Unlocking the Potential of A-Site Ca-Doped LaCo0.2Fe0.8O3-δ: A Redox-Stable Cathode Material Enabling High Current Density in Direct CO2 Electrolysis

Li, Haixia; Wang, Wanhua; Wang, Lucun; Wang, Min; Park, Ka-Young; Lee, Taehee; Heyden, Andreas; Ding, Dong; Chen, Fanglin

doi:10.1021/acsami.3c08561

Title: Unlocking the Potential of A-Site Ca-Doped LaCo_0.2Fe_0.8O_3-δ: A Redox-Stable Cathode Material Enabling High Current Density in Direct CO₂ Electrolysis

Journal Article · 05 September 2023 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.3c08561 · OSTI ID:2205201

Li, Haixia ^[1]; Wang, Wanhua ^[1];

^[2]; Wang, Min ^[2]; Park, Ka-Young ^[1]; Lee, Taehee ^[1];

^[1];

^[2];

^[1]

University of South Carolina, Columbia, SC (United States)
Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Massive carbon dioxide (CO₂) emission from recent human industrialization has affected the global ecosystem and raised great concern for environmental sustainability. The solid oxide electrolysis cell (SOEC) is a promising energy conversion device capable of efficiently converting CO₂ into valuable chemicals using renewable energy sources. However, Sr-containing cathode materials face the challenge of Sr carbonation during CO₂ electrolysis, which greatly affects the energy conversion efficiency and long-term stability. Thus, A-site Ca-doped La1–_xCaxCo_0.2Fe_0.8O_3-δ(0.2 ≤ x ≤ 0.6) oxides are developed for direct CO₂ conversion to carbon monoxide (CO) in an intermediate-temperature SOEC (IT-SOEC). With a polarization resistance as low as 0.18 O cm² in pure CO₂ atmosphere, a remarkable current density of 2.24 A cm^–2 was achieved at 1.5 V with La_0.6Ca_0.4Co_0.2Fe_0.8O_3-δ (LCCF64) as the cathode in La_0.8Sr_0.2Ga_0.83Mg_0.17O_3-δ (LSGM) electrolyte (300 µm) supported electrolysis cells using La_0.6Sr_0.4Co_0.2Fe_0.8O_3-δ(LSCF) as the air electrode at 800 °C. Furthermore, symmetrical cells with LCCF64 as the electrodes also show promising electrolysis performance of 1.78 A cm^–2 at 1.5 V at 800 °C. In addition, stable cell performance has been achieved on direct CO₂ electrolysis at an applied constant current of 0.5 A cm^–2 at 800 °C. The easily removable carbonate intermediate produced during direct CO₂ electrolysis makes LCCF64 a promising regenerable cathode. The outstanding electrocatalytic performance of the LCCF64 cathode is ascribed to the highly active and stable metal/perovskite interfaces that resulted from the in situ exsolved Co/CoFe nanoparticles and the additional oxygen vacancies originated from the Ca₂Fe₂O₅ phase synergistically providing active sites for CO₂ adsorption and electrolysis. Here this study offers a novel approach to design catalysts with high performance for direct CO₂ electrolysis.

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Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: National Aeronautics and Space Administration (NASA); National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 2205201

Report Number(s):: INL/JOU--23-74647-Revision-0

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 37 Vol. 15; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Unlocking the Potential of A-Site Ca-Doped LaCo0.2Fe0.8O3-δ: A Redox-Stable Cathode Material Enabling High Current Density in Direct CO2 Electrolysis

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Title: Unlocking the Potential of A-Site Ca-Doped LaCo_0.2Fe_0.8O_3-δ: A Redox-Stable Cathode Material Enabling High Current Density in Direct CO₂ Electrolysis