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Local Environment Determined Reactant Adsorption Configuration for Enhanced Electrocatalytic Acetone Hydrogenation to
Xuesi Wang1, Yan Jiao1, Laiquan Li1
1School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005, Australia.
Altering the local reaction environment, specifically H+ concentration, controls acetone adsorption on platinum catalysts. This method enhances selectivity for propane production in acetone hydrogenation, avoiding catalyst modification.
Area of Science:
- Heterogeneous catalysis
- Surface chemistry
- Electrocatalysis
Background:
- Controlling reactant adsorption on catalyst surfaces is crucial for selective chemical transformations.
- Existing methods often rely on complex catalyst synthesis or modification.
- Understanding the influence of the local reaction environment is key to optimizing catalytic performance.
Purpose of the Study:
- To demonstrate a simple method for controlling reactant adsorption configuration without catalyst engineering.
- To investigate the effect of local H+ concentration on acetone adsorption and hydrogenation selectivity.
- To elucidate the mechanism by which local acidity influences product distribution in acetone to propane hydrogenation (APH).
Main Methods:
- Electrocatalytic measurements using commercial Pt/Pt-based catalysts.
- In situ spectroscopic characterizations to analyze surface species and adsorption modes.
- Density Functional Theory (DFT) calculations to determine the role of hydrogen coverage and adsorption energies.
Main Results:
- Local H+ concentration significantly influences acetone adsorption, favoring vertical or flat configurations.
- Vertically adsorbed acetone promotes propane production, while flat adsorption suppresses it.
- Increased local acidity enhances APH selectivity by promoting vertical acetone adsorption and suppressing hydrogen evolution.
Conclusions:
- Adjusting the local reaction environment, particularly acidity, is an effective strategy to control adsorption configuration and enhance catalytic selectivity.
- This approach offers a versatile method for optimizing multi-carbon reactant transformations, exemplified by acetone to propane hydrogenation.
- The findings highlight the importance of local surface conditions in dictating catalytic outcomes.
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