%0 Journal Article
%A Chanyeon Kim
%A Justin C Bui
%A Xiaoyan Luo
%A Jason K Cooper
%A Ahmet Kusoglu
%A Adam Z Weber
%A Alexis T Bell
%B Nature Energy
%D 2021
%G eng
%N 11
%P 1026 - 1034
%R 10.1038/s41560-021-00920-8
%T Tailored catalyst microenvironments for CO2 electroreduction to multicarbon products on copper using bilayer ionomer coatings
%U https://www.nature.com/articles/s41560-021-00920-8
%V 6
%8 10/2021
%! Nat Energy
%X <p><span>Electrochemical carbon dioxide reduction (CO</span><sub><span>2</span></sub><span>R) provides a promising pathway for sustainable generation of fuels and chemicals. Copper (Cu) electrocatalysts catalyse CO</span><sub><span>2</span></sub><span>R to valuable multicarbon (C</span><sub><span>2+</span></sub><span>) 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 CO</span><sub><span>2</span></sub><span>/H</span><sub><span>2</span></sub><span>O ratio (via ionomer properties), respectively. When this tailored microenvironment is coupled with pulsed electrolysis, further enhancements in the local ratio of CO</span><sub><span>2</span></sub><span>/H</span><sub><span>2</span></sub><span>O and pH are achieved, leading to selective C</span><sub><span>2+</span></sub><span>&nbsp;production, which increases by 250% (with 90% Faradaic efficiency and only 4% H</span><sub><span>2</span></sub><span>) 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.</span></p>