期刊
CHEMICAL SCIENCE
卷 12, 期 1, 页码 -出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0sc04817h
关键词
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资金
- National Research Foundation of Korea [NRF-2014M3C1A8048818, NRF-2014M1A01030128, NRF-2019K1A3A7A09033397]
- Ministry of Science and ICT (MSIT)
- Korea Research Institute of Standards and Science [KRISS-2017-GP2017-0029]
- National Research Foundation of Korea [2019K1A3A7A09033397, 2014M3C1A8048818] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
Experimental evidence indicates the formation of dense liquid regions in NaCl bulk solution at unprecedentedly high levels of supersaturation, providing new insights into the detailed mechanism of two-step nucleation for many other aqueous solutions. The evolution of solute clusters and breakage of hydration in highly supersaturated conditions were observed, leading to a better understanding of the early stages of nucleation.
For over two decades, NaCl nucleation from a supersaturated aqueous solution has been predicted to occur via a two-step nucleation (TSN) mechanism, i.e., two sequential events, the formation of locally dense liquid regions followed by structural ordering. However, the formation of dense liquid regions in the very early stage of TSN has never been experimentally observed. By using a state-of-the-art technique, a combination of electrostatic levitation (ESL) and in situ synchrotron X-ray and Raman scatterings, we find experimental evidence that indicates the formation of dense liquid regions in NaCl bulk solution at an unprecedentedly high level of supersaturation (S = 2.31). As supersaturation increases, evolution of ion clusters leads to chemical ordering, but no topological ordering, which is a precursor for forming the dense disordered regions of ion clusters at the early stage of TSN. Moreover, as the ion clusters proceed to evolve under highly supersaturated conditions, we observe the breakage of the water hydration structure indicating the stability limit of the dense liquid regions, and thus leading to nucleation. The evolution of solute clusters and breakage of hydration in highly supersaturated NaCl bulk solution will provide new insights into the detailed mechanism of TSN for many other aqueous solutions.
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