Localized mass transport channels for electro-upgrade of dilute CO2 toward high-yield C2+ products
Electrocatalytic upgrade of CO 2 offers a promising approach for recycling of global CO 2 emissions, facilitating the achievement of carbon neutrality. Nevertheless, direct utilization of practical dilute CO 2 is urgently important yet rather difficult, which is hindered by the balance of reaction kinetics and mass transport of CO 2 to the catalytic sites. Herein, we propose coordinating the local environment and active catalyst by constructing covalent organic frameworks (COF) on single-atomic In-doped Cu 2 O (In 1 @Cu 2 O) for a high tolerance of CO 2 inlet concentrations (15% to 100%). The optimized amounts of COF functionalized by the trifluoromethyl group act as the local CO 2 /CO diffusion channels via steric confinement effects and C···F electronic effects. Besides, the formation of key intermediates for C 2+ products is greatly facilitated by the promoted COOH adsorption. Hence, a total current of 81.7 A is realized in a 4 × 100 cm 2 electrolyzer stack with over 770 mmol/h C 2+ products at an inlet of dilute CO 2 . Such a electrode architecture sheds light on the dilute CO 2 electrolysis at the potential industrial scale.
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