A Simple Route to Calcium and Strontium Hydride Clusters

Angew Chem Int Ed Engl. 2017 Sep 18;56(39):11880-11884. doi: 10.1002/anie.201706786. Epub 2017 Aug 23.

Abstract

The first strontium hydride complex has been obtained by simply treating Sr[N(SiMe3 )2 ]2 with PhSiH3 in the presence of PMDTA. The Sr complex Sr6 H9 [N(SiMe3 )2 ]3 ⋅(PMDTA)3 crystallizes as an "inverse cryptand": an interstitial H- is surrounded by a Sr6 H84+ cage decorated with amide and PMDTA ligands. The analogous Ca complex could also be obtained and both retain their solid-state structures in solution: 1 H NMR spectra in C6 D6 show two doublets and one nonet (4:4:1). Up to 90 °C, no coalescence is observed. The Ca cluster was investigated by DFT calculations and shows atypically low charges on Ca (+1.14) and H (-0.59) which signifies an unexpectedly low ionicity. AIM analysis shows hydride⋅⋅⋅hydride bond paths with considerable electron densities in the bond critical point. The clusters thermally decompose into larger, undefined, metal hydride aggregates.

Keywords: alkaline-earth metals; calcium; hydrides; self-assembly; strontium.

Publication types

  • Research Support, Non-U.S. Gov't