Sustainable and environmentally benign catalytic processes are vital for the future to supply the world population with clean energy and industrial products. The replacement of conventional metal or metal oxide catalysts with earth abundant and renewable non-metallic materials has attracted considerable research interests in the field of catalysis and material science. In this talk, we summarize the recent progress in the kinetic and mechanistic studies on nanocarbon catalyzed alkane oxidative dehydrogenation reactions. The presentation attempts to extract general concepts and basic regularities for carbon catalytic process directing us on the way for rational design of novel efficient metal-free catalysts. The nature of the active sites for oxidative dehydrogenation reactions has been revealed through in situ chemical titration strategies. The detailed kinetic analysis and in situ catalyst structure characterization suggests that carbon catalyzed oxidative dehydrogenation reactions involve the redox cycles of the ketonic carbonyl-hydroxyl pairs, and the key physicochemical parameters (activation energy, reaction order and rate/equilibrium constants etc.) of the carbon catalytic systems are proposed and compared with conventional transition metal oxide catalysts. The proposal of the intrinsic catalytic activity provides the possibility for the fair comparisons of different nanocarbon catalysts and the consequent structurefunction relation regularity. Surface modification and hetero-atom doping are proved as the most effective strategies to adjust the catalytic property (activity and product selectivity etc.) of the nanocarbon catalysts. Following the structure-function relations, a novel and highly efficient molebdenum carbide modified nanocarbon catalyst for alkane dehydrogenation is developed. The presentation also exhibit the importance of the in situ structural characterizations for heterogeneous nanocarbon catalysis. The research strategy and methods proposed for carbon catalysts may also shed light on other complicated catalytic systems or fields concerning the applications of carbon materials, such as energy storage and environment protection etc.

Alkane dehydrogenation on nanocarbon catalysts: From reaction mechanism to catalyst design

2019 Spring National Meeting

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