F. Chowdhury , T.L. Rashwan , P. Mondal , M. Behazin , P.G. Keech , J.S. Sharma , M. Krol
{"title":"压实对硫化氢在 MX-80 膨润土中扩散迁移的影响","authors":"F. Chowdhury , T.L. Rashwan , P. Mondal , M. Behazin , P.G. Keech , J.S. Sharma , M. Krol","doi":"10.1016/j.jconhyd.2024.104341","DOIUrl":null,"url":null,"abstract":"<div><p>Canada's deep geological repository (DGR) design includes an engineered barrier system where highly compacted bentonite (HCB) surrounds the copper-coated used fuel containers (UFCs). Microbial-influenced corrosion is a potential threat to long-term integrity of UFC as bisulfide (HS<sup>−</sup>) may be produced by microbial activities under anaerobic conditions and transported via diffusion through the HCB to reach the UFC surface, resulting in corrosion of copper. Therefore, understanding HS<sup>−</sup> transport mechanisms through HCB is critical for accurate prediction of copper corrosion allowance. This study investigated HS<sup>−</sup> transport behaviour through MX-80 bentonite at dry densities 1070–1615 kg m<sup>−3</sup> by performing through-diffusion experiments. Following HS<sup>−</sup> diffusion, bromide (Br<sup>−</sup>) diffusion and Raman spectroscopy analyses were performed to explore possible physical or mineralogical alterations of bentonite caused by interacting with HS<sup>−</sup>. In addition, accessible porosity <span><math><mfenced><mi>ε</mi></mfenced></math></span> was estimated using extended Archie's law. Effective diffusion coefficient of HS<sup>−</sup> was found 2.5 × 10<sup>−12</sup> m<sup>2</sup> s<sup>−1</sup> and 5.0× 10<sup>−12</sup> m<sup>2</sup> s<sup>−1</sup> for dry densities 1330 and 1070 kg m<sup>−3</sup>, respectively. No HS<sup>−</sup> breakthrough was observed for highly compacted bentonite (1535–1615 kg m<sup>−3</sup>) over the experimental timeframe (170 days). Raman spectroscopy results revealed that HS<sup>−</sup> reacted with iron in bentonite and precipitated as mackinawite and, therefore, it was immobilized. Finally, results of this study imply that HS<sup>−</sup> transport towards UFC will be highly controlled by the available iron content and dry density of the buffer material.</p></div>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":null,"pages":null},"PeriodicalIF":4.3000,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0169772224000457/pdfft?md5=797dd44125aa38ea08a2a105b02f855a&pid=1-s2.0-S0169772224000457-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Effect of compaction on bisulfide diffusive transport through MX-80 bentonite\",\"authors\":\"F. Chowdhury , T.L. Rashwan , P. Mondal , M. Behazin , P.G. Keech , J.S. Sharma , M. Krol\",\"doi\":\"10.1016/j.jconhyd.2024.104341\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Canada's deep geological repository (DGR) design includes an engineered barrier system where highly compacted bentonite (HCB) surrounds the copper-coated used fuel containers (UFCs). Microbial-influenced corrosion is a potential threat to long-term integrity of UFC as bisulfide (HS<sup>−</sup>) may be produced by microbial activities under anaerobic conditions and transported via diffusion through the HCB to reach the UFC surface, resulting in corrosion of copper. Therefore, understanding HS<sup>−</sup> transport mechanisms through HCB is critical for accurate prediction of copper corrosion allowance. This study investigated HS<sup>−</sup> transport behaviour through MX-80 bentonite at dry densities 1070–1615 kg m<sup>−3</sup> by performing through-diffusion experiments. Following HS<sup>−</sup> diffusion, bromide (Br<sup>−</sup>) diffusion and Raman spectroscopy analyses were performed to explore possible physical or mineralogical alterations of bentonite caused by interacting with HS<sup>−</sup>. In addition, accessible porosity <span><math><mfenced><mi>ε</mi></mfenced></math></span> was estimated using extended Archie's law. Effective diffusion coefficient of HS<sup>−</sup> was found 2.5 × 10<sup>−12</sup> m<sup>2</sup> s<sup>−1</sup> and 5.0× 10<sup>−12</sup> m<sup>2</sup> s<sup>−1</sup> for dry densities 1330 and 1070 kg m<sup>−3</sup>, respectively. No HS<sup>−</sup> breakthrough was observed for highly compacted bentonite (1535–1615 kg m<sup>−3</sup>) over the experimental timeframe (170 days). Raman spectroscopy results revealed that HS<sup>−</sup> reacted with iron in bentonite and precipitated as mackinawite and, therefore, it was immobilized. Finally, results of this study imply that HS<sup>−</sup> transport towards UFC will be highly controlled by the available iron content and dry density of the buffer material.</p></div>\",\"PeriodicalId\":3,\"journal\":{\"name\":\"ACS Applied Electronic Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.3000,\"publicationDate\":\"2024-05-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S0169772224000457/pdfft?md5=797dd44125aa38ea08a2a105b02f855a&pid=1-s2.0-S0169772224000457-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Electronic Materials\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0169772224000457\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ELECTRICAL & ELECTRONIC\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Electronic Materials","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0169772224000457","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ELECTRICAL & ELECTRONIC","Score":null,"Total":0}
Effect of compaction on bisulfide diffusive transport through MX-80 bentonite
Canada's deep geological repository (DGR) design includes an engineered barrier system where highly compacted bentonite (HCB) surrounds the copper-coated used fuel containers (UFCs). Microbial-influenced corrosion is a potential threat to long-term integrity of UFC as bisulfide (HS−) may be produced by microbial activities under anaerobic conditions and transported via diffusion through the HCB to reach the UFC surface, resulting in corrosion of copper. Therefore, understanding HS− transport mechanisms through HCB is critical for accurate prediction of copper corrosion allowance. This study investigated HS− transport behaviour through MX-80 bentonite at dry densities 1070–1615 kg m−3 by performing through-diffusion experiments. Following HS− diffusion, bromide (Br−) diffusion and Raman spectroscopy analyses were performed to explore possible physical or mineralogical alterations of bentonite caused by interacting with HS−. In addition, accessible porosity was estimated using extended Archie's law. Effective diffusion coefficient of HS− was found 2.5 × 10−12 m2 s−1 and 5.0× 10−12 m2 s−1 for dry densities 1330 and 1070 kg m−3, respectively. No HS− breakthrough was observed for highly compacted bentonite (1535–1615 kg m−3) over the experimental timeframe (170 days). Raman spectroscopy results revealed that HS− reacted with iron in bentonite and precipitated as mackinawite and, therefore, it was immobilized. Finally, results of this study imply that HS− transport towards UFC will be highly controlled by the available iron content and dry density of the buffer material.