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Title: Fe-saponite growth on low-carbon and stainless steel in hydrothermal-bentonite experiments

Abstract

Hydrothermal experiments on engineered barrier system (EBS) materials were conducted to characterize high temperature interactions between bentonite and candidate waste container steels (304SS, 316SS, low-C steel) for deep geological disposition of nuclear spent fuel. In this study, hydrothermal experiments were performed using Dickson reaction cells at temperatures and pressure of up to 300 °C and 15–16 MPa, respectively, for four to six weeks. Wyoming bentonite was saturated with a 1900 ppm K-Ca-Na-Cl solution in combination with stainless and low-C steel coupons. Authigenic Fe-saponite precipitated utilizing steel as a growth substrate with Fe being supplied by steel corrosion. Concurrent with Fe-saponite formation, sulfides precipitated from sulfide-bearing fluids, from pyrite dissolution, near the steel interface. Sulfide mineral formation is dependent on the steel substrate composition: stainless steel produced pentlandite ((Ni, Fe) 9S 8) and millerite (NiS), whereas low C steel generated pyrrhotite (Fe 7S 8). The presence of sulfides suggests highly reduced environments at the steel-clay barrier interface potentially influencing overall steel corrosion rates and (re)passivation mechanisms. Finally, results of this research show that nuclear waste steel container material may act as a substrate for mineral growth in response to corrosion during hydrothermal interactions with bentonite barriers.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [3]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  3. Tulane Univ., New Orleans, LA (United States). Dept. of Geology
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5)
OSTI Identifier:
1474633
Alternate Identifier(s):
OSTI ID: 1477468; OSTI ID: 1479985
Report Number(s):
SAND-2018-2143J; LA-UR-18-21040
Journal ID: ISSN 0022-3115
Grant/Contract Number:  
AC05-00OR22725; AC04-94AL85000; AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Nuclear Materials
Additional Journal Information:
Journal Volume: 511; Journal Issue: C; Journal ID: ISSN 0022-3115
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; Bentonite; Corrosion; Fe-saponite; Steel; Sulfides; Repository; Used-fuel; Earth Sciences; Engineered Barrier Systems, Fe- saponite, H2 generation

Citation Formats

Cheshire, Michael C., A. Caporuscio, Florie, Jove-Colon, Carlos F., and Norskog, Kate E. Fe-saponite growth on low-carbon and stainless steel in hydrothermal-bentonite experiments. United States: N. p., 2018. Web. doi:10.1016/j.jnucmat.2018.09.038.
Cheshire, Michael C., A. Caporuscio, Florie, Jove-Colon, Carlos F., & Norskog, Kate E. Fe-saponite growth on low-carbon and stainless steel in hydrothermal-bentonite experiments. United States. doi:10.1016/j.jnucmat.2018.09.038.
Cheshire, Michael C., A. Caporuscio, Florie, Jove-Colon, Carlos F., and Norskog, Kate E. Thu . "Fe-saponite growth on low-carbon and stainless steel in hydrothermal-bentonite experiments". United States. doi:10.1016/j.jnucmat.2018.09.038. https://www.osti.gov/servlets/purl/1474633.
@article{osti_1474633,
title = {Fe-saponite growth on low-carbon and stainless steel in hydrothermal-bentonite experiments},
author = {Cheshire, Michael C. and A. Caporuscio, Florie and Jove-Colon, Carlos F. and Norskog, Kate E.},
abstractNote = {Hydrothermal experiments on engineered barrier system (EBS) materials were conducted to characterize high temperature interactions between bentonite and candidate waste container steels (304SS, 316SS, low-C steel) for deep geological disposition of nuclear spent fuel. In this study, hydrothermal experiments were performed using Dickson reaction cells at temperatures and pressure of up to 300 °C and 15–16 MPa, respectively, for four to six weeks. Wyoming bentonite was saturated with a 1900 ppm K-Ca-Na-Cl solution in combination with stainless and low-C steel coupons. Authigenic Fe-saponite precipitated utilizing steel as a growth substrate with Fe being supplied by steel corrosion. Concurrent with Fe-saponite formation, sulfides precipitated from sulfide-bearing fluids, from pyrite dissolution, near the steel interface. Sulfide mineral formation is dependent on the steel substrate composition: stainless steel produced pentlandite ((Ni, Fe)9S8) and millerite (NiS), whereas low C steel generated pyrrhotite (Fe7S8). The presence of sulfides suggests highly reduced environments at the steel-clay barrier interface potentially influencing overall steel corrosion rates and (re)passivation mechanisms. Finally, results of this research show that nuclear waste steel container material may act as a substrate for mineral growth in response to corrosion during hydrothermal interactions with bentonite barriers.},
doi = {10.1016/j.jnucmat.2018.09.038},
journal = {Journal of Nuclear Materials},
number = C,
volume = 511,
place = {United States},
year = {2018},
month = {9}
}

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