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Impact of Heteroatom Speciation on the Activity and Stability of Carbon-Based Catalysts for Propane Dehydrogenation
ChemCatChem ( IF 3.8 ) Pub Date : 2021-03-16 , DOI: 10.1002/cctc.202100208
Simon Büchele 1 , Guido Zichittella 1 , Spyridon Kanatakis 1 , Sharon Mitchell 1 , Javier Pérez-Ramírez 2
Affiliation  

Metal-free carbon catalysts represent attractive alternatives to platinum and chromium-containing systems for the on-purpose production of propylene, a crucial chemical building block, via non-oxidative propane dehydrogenation. However, the role of heteroatoms in determining reactivity and stability is poorly understood. Here, the study of a platform of polyaniline-derived and activated carbons, with distinct porous properties, and heteroatom type, content, and speciation, enables establishing improved structure-performance relationships. In-depth characterization reveals that, while several oxygen species potentially catalyze the reaction, carbonyl groups are the main functionality governing the activity. Oxygen loss via propane-driven water evolution is the main deactivation path. Six-fold enhanced stability evidenced over carbon catalysts derived from KOH-post-treated polyanilines demonstrates the importance of controlling the nanostructure for enhancing longevity.

中文翻译:

杂原子形态对丙烷脱氢碳基催化剂活性和稳定性的影响

无金属碳催化剂代表了含铂和铬系统的有吸引力的替代品,用于通过非氧化丙烷脱氢有针对性地生产丙烯,这是一种关键的化学结构单元。然而,人们对杂原子在决定反应性和稳定性方面的作用知之甚少。在这里,对聚苯胺衍生和活性炭平台的研究,具有不同的多孔性质、杂原子类型、含量和形态,能够建立改进的结构-性能关系。深入表征表明,虽然几种氧物质可能催化反应,但羰基是控制活性的主要官能团。氧气损失通过丙烷驱动的水演化是主要的失活途径。由 KOH 后处理的聚苯胺衍生的碳催化剂证明稳定性提高了六倍,这证明了控制纳米结构对提高寿命的重要性。
更新日期:2021-03-16
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