Journal
SCIENCE
Volume 344, Issue 6188, Pages 1138-1142Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1253793
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Funding
- Belgian Fund for Scientific Research-Fonds de la Recherche Scientifique (F.R.S.-FNRS)
- Marie Curie Foundation [CIG322284, CIG334368]
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In nature, aqueous solutions often move collectively along solid surfaces (for example, raindrops falling on the ground and rivers flowing through riverbeds). However, the influence of such motion on water-surface interfacial chemistry is unclear. In this work, we combine surface-specific sum frequency generation spectroscopy and microfluidics to show that at immersed calcium fluoride and fused silica surfaces, flow leads to a reversible modification of the surface charge and subsequent realignment of the interfacial water molecules. Obtaining equivalent effects under static conditions requires a substantial change in bulk solution pH (up to 2 pH units), demonstrating the coupling between flow and chemistry. These marked flow-induced variations in interfacial chemistry should substantially affect our understanding and modeling of chemical processes at immersed surfaces.
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