One-step synthesis of thin-carbon-shell-encapsulated binary cobalt chromium nitrides for oxygen reduction reaction

Abstract

Hydrogen fuel cells are expected to be widely used in transportation and portable power generation. Unfortunately, sluggish cathodic oxygen reduction reaction (ORR) kinetics hamper the commercial application of the fuel cells. The quest for cost effective and highly efficient ORR catalysts is of great importance. Transition metal nitride (TMN) has received widespread attention mainly for its Pt-like characteristics. Here, we propose a new one-step “NH3-free” synthesis of thin-carbon-shell-encapsulated binary cobalt chromium nitrides (Co-CrN@C) using 1,2,4-1H-triazole as the nitrogen/carbon source. The Co-CrN@C exhibits almost ideal four-electron reduction of oxygen and achieves remarkable long-term durability and better methanol tolerance due to high-degree graphitization of the carbon shell. The X-ray photoelectron spectra and the density functional theory calculations unveil the origin of the intrinsic activity of the catalyst and the reaction mechanism. Furthermore, Co-CrN@C exhibits an impressive peak power density (PPD) of 488 mW cm−2, surpassing the 423 mW cm−2 for the Pt/C-driven anion exchange membrane fuel cells. These findings offer an indispensable strategy for rational design of high-efficient and durable non-noble catalysts.