Hydrogen-substituted graphdiyne-assisted ultrafast sparking synthesis of metastable nanomaterials.

Abstract

Metastable nanomaterials, such as single-atom and high-entropy systems, with exciting physical and chemical properties are increasingly important for next-generation technologies. Here, we developed a hydrogen-substituted graphdiyne-assisted ultrafast sparking synthesis (GAUSS) platform for the preparation of metastable nanomaterials. The GAUSS platform can reach an ultra-high reaction temperature of 3,286 K within 8 ms, a rate exceeding 105 K s-1. Controlling the composition and chemistry of the hydrogen-substituted graphdiyne aerogel framework, the reaction temperature can be tuned from 1,640 K to 3,286 K. We demonstrate the versatility of the GAUSS platform with the successful synthesis of single atoms, high-entropy alloys and high-entropy oxides. Electrochemical measurements and density functional theory show that single atoms synthesized by GAUSS enhance the lithium-sulfur redox reaction kinetics in all-solid-state lithium-sulfur batteries. Our design of the GAUSS platform offers a powerful way to synthesize a variety of metastable nanomaterials.