Tuning Metal Elements in Open Frameworks for Efficient Oxygen Evolution and Oxygen Reduction Reaction Catalysts.

Abstract

Electrochemical methods are promising technical routes for future clean energy storage and conversion. Most of the electrochemical methods involve oxygen reactions. Unfavorable kinetics and sluggish reactions are the main challenges for these processes. We report here a facile synthesis of highly efficient oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) catalysts. The catalysts are synthesized through the fine-tuning of metal ions (M, specifically Co, Ni, Zn, and Cu) in Prussian blue analogues (PBAs) and thus termed as M-PBAs. The CoNi-PBA-2 catalyst shows the highest activity toward OER with an onset potential at 280 mV and a Tafel slope of 63 mV dec-1. Zn-PBA catalysts demonstrate high selectivity in two-electron-transfer ORR. The H2O2 yield is as high as 88% at 0 V vs RHE. Density functional theory (DFT) calculations also confirm the high selectivity of Zn-PBA toward H2O2 in ORR.