Litcius/Paper detail

Efficient Synthesis of Dipyrrolobenzenes and Dipyrrolopyrazines <i>via</i> Bidirectional Gold Catalysis: a Combined Synthetic and Photophysical Study

Robin Heckershoff, Tobias Schnitzer, Tim Diederich, Lukas Eberle, Petra Krämer, Frank Röminger, Matthias Rudolph, A. Stephen K. Hashmi

2022Journal of the American Chemical Society26 citationsDOIOpen Access PDF

Abstract

New N-heterocyclic fluorophores are sought-after compounds for organic electronic devices. Here, we report on a straightforward synthesis to access meta/para-dipyrrolobenzenes and para-dipyrrolopyrazines in high yields using a bidirectional gold-catalyzed cyclization strategy. The versatility of our reaction protocol was showcased by preparing dipyrroloarenes with different substituents, various functional groups, and in a multitude of substitution patterns. Furthermore, we showed that the dipyrroloarenes can be post-modified by N-alkylation to improve the solubility or bromination to yield precursors for further derivatization via cross-coupling. Investigation of the photophysical properties of the─mostly unprecedented─dipyrroloarenes identified strong blue emitters such as the diphenyl meta-dipyrrolobenzene with a quantum yield of 98%. Moreover, we showed that changes in the solvent polarity or interactions with Lewis acids such as borane can be used to fine-tune the photophysical properties of the fluorophores.

Topics & Concepts

ChemistryQuantum yieldCombinatorial chemistryYield (engineering)CatalysisHalogenationAlkylationDerivatizationBoraneLewis acids and basesFluorescencePhotochemistryOrganic chemistryPhysicsMaterials scienceMetallurgyQuantum mechanicsHigh-performance liquid chromatographyCatalytic Alkyne ReactionsCyclopropane Reaction MechanismsCatalytic Cross-Coupling Reactions