Local Environment Determined Reactant Adsorption Configuration for Enhanced Electrocatalytic Acetone Hydrogenation to Propane
Xuesi Wang
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia
These authors contributed equally to this work.
Search for more papers by this authorYan Jiao
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia
These authors contributed equally to this work.
Search for more papers by this authorLaiquan Li
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia
Search for more papers by this authorCorresponding Author
Yao Zheng
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia
Search for more papers by this authorCorresponding Author
Shi-Zhang Qiao
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia
Search for more papers by this authorXuesi Wang
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia
These authors contributed equally to this work.
Search for more papers by this authorYan Jiao
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia
These authors contributed equally to this work.
Search for more papers by this authorLaiquan Li
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia
Search for more papers by this authorCorresponding Author
Yao Zheng
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia
Search for more papers by this authorCorresponding Author
Shi-Zhang Qiao
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia
Search for more papers by this authorAbstract
We demonstrate a widely applicable method to alter the adsorption configuration of multi-carbon containing reactants by no catalyst engineering but simply adjusting the local reaction environment of the catalyst surface. Using electrocatalytic acetone to propane hydrogenation (APH) as a model reaction and common commercial Pt/Pt-based materials as catalysts, we found local H+ concentration can significantly influence the adsorption mode of acetone reactant, for example, in vertical or flat mode, and target product selectivity. Electrocatalytic measurement combined with in situ spectroscopic characterizations reveals that the vertically adsorbed acetone is favorable for propane production while the flatly adsorbed mode suppresses the reaction. DFT calculations indicate that the H coverage on catalyst surface plays a decisive role in the adsorption configuration of acetone. The increased local acidity can facilitate the adsorption configuration of acetone from flat to vertical mode and suppress the competing hydrogen evaluation reaction, which consequently enhances the APH selectivity.
Conflict of interest
The authors declare no conflict of interest.
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