What happens when graphdiyne encounters doping for electrochemical energy conversion and storage

Graphdiyne (GDY), the rising-star two-dimensional carbon allotrope, has been widely utilized in electrochemical field owing to its unique properties of highly π-conjugated structure, abundant natural pores, excellent electronic conductivity, and high stability. Nevertheless, the performance of pure GDY does not achieve optimum. The doping of heteroatom into GDY can regulate the electronic structure, promote the ion mobility, and increase the number of active sites of GDY, thereby optimizing its performance. Therefore, heteroatom-doped GDY has attracted considerable attention and many relevant works have been reported, while no review has been conducted to summarize heteroatom-doped GDY. In this work, the preparation methods of heteroatom-doped GDY are first introduced, including in-situ Glaser-Hay coupling method, annealing method, and wet chemical method. Then, the doping of different heteroatoms into GDY such as nitrogen, fluorine, boron, other non-metal atoms, metal single atoms, and co-doping is elaborated. Subsequently, the electrochemical applications of heteroatom-doped GDY in energy conversion and storage are reviewed, including hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, overall water splitting, nitrogen reduction reaction, carbon dioxide reduction reaction, batteries, capacitors, and hydrogen storage. Finally, the existing challenges and opportunities of heteroatom-doped GDY are comprehensively discussed. The above summary indicates that heteroatom-doped GDY displays excellent performance and will open up a broader research horizon. We hope that this review can provide an in-depth understanding of heteroatom-doped GDY, thereby promoting its further development.