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Covalency in AnCl₂ (An = Th-No).

Sophie Cooper¹, Nikolas Kaltsoyannis¹

¹Department of Chemistry, School of Natural Sciences, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK. nikolas.kaltsoyannis@manchester.ac.uk.

Dalton Transactions (Cambridge, England : 2003)

|March 29, 2022

Summary

Covalency in transcurium chlorides is driven by energy matching between actinide 5f orbitals and ligand 3p, not the +2 oxidation state. This study analyzes actinide dichloride (AnCl2) bonding, revealing distinct covalent behaviors across the series.

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Area of Science:

Computational chemistry
Inorganic chemistry
Actinide chemistry

Background:

A link between unexpected covalent behavior in transcurium complexes and the stability of the +2 oxidation state in later actinides has been proposed.
Previous computational studies on actinide trichlorides (AnCl3) indicated energy degeneracy-driven covalency in later actinides.

Purpose of the Study:

To present a comparative computational study of actinide dichlorides (AnCl2).
To analyze the covalency of An-Cl bonds in AnCl2 using various computational metrics.
To elucidate the factors driving covalent behavior in transcurium chlorides.

Main Methods:

Computational methods were employed to study AnCl2 complexes.
Analysis included Natural Bond Orbital (NBO), Natural Resonance Theory (NRT), and Quantum Theory of Atoms In Molecules (QTAIM) metrics.
An-Cl bond lengths were systematically analyzed and compared between different actinide series groups.

Main Results:

An-Cl bond lengths in AnCl2 divide into two sets, with significant increases between Np-Pu and Bk-Cf.
The first group of dichlorides (Th-Np, Cm, Bk) exhibit more covalent bonds than the second group (Pu, Am, Cf-No).
An-Cl covalency decreases across the second half of the series for AnCl2, unlike in AnCl3.

Conclusions:

The observed change in covalent behavior in AnCl2 is attributed to decreased 6d orbital involvement in later elements.
Covalency in AnCl2 is driven by energy matching between actinide 5f orbitals and ligand 3p, not the stability of the +2 oxidation state.
The larger energy difference between 5f and 3p Natural Atomic Orbitals in AnCl2, compared to AnCl3, limits energy degeneracy-driven covalency.