环境条件下大气气溶胶前体形成的计算研究:海盐、水和硫酸分子之间相互作用的案例研究

IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL International Journal of Quantum Chemistry Pub Date : 2024-10-08 DOI:10.1002/qua.27489
Dhyani Vadgama, Rohit Srivastava, Satyam Shinde
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引用次数: 0

摘要

团簇的形成对大气科学和环境化学具有重要影响。这些团聚体的特点是其成分之间存在复杂的相互作用,从而影响其结构、稳定性和生长。对于导致较大气溶胶形成的预核团簇形成的初始阶段,很难进行实验研究。为了了解气溶胶团的形成过程,我们对海盐(氯化钠、氯化钾和氯化镁)、水和硫酸分子之间的相互作用进行了研究。对每个步骤都进行了全面研究,并使用 DLPNO-CCSD(T)/CBS//M06-2X/6-311++G(3df,3pd)计算了热力学参数,以找出分子络合物的稳定性。在所有络合物中,发现簇(SS)1(W)1(SA)3 的结合能最低,原因是形成了 HCl、氢键和弱范德华力。与 H2O 分子相比,海盐与 H2SO4 的相互作用更为有利。加入 H2SO4 会提高簇(SS)1(W)n 的反应活性,而加入 H2O 分子则会降低簇(SS)1(SA)n 的反应活性。然而,在现有的簇 (SS)1(W)n(SA)n 中进一步添加 H2SO4 或 H2O 会增加形成的自由能。此外,我们还研究了温度的影响,结果表明,低温比高温更有利于络合物的形成。热力学参数的负值表明,这些络合物是自发形成的,在较冷区域会放热。
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Computational Study of the Formation of Atmospheric Aerosol Precursors Under Ambient Conditions: A Case Study of the Interaction Between Sea Salt, Water, and Sulfuric Acid Molecules

Cluster formation has significant implications in atmospheric science and environmental chemistry. These clusters are characterized by complex interactions between their constituents, which influence their structure, stability, and growth. Experimental investigations are difficult for the initial stages of prenucleation cluster formation, which leads to larger aerosols. To understand the formation of clusters, the interactions between sea salts (NaCl, KCl, and MgCl2), water, and sulfuric acid molecules have been investigated. Each step has been comprehensively examined and thermodynamic parameters have been computed using DLPNO-CCSD(T)/CBS//M06-2X/6-311++G(3df,3pd) to find the stabilities of the molecular complexes. Among all complexes, the binding energies of cluster (SS)1(W)1(SA)3 are found to be the lowest due to the formation of HCl, hydrogen bonding, and weak van der Waal forces. Sea salts have shown a more favorable interaction with H2SO4 compared to H2O molecules. The addition of H2SO4 increases the reactivity of the cluster (SS)1(W)n, while the addition of H2O molecules reduces the reactivity of the cluster (SS)1(SA)n. However, further addition of H2SO4 or H2O to the existing cluster (SS)1(W)n(SA)n increases the free energy of formation. Furthermore, the influence of temperature was also investigated, suggesting that complex formation is slightly more favorable at lower temperatures than at higher temperatures. The negative values of thermodynamic parameters indicate, that these complexes are spontaneous and exothermic over the colder regions.

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来源期刊
International Journal of Quantum Chemistry
International Journal of Quantum Chemistry 化学-数学跨学科应用
CiteScore
4.70
自引率
4.50%
发文量
185
审稿时长
2 months
期刊介绍: Since its first formulation quantum chemistry has provided the conceptual and terminological framework necessary to understand atoms, molecules and the condensed matter. Over the past decades synergistic advances in the methodological developments, software and hardware have transformed quantum chemistry in a truly interdisciplinary science that has expanded beyond its traditional core of molecular sciences to fields as diverse as chemistry and catalysis, biophysics, nanotechnology and material science.
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