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Title: Importance of interlayer H bonding structure to the stability of layered minerals

Journal Article · · Scientific Reports
 [1];  [2];  [3];  [1];  [1];  [2];  [2];  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy and Environment Directorate
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical and Computational Sciences Directorate
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). National Security Directorate

The exact atomic structures of layered minerals have been difficult to characterize because the layers often possess out-of-plane hydrogen atoms that cannot be detected by many analytical techniques. However, the ordering of these bonds are thought to play a fundamental role in the structural stability and solubility of layered minerals. We report a new strategy of using the intense radiation field of a focused electron beam to probe the effect of differences in hydrogen bonding networks on mineral solubility while simultaneously imaging the dissolution behavior in real time via liquid cell electron microscopy. We show the loss in hydrogens from interlayers of boehmite (?-AlOOH) resulted in 2D nanosheets exfoliating from the bulk that subsequently and rapidly dissolved. However gibbsite (?-Al(OH)3), with its higher concentration of OH terminating groups, was more accommodating to the deprotonation and stable under the beam.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5); USDOE Office of Science (SC), Biological and Environmental Research (BER); PNNL Laboratory Directed Research and Development (LDRD) Program
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
1430728
Alternate ID(s):
OSTI ID: 1512401
Report Number(s):
PNNL-SA-126728; PII: 13452
Journal Information:
Scientific Reports, Vol. 7; ISSN 2045-2322
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 36 works
Citation information provided by
Web of Science

References (58)

Optimized hydrogen positions for aluminium and iron containing hydroxide minerals journal February 2007
Vibrational Spectroscopy and Dehydroxylation of Aluminum (Oxo)Hydroxides: Gibbsite journal April 1999
Boehmite Dissolution Model Based on Simulant Data journal May 2010
Structural controls on OH site availability and reactivity at iron oxyhydroxide particle surfaces journal January 2012
Simulations of H2O2 concentration profiles in the water surrounding spent nuclear fuel journal January 2008
The formation of cerium( iii ) hydroxide nanoparticles by a radiation mediated increase in local pH journal January 2017
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides journal September 1976
New Mechanism for H 2 Formation in Water journal November 2000
Assignment of the structural OH stretching bands of gibbsite journal May 2000
Radiolytic hydrogen generation from aluminum oxyhydroxide solids: theory and experiment journal November 2014
A glance into aluminum toxicity and resistance in plants journal August 2008
Optical modulators with 2D layered materials journal March 2016
Transmission Electron Microscopy book January 1996
Electron beam damage studies of synthetic 6-line ferrihydrite and ferritin molecule cores within a human liver biopsy journal July 2006
The Effect of Geological Parameters on Radiation Damage in Rock Salt: Application to Rock Salt Repositories journal June 1996
Molecular cluster models of aluminum oxide and aluminum hydroxide surfaces journal October 1998
Aluminium Toxicity in Roots: An Investigation of Spatial Sensitivity and the Role of the Root Cap journal January 1993
Solubility of boehmite in concentrated sodium hydroxide solutions: model development and assessment journal January 2001
Dissolution of gibbsite: Direct observations using fluid cell atomic force microscopy journal January 2003
Electron–Water Interactions and Implications for Liquid Cell Electron Microscopy journal September 2014
Desorption of Nitric Acid From Boehmite and Gibbsite journal July 2008
Kinetics of Self-Trapped Holes in Alkali-Halide Crystals: Experiments in NaI(Tl) and KI(Tl) journal December 1973
Two-Dimensional Nanosheets Produced by Liquid Exfoliation of Layered Materials journal February 2011
Transmission Electron Microscopy book January 2009
An ab Initio Study of the Structure and Properties of Aluminum Hydroxide:  Gibbsite and Bayerite journal October 2001
Structure and Stability of Aluminum Hydroxides:  A Theoretical Study journal May 2002
Dissolution/precipitation kinetics of boehmite and gibbsite: Application of a pH-relaxation technique to study near-equilibrium rates journal May 2008
Aluminium cycling in the soil-plant-animal-human continuum journal November 2004
Leaching behaviour of high surface area synthetic boehmite in NaOH solution journal May 2013
Modeling the Sodium Recovery Resulting from Using Concentrated Caustic for Boehmite Dissolution journal October 2011
Aluminum enhances inflammation and decreases mucosal healing in experimental colitis in mice text January 2014
Structure and stability of aluminium trihydroxides bayerite and gibbsite: A quantum mechanical ab initio study with the Crystal06 code journal November 2008
Conditions for Critical Effects in the Mass Action Kinetics Equations for Water Radiolysis journal October 2014
Aluminum enhances inflammation and decreases mucosal healing in experimental colitis in mice journal October 2013
Luminescence Database I—Minerals and Materials journal March 2008
Gibbsite Solubility in Hanford Nuclear Waste Approached from above and below Saturation journal May 2016
Dehydroxylation of Aluminum (Oxo)Hydroxides Using Infrared Emission Spectroscopy. Part II: Boehmite journal May 1999
Study of the Formation Mechanism of Boehmite with Different Morphology upon Surface Hydroxyls and Adsorption of Chloride Ions journal July 2013
Radiolytic Events in Nanostructured Aluminum Hydroxides journal March 2017
The prediction of nuclear fuel (UO2) dissolution rates under waste disposal conditions journal August 1992
Aluminium-induced reduction of plant growth in alfalfa (Medicago sativa) is mediated by interrupting auxin transport and accumulation in roots journal July 2016
Wide Band Gap Scintillation Materials: Progress in the Technology and Material Understanding journal April 2000
Uranyl interaction with the hydrated (001) basal face of gibbsite: A combined theoretical and spectroscopic study journal December 2008
Liquid Exfoliation of Layered Materials journal June 2013
Electron microscopy of specimens in liquid journal October 2011
Dehydroxylation sequences of gibbsite and boehmite: study of differences between soak and flash calcination and of particle-size effects journal January 1996
Theoretical studies on the reaction mechanisms of AlOOH- and γ-Al2O3-catalysed methanol dehydration in the gas and liquid phases journal November 2011
Aluminum speciation and equilibria in aqueous solution: I. The solubility of gibbsite in the system Na-K-Cl-OH-Al(OH)4 from 0 to 100°C journal March 1992
Mechanisms of radiation damage in beam-sensitive specimens, for TEM accelerating voltages between 10 and 300 kV journal July 2012
Transition alumina phases induced by heat treatment of boehmite: An X-ray diffraction and infrared spectroscopy study journal May 2009
Choice of operating voltage for a transmission electron microscope journal October 2014
Can Cr( iii ) substitute for Al( iii ) in the structure of boehmite? journal January 2016
One-dimensional nanowires of pseudoboehmite (aluminum oxyhydroxide γ-AlOOH) journal October 2016
Erratum to Wide Band Gap Scintillation Materials: Progress in the Technology and Material Understanding journal August 2000
Hydrogen bonds and local symmetry in the crystal structure of gibbsite journal September 2010
Factors influencing quantitative liquid (scanning) transmission electron microscopy journal January 2014
EMAG–NANO 2005: Imaging, Analysis and Fabrication on the Nanoscale journal January 2006
Oxidation of UO2 fuel by the products of gamma radiolysis of water journal August 1992

Cited By (4)

Electron irradiation induced amorphous SiO2 formation at metal oxide/Si interface at room temperature; electron beam writing on interfaces journal February 2018
Intensive study on structure transformation of muscovite single crystal under high-dose γ -ray irradiation and mechanism speculation journal July 2019
Improving in situ liquid SEM imaging of particles journal September 2019
Electronic response of aluminum-bearing minerals journal July 2018

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