This chapter explains the effect of compositional modification on the magnetoelectric coefficient in sintered piezoelectric – magnetostrictive composites. It was found that 15 at% doping of Pb(Zn1/3Nb2/3)O3 [PZN] in Pb(Zr0.52Ti0.48)O3 [PZT] enhances the piezoelectric and magnetoelectric properties of a PZT – 20 at% Ni0.8Zn0.2Fe2O4 [NZF] composite. The effect of doping on the ferromagnetic phase was also investigated. With increases in Zn concentration, it was found that the coercive field and Curie temperature of Ni(1-x)ZnxFe2O4 [NZF] decreases, while its saturation magnetization has a maxima at 30 mole% Zn. X-ray diffraction revealed that the lattice constant of NZF increases from 8.32 Å for 0 at% Zn to 8.39 Å for 50 at% Zn. The magnetoelectric coefficient was found to have a maxima of 144 mV/cm.Oe at 30 at% Zn. To understand better, the effect of 40% (by mole) Zn substitution on structural, piezoelectric, ferromagnetic and magnetoelectric properties of Pb(Zr0.52Ti0.48)O3 - CoFe2O4 (PZT - CFO) sintered composite is also explained. X-ray diffraction of Co0.6Zn0.4Fe2O4 (CZF) showed the shift in almost all diffraction peaks to lower diffraction angle confirming the increase in lattice parameter in all three direction from 8.378 (for CFO) to 8.395 Å for (Co,Zn)Fe2O4 (CZF). SEM and TEM results showed defect structure (cleavage, twins, strain fields) in the CZF particle, which is a clear indication of misfit strain developed due to lattice expansion. Magnetic properties measured over temperature (5 K – 1000 K) showed increased magnetization but lower magnetic Curie temperature in PZT - CZF particle. Magnetoelectric coefficient measured as function of ferrite concentration showed an increase of more than 100% after doping the CFO phase with 40% Zn. This enhancement can be attributed to increase in the lattice strain, magnetic permeability and decrease in coercivity.
