Title: Nonlinear dynamics and instability of aqueous dissolution of silicate glasses and minerals

Abstract

Aqueous dissolution of silicate glasses and minerals plays a critical role in global biogeochemical cycles and climate evolution. The reactivity of these materials is also important to numerous engineering applications including nuclear waste disposal. The dissolution process has long been considered to be controlled by a leached surface layer in which cations in the silicate framework are gradually leached out and replaced by protons from the solution. This view has recently been challenged by observations of extremely sharp corrosion fronts and oscillatory zonings in altered rims of the materials, suggesting that corrosion of these materials may proceed directly through congruent dissolution followed by secondary mineral precipitation. Here we show that complex silicate material dissolution behaviors can emerge from a simple positive feedback between dissolution-induced cation release and cation-enhanced dissolution kinetics. This self-accelerating mechanism enables a systematic prediction of the occurrence of sharp dissolution fronts (vs. leached surface layers), oscillatory dissolution behaviors and multiple stages of glass dissolution (in particular the alteration resumption at a late stage of a corrosion process). In conclusion, our work provides a new perspective for predicting long-term silicate weathering rates in actual geochemical systems and developing durable silicate materials for various engineering applications.

Authors:

Wang, Yifeng ^[1]; Jove-Colon, Carlos F. ^[1]; Kuhlman, Kristopher L. ^[1]

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+ Show Author Affiliations

1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Publication Date:

Fri Jul 22 00:00:00 EDT 2016

Research Org.:

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Org.:

USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5)

OSTI Identifier:

1313074

Report Number(s):

SAND2016-4035J
Journal ID: ISSN 2045-2322; 639042

Grant/Contract Number:  

AC04-94AL85000

Resource Type:

Accepted Manuscript

Journal Name:

Scientific Reports

Additional Journal Information:

Journal Volume: 6; Journal ID: ISSN 2045-2322

Publisher:

Nature Publishing Group

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY