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

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Lingting Ye, Minyi Zhang, Ping Huang, Guocong Guo, Maochun Hong, Chunsen Li, John T. S. Irvine, Kui Xie

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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.
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Original languageEnglish
Article number14785
JournalNature Communications
Volume8
DOIs
Publication statusPublished - 16 Mar 2017

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