CO、CO2、H2S、NH3、NO、NO2 和 SO2 与 Zn12O12 和 Zn24 原子团簇的气相相互作用,ACS Omega

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CO、CO2、H2S、NH3、NO、NO2 和 SO2 与 Zn12O12 和 Zn24 原子团簇的气相相互作用
ACS Omega ( IF 3.7 ) Pub Date : 2023-05-30 , DOI: 10.1021/acsomega.3c01177
Mohsen Doust Mohammadi ₁ , Hitler Louis ₂ , Udochukwu G Chukwu ₂ , Somnath Bhowmick ₁ , Michael E Rasaki ₂ , George Biskos _{1,

3}

Affiliation

大气污染物对人类健康构成很高的风险，因此有必要捕获并最好将其从环境空气中去除。_{在这项工作中，我们研究了CO、CO 2}、H ₂ S、NH ₃、NO、NO ₂和SO ₂气体等污染物与Zn ₂₄和Zn ₁₂ O ₁₂之间的分子间相互作用。原子团簇，在元混合函数 TPSSh 和 LANl2Dz 基组上使用密度泛函理论 (DFT)。计算了这些气体分子在两种团簇外表面上的吸附能，发现它们具有负值，表明分子团簇具有很强的相互作用。_{在SO 2}和Zn ₂₄簇之间观察到最大的吸附能。一般来说，Zn ₂₄簇似乎比 Zn ₁₂ O _{12更有效地吸附 SO}₂、NO ₂和 NO ，而后者更适合吸附 CO、CO ₂、H ₂ S 和 NH ₃。前沿分子轨道(FMO)分析表明Zn ₂₄对NH ₃、NO、NO ₂和SO ₂的吸附表现出较高的稳定性，吸附能落在化学吸附范围内。Zn ₁₂ O _{12团簇在吸附 CO、H}₂ S、NO 和 NO ₂后显示出带隙的特征性减小，表明电导率增加。自然键轨道（NBO）分析还表明原子簇和气体之间存在强烈的分子间相互作用。根据非共价相互作用 (NCI) 和分子中原子量子理论 (QTAIM) 分析确定，这种相互作用被认为是强且非共价的。总体而言，我们的结果表明 Zn ₂₄和 Zn ₁₂ O ₁₂簇都是促进吸附的良好候选物种，因此可以用于不同的材料和/或系统中以增强与 CO、H 2 _S、NO 或 NO 的相互作用₂ .

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Gas-Phase Interaction of CO, CO2, H2S, NH3, NO, NO2, and SO2 with Zn12O12 and Zn24 Atomic Clusters

Atmospheric pollutants pose a high risk to human health, and therefore it is necessary to capture and preferably remove them from ambient air. In this work, we investigate the intermolecular interaction between the pollutants such as CO, CO₂, H₂S, NH₃, NO, NO₂, and SO₂ gases with the Zn₂₄ and Zn₁₂O₁₂ atomic clusters, using the density functional theory (DFT) at the meta-hybrid functional TPSSh and LANl2Dz basis set. The adsorption energy of these gas molecules on the outer surfaces of both types of clusters has been calculated and found to have a negative value, indicating a strong molecular-cluster interaction. The largest adsorption energy has been observed between SO₂ and the Zn₂₄ cluster. In general, the Zn₂₄ cluster appears to be more effective for adsorbing SO₂, NO₂, and NO than Zn₁₂O₁₂, whereas the latter is preferable for the adsorption of CO, CO₂, H₂S, and NH₃. Frontier molecular orbital (FMO) analysis showed that Zn₂₄ exhibits higher stability upon adsorption of NH₃, NO, NO₂, and SO₂, with the adsorption energy falling within the chemisorption range. The Zn₁₂O₁₂ cluster shows a characteristic decrease in band gap upon adsorption of CO, H₂S, NO, and NO₂, suggesting an increase in electrical conductivity. Natural bond orbital (NBO) analysis also suggests the presence of strong intermolecular interactions between atomic clusters and the gases. This interaction was recognized to be strong and noncovalent, as determined by noncovalent interaction (NCI) and quantum theory of atoms in molecules (QTAIM) analyses. Overall, our results suggest that both Zn₂₄ and Zn₁₂O₁₂ clusters are good candidate species for promoting adsorption and, thus, can be employed in different materials and/or systems for enhancing interaction with CO, H₂S, NO, or NO₂.

更新日期：2023-05-30

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