Particle arrangements in clay slurries: The case against the honeycomb structure

Amer Deirieh; Irene Y. Chang; Michael L. Whittaker; Steven Weigand; Denis Keane; James Rix; John T. Germaine; Derk Joester; Peter B. Flemings

doi:10.1016/j.clay.2017.11.010

Particle arrangements in clay slurries: The case against the honeycomb structure

Amer Deirieh^*, Irene Y. Chang, Michael L. Whittaker, Steven Weigand, Denis Keane, James Rix, John T. Germaine, Derk Joester, Peter B. Flemings

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

34 Scopus citations

Abstract

The properties of clay slurries (porosity ~ 0.75) impact a wide range of materials such as commercial clay dispersions and sedimentary deposits. Their material behavior, and in particular the gelation of clay slurries, is thought to be governed by clay particle interactions. In the literature, such interactions are rarely directly probed, but rather inferred from structures observed by cryo-electron microscopy. For example, the honeycomb structure is a widely accepted textbook model that is used to rationalize the observed behavior of clay slurries. Using high-pressure freezing, cryo-electron microscopy, and cryo-synchrotron wide-angle X-ray scattering, this study shows that the honeycomb-structure is an artifact of sample preparation. When samples are high-pressure frozen, individual clay particles and aggregates of particles arrange in a random orientation rather than the closed-cell structure dominated by face-face and face-edge contacts observed in plunge frozen samples. These results substantially contribute to the understanding of the gelation mechanism and particle interactions in colloidal clay slurries, and provide valuable input parameters for meso-scale modeling efforts of clay dispersions and sedimentary deposits to upscale their mechanical properties to the macroscale.

Original language	English (US)
Pages (from-to)	166-172
Number of pages	7
Journal	Applied Clay Science
Volume	152
DOIs	https://doi.org/10.1016/j.clay.2017.11.010
State	Published - Feb 2018

Funding

Shell, the UT GeoFluids consortium at the University of Texas at Austin , the NSF ( MRI-1229693 ), the Northwestern University Materials Research Center ( NSF DMR-1121262 ), and the International Institute for Nanotechnology (IIN) in part supported this work. Part of this work was performed at the Center for Nanoscale Systems (CNS) at Harvard University, a member of the National Nanotechnology Infrastructure Network (NNIN) supported by the National Science Foundation ( ECS-0335765 ), and at NUANCE-EPIC and OMM, Northwestern University core facilities that are supported by the MRSEC Program ( NSF DMR-1121262 ) at the Materials Research Center. EPIC (NUANCE Center- Northwestern University ), further received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource ( NSF NNCI-1542205 ); the International Institute for Nanotechnology (IIN); and the State of Illinois, through the IIN. We thank Adam Graham at CNS for technical assistance. Part of this work was performed at the DuPont-Northwestern-Dow Collaborative Access Team (DND-CAT) located at Sector 5 of the Advanced Photon Source (APS). DND-CAT is supported by Northwestern University, E.I. DuPont de Nemours & Co., and The Dow Chemical Company. The APS is operated by Argonne National Laboratory under Contract No. DE-AC02-06CH11357.

Keywords

Clay colloids
Clay microstructure
Cryo SEM imaging
High pressure freezing
Honeycomb structure
Illite-Smectite
Plunge freezing

ASJC Scopus subject areas

Water Science and Technology
Soil Science
Geology
Geochemistry and Petrology

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10.1016/j.clay.2017.11.010

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@article{0bcc369d284543ccafca580cb94b2b40,

title = "Particle arrangements in clay slurries: The case against the honeycomb structure",

abstract = "The properties of clay slurries (porosity ~ 0.75) impact a wide range of materials such as commercial clay dispersions and sedimentary deposits. Their material behavior, and in particular the gelation of clay slurries, is thought to be governed by clay particle interactions. In the literature, such interactions are rarely directly probed, but rather inferred from structures observed by cryo-electron microscopy. For example, the honeycomb structure is a widely accepted textbook model that is used to rationalize the observed behavior of clay slurries. Using high-pressure freezing, cryo-electron microscopy, and cryo-synchrotron wide-angle X-ray scattering, this study shows that the honeycomb-structure is an artifact of sample preparation. When samples are high-pressure frozen, individual clay particles and aggregates of particles arrange in a random orientation rather than the closed-cell structure dominated by face-face and face-edge contacts observed in plunge frozen samples. These results substantially contribute to the understanding of the gelation mechanism and particle interactions in colloidal clay slurries, and provide valuable input parameters for meso-scale modeling efforts of clay dispersions and sedimentary deposits to upscale their mechanical properties to the macroscale.",

keywords = "Clay colloids, Clay microstructure, Cryo SEM imaging, High pressure freezing, Honeycomb structure, Illite-Smectite, Plunge freezing",

author = "Amer Deirieh and Chang, {Irene Y.} and Whittaker, {Michael L.} and Steven Weigand and Denis Keane and James Rix and Germaine, {John T.} and Derk Joester and Flemings, {Peter B.}",

note = "Funding Information: Shell, the UT GeoFluids consortium at the University of Texas at Austin , the NSF ( MRI-1229693 ), the Northwestern University Materials Research Center ( NSF DMR-1121262 ), and the International Institute for Nanotechnology (IIN) in part supported this work. Part of this work was performed at the Center for Nanoscale Systems (CNS) at Harvard University, a member of the National Nanotechnology Infrastructure Network (NNIN) supported by the National Science Foundation ( ECS-0335765 ), and at NUANCE-EPIC and OMM, Northwestern University core facilities that are supported by the MRSEC Program ( NSF DMR-1121262 ) at the Materials Research Center. EPIC (NUANCE Center- Northwestern University ), further received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource ( NSF NNCI-1542205 ); the International Institute for Nanotechnology (IIN); and the State of Illinois, through the IIN. We thank Adam Graham at CNS for technical assistance. Part of this work was performed at the DuPont-Northwestern-Dow Collaborative Access Team (DND-CAT) located at Sector 5 of the Advanced Photon Source (APS). DND-CAT is supported by Northwestern University, E.I. DuPont de Nemours & Co., and The Dow Chemical Company. The APS is operated by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Publisher Copyright: {\textcopyright} 2017 Elsevier B.V.",

year = "2018",

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doi = "10.1016/j.clay.2017.11.010",

language = "English (US)",

volume = "152",

pages = "166--172",

journal = "Applied Clay Science",

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T2 - The case against the honeycomb structure

AU - Deirieh, Amer

AU - Chang, Irene Y.

AU - Whittaker, Michael L.

AU - Weigand, Steven

AU - Keane, Denis

AU - Rix, James

AU - Germaine, John T.

AU - Joester, Derk

AU - Flemings, Peter B.

N1 - Funding Information: Shell, the UT GeoFluids consortium at the University of Texas at Austin , the NSF ( MRI-1229693 ), the Northwestern University Materials Research Center ( NSF DMR-1121262 ), and the International Institute for Nanotechnology (IIN) in part supported this work. Part of this work was performed at the Center for Nanoscale Systems (CNS) at Harvard University, a member of the National Nanotechnology Infrastructure Network (NNIN) supported by the National Science Foundation ( ECS-0335765 ), and at NUANCE-EPIC and OMM, Northwestern University core facilities that are supported by the MRSEC Program ( NSF DMR-1121262 ) at the Materials Research Center. EPIC (NUANCE Center- Northwestern University ), further received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource ( NSF NNCI-1542205 ); the International Institute for Nanotechnology (IIN); and the State of Illinois, through the IIN. We thank Adam Graham at CNS for technical assistance. Part of this work was performed at the DuPont-Northwestern-Dow Collaborative Access Team (DND-CAT) located at Sector 5 of the Advanced Photon Source (APS). DND-CAT is supported by Northwestern University, E.I. DuPont de Nemours & Co., and The Dow Chemical Company. The APS is operated by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Publisher Copyright: © 2017 Elsevier B.V.

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N2 - The properties of clay slurries (porosity ~ 0.75) impact a wide range of materials such as commercial clay dispersions and sedimentary deposits. Their material behavior, and in particular the gelation of clay slurries, is thought to be governed by clay particle interactions. In the literature, such interactions are rarely directly probed, but rather inferred from structures observed by cryo-electron microscopy. For example, the honeycomb structure is a widely accepted textbook model that is used to rationalize the observed behavior of clay slurries. Using high-pressure freezing, cryo-electron microscopy, and cryo-synchrotron wide-angle X-ray scattering, this study shows that the honeycomb-structure is an artifact of sample preparation. When samples are high-pressure frozen, individual clay particles and aggregates of particles arrange in a random orientation rather than the closed-cell structure dominated by face-face and face-edge contacts observed in plunge frozen samples. These results substantially contribute to the understanding of the gelation mechanism and particle interactions in colloidal clay slurries, and provide valuable input parameters for meso-scale modeling efforts of clay dispersions and sedimentary deposits to upscale their mechanical properties to the macroscale.

AB - The properties of clay slurries (porosity ~ 0.75) impact a wide range of materials such as commercial clay dispersions and sedimentary deposits. Their material behavior, and in particular the gelation of clay slurries, is thought to be governed by clay particle interactions. In the literature, such interactions are rarely directly probed, but rather inferred from structures observed by cryo-electron microscopy. For example, the honeycomb structure is a widely accepted textbook model that is used to rationalize the observed behavior of clay slurries. Using high-pressure freezing, cryo-electron microscopy, and cryo-synchrotron wide-angle X-ray scattering, this study shows that the honeycomb-structure is an artifact of sample preparation. When samples are high-pressure frozen, individual clay particles and aggregates of particles arrange in a random orientation rather than the closed-cell structure dominated by face-face and face-edge contacts observed in plunge frozen samples. These results substantially contribute to the understanding of the gelation mechanism and particle interactions in colloidal clay slurries, and provide valuable input parameters for meso-scale modeling efforts of clay dispersions and sedimentary deposits to upscale their mechanical properties to the macroscale.

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KW - Honeycomb structure

KW - Illite-Smectite

KW - Plunge freezing

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ER -

Particle arrangements in clay slurries: The case against the honeycomb structure

Abstract

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Keywords

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