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Exploring the Mechanism of the Electrochemical Polymerization of CO2 to Hard Carbon over CeO2(110)
Institute of Theoretical Chemistry, Ulm University, Oberberghof 7, 89081 Ulm, Germany.
Institute of Theoretical Chemistry, Ulm University, Oberberghof 7, 89081 Ulm, Germany.
Institute of Theoretical Chemistry, Ulm University, Oberberghof 7, 89081 Ulm, Germany.ORCID iD: 0000-0003-4037-7331
Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Institute of Theoretical Chemistry, Ulm University, Oberberghof 7, 89081 Ulm, Germany; Wallenberg Initiative Materials Science for Sustainability (WISE), Luleå University of Technology, 971 87 Luleå, Sweden.ORCID iD: 0000-0003-3883-2868
2024 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 128, no 15, p. 6280-6293Article in journal (Refereed) Published
Abstract [en]

Conversion of CO2 to hard carbon is an interesting technology for the removal of carbon dioxide from the atmosphere. Recently, it was shown that CeO2 can selectively catalyze this reaction, but we still lack information regarding the reaction mechanism. Using density functional theory modeling, we explore possible reaction mechanisms that allow for the polymerization of CO2. According to our computations, the reaction is initialized by the adsorption of CO2 in an oxygen vacancy. Owing to the rich defect chemistry of ceria, a large number of suitable sites are available at the surface. C–C bond formation is achieved through an aldol condensation-type mechanism which comprises the electrochemical elimination of water to form a carbene. This carbene then performs a nucleophilic attack on CO2. The reaction mechanism possesses significant similarities to the corresponding reactions in synthetic organic chemistry. Since the mechanism is completely generic, it allows for all relevant steps of the formation of hard carbon like chain growth, chain linkage, and the formation of side chains or aromatic rings. Surprisingly, ceria mainly serves as an anchor for CO2 in an oxygen vacancy, while all other subsequent reaction steps are almost completely independent from the catalyst. These insights are important for the development of novel catalysts for CO2 reduction and may also lead to new reactions for the electrosynthesis of organic molecules. 

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2024. Vol. 128, no 15, p. 6280-6293
National Category
Physical Chemistry
Research subject
Applied Physics
Identifiers
URN: urn:nbn:se:ltu:diva-105037DOI: 10.1021/acs.jpcc.3c08356Scopus ID: 2-s2.0-85189973481OAI: oai:DiVA.org:ltu-105037DiVA, id: diva2:1850148
Note

Validerad;2024;Nivå 2;2024-04-22 (joosat);

Full text: CC BY license;

Funder: German Bundesministerium für Bildung und Forschung (BMBF) project NETPEC (grant number: 01LS2103A); Dr. Barbara-Mez-Starck foundation;

Available from: 2024-04-09 Created: 2024-04-09 Last updated: 2024-04-22Bibliographically approved

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Busch, Michael

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