DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · Nature Communications
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)

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.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Swiss National Science Foundation (SNSF)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1606894
Journal Information:
Nature Communications, Vol. 10, Issue 1; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 66 works
Citation information provided by
Web of Science

References (66)

First developments towards closing the nutrient cycle in a biofuel production process journal March 2015
Water adsorption in carbons described by the dubinin–astakhov and dubinin–serpinski equations journal January 1994
Surface Tension and Molecular Correlations near the Critical Point journal December 1965
Relation between the Widom line and the dynamic crossover in systems with a liquid-liquid phase transition journal November 2005
Widom Delta of Supercritical Gas–Liquid Coexistence journal March 2018
Biofuels Production by Biomass Gasification: A Review journal March 2018
Kinetically Forbidden Transformations of Water Molecular Assemblies in Hydrophobic Micropores journal June 2011
Thermochemical biofuel production in hydrothermal media: A review of sub- and supercritical water technologies journal January 2008
The ICON beamline – A facility for cold neutron imaging at SINQ
  • Kaestner, A. P.; Hartmann, S.; Kühne, G.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 659, Issue 1 https://doi.org/10.1016/j.nima.2011.08.022
journal December 2011
One-dimensional tomography: a comparison of Abel, onion-peeling, and filtered backprojection methods journal January 1992
Frame overlap Bragg edge imaging journal September 2020
Thermochemical biofuel production in hydrothermal media: A review of sub- and supercritical water technologies journal January 2008
Kinetically Forbidden Transformations of Water Molecular Assemblies in Hydrophobic Micropores journal June 2011
The Potential Theory of Adsorption of Gases and Vapors for Adsorbents with Energetically Nonuniform Surfaces. journal April 1960
Supercritical Water as a Solvent journal August 2005
Widom delta of supercritical gas-liquid coexistence text January 2018
Equation of State in the Neighborhood of the Critical Point journal December 1965
Surface Tension and Molecular Correlations near the Critical Point journal December 1965
Water adsorption in active carbons described by the Dubinin–Astakhov equation journal January 1994
Supercritical water gasification journal September 2008
Mechanism of heterogeneous adsorption in the storage of hydrogen in carbon fibers activated with supercritical water and steam journal July 2011
Organic Chemical Reactions in Supercritical Water journal February 1999
Treatment of municipal sewage sludge in supercritical water: A review journal February 2016
Understanding biomass fractionation in subcritical & supercritical water journal March 2018
The IAPWS Formulation 1995 for the Thermodynamic Properties of Ordinary Water Substance for General and Scientific Use journal June 2002
Chasing quantitative biases in neutron imaging with scintillator-camera detectors: a practical method with black body grids journal January 2018
Membrane distillation: Perspectives for sustainable and improved desalination journal December 2017
Structural mechanism of water adsorption in hydrophobic micropores from in situ small angle X-ray scattering journal December 2000
The Widom line as the crossover between liquid-like and gas-like behaviour in supercritical fluids journal June 2010
Production methods for nanodrug particles using the bottom-up approach journal May 2011
Production methods for nanodrug particles using the bottom-up approach journal May 2011
Total Neutron Cross Section of Water journal August 1968
Green materials synthesis with supercritical water journal January 2011
Geologic controls on supercritical geothermal resources above magmatic intrusions journal July 2015
A novel process and material for the separation of carbon dioxide and hydrogen sulfide gas mixtures journal January 1997
Neutron radiography and numerical simulation of mixing behavior in a reactor for supercritical hydrothermal synthesis journal December 2013
Properties of the Radiography Facility Neutra at sinq and its Potential for use as European Reference Facility journal January 2001
Equilibration-time and pore-width dependent hysteresis of water adsorption isotherm on hydrophobic microporous carbons journal January 2010
Widom line and dynamical crossovers as routes to understand supercritical water journal December 2014
Going supercritical journal July 2010
Going supercritical journal July 2010
Equilibration-time and pore-width dependent hysteresis of water adsorption isotherm on hydrophobic microporous carbons journal January 2010
Neutron radiography and numerical simulation of mixing behavior in a reactor for supercritical hydrothermal synthesis journal December 2013
Clustering of water molecules in ultramicroporous carbon: In-situ small-angle neutron scattering journal January 2017
Properties of the Radiography Facility Neutra at sinq and its Potential for use as European Reference Facility journal January 2001
Widom line and dynamical crossovers as routes to understand supercritical water journal December 2014
Green materials synthesis with supercritical water journal January 2011
Membrane distillation: Perspectives for sustainable and improved desalination journal December 2017
Supercritical water gasification journal September 2008
Understanding biomass fractionation in subcritical & supercritical water journal March 2018
Similarity law for Widom lines and coexistence lines journal May 2017
Seven questions about supercritical fluids - towards a new fluid state diagram conference January 2017
Supercritical water gasification of biomass for hydrogen production – Review journal March 2018
Steam tables for pure water as an ActiveX component in Visual Basic 6.0 journal November 2003
Geologic controls on supercritical geothermal resources above magmatic intrusions text January 2015
The Widom line as the crossover between liquid-like and gas-like behaviour in supercritical fluids journal June 2010
Crossing the Widom-line – Supercritical pseudo-boiling journal March 2015
Supercritical water gasification of biomass for hydrogen production – Review journal March 2018
Widom delta of supercritical gas-liquid coexistence text January 2018
The IAPWS Formulation 1995 for the Thermodynamic Properties of Ordinary Water Substance for General and Scientific Use journal June 2002
Supercritical Water as a Solvent journal April 2005
Organic Chemical Reactions in Supercritical Water journal February 1999
Applications of subcritical and supercritical water conditions for extraction, hydrolysis, gasification, and carbonization of biomass: a critical review journal June 2017
First developments towards closing the nutrient cycle in a biofuel production process journal March 2015
The Potential Theory of Adsorption of Gases and Vapors for Adsorbents with Energetically Nonuniform Surfaces. journal April 1960
Dual Spectrum Neutron Radiography: Identification of Phase Transitions between Frozen and Liquid Water journal June 2014

Cited By (1)

The use of process simulation in supercritical fluids applications journal January 2020