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Self-assembled metallasupramolecular cages towards light harvesting systems for oxidative cyclization

Kumar, A and Saha, R and Mukherjee, PS (2021) Self-assembled metallasupramolecular cages towards light harvesting systems for oxidative cyclization. In: Chemical Science, 12 (14). pp. 5319-5329.

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Official URL: https://doi.org/10.1039/d1sc00097g


Designing artificial light harvesting systems with the ability to utilize the output energy for fruitful application in aqueous medium is an intriguing topic for the development of clean and sustainable energy. We report here facile synthesis of three prismatic molecular cages as imminent supramolecular optoelectronic materialsviatwo-component coordination-driven self-assembly of a new tetra-imidazole donor (L) in combination with 180°/120° di-platinum(ii) acceptors. Self-assembly of 180°trans-Pt(ii) acceptorsA1andA2withLleads to the formation of cages Pt4L2(1a) and Pt8L2(2a) respectively, while 120°-Pt(ii) acceptorA3withLgives the Pt8L2(3a) metallacage. PF6�analogues (1b,2band3b) of the metallacages possess a high molar extinction coefficient and large Stokes shift.1b-3bare weakly emissive in dilute solution but showed aggregation induced emission (AIE) in a water/MeCN mixture as well as in the solid state. AIE active2band3bin aqueous (90 water/MeCN mixture) medium act as donors for fabricating artificial light harvesting systemsviaFörster resonance energy transfer (FRET) with organic dye rhodamine-B (RhB) with high energy efficiency and good antenna effect. The metallacages2band3brepresent an interesting platform to fabricate new generation supramolecular aqueous light harvesting systems with high antenna effect. Finally, the harvested energy of the LHSs (2b+RhB) and (3b+RhB) was utilized successfully for efficient visible light induced photo-oxidative cross coupling cyclization ofN,N-dimethylaniline (4) with a series ofN-alkyl/aryl maleimides (5) in aqueous acetonitrile with dramatic enhancement in yields compared to the reactions withRhBor cages alone. © The Royal Society of Chemistry 2021.

Item Type: Journal Article
Publication: Chemical Science
Publisher: Royal Society of Chemistry
Additional Information: The copyright for this article belongs to Authors
Keywords: Antennas; Coordination reactions; Cyclization; Energy efficiency; Energy transfer; Harvesting; Image enhancement; Light; Metals; Mixtures; Rhodamine B; Rhodium compounds; Supramolecular chemistry, Aggregation-induced emissions; Artificial light harvesting; Coordination-driven self assembly; Cross-coupling-cyclization; High energy efficiency; Light-harvesting systems; Molar extinction coefficient; Resonance energy transfer, Platinum compounds
Department/Centre: Division of Chemical Sciences > Inorganic & Physical Chemistry
Date Deposited: 14 Jul 2021 10:12
Last Modified: 14 Jul 2021 10:12
URI: http://eprints.iisc.ac.in/id/eprint/68789

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