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March 4, 2026Nano Letters0 citations

Modulating Oxygen Activity via Cation Doping for Efficient High-Temperature Carbon Dioxide Electrolysis

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ZSZhibo ShangSHSuting HeZMZilin Ma

Key Points

  • The research aims to improve CO<sub>2</sub> electrolysis efficiency by modulating oxygen activity through cation doping in solid oxide materials.
  • Employs solid oxide electrolysis cells (SOECs) for CO<sub>2</sub> to CO conversion.
  • Utilizes cation doping in Sr<sub>2</sub>Ti<sub>0.8</sub>Fe<sub>1.2</sub>O<sub>6-δ</sub> to create Sr<sub>2</sub>Ti<sub>0.8</sub>FeNi<sub>0.2</sub>O<sub>6-δ</sub> and Sr<sub>2</sub>Ti<sub>0.8</sub>FeCo<sub>0.2</sub>O<sub>6-δ</sub>.
  • Conducts advanced spectroscopic techniques and density functional theory calculations to analyze changes in oxygen activity.
  • Achieves a current density of 1.15 A cm<sup>-2</sup> and a CO production rate of 8.01 mL min<sup>-1</sup> cm<sup>-2</sup> with the STFC cathode.
  • Reports >99% Faradaic efficiency at 1.6 V and 800 °C.
  • Identifies increased oxygen activity due to Co doping, reducing energy barriers for CO generation.

Abstract

High-temperature solid oxide electrolysis cells (SOECs) offer a promising pathway for CO2-to-CO conversion yet are hindered by cathode inactivity. This study demonstrates cation doping in Sr2Ti0. 8Fe1. 2O6-δ (STF), specifically forming Sr2Ti0. 8FeNi0. 2O6-δ (STFN) and Sr2Ti0. 8FeCo0. 2O6-δ (STFC), as an effective strategy for modulating oxygen activity and enhancing CO2 electrolysis performance. The STFC cathode delivers optimal results, achieving a 1. 15 A cm-2 current density, 8. 01 mL min-1 cm-2 CO production rate, and >99% Faradaic efficiency at 1. 6 V and 800 °C. Advanced spectroscopic techniques combined with density functional theory calculations reveal that Co doping increases oxygen activity, evidenced by an upshifted O 2p band center and reduced oxygen vacancy formation energy. Consequently, CO2 adsorption for carbonate (CO32-) intermediate formation is facilitated, and the energy barrier for CO generation is reduced. A techno-economic assessment projects a competitive CO production cost of 748 per ton. These insights provide fundamental guidelines for the design of high-activity catalysts in high-temperature electrochemical systems.

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Cite This Study

Shang et al. (2026) studied this question.

synapsesocial.com/papers/69a7cd9dd48f933b5eeda279https://doi.org/10.1021/acs.nanolett.5c06238
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