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

Zhibo Shang; Suting He; Zilin Ma; Benchi Chen; Xuepeng Xiang; Yihan Ling; Nian Zhang; Shijun Zhao; Yifeng Li; Yan Chen

doi:10.1021/acs.nanolett.5c06238

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

Zhibo Shang
, Suting He
, Zilin Ma
, Benchi Chen
, Xuepeng Xiang
, Yihan Ling
, Nian Zhang
, Shijun Zhao
, Yifeng Li
, Yan Chen^*

^*Corresponding author for this work

Department of Mechanical Engineering

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

3 Citations (Scopus)

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 Sr₂Ti_0.8Fe_1.2O_6−δ (STF), specifically forming Sr₂Ti_0.8FeNi_0.2O_6−δ (STFN) and Sr₂Ti_0.8FeCo_0.2O_6−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 (CO₃^2–) 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. © 2026 American Chemical Society

Original language	English
Pages (from-to)	3232-3241
Number of pages	10
Journal	Nano Letters
Volume	26
Issue number	9
Online published	2 Mar 2026
DOIs	https://doi.org/10.1021/acs.nanolett.5c06238
Publication status	Published - 11 Mar 2026

Funding

This work was supported by the National Key R&D Program of China (2021YFA1501900). Y.C. acknowledges the support of “TCL Young Scholars Program”. We thank the Shanghai Synchrotron Radiation Facility o f BL02B02 (31124.02.SSRF.BL02B02) for the assistance on XAS measurements. The computational time provided by the National Supercomputer Center in Tianjin is highly acknowledged.

Research Keywords

Advanced Spectroscopy
Carbon Monoxide
Cation Doping
High-Temperature CO2Electrolysis
Oxygen Activity

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title = "Modulating Oxygen Activity via Cation Doping for Efficient High-Temperature Carbon Dioxide Electrolysis",

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. {\textcopyright} 2026 American Chemical Society",

keywords = "Advanced Spectroscopy, Carbon Monoxide, Cation Doping, High-Temperature CO2Electrolysis, Oxygen Activity",

author = "Zhibo Shang and Suting He and Zilin Ma and Benchi Chen and Xuepeng Xiang and Yihan Ling and Nian Zhang and Shijun Zhao and Yifeng Li and Yan Chen",

year = "2026",

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doi = "10.1021/acs.nanolett.5c06238",

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TY - JOUR

T1 - Modulating Oxygen Activity via Cation Doping for Efficient High-Temperature Carbon Dioxide Electrolysis

AU - Shang, Zhibo

AU - He, Suting

AU - Ma, Zilin

AU - Chen, Benchi

AU - Xiang, Xuepeng

AU - Ling, Yihan

AU - Zhang, Nian

AU - Zhao, Shijun

AU - Li, Yifeng

AU - Chen, Yan

PY - 2026/3/11

Y1 - 2026/3/11

N2 - 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. © 2026 American Chemical Society

AB - 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. © 2026 American Chemical Society

KW - Advanced Spectroscopy

KW - Carbon Monoxide

KW - Cation Doping

KW - High-Temperature CO2Electrolysis

KW - Oxygen Activity

UR - https://www.scopus.com/pages/publications/105032373787

UR - https://www.scopus.com/pages/publications/105032373787#tab=impact

U2 - 10.1021/acs.nanolett.5c06238

DO - 10.1021/acs.nanolett.5c06238

M3 - RGC 21 - Publication in refereed journal

SN - 1530-6984

VL - 26

SP - 3232

EP - 3241

JO - Nano Letters

JF - Nano Letters

IS - 9

ER -

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

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