AVS 66th International Symposium & Exhibition
    Fundamental Discoveries in Heterogeneous Catalysis Focus Topic Thursday Sessions
       Session HC+2D+SS-ThM

Invited Paper HC+2D+SS-ThM10
Mythbusting: From Single Crystals in UHV to Catalytic Reactors

Thursday, October 24, 2019, 11:00 am, Room A213

Session: Nanoscale Surface Structure in Heterogeneously-Catalyzed Reactions
Presenter: Christian Reece, Harvard University
Authors: R.J. Madix, Harvard University
C. Reece, Harvard University
Correspondent: Click to Email
For decades it has been an objective of surface science studies of chemical reactivity to make a direct connection to heterogeneous catalysis. Over these years the difficulties encountered in connecting these two areas of research gave rise to the dismissal of this possibility by the catalysis community and the invention of such shorthand terms as “pressure gap” and “materials gap” to express this view. Usually overlooked is also the fact that catalytic reactions are conducted at much higher temperatures than the related studies on single crystal surfaces, so a “temperature gap” also exists. In fact, these regimes of reactivity are directly linked by fundamental knowledge of the identity and rate constants for the operative elementary steps comprising the catalytic cycle under catalytic conditions. Further, for many catalytic materials, its state can be defined by the reaction conditions themselves in quaisi-thermodynamic terms. Connection between the reactivity observed on the single crystals with that on the catalyst surface is possible by the use of a transient pressure method which is conducted over the actual catalyst material under Knudsen flow conditions. Recently we have demonstrated this historically elusive connection between UHV-based studies and catalytic performance for the catalytic oxygen-assisted synthesis of methyl formate from methanol over a nanoporous gold catalyst. The connection is entirely based on the kinetics and mechanism determined on single crystal gold surfaces. A brief history of this development will be discussed and the specifics of how this bridge was built examined.