Leiden University Scholarly Publications

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Ye, C. (2024)

Influence of the electrode-electrolyte interface on electrochemical CO2 reduction reaction and hydrogen evolution reaction

Doctoral Thesis
The goal of this thesis is to understand how interfacial parameters, such as the addition of organic additives, bulk pH or metal cations of the electrolyte, affect the relevant electrocatalytic reactions, i.e. electrochemical CO2 reduction reaction or hydrogen evolution reaction. We firstly investigate the influence of organic additives on CO2RR activity and selectivity, as well as their effects on the interfacial environment during CO2RR. The focus then shifts to a well-defined surface, where we closely examine the role of metal cations on CO2RR using a palladium monolayer modified Pt(111) surface (PdMLPt(111)) in a pH 3 electrolyte. Further, we investigate the influence of metal cations on the competing hydrogen evolution reaction (HER) in mildly acidic media, which is relevant for optimizing CO2RR performance. Finally, we expand the scope to industrially relevant conditions by studying the influence of bulk electrolyte pH on CO2RR product distribution using a copper gas...Show moreThe goal of this thesis is to understand how interfacial parameters, such as the addition of organic additives, bulk pH or metal cations of the electrolyte, affect the relevant electrocatalytic reactions, i.e. electrochemical CO2 reduction reaction or hydrogen evolution reaction. We firstly investigate the influence of organic additives on CO2RR activity and selectivity, as well as their effects on the interfacial environment during CO2RR. The focus then shifts to a well-defined surface, where we closely examine the role of metal cations on CO2RR using a palladium monolayer modified Pt(111) surface (PdMLPt(111)) in a pH 3 electrolyte. Further, we investigate the influence of metal cations on the competing hydrogen evolution reaction (HER) in mildly acidic media, which is relevant for optimizing CO2RR performance. Finally, we expand the scope to industrially relevant conditions by studying the influence of bulk electrolyte pH on CO2RR product distribution using a copper gas diffusion electrode (Cu GDE).
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Electrochemical CO2 reduction reaction
Hydrogen evolution reaction
Selectivity
Catalyst
Additive modification
Palladium
Cations
Gas diffusion electrode
Formic acid
Acdic electrolyte
All authors
Ye, C.
Supervisor
Koper, M.T.M.
Co-supervisor
Schouten, K.J.P.
Committee
Ubbink, M.; Tschulink, K.; Kortlever, R.; Jeuken, L.J.C.; Mom, R.V.
Qualification
Doctor (dr.)
Awarding Institution
Leiden Institute of Chemistry (LIC), Faculty of Science, Leiden University
Date
2024-12-05

Funding

Sponsorship
The European Commission, as part of the Marie Sklodowska Curie Innovative Training Network ELCoREL-722614