The synthesis of hitherto unknown thiazole derivatives have been disclosed via purely green approach. This proposed work is novel in terms of C−C bond formation at guanidino carbon in 2‐amino benzimidazole moiety. The unstable benzimidazol‐hemiaminals have been used as a source of reactive intermediates.The catalyst‐free synthesis of diamino benzoyl N‐tosyl thiazole governed bythe sequential chemical conversions, which was steered by simple N‐tosylation of benzimidazol‐hemiaminal. The reaction was internally edge forward by thiazolidine ring opening, N‐tosylation, C−C bond formation and regioselective cleavage of C−N bondat guanidino carbon in a single step. Oxidation of tertiary alcohol to ketone with ring opening by C−N bond cleavage and N‐tosylation are the valuable conversions to accomplish the regioselectivity in the development of new desired thiazole ring. Moreover benzimidazol‐hemiaminal used as a storage of 2‐oxo‐2‐phenylethyl N′‐(1H‐benzo[d]imidazol‐2‐yl)‐N‐phenylcarbamimidothioate which is again highly unstable intermediate. The reverse back step mechanism was developed for the synthesis of thiazoles unlike other hemiaminals. The protocol is free of catalyst and toxic solvents.Use of ionic liquid, shorter reaction time, high yielding and easy isolation of products makes this strategy more environmental‐friendly. The importance of products attributed to the presence of active benzoyl and amino groups. Product thiazoles (T3) (IC50=7.906 μM), (T4) (IC50=5.250 μM) and (T7) (IC50=4.709 μM) were found potent anticancer agents against lung cancer with reference to doxorubicin as standard.

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A current report expresses that Orange Peel Extract use as catalyticmedium for the synthesis of Indoloquinoxaline derivatives from commercially available starting materials. Isatin and O-phenylenediamine in presence of fresh orange peel extractresulted into desired product at room temperature in a given reaction condition. Advantages of this method include greener and cleaner conditions, shorter reaction time, and good to moderate yield of products. A simple one-pot procedure has been developed for the synthesis of Indoloquinoxaline derivatives from readily available starting materials.