Abstract
AbstractAchieving efficient bifunctional oxygen reduction and evolution reactions (ORR/OER) on non‐noble metal catalysts is desirable but remains a significant challenge. Herein, inspired by the experimentally synthesized (phen2N2)FeCl molecule, a stable 2D organometallic framework, namely (phen2N2)FeCl monolayer, is proposed as a qualified candidate by means of constant‐potential first‐principles computations. Unlike most 2D organometallic frameworks that feature pyrrolic coordination, the (phen2N2)FeCl monolayer exhibits a pyridinic‐type FeN4 ligation environment. The unique structure of the monolayer enables a high single‐atom Fe loading in a heterogeneous system, superior to the typical FeNC materials. Constant‐potential energy analysis and microkinetic modeling demonstrate that the monolayer holds great potential for facilitating bifunctional ORR/OER in both the acidic and alkaline conditions, showing theoretical activity higher than the FeNC materials, (phen2N2)FeCl molecule, and Pt/IrO2. Moreover, (phen2N2)MCl monolayers (M = Mn, Co, and Ni) are explored, and the (phen2N2)MnCl monolayer is also identified to have excellent bifunctional activity. This study highlights the rational design of local coordination environments for boosting the electrocatalytic performance of 2D organometallic frameworks.
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