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Externally Regulated Specific Molecular Recognition Driven Pathway Selectivity in Supramolecular Polymerization
Author(s) -
Chakraborty Anwesha,
Manna Rabindra Nath,
Paul Ankan,
Ghosh Suhrit
Publication year - 2021
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.202101492
Subject(s) - supramolecular chemistry , polymerization , monomer , nucleation , stacking , chemistry , polymer chemistry , supramolecular polymers , dimer , crystallography , combinatorial chemistry , molecule , polymer , organic chemistry
Abstract This article reveals 4‐dimethylaminopyridine (DMAP) regulated pathway selectivity in the supramolecular polymerization of a naphthalene‐diimide derivative (NDI‐1), appended with a carboxylic acid group. In decane, NDI‐1 produces ill‐defined aggregate (Agg‐1) due to different H‐bonding motifs of the −COOH group. With one mole equivalent DMAP, the NDI‐1/DMAP complex introduces new nucleation condition and exhibits a cooperative supramolecular polymerization producing J‐aggregated fibrillar nanostructure (Agg‐2). With 10 % DMAP and fast cooling (10 K/min), similar nucleation and open chain H‐bonding with the free monomer in an anti‐parallel arrangement produces identical J‐aggregate (Agg‐2a). With 2.5 % DMAP and slow cooling (1 K/min), a distinct nucleation and supramolecular polymerization pathway emerge leading to the thermodynamically controlled Agg‐3 with face‐to‐face stacking and 2D‐morphology. Slow cooling with 5–10 % DMAP produces a mixture of Agg‐2a and Agg‐3. Computational modelling studies provide valuable insights into the internal order and the pathway complexity.

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