MALDI-TOF and Quantum Chemical Study of Non-stoichiometric Tantalum Oxychloride Clusters

TL;DR

This study combines MALDI-TOF spectroscopy and quantum chemical calculations to analyze non-stoichiometric tantalum oxychloride clusters, revealing their formation, structure, and stability, including cage-like configurations with metal-metal bonds.

Contribution

It presents a combined experimental and theoretical approach to characterize tantalum oxychloride clusters, highlighting their formation mechanisms and stable structural isomers.

Findings

Clusters contain 2 to 15 tantalum atoms.

Cage structures with oxygen bridges are stable.

Metal-metal bonds significantly contribute to stability.

Abstract

Using the MALDI-TOF spectroscopy method, clusters of non-stoichiometric tantalum oxychlorides formed as a result of hydrolysis of nanoscale reaction products of tantalum pentachloride with acetylene and of interaction with oxygen and air moisture in the process of sample preparation were studied. The formation of oxychloride clusters containing from 2 to 15 tantalum atoms is shown. Quantum chemical calculations of the structure and relative thermodynamic stability of the possible isomers are carried out. The stability of cage Ta structures connected by oxygen bridges with significant contribution of metal-metal bond is established