Polycrystalline Pr0.65-xGdxSr0.35MnO3 (x = 0.01, 0.05, 0.1, 0.2, 0.3) manganites were prepared by conventional solid-state method. Structural analysis has revealed a change in structure with x = 0.2, from Rhombohedral (R-3c) to Orthorhombic (Pbnm) symmetry. Small oxygen deficiency was found in the samples. The electrical measurements revealed typical colossal magnetoresistance (CMR) behavior, with single metal–insulator peak at Tp for all investigated samples. The small polaron hopping (SPH) and variable-range hopping (VRH) models were used to describe the electrical conduction above Tp. Magnetic measurements show an increase in magnetization below the Curie temperature, TC. Values of Tc diminish with increasing Gd3+ content. Isothermal measurements around critical points suggest a possible interaction between the 4f-ions and Mn-sublattice The magnetic critical behavior analysis established the tri-critical mean-field model to be the governing model for the series. Large magnetic entropy change ΔSM at near room temperature (278 K) was exhibited by the x = 0.01 sample at 2.2 J/kgK in μ0ΔH = 1 T and 5.36 J/kgK in μ0ΔH = 4 T. The largest |ΔSM| value was shown by the x = 0.1 sample. The values of the relative cooling power (RCP) and the temperature-averaged entropy change (TEC) increased with substitution qualifying these compounds as magnetocaloric materials.
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