Abstract The creation of metal‐metal oxide interfaces is an important approach to fine‐tuning catalyst properties through strong interfacial interactions. This article presents the work on developing interfaces between Pt and CeOxthat improve Pt surface energetics for the hydrogen evolution reaction (HER) within an alkaline electrolyte. The Pt‐CeOxinterfaces are formed by depositing size‐controlled Pt nanoparticles onto a carbon support already coated with ultrathin CeOxnanosheets. This interface structure facilitates substantial electron transfer from Pt to CeOx, resulting in decreased hydrogen binding energies on Pt surfaces, and water dissociation for the HER, as predicted by the density functional theory (DFT) calculations. Electrochemical testing indicates that both Pt specific activity and mass activity are improved by a factor of 2 to 3 following the formation of Pt‐CeOxinterfaces. This study underscores the significance and potential of harnessing robust interfacial effects to enhance electrocatalytic reactions. 
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                            Ultra‐Low Loading Pt/CeO 2 Catalysts: Ceria Facet Effect Affords Improved Pairwise Selectivity for Parahydrogen Enhanced NMR Spectroscopy
                        
                    
    
            Abstract Oxide supports with well‐defined shapes enable investigations on the effects of surface structure on metal–support interactions and correlations to catalytic activity and selectivity. Here, a modified atomic layer deposition technique was developed to achieve ultra‐low loadings (8–16 ppm) of Pt on shaped ceria nanocrystals. Using octahedra and cubes, which expose exclusively (111) and (100) surfaces, respectively, the effect of CeO2surface facet on Pt‐CeO2interactions under reducing conditions was revealed. Strong electronic interactions result in electron‐deficient Pt species on CeO2(111) after reduction, which increased the stability of the atomically dispersed Pt. This afforded significantly higher NMR signal enhancement in parahydrogen‐induced polarization experiments compared with the electron‐rich platinum on CeO2(100), and a factor of two higher pairwise selectivity (6.1 %) in the hydrogenation of propene than any previously reported monometallic heterogeneous Pt catalyst. 
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                            - Award ID(s):
- 1933723
- PAR ID:
- 10236102
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Angewandte Chemie International Edition
- Volume:
- 60
- Issue:
- 8
- ISSN:
- 1433-7851
- Page Range / eLocation ID:
- p. 4038-4042
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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