Dual In Situ Laser Techniques Underpin the Role of Cations in Impacting Electrocatalysts

Understanding the electrode/electrolyte interface is crucial for optimizing electrocatalytic performances. Here, we demonstrate that nature of alkali metal cations can profoundly impact oxygen evolution activity surface-mounted metal–organic framework (SURMOF) derived electrocatalysts, which are based on NiFe(OOH). In situ Raman spectroscopy results show shifts Ni−O bending vibration inversely proportional to mass activities from Cs+ Li+. Particularly, a laser-induced current transient technique was introduced study cation-dependent electric double layer properties and their effects activity. The catalytic trend appeared be closely related potential maximum entropy system, suggesting strong cation interfacial water structure. Our highlight how electrolyte composition used maximize performance SURMOF derivatives toward electrochemical splitting.