Selective high-temperature CO2 electrolysis enabled by oxidized carbon intermediates

  title={Selective high-temperature CO2 electrolysis enabled by oxidized carbon intermediates},
  author={Theis L{\o}ye Skafte and Zixuan Guan and Michael L. Machala and Chirranjeevi Balaji Gopal and Matteo Monti and Lev Martinez and Eugen Stamate and Simone Sanna and Jose A. Garrido Torres and Ethan J. Crumlin and Max Garc{\'i}a‐Melchor and Michal Bajdich and William C. Chueh and Christopher R Graves},
  journal={Nature Energy},
High-temperature CO2 electrolysers offer exceptionally efficient storage of renewable electricity in the form of CO and other chemical fuels, but conventional electrodes catalyse destructive carbon deposition. Ceria catalysts are known carbon inhibitors for fuel cell (oxidation) reactions; however, for more severe electrolysis (reduction) conditions, catalyst design strategies remain unclear. Here we establish the inhibition mechanism on ceria and show selective CO2 to CO conversion well beyond… Expand
25 Citations
A review on cathode processes and materials for electro-reduction of carbon dioxide in solid oxide electrolysis cells
Abstract Excessive emission of CO2 may jeopardize the environment and livelihood of mankind. To achieve a sustainable future, solid oxide electrolysis cells (SOECs) are increasingly attractive as anExpand
CO2 electrolysis – Gas impurities and electrode overpotential causing detrimental carbon deposition
Abstract Applying the solid oxide electrolysis cell (SOEC) for CO2 electrolysis has great potential for efficient large-scale on-site CO production. However, ppb-levels of impurities, e.g. sulphurExpand
Solid Oxide Electrolysis of H2O and CO2 to Produce Hydrogen and Low-Carbon Fuels
  • Yun Zheng, Zhongwei Chen, Jiujun Zhang
  • Electrochemical Energy Reviews
  • 2021
Solid oxide electrolysis cells (SOECs) including the oxygen ion-conducting SOEC (O-SOEC) and the proton-conducting SOEC (H-SOEC) have been actively investigated as next-generation electrolysisExpand
Boosting CO2 electrolysis performance via calcium-oxide-looping combined with in situ exsolved Ni–Fe nanoparticles in a symmetrical solid oxide electrolysis cell
The electrocatalysis of CO2 to valuable chemical products is an important strategy to combat global warming. Symmetrical solid oxide electrolysis cells have been extensively recognized for their CO2Expand
Cathode activation process and CO2 electroreduction mechanism on LnFeO3-δ (Ln=La, Pr and Gd) perovskite cathodes
Abstract LnFeO3-δ (Ln = La, Pr and Gd) as cathodes for CO2 electroreduction are investigated in solid oxide electrolysis cells at 800 °C. Their surface properties, oxygen desorption behaviour, CO2Expand
How Rh surface breaks CO2 molecules under ambient pressure
Strong evidence is revealed for chemical bond cleavage of O‒CO* with ordered intermediates structure formation of (2 × 2)-CO on an atomically flat Rh(111) surface at room temperature by combining scanning tunneling microscopy, X-ray photoelectron spectroscopy at near-ambient pressure, and computational calculations. Expand
Reversible solid-oxide cells for clean and sustainable energy
This review gives first a brief view of the potential availability of sustainable energy. It is clear that over 100 times more solar photovoltaic energy than necessary is readily accessible andExpand
Iron stabilized 1/3 A-site deficient La–Ti–O perovskite cathodes for efficient CO2 electroreduction
CO2 electroreduction in solid oxide electrolysis cells is appealing for energy storage and CO2 fixation. Highly active electrocatalysts with long-term operation stability are vital for theExpand
In situ Dispersed Nano-Au on Zr-Suboxides as Active Cathode for Direct CO2 Electroreduction in Solid Oxide Electrolysis Cells.
  • Lixiao Zhang, Xiaobao Li, +8 authors Weishen Yang
  • Medicine
  • Nano letters
  • 2021
The interface between the Au layer and the electrolyte was reconstructed into nano-Au/Zr-suboxide interfaces, which are active sites that show a much lower reaction activation energy than that of the Au/YSZ interface and promotes Au dispersion and Au nanoparticle stabilization due to the strong interaction between Au and Zr- suboxides. Expand
Highly Active Bifunctional Oxygen Electrocatalytic Sites Realized in Ceria–Functionalized Graphene
DOI: 10.1002/adsu.202000048 batteries.[1–3] However, due to the sluggish kinetics of these reactions, the discovery of efficient catalytic platforms is essential to improve device performance.[4] TheExpand


Carbon deposition and sulfur poisoning during CO2 electrolysis in nickel-based solid oxide cell electrodes
Abstract Reduction of CO2 to CO and O2 in the solid oxide electrolysis cell (SOEC) has the potential to play a crucial role in closing the CO2 loop. Carbon deposition in nickel-based cells is howeverExpand
Surface Chemistry of Perovskite-Type Electrodes During High Temperature CO2 Electrolysis Investigated by Operando Photoelectron Spectroscopy
The correlation of carbonate coverage and cathodic polarization indicates that an electron transfer is required to form the carbonate and thus to activate CO2 on the oxide surface, and the results suggest that acceptor doped oxides with high electron concentration and high oxygen vacancy concentration may be particularly suited for CO2 reduction. Expand
Localized carbon deposition in solid oxide electrolysis cells studied by multiphysics modeling
Abstract Solid oxide electrochemical cells (SOCs) can store electrical energy in the form of chemical fuels with high efficiency by electrolysis of CO 2 and H 2 O . However, achieving commerciallyExpand
Eliminating degradation in solid oxide electrochemical cells by reversible operation.
It is demonstrated that severe electrolysis-induced degradation, which was previously believed to be irreversible, can be completely eliminated by reversibly cycling between electrolysis and fuel-cell modes, similar to a rechargeable battery. Expand
High electrochemical activity of the oxide phase in model ceria-Pt and ceria-Ni composite anodes.
It is demonstrated unambiguously, through the use of ceria-metal structures with well-defined geometries and interfaces, that the near-equilibrium H(2) oxidation reaction pathway is dominated by electrocatalysis at the oxide/gas interface with minimal contributions from the oxide-metal/gas triple-phase boundaries. Expand
Electrochemically modified, robust solid oxide fuel cell anode for direct-hydrocarbon utilization
A main advantage of solid oxide fuel cells (SOFCs) operating at a high temperature (>650 °C) is the flexibility of the fuel they use, specifically as they offer the possibility to utilize methaneExpand
Efficient Reduction of CO2 in a Solid Oxide Electrolyzer
When the economy is based on renewable energy resources, such as wind and solar, the major source of H2 for chemical production and energy storage will be from the electrolysis of water. The abilityExpand
Carbon and Redox Tolerant Infiltrated Oxide Fuel-Electrodes for Solid Oxide Cells
To solve issues of coking and redox instability related to the presence of nickel in typical fuel electrodes in solid oxide cells, Gd-doped CeO2 (CGO) electrodes were studied using symmetric cells.Expand
Surface electrochemistry of CO2 reduction and CO oxidation on Sm-doped CeO(2-x): coupling between Ce(3+) and carbonate adsorbates.
An operando investigation of the surface reaction mechanism on a ceria-based electrochemical cell using ambient pressure X-ray photoelectron spectroscopy shows that the reaction proceeds via a stable carbonate intermediate, the coverage of which is coupled to the surface Ce(3+) concentration. Expand
CO2 activation and carbonate intermediates: an operando AP-XPS study of CO2 electrolysis reactions on solid oxide electrochemical cells.
Through the use of ambient pressure X-ray photoelectron spectroscopy and specially designed ceria-based solid oxide electrochemical cells, carbon dioxide (CO2) electrolysis reactions (CO2 + 2e(-)→ COExpand