A novel protocol for designing a variety of topologically unique multicyclic polymer architectures, such as mono-, bi-, and tricyclic polymers as well as topological isomers, has been proposed on the basis of an electrostatic self-assembly of polymer precursors having five-membered cyclic ammonium salt groups accompanying plurifunctional carboxylate counteranions. Upon dilution in an organic medium at a concentration of below a gram per liter, the multiple aggregates of the polymer precursors completely dissociate into a smallest assembly, and cations and anions balance the charge. The subsequent covalent fixation through the ring-opening reaction of cyclic ammonium salt groups by carboxylate counteranions provides an efficient means for a variety of polymer architectures comprising mono- and multicyclic polymer units.

Summary: Due to its capability of dispensing very small volumes of different liquids in a controlled manner, ink‐jet printing is well suited for combinatorial experiments. The multi‐nozzle ink‐jet delivery system is especially advantageous for parallel chemical synthesis of different materials. We have used ink‐jet printing of an oxidizing agent to pattern a pre‐coated conducting polymer, poly(3,4‐ethylenedioxy)‐thiophene‐poly(styrene sulfonate) (PEDOT‐PSS), yielding electrodes with predefined shapes and a controlled degree of sheet resistivity for use in gray‐scale organic light‐emitting devices (OLEDs). The electrical and optical properties of the PEDOT‐PSS layer are modified via chemical interaction using the oxidizing agent. These experiments were performed using a desktop ink‐jet printer in conjunction with common graphic software which employed color functions such as CMY (cyan, magenta and yellow), HSL (hue, saturation and luminosity) and RGB (red, green and blue).Photographs of gray‐scale OLEDs patterned on PEDOT‐PSS surfaces by an ink‐jet printer on plastic substrates.magnified imagePhotographs of gray‐scale OLEDs patterned on PEDOT‐PSS surfaces by an ink‐jet printer on plastic substrates.

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A series of θ-shaped poly(tetrahydrofuran), poly(THF), of different molecular weights were effectively synthesized by an electrostatic self-assembly and covalent fixation process using a three-armed, star telechelic precursor having N-phenylpyrrolidinium salt groups carrying a trimesate, 1,3,5-benzene tricarboxylate, counteranion (1/trimesate). Under appropriate dilution in acetone, θ-shaped poly(THF)s (2) were obtained in 40-49% isolated yields through the covalent conversion of an electrostatic selfassembly of a single polymer precursor unit with retaining the balance of the charges between cations and anions. The isolated product was unequivocally characterized by means of 1 H NMR, IR, SEC as well as a reversed-phase chromatography (RPC), and MALDI-TOF MASS techniques.

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