TY - JOUR
T1 - Copper sulfide derived nanoparticles supported on carbon for the electrochemical reduction of carbon dioxide
AU - van Oversteeg, Christina H.M.
AU - Tapia Rosales, Marisol
AU - Helfferich, Kristiaan H.
AU - Ghiasi, Mahnaz
AU - Meeldijk, Johannes D.
AU - Firet, Nienke J.
AU - Ngene, Peter
AU - de Mello Donegá, Celso
AU - de Jongh, Petra E.
PY - 2020
Y1 - 2020
N2 - The electrocatalytic reduction of CO2 to produce sustainable fuels and chemicals is attracting great attention. Cu-based catalysts can lead to the production of a range of different molecules, and interestingly the product selectivity strongly depends on the preparation history, although it is not fully understood yet why. We report a novel strategy that allowed us to prepare Cu nanoparticle on carbon catalysts with similar morphologies, but prepared by in-situ reduction of either supported CuS, Cu2S or CuO nanoparticles. For the first time the evolution of the Cu species was followed under CO2 and H+ reduction conditions using in-situ X-ray absorption spectroscopy. Excellent electrochemical contact between the Cu-based nanoparticles, the carbon support and the carbon-paper substrate was observed, resulting in metallic Cu as the predominant phase under typical electrochemical CO2 reduction conditions. Even covering less than 4% of the H2 producing carbon support with Cu-sulfide derived nanoparticles allowed to steer the selectivity to a maximum of 12% Faradaic efficiency for the production of formate. Clear differences between the catalysts derived from CuS, Cu2S or CuO nanoparticles were observed, which was ascribed to the presence of residual sulfur in the catalysts.
AB - The electrocatalytic reduction of CO2 to produce sustainable fuels and chemicals is attracting great attention. Cu-based catalysts can lead to the production of a range of different molecules, and interestingly the product selectivity strongly depends on the preparation history, although it is not fully understood yet why. We report a novel strategy that allowed us to prepare Cu nanoparticle on carbon catalysts with similar morphologies, but prepared by in-situ reduction of either supported CuS, Cu2S or CuO nanoparticles. For the first time the evolution of the Cu species was followed under CO2 and H+ reduction conditions using in-situ X-ray absorption spectroscopy. Excellent electrochemical contact between the Cu-based nanoparticles, the carbon support and the carbon-paper substrate was observed, resulting in metallic Cu as the predominant phase under typical electrochemical CO2 reduction conditions. Even covering less than 4% of the H2 producing carbon support with Cu-sulfide derived nanoparticles allowed to steer the selectivity to a maximum of 12% Faradaic efficiency for the production of formate. Clear differences between the catalysts derived from CuS, Cu2S or CuO nanoparticles were observed, which was ascribed to the presence of residual sulfur in the catalysts.
KW - Carbon support
KW - CO reduction
KW - Copper sulfide
KW - In situ X-ray absorption spectroscopy
KW - Nanoparticles
KW - Sulfidation
UR - http://www.scopus.com/inward/record.url?scp=85092212925&partnerID=8YFLogxK
U2 - 10.1016/j.cattod.2020.09.020
DO - 10.1016/j.cattod.2020.09.020
M3 - Article
AN - SCOPUS:85092212925
SN - 0920-5861
VL - 377
SP - 157
EP - 165
JO - Catalysis Today
JF - Catalysis Today
ER -