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Aminophosphine

In organophosphorus chemistry, aminophosphines are compounds with the formula R<sub>3−n</sub>P(NR<sub>2</sub>)<sub>n</sub> where R is a hydrogen or organic substituent, and n = 0, 1, or 2. At one extreme, the parents H<sub>2</sub>PNH<sub>2</sub> and are lightly studied and fragile. At the other extreme, tris(dimethylamino)phosphine (P(NMe<sub>2</sub>)<sub>3</sub>) is commonly available. Intermediate members are known, such as Ph<sub>2</sub>PN(H)Ph. Aminophosphines are typically colorless and reactive to oxygen. Aminophosphines are pyramidal geometry at phosphorus.

Parent members

The fundamental aminophosphines have the formulae PH<sub>3−n</sub>(NH<sub>2</sub>)<sub>n</sub> (n = 1, 2, or 3). Fundamental aminophosphines can not be isolated in a practical quantities but have been examined theoretically. H<sub>2</sub>NPH<sub>2</sub> is predicted to be more stable than the P(V) tautomer HN=PH<sub>3</sub>.

Secondary amines are more straightforward. Trisaminophosphines are made by treating phosphorus trichloride with secondary amines:

PCl<sub>3</sub> + 6 HNMe<sub>2</sub> → (Me<sub>2</sub>N)<sub>3</sub>P + 3 [H<sub>2</sub>NMe<sub>2</sub>]Cl

where Me = methyl.

Aminophosphine chlorides

The amination of phosphorus trihalides occur sequentially, with each amination proceeding slower than before:

PCl<sub>3</sub> + 2 HNMe<sub>2</sub> → Me<sub>2</sub>NPCl<sub>2</sub> + [H<sub>2</sub>NMe<sub>2</sub>]Cl
Me<sub>2</sub>NPCl<sub>2</sub> + 2 HNMe<sub>2</sub> → (Me<sub>2</sub>N)<sub>2</sub>PCl + [H<sub>2</sub>NMe<sub>2</sub>]Cl
(Me<sub>2</sub>N)<sub>2</sub>PCl + 2 HNMe<sub>2</sub> → (Me<sub>2</sub>N)<sub>3</sub>P + [H<sub>2</sub>NMe<sub>2</sub>]Cl

Monosubstitution selectivity improves with bulky amines such as diisopropylamine. Commercially available aminophosphine chlorides include dimethylaminophosphorus dichloride and bis(dimethylamino)phosphorus chloride.

Methylamine and trifluorophosphine react to give MeN(PF<sub>2</sub>)<sub>2</sub>:

2 PF<sub>3</sub> + 3 MeNH<sub>2</sub> → MeN(PF<sub>2</sub>)<sub>2</sub> + 2 [MeNH<sub>3</sub>]F

MeN(PF<sub>2</sub>)<sub>2</sub> is a bridging ligand in organometallic chemistry.

Aminophosphines can also made from organophosphorus chlorides and amines. Chlorodiphenylphosphine and diethylamine react to give an aminophosphine:

Ph<sub>2</sub>PCl + 2 HNEt<sub>2</sub> → Ph<sub>2</sub>PNEt<sub>2</sub> + [H<sub>2</sub>NEt<sub>2</sub>]Cl

Primary amines react with phosphorus(III) chlorides to give aminophosphines with acidic α-NH centers:

Ph<sub>2</sub>PCl + 2 H<sub>2</sub>NR → Ph<sub>2</sub>PN(H)R + [H<sub>3</sub>NR]Cl

Reactions

Protonolysis

Protic reagents attack the P-N bond. Alcoholysis readily occurs:

Ph<sub>2</sub>PNEt<sub>2</sub> + ROH → Ph<sub>2</sub>POR + HNEt<sub>2</sub>

The P-N bond reverts to the chloride when treated with anhydrous hydrogen chloride:

Ph<sub>2</sub>PNEt<sub>2</sub> + HCl → Ph<sub>2</sub>PCl + HNEt<sub>2</sub>

Transamination similarly converts one aminophosphine to another:

P(NMe<sub>2</sub>)<sub>3</sub> + R<sub>2</sub>NH ⇌ P(NR<sub>2</sub>)(NMe<sub>2</sub>)<sub>2</sub> + HNMe<sub>2</sub>

With tris(dimethylamino)phosphine, dimethylamine evaporation can drive the equilibrium.

Since Grignard reagents do not attack P-NR<sub>2</sub> bond, aminophosphine chlorides are useful reagents in preparing unsymmetrical tertiary phosphines. Illustrative is converting dimethylaminophosphorus dichloride to chlorodimethylphosphine:

2 MeMgBr + Me<sub>2</sub>NPCl<sub>2</sub> → Me<sub>2</sub>NPMe<sub>2</sub> + 2 MgBrCl
Me<sub>2</sub>NPMe<sub>2</sub> + 2 HCl → ClPMe<sub>2</sub> + Me<sub>2</sub>NH<sub>2</sub>Cl

Also, illustrative is the synthesis of 1,2-bis(dichlorophosphino)benzene using (Et<sub>2</sub>N)<sub>2</sub>PCl (Et = ethyl). This route gives C<sub>6</sub>H<sub>4</sub>[P(NEt<sub>2</sub>)<sub>2</sub>]<sub>2</sub>, which is treated with hydrogen chloride:

C<sub>6</sub>H<sub>4</sub>[P(NEt<sub>2</sub>)<sub>2</sub>]<sub>2</sub> + 8 HCl → C<sub>6</sub>H<sub>4</sub>(PCl<sub>2</sub>)<sub>2</sub> + 4 Et<sub>2</sub>NH<sub>2</sub>Cl

Conversion to phosphenium salts

Diaminophosphorus chlorides and tris(dimethylamino)phosphine are precursors to phosphenium ions of the type [(R<sub>2</sub>N)<sub>2</sub>P]<sup>+</sup>:

R<sub>2</sub>PCl + AlCl<sub>3</sub> → [R<sub>2</sub>P<sup>+</sup>]AlCl<sub>4</sub><sup>−</sup>
P(NMe<sub>2</sub>)<sub>3</sub> + 2 HOTf → [P(NMe<sub>2</sub>)<sub>2</sub>]OTf + [H<sub>2</sub>NMe<sub>2</sub>]OTf

Oxidation and quaternization

Typical aminophosphines oxidize. Alkylation, such as by methyl iodide, gives the phosphonium cation.

Addition to carbonyls

In diazaphospholenes the polarity of the P-H bond is inverted compared to traditional secondary phosphines. They have some hydridic character. One manifestation of this polarity is their reactivity toward benzophenone in yet another way.

References