Isomerism of Trimeric Aluminum Complexes in Aqueous Environments: Exploration via DFT-Based Metadynamics Simulation

Research output: Contribution to journalArticleScientificpeer-review

Researchers

  • Giorgio Lanzani
  • Ari P. Seitsonen
  • Marcella Iannuzzi
  • Kari Laasonen

  • Simo O. Pehkonen

Research units

  • University of Oulu
  • University of Zurich
  • Ecole Normale Superieure
  • University of Eastern Finland

Abstract

The chemistry of aluminum or oxo-aluminum in water is still relatively unknown, although it is the basis for many chemical and industrial processes, including flocculation in water treatment plants. Trimeric species have a predominant role in the formation of the Keggin cations, which are the basic building blocks of aluminum-based chemicals. Despite this, details of the structural evolution of these small solvated clusters and how this is related to the processes leading to the formation of larger aggregates are still an open issue. To address these questions, here, we have applied the metadynamics (MTD) simulation technique [Barducci, A.; et with density functional theory-based molecular dynamics to al. Wiley Interdiscip. Rev.: Comput. Mol. Sci. 2010, 1, 826-843] disclose the dynamics and structural conversions of trimeric aluminum complexes in an aqueous environment. The existence of a variety of competing metastable conformations, for example, book-like, cyclic boat, and linear shape conformations, is revealed in the MTD simulation. Furthermore, equilibrium simulations of the various intermediate states encountered along the MTD trajectory are used to assess their (meta)stability, determine the rearrangement of the OH ligands, and discuss the role of the solvating water.

Details

Original languageEnglish
Pages (from-to)11800-11809
Number of pages10
JournalJournal of Physical Chemistry B
Volume120
Issue number45
Publication statusPublished - 17 Nov 2016
MoE publication typeA1 Journal article-refereed

    Research areas

  • TEMPERATURE MOLECULAR-DYNAMICS, IONIZATION MASS-SPECTROMETRY, HYDROLYSIS PRODUCTS, DENSITY, ALCL3-CENTER-DOT-6H(2)O, IDENTIFICATION, EQUILIBRIUM, CLUSTERS, BEHAVIOR, WATER

ID: 10241584