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

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 MnO1.9F0.1 effectively soften the bonding interaction of Mn-O bonds in the IrCl3 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.

Automated summary

This work proposes a light-driven atomic assembly proposal to optimize the spin-entropy-related orbital interaction and charge transfer in electrocatalysis. The introduction of fluorine atoms effectively softens the bonding interaction in the solution, allowing for the formation of orderly atomic-hybridized catalysts. The time-related elemental analysis shows that the dynamic dissolution/redeposition of Ir clusters leads to a reintegration of the reaction pathway with a lower activation energy.