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Spent Fuel and Waste Science and Technology Update on Smectite-to-Illite Transformation: Laboratory Experiments Melissa Mills Sandia National Laboratories SFWST Annual Working Group Meeting Las Vegas, Nevada May 22-24, 2018 Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC., a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA-0003525. SAND2018-5486PE.

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Spent Fuel and Waste Science and Technology

Update on Smectite-to-Illite Transformation:Laboratory Experiments

Melissa MillsSandia National Laboratories

SFWST Annual Working Group Meeting Las Vegas, NevadaMay 22-24, 2018

Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC., a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA-0003525. SAND2018-5486PE.

Spent Fuel and Waste Science andTechnology

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 2

Overview of Activity

Hydrothermal reaction of smectite to illite important for bentonites as a barrier

Understanding the thermal alteration effects is dependent on:– Time– Temperature– Si and K+ concentrations– Solid to liquid ratio– Possibly interlayer cations

Typically thought to take a long time for conversion Conducted laboratory experiments for diagenetic reactions in

Parr Vessel reactors at 200°C for 1 week with variable loadings and exchanged cations (K, Cs, NH4)

Spent Fuel and Waste Science andTechnology

Analysis Techniques

XRD for basal spacing

Cation exchange capacity (CEC)

Recorded mass loss data and pH of reacted solutions

Surface area by BET nitrogen adsorption

Analysis of solutions after reaction by IC, ICP-MS, ICP-OES– Determine dissolved ions

Particle size by Malvern Zetasizer

SEM-EDS for morphology and compositional mapping

XRF for composition

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 3

Spent Fuel and Waste Science andTechnology

Results: XRD

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 4

Na-Form Smectite

Spent Fuel and Waste Science andTechnology

Results: XRD Continued

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 5

K-Form Smectite

Spent Fuel and Waste Science andTechnology

Future R&D

Perform additional characterization techniques– Particle size analysis by Zetasizer

– Composition by XRF

– Morphology by SEM

– Dissolved ions by ICP

Investigate behavior of iron in reaction

Addition of mica to possibly escalate conversion

Addition of quartz to inhibit conversion

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 6

Spent Fuel and Waste Science andTechnology

Additional Slides

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 7

Spent Fuel and Waste Science andTechnology

Results: XRD

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 8

Spent Fuel and Waste Science andTechnology

Results: XRD

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 9

Spent Fuel and Waste Science andTechnology

Results: XRD

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 10

Spent Fuel and Waste Science andTechnology

Results: Surface Area

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 11

28.65 27.94

106.40

46.56

62.8368.24

77.7483.57

52.96

75.40

65.97 62.56 62.5067.30

48.94

67.7960.86

100

120

Surfa

ce A

rea

(m2 /g

)

Raw material

ReactedNa-Smectite Reacted

K-Smectite

ReactedCs-SmectiteReacted

NH4-Smectite

Spent Fuel and Waste Science andTechnology

Results: CEC

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 12

Spent Fuel and Waste Science andTechnology

Results: Mass Loss and pH

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 13

Spent Fuel and Waste Science andTechnology

Results: SEM

5/23/18 Crystalline R&D: Smectite-to-Illite Transformation 14

Smectite to illite transformation of Gulf of Mexico-Eugene Island (GoM-EI) mudrock

SMECTITE-TO-ILLITE CONVERSION IN A GEOTHERMALLY … 40/40-1-53.pdf · clays and clay minerals, vol. 40, no. 1, 53-64, 1992. smectite-to-illite conversion in a geothermally and lithologically

HYDROTHERMAL TREATMENT OF SMECTITE, ILLITE, AND …clays.org/journal/archive/volume 35/35-4-241.pdf · HYDROTHERMAL TREATMENT OF SMECTITE, ILLITE, AND BASALT TO 460~ COMPARISON OF

COMPOSITIONAL END MEMBERS AND THERMODYNAMIC …clays.org/journal/archive/volume 41/41-5-537.pdf · solubility in smectite and illite by critically analyzing compositional data reported

Instructions for use - 北海道大学...studies emphasize the importance of external SiO 2 sources, such as smectite-illite transformation (S-I) reac-tions in accompanying shales

ROLE OF IRON REDUCTION IN THE CONVERSION OF SMECTITE …clays.org/journal/archive/volume 27/27-5-327.pdf · ROLE OF IRON REDUCTION IN THE CONVERSION OF SMECTITE TO ILLITE IN BENTONITES

ILLITE/SMECTITE GEOTHERMOMETRY OF THE PROTEROZOIC … 41/41-2-134.pdf · ILLITE/SMECTITE GEOTHERMOMETRY OF THE PROTEROZOIC ... Waples, 1980; Pollastro and Barker, ... The shape of

ILLITE/SHECTITE(U) i i COLL CRYSTL HANOVER STRUCTURE NH … · the illite and smectite layers and one possible stacking sequence. In this sequence, one of the spacings, RS, is indicated

Effect of coating phyllosilicate clays with hydrous oxides on … · 2014. 3. 6. · phyllosilicate clays (kaolinite, illite, smectite) with and without goethite coating and illitic

X RAY in Illite

Rock-physics modeling of shale during smectite-to-illite ...rpl.uh.edu/papers/2016/201610_RPL_Qin_Rock_physics...increasing salinity or decreasing CEC. For example, smectite typically

Estudo de perfis de meteorização do granito de Terras de ... · Chlorite, illite, C-S and I-S mixed-layers, smectite, kaolinite, gibbsite, lepidocrocite, goethite, calcite and pyrite

XRD ANALYSIS OF ILLITE-SMECTITE …

FRIO SHALE MINERALOGY AND THE STOICHIOMETRY OF THE ...clays.org/journal/archive/volume 45/45-5-618.pdf · FRIO SHALE MINERALOGY AND THE STOICHIOMETRY OF THE SMECTITE-TO-ILLITE REACTION:

SEDIMENTOLOGY OF BAJOCIAN ROCKS FROM THE by STEPHEN … · 6.3a. Clay Mineralogy 215 1. Kaolinite 215 2. Illite 218 3. Mixed layer illite/smectite 218 4. Chlorite 220 6.3b Other Diagenetic

Data report: clay mineral assemblages and illite/smectite

MICROSTRUCTURES, FORMATION MECHANISMS, AND … 36/36-1-1.pdfKey Words--Chlorite, Electron microscopy, Fluid-mineral equilibria, Geothermal field, Illite, Salton Sea, Smectite, Texture

ESTUDO PETROGRÁFICO E PETROLÓGICO DA FORMAÇÃO … · illite/smectite and the mineral pyrophyllite. Although the characteristics of the samples reflect the previous conditions

ROTATIONALLY DISORDERED ILLITE/SMECTITE IN PALEOZOIC …clays.org/journal/archive/volume 43/43-3-271.pdf · Vol. 43, No. 3, 1995 RotationaUy disordered illite/smectite in Paleozoic

OPEN ACCESS minerals · PDF fileMinerals in the coals are mainly made up of quartz, chamosite, kaolinite, mixed-layer illite/smectite ... ASTM D3175-11 [14], and ASTMD3174-11 [15],

COMPOSITIONAL END MEMBERS AND THERMODYNAMIC … 41/41-5-537.pdf · the actual compositional variation in smectite or illite is probably much more restricted than that inferred from

Clay mineralogy and geochemistry of three offshore wells in the …journals.tubitak.gov.tr/earth/issues/yer-16-25-6/yer-25... · The conversion of smectite to illite depends on the

2019 SFWST Roadmap Update – Workshop Methodology and ...€¦ · 2019 SFWST Roadmap Update – Workshop Methodology and Breakout Group Assignments S. David Sevougian Sandia National

Interlayer order in illite/smectite · illite as the first interlayer in a crystallite 600/o of the time and smectite 400/o of the time. Succeeding interlayers also have a 600/o chance

DETERMINATION OF ILLITE-SMECTITE STRUCTURES … 47/47-5-555.pdf · clays and clay minerals, vol. 47, no. 5, 555-566, 1999. determination of illite-smectite structures using multispecimen

CHARACTERIZATION OF THE END OF SMECTITE-TO-ILLITE ... 40/40-1-40.pdf · CHARACTERIZATION OF THE END OF SMECTITE-TO-ILLITE TRANSFORMATION: DECOMPOSITION OF X-RAY PATTERNS BRUNO LANSON

OriginandevolutionofmineralizingfluidsandexplorationoftheC ...diposit.ub.edu/dspace/bitstream/2445/162495/1/674991.pdfUNCORRECTED PROOF Ore Geology Reviewsxxx(2016)xxx-xxx 5 barite,illite,andminordiasporeandrutile.Argillicalterationpro-ducedquartz,kaolinite,illite,illite-smectite,andminorchloritewithCited

parallel reaction kinetics of smectite to illite conversion

Mechanism of illite formation during smectite-to-illite conversion in a

SMECTITE-ILLITE TRANSITION IN BARBADOS ... 40/40-1-65.pdfVol. 40, No. 1, 1992 Smectite-illite transition in Barbados accretionary wedge sediments 67 Figure 3. Summary of stratigraphic

Weathering - exploreiowageology.org€¦ · weathering-resistant Fe and Al oxides. 0 02 g 02 molecules and cations Exchangeable water molecules and cations Illite and smectite have

R1 = rectorite, CCM 34, 125 (1986). - The Mineralogical … = illite-smectite mixed-layer, CCM 34, 125 (1986). R1 = rectorite, CCM 34, 125 (1986). R2 = illite-illite-smectite regular

Microbial effects in promoting the smectite to illite … › dtic › tr › fulltext › u2 › a499115.pdfillite-rich I-S, with a continuously variable ratio in the propor- tions

comparison of structural models of mixed-layer illite/smectite and

M. LEZZERINI, F. STORTI, M. TAMPONI - stsn.it · 150 LEZZERINI M., STORTI F., TAMPONI M. sociazione mineralogica calcite + quarzo + illite + smectite + clorite + strati misti disordinati