First-Principles Calculations of Two-Dimensional Monolayer PdSe₂ for Selective Sensing of Nitrogen-Containing Gases

Abstract

Monolayer palladium diselenide (PdSe 2 ) has attracted increasing attention due to its outstanding physicochemical properties and puckered pentagonal layered structure. In this study, the adsorption of nitrogen-containing gases on the surface of monolayer PdSe 2 has been investigated by first-principles calculations to fully explore its gas-sensing capability. It is found that NH 3 and N 2 O show physisorption, while NO 2 and NO prefer chemisorption, indicating excellent selectivity of monolayer PdSe 2 . Furthermore, the NH 3 and N 2 O (NO 2 and NO) adsorption exhibits a negligible (significant) amount of charge transfer, which in turn leads to a tiny (considerable) change in the electronic structure and magnetic property of the adsorbent surface. In particular, the adsorption of NO 2 and NO introduces additional states around the Fermi level, which induces a dramatic decrease of the band gap and appearance of magnetic moments, and further leads to a huge change of the electrical conductivity of monolayer PdSe 2 . Additionally, the recovery time of the PdSe 2 sensor at room temperature is estimated to be considerably short for NO 2 and NO. Overall, the present work reveals that two-dimensional monolayer PdSe 2 can be used as a promising reusable sensing material featured with high selectivity and excellent sensitivity for environmentally hazardous gas molecules.

Adsorption and Gas-Sensing Performance of the Small-Molecule Gas on ZrSe2 Monolayers: A First-Principles Study

“…As industrialization has grown in recent years, the amount of polluting gases in the air have increased, which are particularly harmful to the environment and public health. − Therefore, it makes sense to remove and capture these toxic gases from the environment using effective methods. In order to identify such air pollutants, highly sensitive sensors with high selectivity, fast response, and recovery of sorbents to toxic substances are urgently needed. − Due to their high surface-to-volume ratio, − two-dimensional (2D) nanomaterials have gained significant interest from researchers in recent years as efficient gas sensors. The discovery of graphene led to studies on the sensing potential of 2D nanostructures.…”

First-Principles Study on the Selective Detection of Toxic Gases by 2D Monolayer PdS2: Insight into Charge Transfer Dynamics and Alignment of Frontier Molecular Orbitals

“…Two-dimensional (2D) materials have been widely investigated due to their large surface-to-volume ratio, high surface activities, and distinct thickness-dependent physical and chemical properties. So far, some intrinsic 2D materials such as graphene, transition metal dichalcogenides (TMDCs), − boron–phosphorus, phosphorene, and silicene have been extensively studied as gas-sensing materials due to their excellent selectivity and sensitivity. According to the different charge transfer mechanisms, the gas molecules adsorbing on the surface of the 2D materials can act as electron donors or acceptors.…”

“…20−24 Recent experiments and calculations have been conducted on monolayer and few-layer PdSe 2 gas sensors, and it has been found that PdSe 2 is a promising sensing material exhibiting sensitive responses toward nitrogen dioxide (NO 2 ) gas and good reusability at room temperature. 5,25,26 Unfortunately, there are no studies to explore whether the monolayer PdS 2 is suitable for gas sensors up to now.…”

Layer-dependent electronic structures and optical properties of two-dimensional PdSSe

“…[26][27][28][29][30] NMDCs not only possess anisotropic structures, low-energy differences between different crystalline phases and controllable phase transitions compared to conventional TMDCs, but also exhibit promising application potential in field-effect transistors, photodetectors, sensors, photocatalysts and photovoltaic cells. [31][32][33][34][35][36][37] Particularly, the bulk phases of diselenides or disulphides of palladium (PdX 2 , X = S, and Se) crystallize in a peculiar puckered pentagonal structure (2O type), instead of the common 1T, 2H or 3R structure of TMDCs. 38 Although equilateral pentagons with good symmetry are regarded as topological or geometrical defects and cannot be used as planar structural motifs, low-symmetry type-II pentagons can spread over the entire plane and lead to Cairo tessellation.…”

“…26–30 NMDCs not only possess anisotropic structures, low-energy differences between different crystalline phases and controllable phase transitions compared to conventional TMDCs, but also exhibit promising application potential in field-effect transistors, photodetectors, sensors, photocatalysts and photovoltaic cells. 31–37…”