Ion Correlations Decrease Particle Aggregation Rate by Increasing Hydration Forces at InterfacesClick to copy article linkArticle link copied!
- Pravalika ButreddyPravalika ButreddyPhysical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Pravalika Butreddy
- Jaeyoung HeoJaeyoung HeoPhysical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Jaeyoung Heo
- Nikhil RampalNikhil RampalMaterial Sciences Division, Lawrence Livermore National Laboratory, Livermore, California 94550, United StatesMore by Nikhil Rampal
- Tingting LiuTingting LiuChemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United StatesMore by Tingting Liu
- Lili LiuLili LiuPhysical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Lili Liu
- William SmithWilliam SmithY-12 National Security Complex, Oak Ridge, Tennessee 37830, United StatesMore by William Smith
- Xin ZhangXin ZhangPhysical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Xin Zhang
- Micah P. PrangeMicah P. PrangePhysical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Micah P. Prange
- Benjamin A. LeggBenjamin A. LeggPhysical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Benjamin A. Legg
- Gregory K. SchenterGregory K. SchenterPhysical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Gregory K. Schenter
- James J. De YoreoJames J. De YoreoPhysical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesDepartment of Materials Science and Engineering, University of Washington, Seattle, Washington 98195, United StatesMore by James J. De Yoreo
- Jaehun Chun*Jaehun Chun*Email: [email protected]Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesDepartment of Chemical Engineering, CUNY City College of New York, New York, New York 10031, United StatesMore by Jaehun Chun
- Andrew G. Stack*Andrew G. Stack*Email: [email protected]Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United StatesMore by Andrew G. Stack
- Elias Nakouzi*Elias Nakouzi*Email: [email protected]Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Elias Nakouzi
Abstract
The connection between solution structure, particle forces, and emergent phenomena at solid–liquid interfaces remains ambiguous. In this case study on boehmite aggregation, we established a connection between interfacial solution structure, emerging hydration forces between two approaching particles, and the resulting structure and kinetics of particle aggregation. In contrast to expectations from continuum-based theories, we observed a nonmonotonic dependence of the aggregation rate on the concentration of sodium chloride, nitrate, or nitrite, decreasing by 15-fold in 4 molal compared to 1 molal solutions. These results are accompanied by an increase in repulsive hydration forces and interfacial oscillatory features from 0.27–0.31 nm in 0.01 molal to 0.38–0.52 nm in 2 molal. Moreover, molecular dynamics (MD) simulations indicated that these changes correspond to enhanced ion correlations near the interface and produced loosely bound aggregates that retain electrolyte between the particles. We anticipate that these results will enable the prediction of particle aggregation, attachment, and assembly, with broad relevance to interfacial phenomena.
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