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Title: Visualization of supercritical water pseudo-boiling at Widom line crossover

Abstract

Supercritical water is a green solvent used in many technological applications including materials synthesis, nuclear engineering, bioenergy, or waste treatment and it occurs in nature. Despite its relevance in natural systems and technical applications, the supercritical state of water is still not well understood. Recent theories predict that liquid-like (LL) and gas-like (GL) supercritical water are metastable phases, and that the so-called Widom line zone is marking the crossover between LL and GL behavior of water. With neutron imaging techniques, we succeed to monitor density fluctuations of supercritical water while the system evolves rapidly from LL to GL as the Widom line is crossed during isobaric heating. Our observations show that the Widom line of water can be identified experimentally and they are in agreement with the current theory of supercritical fluid pseudo-boiling. This fundamental understanding allows optimizing and developing new technologies using supercritical water as a solvent.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [4]; ORCiD logo [5]; ORCiD logo [6]; ORCiD logo [7]
  1. Paul Scherrer Inst. (PSI), Villigen (Switzerland). Lab. for Bioenergy and Catalysis (LBK), ENE Division; Inst. of Physical Chemistry "Ilie Murgulescu", Bucharest, (Romania)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  3. Paul Scherrer Inst. (PSI), Villigen (Switzerland). Electrochemistry Lab. (LEC), ENE Division, and Lab. for Neutron Scattering and Imaging (LNS), NUM Division
  4. Paul Scherrer Inst. (PSI), Villigen (Switzerland). Lab. for Scientific Computing and Modelling (LSM), NES Division; Federal Inst. of Technology, Zurich (Switzerland)
  5. Paul Scherrer Inst. (PSI), Villigen (Switzerland). Lab. for Scientific Computing and Modelling (LSM), NES Division
  6. Paul Scherrer Inst. (PSI), Villigen (Switzerland). Lab. for Bioenergy and Catalysis (LBK), ENE Division
  7. Paul Scherrer Inst. (PSI), Villigen (Switzerland). Lab. for Bioenergy and Catalysis (LBK), ENE Division; Ecole Polytechnique Federale Lausanne (Switzlerland)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Swiss National Science Foundation (SNSF)
OSTI Identifier:
1606894
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Maxim, Florentina, Contescu, Cristian, Boillat, Pierre, Niceno, Bojan, Karalis, Konstantinos, Testino, Andrea, and Ludwig, Christian. Visualization of supercritical water pseudo-boiling at Widom line crossover. United States: N. p., 2019. Web. https://doi.org/10.1038/s41467-019-12117-5.
Maxim, Florentina, Contescu, Cristian, Boillat, Pierre, Niceno, Bojan, Karalis, Konstantinos, Testino, Andrea, & Ludwig, Christian. Visualization of supercritical water pseudo-boiling at Widom line crossover. United States. https://doi.org/10.1038/s41467-019-12117-5
Maxim, Florentina, Contescu, Cristian, Boillat, Pierre, Niceno, Bojan, Karalis, Konstantinos, Testino, Andrea, and Ludwig, Christian. Tue . "Visualization of supercritical water pseudo-boiling at Widom line crossover". United States. https://doi.org/10.1038/s41467-019-12117-5. https://www.osti.gov/servlets/purl/1606894.
@article{osti_1606894,
title = {Visualization of supercritical water pseudo-boiling at Widom line crossover},
author = {Maxim, Florentina and Contescu, Cristian and Boillat, Pierre and Niceno, Bojan and Karalis, Konstantinos and Testino, Andrea and Ludwig, Christian},
abstractNote = {Supercritical water is a green solvent used in many technological applications including materials synthesis, nuclear engineering, bioenergy, or waste treatment and it occurs in nature. Despite its relevance in natural systems and technical applications, the supercritical state of water is still not well understood. Recent theories predict that liquid-like (LL) and gas-like (GL) supercritical water are metastable phases, and that the so-called Widom line zone is marking the crossover between LL and GL behavior of water. With neutron imaging techniques, we succeed to monitor density fluctuations of supercritical water while the system evolves rapidly from LL to GL as the Widom line is crossed during isobaric heating. Our observations show that the Widom line of water can be identified experimentally and they are in agreement with the current theory of supercritical fluid pseudo-boiling. This fundamental understanding allows optimizing and developing new technologies using supercritical water as a solvent.},
doi = {10.1038/s41467-019-12117-5},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {9}
}

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    Works referencing / citing this record:

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