Enhancing CO2 electrolysis through synergistic control of non-stoichiometry and doping to tune cathode surface structures

Lingting Ye, Minyi Zhang, Ping Huang, Guocong Guo, Maochun Hong, Chunsen Li (), John T. S. Irvine () and Kui Xie ()
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Lingting Ye: Key Lab of Design & Assembly of Functional Nanostructure, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences
Minyi Zhang: State Key Lab of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences
Ping Huang: Key Lab of Design & Assembly of Functional Nanostructure, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences
Guocong Guo: State Key Lab of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences
Maochun Hong: State Key Lab of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences
Chunsen Li: State Key Lab of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences
John T. S. Irvine: Key Lab of Design & Assembly of Functional Nanostructure, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences
Kui Xie: Key Lab of Design & Assembly of Functional Nanostructure, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences

Nature Communications, 2017, vol. 8, issue 1, 1-10

Abstract: 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 CO2 reduction 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 CO2 adopts 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 CO2 electrolysis.

Date: 2017
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DOI: 10.1038/ncomms14785

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