“…Graphdiyne [15], a new kind of carbon allotrope, is composed of benzene rings (sp 2 -hybridized carbons) and diyne links (-C≡C−C≡C−, sp-hybridized carbons). Due to their unique electronic structures and novel triangular molecular pores, GDY and GDY-based materials have shown great potential in the fields of energy storage and conversion [16,17], catalysis [18,19], electronics, and intelligent devices [20,21]. Generally, in electrocatalytic reactions, a large active surface and pores can facilitate the diffusion and benefit the transfer of small ions and molecules [22,23], rendering GDY a highly efficient electrocatalyst in oxygen reduction reaction (ORR) [24], oxygen evolution reaction (OER) [25], hydrogen evolution reaction (HER) [26], overall water splitting (OWS) [27], electrochemical CO 2 reduction (ECCO 2 R) [28], and nitrogen reduction reaction (NRR) [29].…”