Light‐driven Orderly Assembly of Ir‐atomic Chains to Integrate a Dynamic Reaction Pathway for Acidic Oxygen Evolution

Abstract This work suggests an intriguing light‐driven atomic assembly proposal to orderly configure the distribution of reactive sites to optimize the spin‐entropy‐related orbital interaction and charge transfer from electrocatalysts to intermediates. Herein, the introduced fluorine (F) atoms acting as photo‐corrosion centres in MnO 1.9 F 0.1 effectively soften the bonding interaction of Mn−O bonds in the IrCl 3 solution. Therefore, partial Mn atoms can be successively replaced to form orderly atomic‐hybridized catalysts with a spin‐related low entropy due to the coexistence of Ir‐atomic chains and clusters. The time‐related elemental analysis demonstrates that the dynamic dissolution/redeposition of Ir clusters in acidic oxygen evolution leads to a reintegration of the reaction pathway to seek the switchable rate‐limiting step with a lower activation energy.