Tuning ice nucleation with counterions on polyelectrolyte brush surfaces.

Tuning ice nucleation with counterions on polyelectrolyte brush surfaces.
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DOI:
10.1126/sciadv.1600345
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发表时间:
2016-06
期刊:
影响因子:
13.6
通讯作者:
Wang J
Wang J
中科院分区:
综合性期刊1区
文献类型:
--
作者:
He Z;Xie WJ;Liu Z;Liu G;Wang Z;Gao YQ;Wang J

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这项工作是第一次表明,在离子表面上调整HIN的离子特异性如下霍夫迈斯特系列。离子表面上的非均质冰核(HIN)普遍存在于大范围的大气气溶胶和生物界面中。尽管它在卷云形成和细胞、器官和组织的冷冻保存中非常重要,但尚不清楚离子对冰成核的特定影响是否存在。受益于离子在刷(PB)/水界面上可以可逆交换的事实,我们报道了离子对PB表面HIN的影响,并且我们发现离子在调节HIN中的显著效率遵循Hofmeister系列。此外,还展示了高达7.8°C的大HIN温度窗口。通过建立冰状水分子的分数之间的相关性和动力学的结构转换从液体到冰状水分子在PB/水界面与不同的抗衡离子,我们表明,我们的分子动力学模拟分析是一致的实验观察的离子特异性HIN的效果。
This work is the first to show that the ion specificity in tuning HIN on ionic surfaces follows the Hofmeister series. Heterogeneous ice nucleation (HIN) on ionic surfaces is ubiquitous in a wide range of atmospheric aerosols and at biological interfaces. Despite its great importance in cirrus cloud formation and cryopreservation of cells, organs, and tissues, it remains unclear whether the ion-specific effect on ice nucleation exists. Benefiting from the fact that ions at the polyelectrolyte brush (PB)/water interface can be reversibly exchanged, we report the effect of ions on HIN on the PB surface, and we discover that the distinct efficiency of ions in tuning HIN follows the Hofmeister series. Moreover, a large HIN temperature window of up to 7.8°C is demonstrated. By establishing a correlation between the fraction of ice-like water molecules and the kinetics of structural transformation from liquid- to ice-like water molecules at the PB/water interface with different counterions, we show that our molecular dynamics simulation analysis is consistent with the experimental observation of the ion-specific effect on HIN.