We present magnetotransport and 209 Bi nuclear magnetic resonance (NMR) data on a series of single crystals of Bi2Se3, Bi2Te2Se and CuxBi2Se3 with varying carrier concentrations. The Knight shift of the bulk nuclei is strongly correlated with the carrier concentration via a hyperfine coupling of 27 µeV, which may have important consequences for scattering of the protected surface states. Surprisingly we find that the NMR linewidths and the spin lattice relaxation rate appear to be dominated by the presence of localized spins, which may be related to the presence of Se vacancies.