AVS 65th International Symposium & Exhibition | |
Surface Science Division | Wednesday Sessions |
Session SS+HC-WeM |
Session: | Catalytic Alloys: Understanding Heterogeneity |
Presenter: | Jin-Hao Jhang, Yale University |
Authors: | J.-H. Jhang, Yale University G.S. Hutchings, Yale University J.A. Boscoboinik, Center for Functional Nanomaterials Brookhaven National Laboratory E.I. Altman, Yale University |
Correspondent: | Click to Email |
The participation of water in zeolites is widely seen in catalysis, ion-exchange, and wastewater treatment. Water adsorption, dissociation and desorption all play critical roles in forming catalytically active Brønsted and Lewis acid sites. Recently, two-dimensional (2D) silica and aluminosilicate bilayers were fabricated on different substrates successfully. Prior studies have suggested that protonated 2D aluminosilicate can be formed and these protonated sites may be analogous to those in acid zeolites. Thereby, the 2D aluminosilicate shows its potential as a zeolite model. In this work, we studied water chemistry on 2D silica and aluminosilicate grown on a Pd(111) substrate by combining density function theory (DFT), thermal desorption spectroscopy (TDS), and ambient pressure photoelectron spectroscopy (AP-PES). We found that protonated 2D aluminosilicate on Pd(111) is thermally stable with both dehydrogenation and dehydration of the protonated surface energetically infeasible under 1000 K. Based on the theoretical and experimental results, once the aluminosilicate surface is protonated, no further water dissociation will take place. The AP-PES study suggests that molecular water can penetrates through the 2D bilayers and stays at the bilayer-substrate interface, leading to core-level shifts in the 2D bilayers due to changes of dipole moments. These findings show that the Brønsted acid sites on the Pd-supported 2D aluminosilicate are robust, and thereby provide fundamental information on the more complex zeolite surfaces.