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 38.9 mV at −10 mA cm−2 in an alkaline medium. Importantly, the cell voltage of water electrolysis can be significantly reduced to only 1.35 V at a current of 10 mA 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.

Coupling Ferrocyanide-Assisted PW/PB Redox with Efficient Direct Seawater Electrolysis for Hydrogen Production

“…The stability of the system was also evaluated by way of chronoamperometry, which showed that this approach exhibited considerable stability at 100 mA cm –2 with a retention rate of 95% within 45 h (Figure S18). To emphasize the advantage and potential of [Fe­(CN) 6 ] 4– -assisted PW/PB redox-coupled hydrogen production system, Figure e and Table S1 show the cell voltage, electricity consumption, and cell life of this work at a certain current density and compare it with those from different state-of-the-art seawater splitting experiments reported in the literature. ,− Our approach undoubtedly showed significant advantages in efficiency, energy consumption, and sustainability in H 2 production.…”

Innovative Electrochemical Strategies for Hydrogen Production: From Electricity Input to Electricity Output

“…[51] Qiu and co-workers synthesized 5,5'-azotetrazolate by electrooxidation of 5-amino-1H-tetrazole coupled with HER. [52] What's more, alkene oxidation can also be employed as an alternative anodic reaction coupled with cathodic HER (Figure 5f). Sargent and co-workers coupled the electrooxidation of ethylene with H 2 production to produce ethylene glycol by a gold-doped palladium catalyst in aqueous 0.1 M NaClO 4 medium.…”

Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application

“…To overcome this problem, PGM-based SACs and DACs have been widely studied in HER process, such as catalysts containing Pt-, [192] Pd-, [193] Rusingle/dual atom sites. [194] For example, Yang et al trap atomic Pt in defective graphene matrix to form the Pt-C 3 configuration (named as Pt@DG, Figure 14a), which gives ultrahigh activity in HER process under both acidic and alkaline conditions. [55] As shown in Figure 14b, in acidic HER process, a much decreased overpotential (30 mV) at a current density of 10 mA cm −2 of Pt@DG is achieved compared to that of Pt/C.…”