Microstructure and Oxygen Evolution Property of Prussian Blue Analogs Prepared by Mechanical Grinding

Solvent-free mechanochemical synthesis of efficient and low-cost double perovskite (DP), like a cage of Prussian blue (PB) and PB analogs (PBAs), is a promising approach for different applications such as chemical sensing, energy storage, and conversion. Although the solvent-free mechanochemical grinding approach has been extensively used to create halide-based perovskites, no such reports have been made for cyanide-based double perovskites. Herein, an innovative solvent-free mechanochemical synthetic strategy is demonstrated for synthesizing Fe4[Fe(CN)6]3, Co3[Fe(CN)6]2, and Ni2[Fe(CN)6], where defect sites such as carbon-nitrogen vacancies are inherently introduced during the synthesis. Among all the synthesized PB analogs, the Ni analog manifests a considerable electrocatalytic oxygen evolution reaction (OER) with a low overpotential of 288 mV to obtain the current benchmark density of 20 mA cm-2. We hypothesize that incorporating defects, such as carbon-nitrogen vacancies, and synergistic effects contribute to high catalytic activity. Our findings pave the way for an easy and inexpensive large-scale production of earth-abundant non-toxic electrocatalysts with vacancy-mediated defects for oxygen evolution reaction.