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Reversible Dihydrogen Activation and Catalytic H/D Exchange with Group 10 Heterometallic Complexes**
Dr. Martí Garçon Dr. Andreas Phanopoulos Dr. Andrew J. P. White Prof. Dr. Mark R. Crimmin 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2023,135(2):e202213001
Reaction of a hexagonal planar palladium complex featuring a [PdMg3H3] core with H2 is reversible and leads to the formation of a new [PdMg2H4] tetrahydride species alongside an equivalent of a magnesium hydride co-product [MgH]. While the reversibility of this process prevented isolation of [PdMg2H4], analogous [PtMg2H4] and [PtZn2H4] complexes could be isolated and characterised through independent syntheses. Computational analysis (DFT, AIM, NCIPlot) of the bonding in a series of heterometallic tetrahydride compounds (Ni–Pt; Mg and Zn) suggests that these complexes are best described as square planar with marginal metal-metal interactions; the strength of which increases slightly as group 10 is descended and increases from Mg to Zn. DFT calculations support a mechanism for H2 activation involving a ligand-assisted oxidative addition to Pd. These findings were exploited to develop a catalytic protocol for H/D exchange into magnesium hydride and zinc hydride bonds. 相似文献