Ionic Exchange of Metal–Organic Frameworks to Access Single Nickel Sites for Efficient Electroreduction of CO₂

Abstract

Single-atom catalysts often exhibit unexpected catalytic activity for many important chemical reactions because of their unique electronic and geometric structures with respect to their bulk counterparts. Herein we adopt metal-organic frameworks (MOFs) to assist the preparation of a catalyst containing single Ni sites for efficient electroreduction of CO₂. The synthesis is based on ionic exchange between Zn nodes and adsorbed Ni ions within the cavities of the MOF. This single-atom catalyst exhibited an excellent turnover frequency for electroreduction of CO₂ (5273 h^-1), with a Faradaic efficiency for CO production of over 71.9% and a current density of 10.48 mA cm^-2 at an overpotential of 0.89 V. Our findings present some guidelines for the rational design and accurate modulation of nanostructured catalysts at the atomic scale.