Graphdiyne-Based Two-Dimensional Nanomaterials for Next-Generation “Beyond Li-Ion” Batteries

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Two-dimensional (2D) carbon nanomaterials represent a promising avenue for the development of next-generation energy storage systems. Particularly, graphdiyne-based 2D nanomaterials have emerged as optimistic candidates due to their unique structural and electronic properties. Graphdiyne, an emerging carbon allotrope with the consolidation of diacetylenic linkages and sp2 hybridized carbon atoms, offers remarkable surface area, mechanical strength, and chemical stability. Herein, we developed a lithiophilic hydrogen substituted graphdiyne aerogel host for Li metal batteries. The hydrogen substituted graphdiyne aerogel’s lithiophilic nature and hierarchical pores drive molten Li infusion and reduce local current density within the three-dimensional host, thus achieving dendrite-free Li metal anodes. By regulating electron and ion transport within the host simultaneously, uniform lithium stripping/platting is fulfilled, thereby effectively mitigating lithium dendritic growth and enhancing lithium utilization. A symmetric cell with lithium-infused hydrogen substituted graphdiyne aerogel exhibits a low overpotential of 88 mV at 2 mA cm-2, and stable cycling of 300 cycles in carbonate electrolytes. Paired with a lithium iron phosphate cathode, a full-cell battery demonstrates excellent rate capability and long-term stability with 98.1% capacity retention after 170 cycles at 0.4 C. Moving beyond Li metal batteries, we incorporated cobalt single atom sites into hydrogen substituted graphdiyne for all-solid-state lithium-sulfur batteries. Porous hydrogen substituted graphdiyne aerogel suppressed the amount of soluble sulfur species in the solid polymer electrolytes. Furthermore, the catalytic effect of cobalt single atom sites enhanced the lithium-sulfur reaction kinetics and cycling performance of all-solid-state lithium-sulfur batteries. Our work sheds light on developing graphdiyne-based 2D nanomaterials in revolutionizing next-generation energy storage technologies and in addressing the challenges posed by the ever-increasing demand for efficient and sustainable energy storage solutions.