title: Enhancing CO2electrolysis through synergistic control of non-stoichiometry and doping to tune cathode surface structures.
abstract: Sustainable future energy scenarios require significant efficiency improvements in both electricity generation and storage. High-temperature solid oxide cells, and in particular carbon dioxide electrolysers, afford chemical storage of available electricity that can both stabilize and extend the utilization of renewables. Here we present a double doping strategy to facilitate CO2reduction at perovskite titanate cathode surfaces, promoting adsorption/activation by making use of redox active dopants such as Mn linked to oxygen vacancies and dopants such as Ni that afford metal nanoparticle exsolution. Combined experimental characterization and first-principle calculations reveal that the adsorbed and activated CO2adopts an intermediate chemical state between a carbon dioxide molecule and a carbonate ion. The dual doping strategy provides optimal performance with no degradation being observed after 100 h of high-temperature operation and 10 redox cycles, suggesting a reliable cathode material for CO2electrolysis.
authors.affiliation: Key Lab of Design &Assembly of Functional Nanostructure, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
authors.forename: Lingting
authors.initials: L
authors.lastname: Ye
authors.affiliation: State Key Lab of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
authors.forename: Minyi
authors.initials: M
authors.lastname: Zhang
authors.affiliation: Key Lab of Design &Assembly of Functional Nanostructure, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
authors.forename: Ping
authors.initials: P
authors.lastname: Huang
authors.affiliation: State Key Lab of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
authors.forename: Guocong
authors.initials: G
authors.lastname: Guo
authors.affiliation: State Key Lab of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
authors.forename: Maochun
authors.initials: M
authors.lastname: Hong
authors.affiliation: State Key Lab of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
authors.forename: Chunsen
authors.initials: C
authors.lastname: Li
authors.affiliation: Key Lab of Design &Assembly of Functional Nanostructure, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.|School of Chemistry, University of St Andrews, St Andrews, Fife KY16 9ST, Scotland, UK.
authors.forename: John T S
authors.initials: JT
authors.lastname: Irvine
authors.affiliation: Key Lab of Design &Assembly of Functional Nanostructure, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
authors.forename: Kui
authors.initials: K
authors.lastname: Xie