Molecular Chirality and Cloud Activation Potentials of Dimeric α-Pinene Oxidation Products

Molecular Chirality and Cloud Activation Potentials of Dimeric α-Pinene Oxidation Products
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DOI:
10.1021/jacs.1c07509
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发表时间:
2021-10-04
影响因子:
15
通讯作者:
Thomson, Regan J.
Thomson, Regan J.
中科院分区:
化学1区
文献类型:
--
作者:
Bellcross, Aleia;Be, Ariana Gray;Thomson, Regan J.

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报道了具有不同末端官能团和主链立体化学的十种大气相关α-蒎烯衍生的二聚体的表面活性。我们发现类似的非对映异构体的相同的二聚体之间的表面活性的差异为10%,表明表面活性取决于骨干立体化学。我们的标准品的辛醇-水(K-OW)和辛醇-硫酸铵分配系数(K-OAS)测量结果与表面活性测量结果一致,表面活性更高的二聚体表现出更高的疏水性。我们的研究结果建立了二次有机气溶胶粒子的分子手性和云激活潜力之间的联系。考虑到生物源排放物的对映体过量的日变化,这种联系对生物圈的可能贡献:大气反馈以及气溶胶粒子粘度和相分离进行了讨论。
The surface activity of ten atmospherically relevant a-pinene-derived dimers having varying terminal functional groups and backbone stereochemistry is reported. We find similar to 10% differences in surface activity between diastereomers of the same dimer, demonstrating that surface activity depends upon backbone stereochemistry. Octanol-water (K-OW) and octanol-ammonium sulfate partitioning coefficient (K-OAS) measurements of our standards align well with the surface activity measurements, with the more surface-active dimers exhibiting increased hydrophobicity. Our findings establish a link between molecular chirality and cloud activation potential of secondary organic aerosol particles. Given the diurnal variations in enantiomeric excess of biogenic emissions, possible contributions of such a link to biosphere:atmosphere feedbacks as well as aerosol particle viscosity and phase separation are discussed.