Hydrogen Substituted Graphdiyne Assisted Ultra-Fast Sparking Synthesis of Metastable Nanomaterials for Li-S Batteries

Metastable nanomaterials, such as single atom and high entropy systems, with exciting physical and chemical properties, are increasingly crucial for next-generation technologies. The origin of these properties results from electronic and bonding structures far from equilibrium although the synthesis of metastable nanomaterials remains challenging. For example, extreme heating and cooling rates are often required to prevent cluster formation of single atoms and phase separation of high entropy alloys. Here, we developed a hydrogen substituted graphdiyne-assisted ultra-fast sparking synthesis platform for the preparation of metastable nanomaterials. Controlling the composition and chemistry of the hydrogen substituted graphdiyne aerogel framework, the reaction temperature can be tuned from 1640 K to 3286 K within milliseconds. We demonstrate the versatility of the ultra-fast high-temperature platform with the successful synthesis of single atoms, high entropy alloys, and high entropy oxides. Electrochemical measurements and density functional theories show that single atoms synthesized by the platform enhance the lithium-sulfur redox reaction kinetics, enabling high-performance all-solid-state lithium-sulfur batteries. Our design of the ultra-fast high-temperature platform offers a new powerful way to synthesize a variety of metastable nanomaterials.