Harnessing the Synergistic Effects of Ir Co‐Decorated NiMn‐LDH: a Multi‐Analytical Approach to Boost Electrocatalytic Overall Water Splitting Activity in Alkaline Condition

Abstract Fine control over the Ir precursor to the Nickel‐based layered double hydroxides (LDHs) is significant for decorating both single atoms (SA) and nanoclusters (NC), thus modulating catalytic kinetics and improving overall performance. In this study, NiMn‐LDH is synthesized and co‐decorated it with Iridium, introducing a new pathway for developing efficient bifunctional electrocatalysts in water‐splitting technologies. Additionally, a typical fibrous material has developed by immobilizing. onto PAN (polyacrylonitrile) nanofibers () using a feasible electrospinning technique. Notably, the catalyst exhibits low overpotentials of 249 and 110 mV for oxygen (OER) and hydrogen evolution reactions (HER) at 10 mA cm − 2 , and a low cell voltage of 1.65 V for total water splitting (TWS). Additionally, remained stable and effective in alkaline OER, HER, and TWS for over 50 h. Furthermore, X‐ray adsorption near‐edge spectrum (XANES) experiments, together with theoretical calculations, show that the synergistic effect of Ir SA and which helps to enhance the catalytic activity, promoting electron rearrangement and lowering the reaction energy barrier.