Reactivity Switch of Platinum with Gallium: From Reverse Water Gas Shift to Methanol Synthesis
OPEN ACCESS
Loading...
Author / Producer
Date
2024-04-17
Publication Type
Journal Article
ETH Bibliography
yes
OPEN ACCESS
Data
Rights / License
Abstract
The development of efficient catalysts for the hydrogenation of CO2 to methanol using "green" H-2 is foreseen to be a key step to close the carbon cycle. In this study, we show that small and narrowly distributed alloyed PtGa nanoparticles supported on silica, prepared via a surface organometallic chemistry (SOMC) approach, display notable activity for the hydrogenation of CO2 to methanol, reaching a 7.2 mol(CH3OH) h(-1) mol(Pt)(-1) methanol formation rate with a 54% intrinsic CH3OH selectivity. This reactivity sharply contrasts with what is expected for Pt, which favors the reverse water gas shift reaction, albeit with poor activity (2.6 mol(CO2) h(-1) mol(Pt)(-1)). In situ XAS studies indicate that ca. 50% of Ga is reduced to Ga-0 yielding alloyed PtGa nanoparticles, while the remaining 50% persist as isolated Ga-III sites. The PtGa catalyst slightly dealloys under CO2 hydrogenation conditions and displays redox dynamics with PtGa-GaOx interfaces responsible for promoting both the CO2 hydrogenation activity and methanol selectivity. Further tailoring the catalyst interface by using a carbon support in place of silica enables to improve the methanol formation rate by a factor of similar to 5.
Permanent link
Publication status
published
External links
Editor
Book title
Journal / series
Volume
146 (15)
Pages / Article No.
10806 - 10811
Publisher
American Chemical Society
Event
Edition / version
Methods
Software
Geographic location
Date collected
Date created
Subject
Organisational unit
03872 - Copéret, Christophe / Copéret, Christophe
Notes
Funding
180544 - NCCR Catalysis (phase I) (SNF)
192050 - Molecular Approach and Understanding in Heterogeneous Catalysis (SNF)
192050 - Molecular Approach and Understanding in Heterogeneous Catalysis (SNF)