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

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 4d 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.