Electrochemical carbon dioxide reduction (CO2R) provides a promising pathway for sustainable generation of fuels and chemicals. Copper (Cu) electrocatalysts catalyse CO2R to valuable multicarbon (C2+) products, but their selectivity depends on the local microenvironment near the catalyst surface. Here we systematically explore and optimize this microenvironment using bilayer cation- and anion-conducting ionomer coatings to control the local pH (via Donnan exclusion) and CO2/H2O ratio (via ionomer properties), respectively. When this tailored microenvironment is coupled with pulsed electrolysis, further enhancements in the local ratio of CO2/H2O and pH are achieved, leading to selective C2+ production, which increases by 250% (with 90% Faradaic efficiency and only 4% H2) compared with static electrolysis over bare Cu. These results underscore the importance of tailoring the catalyst microenvironment as a means of improving overall performance in electrochemical syntheses.
BT - Nature Energy DA - 10/2021 DO - 10.1038/s41560-021-00920-8 IS - 11 LA - eng N2 -Electrochemical carbon dioxide reduction (CO2R) provides a promising pathway for sustainable generation of fuels and chemicals. Copper (Cu) electrocatalysts catalyse CO2R to valuable multicarbon (C2+) products, but their selectivity depends on the local microenvironment near the catalyst surface. Here we systematically explore and optimize this microenvironment using bilayer cation- and anion-conducting ionomer coatings to control the local pH (via Donnan exclusion) and CO2/H2O ratio (via ionomer properties), respectively. When this tailored microenvironment is coupled with pulsed electrolysis, further enhancements in the local ratio of CO2/H2O and pH are achieved, leading to selective C2+ production, which increases by 250% (with 90% Faradaic efficiency and only 4% H2) compared with static electrolysis over bare Cu. These results underscore the importance of tailoring the catalyst microenvironment as a means of improving overall performance in electrochemical syntheses.
PY - 2021 SP - 1026 EP - 1034 ST - Nat Energy T2 - Nature Energy TI - Tailored catalyst microenvironments for CO2 electroreduction to multicarbon products on copper using bilayer ionomer coatings UR - https://www.nature.com/articles/s41560-021-00920-8 VL - 6 ER -