Dataset for Modulating the Dynamics of Brønsted Acid Sites on PtWOx Inverse Catalyst

Published: 4 February 2022| Version 1 | DOI: 10.17632/hp45n9ykd6.1
, Shizhong Liu, Weiqing Zheng, Renjing Huang, Cong Wang, Ajibola Lawal, Konstantinos Alexopoulos, Sibao Liu, Yunzhu Wang, Kewei Yu, J. Anibal Boscoboinik, Yuefeng Liu, Xi Liu, Anatoly I. Frenkel, Omar A. Abdelrahman, Raymond J. Gorte, Stavros Caratzoulas, Dionisios G. Vlachos


Brønsted acid sites on the oxide overlayers of metal-metal oxide (M-MO) inverse catalysts are often hypothesized to drive selective C-O bond activation. However, the Brønsted acid site nature and dynamics under working conditions remain poorly understood due to multiple materials functionalities. Here, we investigate the formation and the dynamics of Brønsted acid and redox sites on PtWOx/C under working conditions. DFT-based thermodynamic calculations and microkinetic modeling reveal a complex interplay between Brønsted acid and redox sites and potentially fast catalyst dynamics at comparable time scales to the Bronsted acid catalyzed dehydration chemistry. Combining in situ characterization and probe chemistry, we demonstrate that the density of Brønsted acid sites on the PtWOx/C inverse catalyst could be modulated by up to two orders of magnitude by altering the reaction parameters and by the chemistry itself. We elicit an order of magnitude increase in the acid-catalyzed dehydration average reaction rate by periodic hydrogen pulsing.