Impact of Heteroatom Speciation on the Activity and Stability of Carbon‐Based Catalysts for Propane Dehydrogenation

Abstract

AbstractMetal‐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.