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“双亚稳”水中空化和冰核形成的研究:延时摄影和中子衍射。

Studies of cavitation and ice nucleation in 'doubly-metastable' water: time-lapse photography and neutron diffraction.

机构信息

College of Engineering, Swansea University, Swansea SA2 8PP, UK.

出版信息

Phys Chem Chem Phys. 2012 Oct 14;14(38):13255-61. doi: 10.1039/c2cp41925d.

Abstract

High-speed photographic studies and neutron diffraction measurements have been made of water under tension in a Berthelot tube. Liquid water was cooled below the normal ice-nucleation temperature and was in a doubly-metastable state prior to a collapse of the liquid state. This transition was accompanied by an exothermic heat release corresponding with the rapid production of a solid phase nucleated by cavitation. Photographic techniques have been used to observe the phase transition over short time scales in which a solidification front is observed to propagate through the sample. Significantly, other images at a shorter time interval reveal the prior formation of cavitation bubbles at the beginning of the process. The ice-nucleation process is explained in terms of a mechanism involving hydrodynamically-induced changes in tension in supercooled water in the near vicinity of an expanding cavitation bubble. Previous explanations have attributed the nucleation of the solid phase to the production of high positive pressures. Corresponding results are presented which show the initial neutron diffraction pattern after ice-nucleation. The observed pattern does not exhibit the usual crystalline pattern of hexagonal ice [I(h)] that is formed under ambient conditions, but indicates the presence of other ice forms. The composite features can be attributed to a mixture of amorphous ice, ice-I(h)/I(c) and the high-pressure form, ice-III, and the diffraction pattern continues to evolve over a time period of about an hour.

摘要

高速摄影研究和中子衍射测量已经在 Berthelot 管中对拉伸状态下的水进行了研究。在液体状态崩溃之前,将液态水冷却到正常冰成核温度以下,并处于双亚稳状态。这种转变伴随着放热释放,伴随着空化快速产生的固相的成核。摄影技术已被用于在短时间尺度内观察相变,在该时间尺度内,可以观察到凝固前沿通过样品传播。重要的是,在较短的时间间隔内的其他图像显示出在该过程开始时先前形成的空化气泡。冰成核过程是根据涉及在接近膨胀空化气泡的过冷水中的张力的水力诱导变化的机制来解释的。以前的解释将固相的成核归因于高压的产生。呈现了相应的结果,显示了冰成核后的初始中子衍射图案。观察到的图案不表现出在环境条件下形成的六方冰[I(h)]的通常结晶图案,而是表明存在其他冰形式。复合特征可归因于无定形冰、冰-I(h)/I(c)和高压形式冰-III 的混合物,并且衍射图案在大约一个小时的时间段内继续演变。

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