Real-time in situ observations of reaction and transport phenomena during silicate glass corrosion by fluid-cell Raman spectroscopy

Nature Materials
Thorsten GeislerMoritz B K Fritzsche

Abstract

Borosilicate glass is an important material used in various industries due to its chemical durability, such as for the immobilization of high-level nuclear waste. However, it is susceptible to aqueous corrosion, recognizable by the formation of surface alteration layers (SALs). Here, we report in situ fluid-cell Raman spectroscopic experiments providing real-time insights into reaction and transport processes during the aqueous corrosion of a borosilicate glass. The formation of a several-micrometre-thick water-rich zone between the SAL and the glass, interpreted as an interface solution, is detected, as well as pH gradients at the glass surface and within the SAL. By replacing the solution with a deuterated solution, it is observed that water transport through the SAL is not rate-limiting. The data support an interface-coupled dissolution-reprecipitation process for SAL formation. Fluid-cell Raman spectroscopic experiments open up new avenues for studying solid-water reactions, with the ability to in situ trace specific sub-processes in real time by using stable isotopes.

References

Feb 9, 2008·Dalton Transactions : an International Journal of Inorganic Chemistry·Wolfram W RudolphErich Königsberger
Oct 28, 2008·Nature Materials·Céline CailleteauOlivier Spalla
Mar 29, 2014·Science·Andrew Putnis
Feb 20, 2015·Nature Communications·Stéphane GinThibault Charpentier
Jul 23, 2016·Scientific Reports·Yifeng WangKristopher L Kuhlman
Nov 8, 2017·Scientific Reports·Moritz LiesegangGregor Neusser
Jun 6, 2018·Nature Communications·Stéphane GinJincheng Du

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Methods Mentioned

BETA
electron microprobe
transmission electron microscopy
X-ray

Software Mentioned

MATLAB
PHREEQC

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