behaviour was exhibited by catalysts with dispersed Pd particles. By contrast, the formation of ion-exchanged Pd2+ and large Pd particles appeared to have a detrimental effect on the oxidation-reduction behaviour and the conversion of CH4. The formation of ion-exchanged Pd2+ and large Pd particles was limited by using a highly siliceous beta zeolite support with a low capacity for cation exchange. The same effect was also found using a small-pore SSZ-13 zeolite due to the lower mobility of Pd species. It was found that the zeolite support material should be carefully selected so that the well-dispersed Pd particles remain, and the formation of ion-exchanged Pd2+ is minimized.



中文翻译:

沸石负载钯的结构和性能完全氧化甲烷

利用负载在 H-β 和 H-SSZ-13 上的 Pd 研究了沸石载体材料的影响及其对 CH 4氧化活性的影响。CH之间的相关性4氧化活性,Si / Al比(SAR),沸石骨架,氧化还原行为和Pd物种存在的类型,发现通过催化活性测量与多种表征方法(operando XAS,NH组合3 -TPD、SAXS、STEM 和 NaCl 滴定)。Operando XAS 分析表明高 CH 4催化剂在富和贫条件之间切换时,氧化活性经历了金属和氧化 Pd 状态之间的快速转变。这种行为由具有分散 Pd 颗粒的催化剂表现出来。相比之下,离子交换的 Pd 2+和大 Pd 颗粒的形成似乎对氧化还原行为和 CH 4的转化具有不利影响。离子交换 Pd 2+的形成大 Pd 颗粒通过使用具有低阳离子交换能力的高硅质 β 沸石载体受到限制。由于 Pd 物质的迁移率较低,使用小孔 SSZ-13 沸石也发现了相同的效果。发现应仔细选择沸石载体材料,以便保留良好分散的 Pd 颗粒,并使离子交换 Pd 2+的形成最小化。

更新日期:2020-12-28
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