(Invited) Dynamics in the Electrocatalytic Reduction of CO2
Authors: Roldan Cuenya Beatriz 
Published: September 2023

Climate change concerns have spurred a growing interest in developing environmentally friendly technologies for energy generation, such as green H2 from water splitting. Moreover, the electrochemical reduction of CO2 (CO2RR) into value-added chemicals and fuels offers an additional possibility to store renewable energy into chemical bonds. It is therefore of particular interest to develop efficient, selective and durable electrocatalysts that can operate under mild reaction conditions. The latter however requires fundamental understanding of their structure and surface composition under reaction conditions. It should be kept in mind that even morphologically and chemically well-defined pre-catalysts will be susceptible to drastic modifications under operando conditions, especially when the reaction conditions themselves change periodically.

This talk will illustrate how of a multi-technique in-situ/operando experimental approach is able provide in depth mechanistic insights into CO2RR1,2. A synergistic combination of LC-TEM, EC-AFM, NAP-XPS, XAS, XRD, GC/MS, and Raman Spectroscopy, coupled with machine learning-based data analysis, has been employed to investigate the time-dependent chemical and structural changes in mono and bimetallic CO2 electrocatalysts under reaction conditions.

Some of the aspects that will be discussed here include: (i) the design of size- and shape-controlled catalytically active nanoparticle (NP) pre-catalysts (Cu2O cubes, ZnO@Cu2O cubic NPs), (ii) the understanding of the active state formation (e.g for well-defined Cu(100), Cu(111) surfaces) and the correlation between the dynamically evolving structure and composition of the electrocatalysts under operando reaction conditions and their activity and selectivity. Our studies are expected to open up new routes for the reutilization of CO2 through its direct conversion into industrially valuable chemicals and fuels such as ethylene and ethanol.

References

[1] J. Timoshenko, A. Bergmann, B. Roldan Cuenya et al., Nature Catalysis
(2022), 5, 259–267.

[2] M. Rüscher, A. Herzog, J. Timoshenko, H. Jeon, W. Frandsen, S. Kühl, B. Roldan Cuenya Catalysis Science & Technology (2022)12, 3028–3043. Climate change concerns have spurred a growing interest in developing environmentally friendly technologies for energy generation, such as green H2 from water splitting. Moreover, the electrochemical reduction of CO2 (CO2RR) into value-added chemicals and fuels offers an additional possibility to store renewable energy into chemical bonds. It is therefore of particular interest to develop efficient, selective and durable electrocatalysts that can operate under mild reaction conditions. The latter however requires fundamental understanding of their structure and surface composition under reaction conditions. It should be kept in mind that even morphologically and chemically well-defined pre-catalysts will be susceptible to drastic modifications under operando conditions, especially when the reaction conditions themselves change periodically.

This talk will illustrate how of a multi-technique in-situ/operando experimental approach is able provide in depth mechanistic insights into CO2RR1,2. A synergistic combination of LC-TEM, EC-AFM, NAP-XPS, XAS, XRD, GC/MS, and Raman Spectroscopy, coupled with machine learning-based data analysis, has been employed to investigate the time-dependent chemical and structural changes in mono and bimetallic CO2 electrocatalysts under reaction conditions.

Some of the aspects that will be discussed here include: (i) the design of size- and shape-controlled catalytically active nanoparticle (NP) pre-catalysts (Cu2O cubes, ZnO@Cu2O cubic NPs), (ii) the understanding of the active state formation (e.g for well-defined Cu(100), Cu(111) surfaces) and the correlation between the dynamically evolving structure and composition of the electrocatalysts under operando reaction conditions and their activity and selectivity. Our studies are expected to open up new routes for the reutilization of CO2 through its direct conversion into industrially valuable chemicals and fuels such as ethylene and ethanol.

References

[1] J. Timoshenko, A. Bergmann, B. Roldan Cuenya et al., Nature Catalysis
(2022), 5, 259–267.

[2] M. Rüscher, A. Herzog, J. Timoshenko, H. Jeon, W. Frandsen, S. Kühl, B. Roldan Cuenya Catalysis Science & Technology (2022)12, 3028–3043.