Rational Designing Microenvironment of Gas-Diffusion Electrodes via Microgel-Augmented CO2 Availability for High-Rate and Selective CO2 Electroreduction to Ethylene

Rational Designing Microenvironment of Gas-Diffusion Electrodes via Microgel-Augmented CO2 Availability for High-Rate and Selective CO2 Electroreduction to Ethylene

Efficient electrochemical CO2 reduction reaction (CO2RR) requires advanced gas-diffusion electrodes (GDEs) with tunned microenvironment to overcome low CO2 availability in the vicinity of catalyst layer. Herein, for the first time, pyridine-containing microgels-augmented CO2 availability is presented in Cu2O-based GDE for high-rate CO2 reduction to ethylene, owing to the presence of CO2-phil microgels with amine moieties. Microgels as three-dimensional polymer networks act as CO2 micro-reservoirs to engineer the GDE microenvironment and boost local CO2 availability. The superior ethylene production performance of the GDE modified by 4-vinyl pyridine microgels, as compared with the GDE with diethylaminoethyl methacrylate microgels, indicates the bifunctional effect of pyridine-based microgels to enhance CO2 availability, and electrocatalytic CO2 reduction. While the Faradaic efficiency (FE) of ethylene without microgels was capped at 43% at 300 mA cm−2, GDE with the pyridine microgels showed 56% FE of ethylene at 700 mA cm−2. A similar trend was observed in zero-gap design, and GDEs showed 58% FE of ethylene at −4.0 cell voltage (>350 mA cm−2 current density), resulting in over 2-fold improvement in ethylene production. This study showcases the use of CO2-phil microgels for a higher rate of CO2RR-to-C2+, opening an avenue for several other microgels for more selective and efficient CO2 electrolysis.