High Activity Single Metal Atom Twisted Bilayer Graphene Catalyst for Oxygen Evolution Reaction: A DFT Study

Single‐atom catalysts (SACs) with high activity and selectivity are regarded as excellent OER catalysts, but easily corroded under acidic environment. Here, we employed density functional theory (DFT) calculations to design a series of SACs protected by twisted bilayer graphene (tBLG) “chainmail.” Charge transfer analysis showed that the carbon layer could serve as an intermediate between transition metal atom and reactants. In addition, rotation operation on bilayer graphene was applied to further enhance the catalytic performance. Thermodynamic free energy diagrams of eight types metal atoms and five rotation angles were systematically discussed. A volcano plot of overpotentials among all the studied single metal atom twisted bilayer graphene catalysts can be described by (). The designed Ni‐tBLG catalyst (rotation angle is 21.8°) exhibited the best performance with the lowest OER overpotential of 0.35 V. These results revealed that the selected single metal atom twisted bilayer graphene catalysts with high activity and stability could be treated as efficient OER catalysts.