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

作者：Ma, Yiping; Gong, Xujia; Xiao, Feng; Liu, Yunhui; Ming, Xing^*

来源：ACS Applied Nano Materials, 2023, 6(13): 12470-12478.

DOI：10.1021/acsanm.3c02177

• PdS2
• gas sensor
• frontier molecularorbitals
• charge transfer
• first principles

Detecting toxic gas molecules is of great significancefor industryand public health. However, how to select and design highly sensitiveand selective gas sensors has been a great challenge. In the presentstudy, we explore the adsorption properties of monolayer PdS2 for the NH3, N2O, NO2, NO, CO,H2S, SO2, SO2F2, and SOF2 toxic gas molecules by first-principles calculations. Bycombined analyses of adsorption energy, adsorption distance, chargetransfer, electronic structure, work function, and recovery time,the selectivity and sensitivity of the monolayer PdS2 toNO(2), NO, and SO2 toxic gas molecules are identified.The adsorptions of NO2, NO, and SO2 lead toobvious changes of the electronic structure and charge transfer forthe monolayer PdS2, which are further analyzed based onthe frontier molecular orbitals theory. Additionally, NO adsorptioneffectively leads the work function of monolayer PdS2 toreduce by 17%, and the recovery time of the monolayer PdS2 sensor at room temperature is estimated to be considerably shortfor NO2, NO, and SO2 gases. The present studynot only uncovered that the monolayer PdS2 can be usedas a promising reusable sensing material featured with high selectivityand excellent sensitivity for environmentally hazardous gas moleculesbut also proposed a strategy for screening suitable sensing materialby comparing the frontier molecular orbitals of the gas moleculeswith the band edges of the candidate adsorption materials, which willattract more attention from the wide audience working in the low-dimensionalmaterial system.

• 单位
  中山大学; 桂林理工大学