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Chen, Chun‐Hsing

Publications and source records attributed to Chen, Chun‐Hsing.

Heteroleptic Square Planar Cobalt(I/II) Complexes

Reduction of the cobalt(II) chloride complex, Ph 2 B( t BuIm) 2 Co(THF)Cl (1) in the presence of t BuN≡C affords the diamagnetic, square planar cobalt(I) complex Ph 2 B( t BuIm) 2 Co(C≡N t Bu) 2 (2). This is a rare example of a 16-electron cobalt(I) complex that is structurally related to square planar noble metal complexes. Accordingly, the electronic structure of 2, as calculated by DFT, reveals that the HOMO is largely d z 2 in character. Complex 2 is readily oxidized to its cobalt(II) congener [Ph 2 B( t BuIm) 2 Co(C=N t Bu) 2 ]BPh 4 (3-BPh 4 ), whose EPR spectral parameters are characteristic of low-spin d 7 with an unpaired electron in an orbital of d z 2 parentage. Further, this is also consistent with the results of DFT calculations. Despite its 16-electron configuration and the d z 2 parentage of the HOMO, the only tractable reactions of 2 involve one electron oxidation to afford 3.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Pincers with diverse donors and their interconversion: application to Ni(II)

Abstract A pincer ligand composed of a pyridine with ortho positions substituted by a bulky phosphine arm and a pyrazole arm (PNNH) is installed on nickel(II) to yield the diamagnetic planar complex [(PNNH)NiCl]Cl. The chloride anion can be replaced by BPh 4 − by a metathesis. The acidic pyrazole proton can be removed with LiN(SiMe 3 ) 2 to yield the square planar neutral molecule (PNN − )NiCl. The coordinated chloride can be metathetically replaced by azide to yield diamagnetic (PNN − )Ni(N 3 ). To evaluate changing the phosphine donor for a phosphine sulfide, the corresponding pincer ligand SPNNH was synthesized and installed on NiBr 2 . The reduced steric bulk from the more distant phosphorous keeps both halides coordinated in the paramagnetic molecular species (SPNNH)NiBr 2 . Several attempts to dehydrobrominate this species result in synthesis and characterization of two unexpected products. One effort revealed that the electrophilic character of P(V) leaves the phosphorus atom in (SPNNH)NiBr 2 vulnerable to nucleophilic attack, resulting in a P/C cleavage product which was characterized.

Cabelof, Alyssa C.↗