An Integrated Design with new Metal-Functionalized Covalent Organic Frameworks for the Effective Electroreduction of...

One of the long-standing issues that prohibits large-scale CO₂ reutilization is the low aqueous solubility of CO₂ and the incurring inefficient mass transport of CO₂ . Herein, we suggest a feasible way to promote the CO₂ reutilization by integrating the storage and reduction, with a new covalent organic framework (COF) series constituted by cobalt-phthalocyanine and boronic acid linkers. We find that the porous structure of the cobalt COF is competitive in the CO₂ storage and can sustain a high CO₂ concentration around the reduction center, whereas the mass transport of CO₂ as well as the efficiency of the CO₂ reduction is significantly improved. The predicted cobalt COF exhibits an overpotential of 0.27 V and a CO production rate, which is 97.7 times higher than in aqueous solution, for the CO₂ reduction. Our work provides a promising candidate for the CO₂ reutilization, with valuable insights and an important prototype for future practical design.