RT journal article
T1 Improved electrochemical conversion of CO2 to multicarbon products by using molecular doping
A1 Wu, Huali
A1 Li, Ji
A1 Qi, Kun
A1 Zhang, Yang
A1 Petit, Eddy
A1 Wang, Wensen
A1 Flaud, Valérie
A1 Onofrio, Nicolas
A1 Rebiere, Bertrand
A1 Huang, Lingqi
A1 Salameh, Chrystelle
A1 Lajaunie, Luc Cyrille Jacques
A1 Miele, Philippe
A1 Voiry, Damien
A2 Ciencia de los Materiales e Ingeniería Metalúrgica y Química Inorgánica
AB The conversion of CO2 into desirable multicarbon products via the electrochemical reduction reaction holds promise to achieve a circular carbon economy. Here, we report a strategy in which we modify the surface of bimetallic silver-copper catalyst with aromatic heterocycles such as thiadiazole and triazole derivatives to increase the conversion of CO2 into hydrocarbon molecules. By combining operando Raman and X-ray absorption spectroscopy with electrocatalytic measurements and analysis of the reaction products, we identified that the electron withdrawing nature of functional groups orients the reaction pathway towards the production of C2+ species (ethanol and ethylene) and enhances the reaction rate on the surface of the catalyst by adjusting the electronic state of surface copper atoms. As a result, we achieve a high Faradaic efficiency for the C2+ formation of approximate to 80% and full-cell energy efficiency of 20.3% with a specific current density of 261.4 mA cm(-2) for C2+ products.Strategies to systematically tune CO2 electroreduction to multicarbon products are of high interests. Here the authors report electron withdrawing functional group alters the reaction pathway towards C2+ products by adjusting the oxidation state of surface copper.
PB NATURE RESEARCH
SN 2041-1723
YR 2021
FD 2021-12
LK http://hdl.handle.net/10498/26276
UL http://hdl.handle.net/10498/26276
LA eng
NO D.V., K.Q., and H.L.W. acknowledge funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement no. 804320). L.L., D.V., and H.L.W acknowledge the use of TEM instrumentation provided by the Nation Facility ELECMI ICTS (`Division de Microscopia Electronica', Universidad de Cadiz, DME-UCA). L.L. acknowledges funding from the Andalusian regional government (FEDER-UCA-18-106613), the European Union's Horizon 2020 research and innovation program (grant agreement 823717-ESTEEM3), and the Spanish Ministerio de Economia y Competitividad (PID2019-107578GA-I00). K.Q. and Y.Z. acknowledge financial support from the China Postdoctoral Science Foundation (2018M633127) and the Natural Science Foundation of Guangdong Province (2018A030310602). J.L. acknowledge financial support from the National Natural Science Foundation of China (21808134). We thank Soleil Synchrotron and Andrea Zitolo for allocating beamtime at beamline Samba within the proposal 20200732.
DS Repositorio Institucional de la Universidad de Cádiz
RD 06-nov-2026