Tuning covalence for phosphorus-mediated C-C coupling in carbon monoxide electroreduction to multicarbon oxygenates
Year: 2026
Type: preprint
Abstract: Electrochemical carbon monoxide reduction (COR) is a promising route for sustainable production of multicarbon chemicals from CO2, as it bypasses the large carbon losses of direct CO2 electroreduction. In most electrocatalysts currently explored to tune COR selectivity towards highadded value multicarbon oxygenated molecules, like acetate and ethanol, copper is the catalytic site of C-C bond formation. Herein, we show that by designing nanoparticles of a strongly covalent copper compound, CuSi2P3, we retain isolated copper atoms during COR and trigger the intervention of phosphorus atoms as C-C coupling sites, without directly involving copper atoms. This profound change in COR mechanism results in a high selectivity towards C2 molecules (80 % Faradaic efficiency), especially oxygenates (73%), at a current density of -150 mA cm-2. This work reveals the importance of tailoring, via the crystal structure, the local environment of metal atoms, to achieve original selectivity in COR with new families of electrocatalysts.
Source: ChemRxiv
Authors: Anissa Ghoridi, Carlos V. M. Inocêncio, Hong Phong Duong, Ngoc-Huan Tran, Zubair Ahmed, Isabel Gómez-Recio, Maria Luisa Ruiz-Gonzàlez, Stephan Steinmann, Preeti Verma, Claudia Morais, Nadia Guignard, Antoine Miche, Sandra Casale, Christel Gervais, Cristina Coelho Diogo, Isabelle Génois, Andrea Zitolo, Christoph Sahle, Alessandro Longo, José Maria González-Calbet, Marc Fontecave, David Portehault
Institutions: Centre National de la Recherche Scientifique, Sorbonne Université, Chimie de la Matière Condensée de Paris, Collège de France, Laboratoire de chimie des processus biologiques, Universidad Complutense de Madrid, École Normale Supérieure de Lyon, Laboratoire de Chimie, Université de Poitiers, Institut de Chimie des Milieux et des Matériaux de Poitiers, Laboratoire de Réactivité de Surface, Synchrotron SOLEIL, European Synchrotron Radiation Facility
Language: English
Field: Energy
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W7223178815