Max Planck Institute for Dynamics and Self-Organization , Am Fassberg, 37077 Göttingen, Germany.
ACS Nano. 2017 Dec 26;11(12):12723-12731. doi: 10.1021/acsnano.7b07472. Epub 2017 Nov 10.
The classic regelation experiment of Thomson in the 1850s deals with cutting an ice cube, followed by refreezing. The cutting was attributed to pressure-induced melting but has been challenged continuously, and only lately consensus emerged by understanding that compression shortens the O:H nonbond and lengthens the H-O bond simultaneously. This H-O elongation leads to energy loss and lowers the melting point. The hot debate survived well over 150 years, mainly due to a poorly defined heat exchange with the environment in the experiment. In our current experiment, we achieved thermal isolation from the environment and studied the fully reversible ice-liquid water transition for water confined between graphene and muscovite mica. We observe a transition from two-dimensional (2D) ice into a quasi-liquid phase by applying a pressure exerted by an atomic force microscopy tip. At room temperature, the critical pressure amounts to about 6 GPa. The transition is completely reversible: refreezing occurs when the applied pressure is lifted. The critical pressure to melt the 2D ice decreases with temperature, and we measured the phase coexistence line between 293 and 333 K. From a Clausius-Clapeyron analysis, we determine the latent heat of fusion of two-dimensional ice at 0.15 eV/molecule, being twice as large as that of bulk ice.
20 世纪 50 年代,汤姆森进行了经典的规则分割实验,涉及切割冰块,然后重新冻结。切割归因于压力诱导的熔化,但一直受到质疑,直到最近才通过理解压缩同时缩短 O:H 非键和延长 H-O 键而达成共识。这种 H-O 伸长导致能量损失并降低熔点。这个激烈的争论持续了 150 多年,主要是由于实验中与环境的热交换定义不明确。在我们目前的实验中,我们实现了与环境的热隔离,并研究了在石墨烯和白云母之间受限的水的完全可逆的冰-液态水转变。我们通过施加原子力显微镜针尖施加的压力观察到二维(2D)冰向准液相的转变。在室温下,临界压力约为 6 GPa。该转变是完全可逆的:当施加的压力被解除时,重新冻结发生。二维冰的熔融临界压力随温度而降低,我们测量了 293 到 333 K 之间的相共存线。通过克劳修斯-克拉佩龙分析,我们确定了二维冰的熔融潜热为 0.15 eV/分子,是块状冰的两倍。