Green Electrosynthesis of 5,5'-Azotetrazolate Energetic Materials Plus Energy-Efficient Hydrogen Production Using Ruthenium Single-Atom Catalysts.

Abstract

Water electrolysis involves two parallel reactions, that is, oxygen evolution (OER) and hydrogen evolution (HER), in which sluggish OER is a significant limiting step that results in high energy consumption. Coupling the thermodynamically favorable electrooxidation of organic alternatives to value-added fine chemicals HER is a promising approach for the simultaneous cost-effective production of value-added chemicals and hydrogen. Here, a new coupling system for the green electrochemical synthesis of organic energetic materials (EMs) plus hydrogen production using single-atom catalysts is introduced. The catalysts are prepared by the facile galvanostatic deposition of ruthenium single atoms on the molybdenum selenide and reveal a low HER overpotential of 38.9mV at -10mA cm-2 in an alkaline medium. Importantly, the cell voltage of water electrolysis can be significantly reduced to only 1.35V at a current of 10mA cm-2 by coupling water splitting with the electrooxidation of 5-amino-1H-tetrazole to synthesize 5,5'-azotetrazolate energetic material. These materials are traditionally synthesized under harsh conditions involving a strong oxidizing agent, high-temperature conditions, and difficult separation of by-products. This study provides a green and efficient method of synthesizing organic EMs while simultaneously producing hydrogen.