Analyzing the Complete Carbon Balance in High Current Density Electrochemical CO2 Reduction Reactors
Brian Seger a, Gaston Larrazabal a, Ming Ma a, Ib Chorkendorff a, Kasper Therkildsen b
a Technical University of Denmark (DTU), Denmark
b Siemens Corporate Technologies, Günther-Scharowsky-Str.1, Erlangen, 91058, Germany
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting19 (NFM19)
#SolCat19. (Photo)electrocatalysis for sustainable carbon utilization: mechanisms, methods, and reactor development
Berlin, Germany, 2019 November 3rd - 8th
Organizer: Matthew Mayer
Oral, Brian Seger, presentation 013
DOI: https://doi.org/10.29363/nanoge.nfm.2019.013
Publication date: 18th July 2019

This talk will focus on understanding the complete carbon balance on electrochemical CO2 reduction reactors operating at industrial relevant current densities (100-500 mA/cm2).  Both a gas diffusion approach with a liquid catholyte as well as a zero gap membrane electrode assembly (MEA) approach will be discussed. 

In the MEA approach, a Ag membrane was used as a CO2 reduction cathode and a greater than 95% faradaic efficiency to CO is obtained at 200 mA/cm2 (~ 3.1 V).  Insertion of a reference electrode allowed us to roughly attribute losses to either cathode, anode, or the membrane.  Gas chromatography of the anode, in addition to the cathode, shows both the faradaic efficiency of oxygen evolution as well as the CO2 crossover across an anion exchange membrane and how this varies as a function of current.  The production of formate is analyzed as well as its crossover to the anode. 

For the gas diffusion electrode approach, sputtered Cu was used as a cathodic catalyst.  As expected, high faradaic efficiencies to ethylene and ethanol were seen as well as other multi-carbon products.  CO2 reduction products diffusing through to the anode were analyzed as well as oxygen and CO2. CO2 crossover and oxygen evolution faradaic efficiencies as a function of operating current and other reactor parameters will be discussed.  This talk will also demonstrated the role of varying electrolyte pH and how this effects performance from an overall carbon balance standpoint.

This work was funded by both the V-Sustain grant from the Villum Foundation V-SUSTAIN (Grant # 9455) and the ECOEthylene project from Innovation Fund Denmark (Grant # 8057-00018B)

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