Insights into the mechanism and kinetics of dissolution of aluminoborosilicate glasses in acidic media: Impact of high ionic field strength cations

Achieving thinner and higher performance display/substrate glasses and transparent glass-ceramics with tunable properties requires a precise control of acid-etching process, thus necessitating a comprehensive understanding of glass composition–structure–dissolution behavior relationships in acidic m...

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Published inActa materialia Vol. 242; p. 118468
Main Authors Qin, Qianhui, Stone-Weiss, Nicholas, Zhao, Tongyao, Mukherjee, Pinaki, Ren, Jinjun, Mauro, John C., Goel, Ashutosh
Format Journal Article
LanguageEnglish
Published Elsevier Ltd 01.01.2023
Subjects
Corrosion
Non-metallic glasses (silicates)
Structure–property relationship
Corrosion
Non-metallic glasses (silicates)
Structure–property relationship
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Abstract Achieving thinner and higher performance display/substrate glasses and transparent glass-ceramics with tunable properties requires a precise control of acid-etching process, thus necessitating a comprehensive understanding of glass composition–structure–dissolution behavior relationships in acidic medium. Unfortunately, the literature on this subject has been focused only on a narrow set of glass chemistries. Therefore, consensus on the mechanisms that govern the acidic dissolution of multicomponent silicate glasses over a broad compositional space is still lacking. The present work employs a suite of state-of-the-art spectroscopic techniques, including 1D and 2D NMR, TEM-EELS, ICP-OES, and XPS, to provide an insight into the mechanism and kinetics of corrosion of alkali/alkaline-earth aluminoborosilicate glasses (comprising high field strength cations – HFSCs, i.e., La3+, Ti4+, Zr4+ and Nb5+) in acidic media (HCl; pH = 2). Incorporating the HFSCs into the glasses induces significant structural changes in their network, thus, impacting the forward rate dissolution kinetics. Based on the results, we hypothesize that the glasses dissolve at pH = 2 through an ‘interfacial dissolution – re-precipitation mechanism (IDPM)’ and ‘in-situ recondensation’ coupled pattern, wherein the IDPM results in a Si-rich alteration layer, followed by local recondensation occurring due to limited kinetics near the interfacial solution between the uncorroded glass surface and the outer alteration layer. [Display omitted]
AbstractList Achieving thinner and higher performance display/substrate glasses and transparent glass-ceramics with tunable properties requires a precise control of acid-etching process, thus necessitating a comprehensive understanding of glass composition–structure–dissolution behavior relationships in acidic medium. Unfortunately, the literature on this subject has been focused only on a narrow set of glass chemistries. Therefore, consensus on the mechanisms that govern the acidic dissolution of multicomponent silicate glasses over a broad compositional space is still lacking. The present work employs a suite of state-of-the-art spectroscopic techniques, including 1D and 2D NMR, TEM-EELS, ICP-OES, and XPS, to provide an insight into the mechanism and kinetics of corrosion of alkali/alkaline-earth aluminoborosilicate glasses (comprising high field strength cations – HFSCs, i.e., La3+, Ti4+, Zr4+ and Nb5+) in acidic media (HCl; pH = 2). Incorporating the HFSCs into the glasses induces significant structural changes in their network, thus, impacting the forward rate dissolution kinetics. Based on the results, we hypothesize that the glasses dissolve at pH = 2 through an ‘interfacial dissolution – re-precipitation mechanism (IDPM)’ and ‘in-situ recondensation’ coupled pattern, wherein the IDPM results in a Si-rich alteration layer, followed by local recondensation occurring due to limited kinetics near the interfacial solution between the uncorroded glass surface and the outer alteration layer. [Display omitted]
ArticleNumber 118468
Author Mukherjee, Pinaki
Stone-Weiss, Nicholas
Qin, Qianhui
Mauro, John C.
Zhao, Tongyao
Goel, Ashutosh
Ren, Jinjun
Author_xml – sequence: 1
  givenname: Qianhui
  surname: Qin
  fullname: Qin, Qianhui
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  givenname: Nicholas
  orcidid: 0000-0001-7139-1940
  surname: Stone-Weiss
  fullname: Stone-Weiss, Nicholas
  organization: Department of Materials Science and Engineering, Rutgers, The State University of New Jersey, Piscataway, NJ 08854, United States
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  givenname: Tongyao
  surname: Zhao
  fullname: Zhao, Tongyao
  organization: Key Laboratory of Materials for High-Power Laser, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800, China
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  givenname: Pinaki
  surname: Mukherjee
  fullname: Mukherjee, Pinaki
  organization: Department of Materials Science and Engineering, Michigan Technological University, Houghton, MI 49931, United States
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  givenname: Jinjun
  surname: Ren
  fullname: Ren, Jinjun
  organization: Key Laboratory of Materials for High-Power Laser, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800, China
– sequence: 6
  givenname: John C.
  surname: Mauro
  fullname: Mauro, John C.
  organization: Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA 16802, United States
– sequence: 7
  givenname: Ashutosh
  surname: Goel
  fullname: Goel, Ashutosh
  email: ag1179@soe.rutgers.edu
  organization: Department of Materials Science and Engineering, Rutgers, The State University of New Jersey, Piscataway, NJ 08854, United States
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Snippet Achieving thinner and higher performance display/substrate glasses and transparent glass-ceramics with tunable properties requires a precise control of...
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SubjectTerms Corrosion
Non-metallic glasses (silicates)
Structure–property relationship
Title Insights into the mechanism and kinetics of dissolution of aluminoborosilicate glasses in acidic media: Impact of high ionic field strength cations
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