Abstract
The design of crystalline polymers is intellectually stimulating and synthetically challenging, especially when the polymerization of any monomer occurs in a linear dimension. Such linear growth often leads to entropically driven chain entanglements and thus is detrimental to attempts to realize the full potential of conjugated molecular structures. Here we report the polymerization of two-monomer-connected precursors (TMCPs) in which two pyrrole units are linked through a connector, yielding highly crystalline polymers. The simultaneous growth of the TMCP results in a close-packed crystal in polypyrrole (PPy) at the molecular scale with either a hexagonal close-packed or face-centred cubic structure, as confirmed by high-voltage electron microscopy, and the structure that formed could be controlled by simply changing the connector. The electrical conductivity of the TMCP-based PPy is almost 35 times that of single-monomer-based PPy, demonstrating its promise for application in diverse fields.
Highlights
The design of crystalline polymers is intellectually stimulating and synthetically challenging, especially when the polymerization of any monomer occurs in a linear dimension
We identified a primary metallic crystalline structure at the molecular scale in the P(Py:disulfonic acids (DSAs):Py)s (where a P(Py:DSA:Py) is a polymer synthesized from a two-monomer-connected precursors (TMCPs) composed of Py and a DSA) that could manifest as either hexagonal close-packed (HCP) or face-centred cubic (FCC); the structure that formed could be controlled by changing the connector
When polymerization proceeds with a TMCP, unlike for a single monomer, the four reactive sites of the TMCP impose a constraint on the direction of propagation, thereby preventing randomly oriented chain growth (Fig. 1a)
Summary
The design of crystalline polymers is intellectually stimulating and synthetically challenging, especially when the polymerization of any monomer occurs in a linear dimension. Several efforts have been made[17,18,19] to synthesize crystalline polymers via simple processes and to study their crystal structures using high-resolution transmission electron microscopy (HRTEM) and X-ray diffraction.
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