We now describe an additional useful and more surprising dimension to the selectivity displayed by this reagent combination in the alkylation of arylenediamines. When we initially exposed a phenylenediamine to the NaY-catalysed dialkyl carbonate alkylation reaction conditions, we had expected to observe N,N′-dialkylation. In fact these conditions lead to highly selective—sometimes specific—mono-N-alkylation of just one of the amino groups ...