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ReferencesScans of 1 H and 13 C Spectra S11 S12-S63were purchased from Aldrich and used without further purification. The solvents were purchased and dried according to standard procedure prior to use. 1 1 H NMR (400 MHz) spectra were recorded with a Varian 400 spectrometer. Infrared (IR) spectra recorded on a Perkin Elmer Spectrum one FT-IR spectrometer. VKSI Medico Centrifuge machine was used for our experimental procedure for the synthesis of substituted cyanamides.

General. Amines, CS2, DIB, Et3N, Pyridine, KOH, and NaOH were purchased from Aldrich and used without further purification. The solvents were purchased and dried according to standard procedure prior to use. 1 1 H NMR (400 MHz) spectra were recorded with a Varian 400 spectrometer. Infrared (IR) spectra recorded on a Perkin Elmer Spectrum one FT-IR spectrometer.General Procedure for Aryl/Alkyl isothiocyanate: In a 10 mL round bottom flask containing a magnetic stir bar, Amine (1.0 equivalent), NaOH (1.5 equivalent) and TPGS-750-M/H2O (1wt%, 0.4 mL, 1.0 M) were sequentially added. The reaction mixture was stirred at room temperature for 2h. After starting material was completely consumed, as monitored by TLC, DIB (1.5 equivalent) and NaOH (1.5 equivalents) were sequentially added and stirring continued for 60 minutes. Then ethyl acetate (2 x 1mL) was added to the reaction mixture, which was stirred for 5 minutes. The organic layer was transferred using a Pasteur pipet and evaporated under reduced pressure to give the crude product. The residue was purified by column chromatography over silica gel by using 100% hexane as eluent to obtain isothiocyanate derivative .

Consecutive addition/domino C–S cross-coupling reaction has been developed for the synthesis of 2-arylthio arylcyanamides.