期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 142, 期 13, 页码 6093-6102出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b12530
关键词
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资金
- US Department of Energy (DOE), Office of Basic Energy Sciences (BES) at Pacific Northwest National Laboratory (PNNL)
- BES Division of Materials Science and Engineering, Synthesis and Processing Sciences Program
- BES Chemical Sciences, Geosciences, and Biosciences Division, Geosciences Program [DE-SC0019071]
- DOE [DE-AC05-76RL01830]
When hydrolyzable cations such as aluminum interact with solid-water interfaces, macroscopic interfacial properties (e.g., surface charge and potential) and interfacial phenomena (e.g., particle adhesion) become tightly linked with the microscopic details of ion adsorption and speciation. We use in situ atomic force microscopy to directly image individual aluminum ions at a mica-water interface and show how adsorbate populations change with pH and aluminum activity. Complementary streaming potential measurements then allow us to build a triple layer model (TLM) that links surface potentials to adsorbate populations, via equilibrium binding constants. Our model predicts that hydrolyzed species dominate the mica-water interface, even when unhydrolyzed species dominate the solution. Ab initio molecular dynamics (AIMD) simulations confirm that aluminum hydrolysis is strongly promoted at the interface. The TLM indicates that hydrolyzed adsorbates are responsible for surface-potential inversions, and we find strong correlations between hydrolyzed adsorbates and particle-adhesion forces, suggesting that these species mediate adhesion by chemical bridging.
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