Spherical Murray-Type Assembly of Co-N-C Nanoparticles as a High-Performance Trifunctional Electrocatalyst

Future renewable energy conversion requires advanced electrocatalysis technologies for hydrogen production, fuel cells, and metal-air batteries. Highly efficient trifunctional nonprecious electrocatalysts are a critical precious metal replacement for the economically viable electrocatalysis of oxygen reduction and water splitting, both of which are a triphase electrode process. Electrocatalysts with a refined porous structure and active composition beneficial for three-phase reactions are broadly pursued. Herein, a highly promising trifunctional spherical Murray assembly of Co-N-C nanoparticles was derived from low-cost Prussian blue analogues for the oxygen reduction reaction and water splitting. The Murray-type architecture with a tunable porous hierarchy for efficient mass transfer and the combination of a Co-N-C active composition are key for the improved electrocatalytic performance. Acid-leaching produced an optimized Murray-type durable and methanol-tolerant Co-N-C electrocatalyst that achieved an onset potential of 0.94 V [vs reversible hydrogen electrode (RHE)] and a half wave potential of 0.84 V (vs RHE) as well as a large diffusion-limited current density of 5.7 mA cm(-2) for the oxygen reduction reaction, which is comparable to Pt/C. In addition, it displayed low onset overpotentials of similar to 150 and similar to 350 mV corresponding to the hydrogen evolution reaction and oxygen evolution reaction, respectively, highlighting its great potential to be used in overall water splitting with a total splitting voltage of 1.73 V. This work highlights the importance of Murray-type electrocatalysts for multiphase energy-related reactions.