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Bromide abstraction from the three-coordinate Ni(i) ring-expanded N-heterocyclic carbene complex [Ni(6-Mes)(PPh 3 )Br] (1; 6-Mes = 1,3-bis(2,4,6-trimethylphenyl)-3,4,5,6-tetrahydropyrimidin-2-ylidene) with TlPF 6 in THF yields the T-shaped cationic solvent complex, [Ni(6-Mes)(PPh 3 )(THF)][PF 6 ] (2), whereas treatment with NaBAr F  4 in Et 2 O affords the dimeric Ni(i) product, [{Ni(6-Mes)(PPh 3 )} 2 (μ-Br)][BAr F  4 ] (3). Both 2 and 3 act as latent sources of the cation [Ni(6-Mes)(PPh 3 )] + , which can be trapped by CO to give [Ni(6-Mes)(PPh 3 )(CO)] + (5). Addition of [(Et 3 Si) 2 (μ-H)][B(C 6 F 5 ) 4 ] to 1 followed by work up in toluene results in the elimination of phosphine as well as halide to afford a co-crystallised mixture of [Ni(6-Mes)(η 2 -C 6 H 5 Me)][B(C 6 F 5 ) 4 ] (4), and [6MesHC 6 H 5 Me][B(C 6 F 5 ) 4 ]. Treatment of 1 with sodium salts of more strongly coordinating anions leads to substitution products. Thus, NaBH 4 yields the neutral, diamagnetic dimer [{Ni(6-Mes)} 2 (BH 4 ) 2 ] (6), whereas NaBH 3 (CN) gives the paramagnetic monomeric cyanotrihydroborate complex [Ni(6-Mes)(PPh 3 )(NCBH 3 )] (7). Treatment of 1 with NaO t Bu/NHPh 2 affords the three-coordinate Ni(i) amido species, [Ni(6-Mes)(PPh 3 )(NPh 2 )] (8). The electronic structures of 2, 5, 7 and 8 have been analysed in comparison to that of previously reported 1 using a combination of EPR spectroscopy and density functional theory.

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Mono- and dinuclear Ni(<scp>i</scp>) products formed upon bromide abstraction from the Ni(<scp>i</scp>) ring-expanded NHC complex [Ni(6-Mes)(PPh<sub>3</sub>)Br]

Mono- and dinuclear Ni(i) products formed upon bromide abstraction from the Ni(i) ring-expanded NHC complex [Ni(6-Mes)(PPh3)Br]

Mono- and dinuclear Ni(i) products formed upon bromide abstraction from the Ni(i) ring-expanded NHC complex [Ni(6-Mes)(PPh₃)Br]