Reactivity Descriptor in Solid Acid Catalysis: Predicting Turnover Frequencies for Propene Methylation in Zeotypes.
Recent work has reported the discovery of metal surface catalysts by employing a descriptor-based approach, establishing a correlation between a few well-defined properties of a material and its catalytic activity. This theoretical work aims for a similar approach in solid acid catalysis, focusing on the reaction between propene and methanol catalyzed by Brønsted acidic zeotype catalysts. Experimentally, the ammonia heat of adsorption is often used as a measure of the strength of acid sites. Using periodic DFT calculations, we show that this measure can be used to establish scaling relations for the energy of intermediates and transition states, effectively describing the reactivity of the acid site. This allows us to use microkinetic modeling to predict a quantitative relation between the ammonia heat of adsorption and the rate of propene methylation from first principles. We propose that this is the first step toward descriptor-based design of solid acid catalysts.
†SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States.|‡Shanghai Research Institute of Petrochemical Technology SINOPEC, Shanghai 201208, China.
Chuan-Ming
CM
Wang
†SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States.|¶Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States.
Rasmus Y
RY
Brogaard
†SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States.|§Inorganic Chemistry and Catalysis Group, Debye Institute for Nanomaterials Science, Faculty of Science, Utrecht University, 3584 CG Utrecht, The Netherlands.
Bert M
BM
Weckhuysen
†SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States.|¶Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States.
Jens K
JK
Nørskov
†SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States.
Felix
F
Studt
acid catalysis; ammonia; density functional theory; scaling relations; zeolites