Engineering Catalyst–Electrolyte Microenvironments to Optimize the Activity and Selectivity for the Electrochemical Reduction of CO2 on Cu and Ag

• DOI: 10.1021/acs.accounts.1c00650
• Publication Date: 2022-02-01T17:08:57Z
• Authors: Justin C. Bui; Chanyeon Kim; Alex J. King; Oyinkansola Romiluyi; Ahmet Kusoglu; Adam Z. Weber; Alexis T. Bell
• Keywords: Selective catalytic reduction; Gas diffusion electrode

ConspectusThe electrochemical reduction of carbon dioxide (CO2R) driven by renewably generated electricity (e.g., solar and wind) offers a promising means for reusing the CO2 released during production cement, steel, aluminum as well ammonia methanol. If could be removed from atmosphere at acceptable costs (i.e., <$100/t CO2), then CO2R used to produce carbon-containing chemicals fuels in fully sustainable manner. Economic considerations dictate that current densities must range 0.1 1 A/cm2 selectivity toward targeted product high order minimize separation costs. Industrially relevant operating conditions can achieved using gas diffusion electrodes (GDEs) maximize transport species cathode combining such with solid-electrolyte membrane eliminating ohmic losses associated liquid electrolytes. Additionally, attained careful tuning microenvironment near catalyst surface pH, concentrations H2O, identities cations double layer adjacent surface).We begin this Account discussion our experimental theoretical work aimed optimizing microenvironments CO2R. We first examine effects morphology on multicarbon (C2+) products over Cu-based catalysts explore role mass transfer combined kinetics buffer reactions local concentration pH surface. This is followed dependence dynamics formation specific both Cu Ag catalysts. Next, we impact electrolyte cation identity rate distribution products. Subsequently, look utilizing pulsed electrolysis tune The last part demonstrates ionomer-coated combination enable attainment very (>90%) C2+ an aqueous electrolyte. extended consider difference catalyst–nanoparticle microenvironment, present electrode assembly (MEA), respect planar immersed