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Newman–Kwart rearrangement

The Newman–Kwart rearrangement is a type of rearrangement reaction in which the aryl group of an O-aryl thiocarbamate, ArOC(=S)NMe<sub>2</sub>, migrates from the oxygen atom to the sulfur atom, forming an S-aryl thiocarbamate, ArSC(=O)NMe<sub>2</sub>. The reaction is named after its discoverers, Melvin Spencer Newman and Harold Kwart. The reaction is a manifestation of the double bond rule. The Newman–Kwart reaction represents a useful synthetic tool for the preparation of thiophenol derivatives.

Mechanism

The Newman–Kwart rearrangement is intramolecular. It is generally believed to be a concerted process, proceeding via a four-membered cyclic transition state (rather than a two-step process passing through a discrete reactive intermediate). The enthalpy of activation for this transition state is generally quite high for typical substrates (ΔH<sup>‡</sup> ~ 30 to 40 kcal/mol), necessitating high reaction temperatures (200 to 300 °C, Ph<sub>2</sub>O as solvent or heat).

A Pd-catalyzed process and conditions under photoredox catalysis (both proceeding through complex multistep mechanisms) are known. These catalytic processes allow for much milder reaction conditions to be used (100 °C for Pd catalysis, ambient temperature for photoredox).

Use for preparation of thiophenols

The Newman–Kwart rearrangement is an important prelude to the synthesis of thiophenols. A phenol (1) is deprotonated with a base followed by treatment with a thiocarbamoyl chloride (2) to form an O-aryl thiocarbamate (3). Heating 3 to around 250&nbsp;°C causes it undergo Newman–Kwart rearrangement to an S-aryl thiocarbamate (4). Alkaline hydrolysis or similar cleavage yields a thiophenol (5).

See also

References