Electrolyte Engineering towards Efficient Water Splitting at Mild pH

The development of processes for the conversion of H2O and CO2 driven by electricity generated by renewable means is essential to achieving sustainable energy and chemical cycles, in which the electrocatalytic oxygen evolution reaction (OER) is one of the bottlenecks. In this study, the influences of the electrolyte molarity and identity on the OER at alkaline to neutral pH were investigated at an appreciable current density of around 10 mAcm(-2), revealing both the clear boundary of reactant switching between H2O/OH-, owing to the diffusion limitation of OH-, and the substantial contribution of the mass transport of the buffered species in buffered mild-pH conditions. These findings suggest a strategy of electrolyte engineering: tuning the electrolyte properties to maximize the mass-transport flux. The concept is successfully demonstrated for the OER, as well as overall water electrolysis in buffered mild-pH conditions, shedding light on the development of practical solar fuel production systems.