Ruthenium‐Doped Cobalt–Chromium Layered Double Hydroxides for Enhancing Oxygen Evolution through Regulating Charge Transfer

Abstract Exploring the origin of transition metal (TM) lattice‐doped layered double hydroxides (LDHs) toward the oxygen evolution reaction (OER) plays a crucial role in engineering efficient electrocatalysts. Without understanding the physics behind the TM‐induced catalytic enhancements, it would be challenging to design the next generation of electrocatalysts. Herein, single Ru atoms are introduced into a CoCr LDHs lattice to improve activity. In 0.1 m KOH, CoCrRu LDHs require only 290 mV overpotential to drive to 10 mA cm−2 and show a Tafel slope of 56.12 mV dec−1. Electronic structure analyses based on density functional theory confirm that promoted OER activity originates from synergetic charge transfer among Ru, Cr, and Co elements. Specifically, Ru dopants can downshift d states of Co and enhance electron donation of Cr to oxygenates, which essentially breaks the scaling relation and achieves higher activity. This work provides insights into how single atomic Ru dopant tunes the electronic structures of its neighbor's active site Co and thus increases OER activities.