Efficient multicarbon formation in acidic CO2 reduction via tandem electrocatalysis
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Materials Science↗
Engineering topics
Ozden, Adnan
Publications and source records attributed to Ozden, Adnan.
Coordination Polymer Electrocatalysts Enable Efficient CO‐to‐Acetate Conversion
Abstract Upgrading carbon dioxide/monoxide to multi‐carbon C 2+ products using renewable electricity offers one route to more sustainable fuel and chemical production. One of the most appealing products is acetate, the profitable electrosynthesis of which demands a catalyst with higher efficiency. Here, a coordination polymer (CP) catalyst is reported that consists of Cu(I) and benzimidazole units linked via Cu(I)‐imidazole coordination bonds, which enables selective reduction of CO to acetate with a 61% Faradaic efficiency at −0.59 volts versus the reversible hydrogen electrode at a current density of 400 mA cm −2 in flow cells. The catalyst is integrated in a cation exchange membrane‐based membrane electrode assembly that enables stable acetate electrosynthesis for 190 h, while achieving direct collection of concentrated acetate (3.3 molar) from the cathodic liquid stream, an average single‐pass utilization of 50% toward CO‐to‐acetate conversion, and an average acetate full‐cell energy efficiency of 15% at a current density of 250 mA cm −2 .
Luo, Mingchuan↗
Energy- and carbon-efficient CO 2 /CO electrolysis to multicarbon products via asymmetric ion migration–adsorption
Carbon dioxide/monoxide (CO 2 /CO) electrolysis provides a means to convert emissions into multicarbon products. However, impractical energy and carbon efficiencies limit current systems. Here we show that these inefficiencies originate from uncontrolled gas/ion distributions in the local reaction environment. Understanding of the flows of cations and anions motivated us to seek a route to block cation migration to the catalyst surface-a strategy we instantiate using a covalent organic framework (COF) in bulk heterojunction with a catalyst. The pi-conjugated hydrophobic COFs constrain cation (potassium) diffusion via cation-pi interactions, while promoting anion (hydroxide) and gaseous feedstock adsorption on the catalyst surface. So as a result, a COF-mediated catalyst enables electrosynthesis of multicarbon products from CO for 200 h at a single-pass carbon efficiency of 95%, an energy efficiency of 40% and a current density of 240 mA cm -2 .
42 ENGINEERING↗