An Integrated Design with new Metal‐Functionalized Covalent Organic Frameworks for the Effective Electroreduction of CO 2

One of the long‐standing issues that prohibits large‐scale CO 2 reutilization is the low aqueous solubility of CO 2 and the incurring inefficient mass transport of CO 2 . Herein, we suggest a feasible way to promote the CO 2 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 CO 2 storage and can sustain a high CO 2 concentration around the reduction center, whereas the mass transport of CO 2 as well as the efficiency of the CO 2 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 CO 2 reduction. Our work provides a promising candidate for the CO 2 reutilization, with valuable insights and an important prototype for future practical design.