Oxygen-induced changes to selectivity-determining steps in electrocatalytic CO2 reduction

Autor:	Andrew A. Peterson, Yin-Jia Zhang
Rok vydání:	2015
Předmět:	chemistry Oxidation state Electrode Inorganic chemistry General Physics and Astronomy chemistry.chemical_element Density functional theory Physical and Theoretical Chemistry Selectivity Electrocatalyst Oxygen Oxygen binding Catalysis
Zdroj:	Physical Chemistry Chemical Physics. 17:4505-4515
ISSN:	1463-9084 1463-9076
DOI:	10.1039/c4cp03783a
Popis:	The state of the electrocatalyst surface-including the oxidation state of the catalyst and the presence of spectator species-is investigated on Cu surfaces with density functional theory in order to understand predicted ramifications on the selectivity and efficiency of CO2 reduction. We examined the presence of oxygen-based species, including the fully oxidized Cu2O surface, the partially oxidized Cu(110)-(2 × 1)O surface, and the presence of OH spectators. The relative oxygen binding strength among these surfaces can help to explain the experimentally observed selectivity change between CH4 and CH3OH on these electrodes; this suggests that the oxygen-binding strength may be a key parameter which predicts the thermodynamically preferred selectivity for pathways proceeding through a methoxy (CH3O) intermediate. This study shows the importance of the local surface environment in the product selectivity of electrocatalysis, and suggests a simple descriptor that can aid in the design of improved electrocatalytic materials.
Databáze:	OpenAIRE
Externí odkaz:	https://explore.openaire.eu/search/publication?articleId=doi_dedup___::23cd4b045983274acd831f66c8e99a50 https://doi.org/10.1039/c4cp03783a Zobrazit plný text záznamu