Predicting Outcomes of Nanoparticle Attachment by Connecting Atomistic, Interfacial, Particle, and Aggregate Scales

Lili Liu, Benjamin A. Legg, William Smith, Lawrence M. Anovitz, Xin Zhang, Reed Harper, Carolyn I. Pearce, Kevin M. Rosso, Andrew G. Stack, Markus Bleuel, David F.R. Mildner, Gregory K. Schenter, Aurora E. Clark, James J. De Yoreo, Jaehun Chun, Elias Nakouzi

Research output: Contribution to journalArticlepeer-review

11 Scopus citations

Abstract

Predicting nanoparticle aggregation and attachment phenomena requires a rigorous understanding of the interplay among crystal structure, particle morphology, surface chemistry, solution conditions, and interparticle forces, yet no comprehensive picture exists. We used an integrated suite of experimental, theoretical, and simulation methods to resolve the effect of solution pH on the aggregation of boehmite nanoplatelets, a case study with important implications for the environmental management of legacy nuclear waste. Real-time observations showed that the particles attach preferentially along the (010) planes at pH 8.5 and the (101) planes at pH 11. To rationalize these results, we established the connection between key physicochemical phenomena across the relevant length scales. Starting from molecular-scale simulations of surface hydroxyl reactivity, we developed an interfacial-scale model of the corresponding electrostatic potentials, with subsequent particle-scale calculations of the resulting driving forces allowing successful prediction of the attachment modes. Finally, we scaled these phenomena to understand the collective structure at the aggregate-scale. Our results indicate that facet-specific differences in surface chemistry produce heterogeneous surface charge distributions that are coupled to particle anisotropy and shape-dependent hydrodynamic forces, to play a key role in controlling aggregation behavior.

Original languageEnglish
Pages (from-to)15556-15567
Number of pages12
JournalACS Nano
Volume17
Issue number16
DOIs
StatePublished - Aug 22 2023

Funding

This work was supported by IDREAM (Interfacial Dynamics in Radioactive Environments and Materials), an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science (SC), Basic Energy Sciences (BES), at Pacific Northwest National Laboratory (PNNL) (FWP 68932). PNNL is a multiprogram national laboratory operated for the DOE by Battelle Memorial Institute under Contract DE-AC05-76RL0-1830. We acknowledge the support of the National Institute of Standards and Technology, Center for Neutron Research, U.S. Department of Commerce, in providing the research neutron facilities used in this work. Access to both NBG30 SANS and BT5 USANS was provided by the Center for High Resolution Neutron Scattering, a partnership between the National Institute of Standards and Technology and the National Science Foundation under Agreement No. DMR-1508249. Certain commercial equipment, instruments, materials and software are identified in this paper to foster understanding. Such identification does not imply recommendation or endorsement by the National Institute of Standards and Technology or the Department of Energy, nor does it imply that the materials or equipment identified are necessarily the best available for the purpose.

Keywords

  • DLVO theory
  • aggregation
  • anisotropic particles
  • interparticle forces
  • multiscale
  • oriented attachment

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