Previous theoretical studies have consistently shown that pristine SiC monolayers exhibit weak interactions with most hazardous gas molecules, limiting their applicability in gas capture, sensing, and catalysis. To overcome this limitation, this work employs first-principles density functional theory to investigate Zr substitutional doping as a strategy to activate the SiC surface and enhance its adsorption performance. Comprehensive analyses, including structural, electronic, charge-density difference (CDD), electron localization function (ELF), work function (WF), and recovery time, were conducted. Zr doping significantly strengthens gas adsorption and improves sensitivity. NO2, NO, NH3, CO, and COS exhibit strong chemisorption on Zr–SiC, whereas CO2 remains weakly physisorbed. Pronounced work-function shifts, particularly for NO2 and NO, demonstrate the strong potential of Zr–SiC for work-function-based gas sensing. Recovery-time analysis further indicates that these systems can operate effectively as toxic-gas sensors with moderate thermal activation. Overall, Zr doping is an effective approach for enhancing the capturing and gas-sensing performance of SiC monolayers, while also opening pathways for future exploration in catalytic applications.
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