Enhanced Charge Transfer Process and Chemical Sensing Ability Over a Lattice Rearrangement Strategy via Monatomic Ag Embedded Graphdiyne

ABSTRACT Despite the graphdiyne (GDY) has been theoretically predicted to be a promising candidate for chemical sensor applications due to its distinctive intrinsic structure and properties, significant challenges still remain in practical applications. Here, we demonstrate a regulated charge‐transfer pathway and a sensing ability enhancement strategy through pore‐confined monatomic Ag‐induced lattice rearrangement of GDY. The planar and axially asymmetric multi‐coordination configuration and pore confinement effect between Ag and the nitrogen‐substituted GDY skeleton enable a high Ag loading of 10.2 wt.%. Meanwhile, the lattice structure of GDY is tailored by a single atom of Ag, presenting a perfect hexagonal crystal structure with ultrahigh crystallinity, enabling an efficient charge transfer channel during the gas interaction process. Moreover, the reorientation of the 4 d orbitals of the Ag atom endows a stronger d − p interaction with the adsorbate. As expected, the sensor denoted as Ag _SAs /GDY demonstrates remarkable performance for ethanol detection over the entire low temperature range (<100°C). This work provides a new insight into enhancing the sensing activity at the atomic level and offers a general approach for the future design and development of other high‐loading monatomic materials on carbon substrates.