Random Occupation of Multimetal Sites in Transition Metal‐Organic Frameworks for Boosting the Oxygen Evolution Reaction

Developing robust oxygen evolution reaction (OER) electrocatalysts with excellent performance is essential for the conversion of renewable electricity to clean fuel. Herein, we present a facile concept for the synthesis of efficient high‐entropy metal‐organic frameworks (HEMOFs) as electrocatalysts in a one‐step solvothermal synthesis. This strategy allows control of the microstructure and corresponding lattice distortion by tuning the metal ion composition. As a result, the OER activity was improved by optimizing the coordination environment of the metal catalytic center. The optimized Co‐rich HEMOFs exhibited a low overpotential of 310 mV at a current density of 10 mA cm−2, better than a RuO2 catalyst tested under the same conditions. The finding of lattice distortion of the HEMOFs provides a new strategy for developing high‐performance electrocatalysts for energy conversion.