Integration of High‐ <i>p</i> , Low‐ <i>T</i> CO ₂ Electrolysis with Pressure Swing Adsorption Purification

Abstract Herein, a high‐pressure low‐temperature CO 2 electrolysis (LTCE) cell is coupled with a pressure swing adsorption (PSA) unit to maximize CO production and product‐gas purity to compare cascade and full‐recycle operation. The inlet CO 2 governs LTCE selectivity with CO 2 ‐rich feeds yielding CO &gt;90% with minimal H 2 , with CO 2 conversion being 22.4%; diluted CO 2 &lt;70 vol.% lowers CO selectivity to 75.3%. Similarly, PSA yield ranges between 25.4 and 33.4% depending on the input CO concentration, enabling negligible CO 2 in the product (≤0.025 vol.%). Compared to the cascade (≈6% CO yield), the full recycle system yields 99.99% CO (88.3 vol.% CO). Even at end‐of‐life scenarios for the LTCE cell with CO selectivity ≈35% near quantitative CO yield (99.6%) in recycle operation is possible.