A Facile Strategy for Constructing a Carbon‐Particle‐Modified Metal–Organic Framework for Enhancing the Efficiency of CO2 Electroreduction into Formate

Electrocatalytic reduction of CO2 by metal–organic frameworks (MOFs) has been widely investigated, but insufficient conductivity limits application. Herein, a porous 3D In‐MOF {(Me2NH2)[In(BCP)]⋅2 DMF}n (V11) with good stability was constructed with two types of channels (1.6 and 1.2 nm diameter). V11 exhibits moderate catalytic activity in CO2 electroreduction with 76.0 % of Faradaic efficiency for formate (FEHCOO‐). Methylene blue molecules of suitable size and pyrolysis temperature were introduced and transformed into carbon particles (CPs) after calcination. The performance of the obtained CPs@V11 is significantly improved both in FEHCOO‐ (from 76.0 % to 90.1 %) and current density (2.2 times). Control experiments show that introduced CPs serve as accelerant to promote the charges and mass transfer in framework, and benefit to sufficiently expose active sites. This strategy can also work on other In‐MOFs, demonstrating the universality of this method for electroreduction of CO2. To improve the catalytic performance of MOFs in CO2RR, a strategy to introduce suitable precursor to in situ generate carbon nanoparticles was adopted. Introduced carbon nanoparticles serve as accelerant to promote the charges and mass transfer in the framework, and sufficiently expose active sites. This strategy gives impetus to construct more effective catalysts for electroreduction of CO2.