MicroED characterization of a robust cationic σ-alkane complex stabilized by the [B(3,5-(SF(5))(2)C(6)H(3))(4)](-) anion, via on-grid solid/gas single-crystal to single-crystal reactivity

利用微区电子衍射(MicroED)表征了由[B(3,5-(SF(5))(2)C(6)H(3))(4)](-)阴离子稳定的稳定阳离子σ-烷烃配合物,通过网格上固/气单晶到单晶反应

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Abstract

Microcrystalline (∼1 μm) [Rh(Cy(2)PCH(2)CH(2)PCy(2))(norbornadiene)][S-BAr(F)(4)], [S-BAr(F)(4)] = [B(3,5-(SF(5))(2)C(6)H(3))(4)](-), reacts with H(2) in a single-crystal to single-crystal transformation to form the σ-alkane complex [Rh(Cy(2)PCH(2)CH(2)PCy(2))(norbornane)][S-BAr(F)(4)], for which the structure was determined by microcrystal Electron Diffraction (microED), to 0.95 Å resolution, via an on-grid hydrogenation, and a complementary single-crystal X-ray diffraction study on larger, but challenging to isolate, crystals. Comparison with the [BAr(F)(4)](-) analogue [Ar(F) = 3,5-(CF(3))(2)(C(6)H(3))] shows that the [S-BAr(F)(4)](-) anion makes the σ-alkane complex robust towards decomposition both thermally and when suspended in pentane. Subsequent reactivity with dissolved ethene in a pentane slurry, forms [Rh(Cy(2)PCH(2)CH(2)PCy(2))(ethene)(2)][S-BAr(F)(4)], and the catalytic dimerisation/isomerisation of ethene to 2-butenes. The increased stability of [S-BAr(F)(4)](-) salts is identified as being due to increased non-covalent interactions in the lattice, resulting in a solid-state molecular organometallic material with desirable stability characteristics.

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