Electrocatalysis at Organic-Metal Interfaces: Identification of Structure-Reactivity Relationships for CO2 Reduction at Modified Cu Surfaces.
Aya K BuckleyMichelle LeeTao ChengRoman V KazantsevDavid M LarsonWilliam A Goddard IiiF Dean TosteFrancesca M TomaPublished in: Journal of the American Chemical Society (2019)
The limited selectivity of existing CO2 reduction catalysts and rising levels of CO2 in the atmosphere necessitate the identification of specific structure-reactivity relationships to inform catalyst development. Herein, we develop a predictive framework to tune the selectivity of CO2 reduction on Cu by examining a series of polymeric and molecular modifiers. We find that protic species enhance selectivity for H2, hydrophilic species enhance formic acid formation, and cationic hydrophobic species enhance CO selectivity. ReaxFF reactive molecular dynamics simulations indicate that the hydrophilic/hydrophobic modifiers influence the formation of surface hydrides, which yield formic acid or H2. These observations offer insights into how these modifiers influence catalytic behavior at the non-precious Cu surface and may aid in the future implementation of organic structures in CO2 reduction devices.
Keyphrases
- molecular dynamics simulations
- ionic liquid
- aqueous solution
- metal organic framework
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- liquid chromatography
- structural basis
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- molecular docking
- high resolution
- current status
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- single molecule
- water soluble
- bioinformatics analysis
- simultaneous determination
- tandem mass spectrometry
- solid phase extraction
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- crystal structure