Theoretical Insights into Adsorption Behaviors of a Nickel-Decorated Graphdiyne-like Boron Nitride Monolayer as a Single-Atom Adsorbent

As an emerging class of materials with active metal atoms individually anchored on the support, single-atom adsorbents exhibit a unique appeal due to the high atomic utilization rate, specific activity, and uniquely defined active sites. Atomic-level insights into the unique adsorption behaviors are highly desirable for the design of single-atom adsorbents. However, comprehending the inherent mechanism of adsorption on single-atom adsorbents remains a challenge. Herein, a great deal of effort has been devoted to determining the gas adsorption mechanism over the single nickel atom-decorated graphdiyne and graphdiyne-like boron nitride monolayer using density functional theory calculations. The results demonstrate that due to the incorporation of the nickel atom, the two kinds of single-atom adsorbents both show an improved adsorption capacity in comparison to those of the corresponding pristine forms, which agrees with the electron donation and back-donation mechanism. Remarkably, a nickel-decorated graphdiyne-like boron nitride monolayer exhibits the highest NO₂ adsorption ability with an interaction energy of -87.4 kcal mol^-1. Besides, the direct ab initio molecular dynamics reveal that a nickel-decorated graphdiyne-like boron nitride monolayer can stabilize the gas molecule due to the intermolecular force. These findings will pave the way for designing efficient and effective gas adsorbents on the metal-decorated graphdiyne-like boron nitride monolayer.