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Summary: The hydrodynamic and conformational properties of polyelectrolyte poly(N,N‐diallyl‐N,N‐dimethylammonium chloride) and its corresponding polybetaine poly(2‐diallyl(methyl)ammonio)acetate) molecules in aqueous solutions with various ionic strength and pH, were studied by viscometry, static and dynamic light scattering methods. It was established that a 1 M NaCl solution is a thermodynamically good solvent for poly(N,N‐diallyl‐N,N‐dimethylammonium chloride). In water solutions conformation of poly(2‐diallyl(methyl)ammonio)acetate) molecules corresponds to polymer coil under θ–conditions. An increase in the concentration of NaCl in water and 0.1M NaOH solutions from 0 to 1 mol/l brings about a sharp gain in the intrinsic viscosity of the polymer and in the hydrodynamic radius of molecules. This effect results from the decomposition of zwitterion pairs responsible for the compact conformation of polymer molecules in water and 0.1 M NaOH. The Kuhn segment length for poly(2‐diallyl(methyl)ammonio)acetate) molecules A = 6.3 nm determined in water and in 0.1 M NaOH solutions practically coincided with A value 6.6 nm, received in 1 M NaCl and in 0.1 M NaOH/1M NaCl. For poly(N,N‐diallyl‐N,N‐dimethylammonium chloride) molecules in 1 M NaCl solutions A = 3.9 nm.

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