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Phosphonium‐containing polyelectrolyte networks (PENs) (P1–P4) were prepared by cyclotrimerization of bis(4‐acetylphenyl)diphenylphosphonium bromide (M1) and 1,4‐diacetylbenzene (M2) with p‐toluene sulfonic acid in various M1:M2 ratios (1,0, 1:1, 1:2, and 1:4). The relative abundance of the PAr4+ units in each PEN was demonstrated to influence thermal stability, alkaline stability, water uptake, surface area, and CO2 uptake in predictable ways. Impressively, PENs with NTf2− counterions (Tf = CF3SO3) did not exhibit 5% mass loss until heating above 400 °C. Alkaline stability, tested by challenging a PEN with 6 M NaOH(aq) at 65 °C for 120 h, increased with increasing PAr4+ content, which reflected the enhanced reactivity of the HO− anion in more hydrophobic materials (i.e., PENs with lower M1:M2 ratios). The specific surface areas estimated by Brunauer‐Emmett‐Teller (BET) analysis for these PENs were above 60 m2/g under N2 and nearly 90 m2/g under CO2. Notably, P3 (in which 33% of monomers comprise a phosphonium moiety) exhibited a CO2 uptake affinity of one CO2 molecule adsorbed for every phosphonium site. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019, 57, 598–604 Phosphonium covalent organic framework materials with various monomer feed rations and phosphonium content were studied for stability, CO2‐uptake, and specific surface area. [ABSTRACT FROM AUTHOR]

The properties of phosphonium polyelectrolytes (PELs) were evaluated in an effort to assess the influence of both side chain and main chain composition. The influence of side chain was examined by comparing properties of a series of PELs having hydrophobic octyloxy side chains to those of structural analogues lacking the side chains. The influence exerted by backbone flexibility/length of spacer between charges was revealed by comparing properties of two series of polymers with a variable number of methylene units between phosphonium charge‐bearing sites. Side chain composition and spacing between phosphonium units lead to noteworthy influence on thermal stability, glass transition, and crystallinity. The molecular structure of PELs also correlates with trends in film morphology and critical surface energy of PEL dip‐cast films. Sensitivity of morphology to humidity or water in the casting solvent was observed. Supramolecular assembly of films via layer‐by‐layer deposition of PELs alternating with anionic polythiophene derivative layers was also undertaken. The linearity of film growth, amount of material deposited in each bilayer, polycation:polyanion ratio, and film roughness all show noteworthy trends that depend on both the presence/absence of side chains and on spacing between ionic centers. The relationship between side chain and spacer on bactericidal activity against Staphylococcus aureus and Escherichia coli was assessed. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019, 57, 24–34 Phosphonium ionomers having different lengths of spacers between cationic sites were prepared. Comparison of multiple properties of these ionomers with or without hydrophobic sidechains were examined. [ABSTRACT FROM AUTHOR]