We study the effects of Zn substitution on single crystals of the low-dimensional multiferroicmaterial Cu3Mo2O9. We report the magnetic field-temperature phase diagram obtained from thetemperature and the magnetic field dependences of the specific heat, the dielectric constant, thedifferential magnetization, and the electric polarization-electric field curve in Cu2.85Zn0.15Mo2O9. We obtain three phases: a paraelectric and a ferroelectric phase, and a ferroelectric phase with alarge coercive electric field. The origin of the last one is discussed based on the charge redistributioneffect on a half-filled Mott insulator. In this phase, the Zn substitution induces a robust localizedferroelectric polarization that increases the coercive electric field.