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Evidence for auto-catalytic mineral dissolution from surface-specific vibrational spectroscopy.

ABSTRACT: The dissolution of minerals in water is typically studied on macroscopic length- and time-scales, by detecting dissolution products in bulk solution and deducing reaction rates from model assumptions. Here, we report a direct, real-time measurement of silica dissolution, by monitoring how dissolution changes the first few interfacial layers of water in contact with silica, using surface-specific spectroscopy. We obtain direct information on the dissolution kinetics of this geochemically relevant mineral. The interfacial concentration of dissolution products saturates at the level of the solubility limit of silica (~millimolar) on the surprisingly short timescale of tens of hours. The observed kinetics reveal that the dissolution rate increases substantially with progressing dissolution, suggesting that dissolution is an auto-catalytic process.

SUBMITTER: Schaefer J

PROVIDER: S-EPMC6102271 | biostudies-literature | 2018 Aug

REPOSITORIES: biostudies-literature

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Evidence for auto-catalytic mineral dissolution from surface-specific vibrational spectroscopy.

Schaefer Jan J Backus Ellen H G EHG Bonn Mischa M

Nature communications 20180820 1

The dissolution of minerals in water is typically studied on macroscopic length- and time-scales, by detecting dissolution products in bulk solution and deducing reaction rates from model assumptions. Here, we report a direct, real-time measurement of silica dissolution, by monitoring how dissolution changes the first few interfacial layers of water in contact with silica, using surface-specific spectroscopy. We obtain direct information on the dissolution kinetics of this geochemically relevant ...[more]

PMID: 30127364

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Project description:Vibrational spectroscopy is an essential tool in chemical analyses, biological assays, and studies of functional materials. Over the past decade, various coherent nonlinear vibrational spectroscopic techniques have been developed and enabled researchers to study time-correlations of the fluctuating frequencies that are directly related to solute-solvent dynamics, dynamical changes in molecular conformations and local electrostatic environments, chemical and biochemical reactions, protein structural dynamics and functions, characteristic processes of functional materials, and so on. In order to gain incisive and quantitative information on the local electrostatic environment, molecular conformation, protein structure and interprotein contacts, ligand binding kinetics, and electric and optical properties of functional materials, a variety of vibrational probes have been developed and site-specifically incorporated into molecular, biological, and material systems for time-resolved vibrational spectroscopic investigation. However, still, an all-encompassing theory that describes the vibrational solvatochromism, electrochromism, and dynamic fluctuation of vibrational frequencies has not been completely established mainly due to the intrinsic complexity of intermolecular interactions in condensed phases. In particular, the amount of data obtained from the linear and nonlinear vibrational spectroscopic experiments has been rapidly increasing, but the lack of a quantitative method to interpret these measurements has been one major obstacle in broadening the applications of these methods. Among various theoretical models, one of the most successful approaches is a semiempirical model generally referred to as the vibrational spectroscopic map that is based on a rigorous theory of intermolecular interactions. Recently, genetic algorithm, neural network, and machine learning approaches have been applied to the development of vibrational solvatochromism theory. In this review, we provide comprehensive descriptions of the theoretical foundation and various examples showing its extraordinary successes in the interpretations of experimental observations. In addition, a brief introduction to a newly created repository Web site (http://frequencymap.org) for vibrational spectroscopic maps is presented. We anticipate that a combination of the vibrational frequency map approach and state-of-the-art multidimensional vibrational spectroscopy will be one of the most fruitful ways to study the structure and dynamics of chemical, biological, and functional molecular systems in the future.

Dataset Information

Evidence for auto-catalytic mineral dissolution from surface-specific vibrational spectroscopy.

Publications

Evidence for auto-catalytic mineral dissolution from surface-specific vibrational spectroscopy.

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