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A Fenton reaction and a corrosion inhibition strategy were designed for enhancing the polishing rate and achieving a corrosion-free Ge1Sb4Te5 film surface during chemical-mechanical planarization (CMP) of three-dimensional (3D) cross-point phase-change random-access memory (PCRAM) cells and 3D cross-point synaptic arrays. The Fenton reaction was conducted with 1,3-propylenediamine tetraacetic acid, ferric ammonium salt (PDTA–Fe) and H2O2. The chemical oxidation degree of GeO2, Sb2O3, and TeO2 evidently increased with the PDTA–Fe concentration in the CMP slurry, such that the polishing rate of the Ge1Sb4Te5 film surface linearly increased with the PDTA–Fe concentration. The addition of a corrosion inhibitor having protonated amine functional groups in the CMP slurry remarkably suppressed the corrosion degree of the Ge1Sb4Te5 film surface after CMP; i.e., the corrosion current of the Ge1Sb4Te5 film surface linearly decreased as the corrosion inhibitor concentration increased. Thus, the proposed Fenton reaction and corrosion inhibitor in the Ge1Sb4Te5 film surface CMP slurry could achieve an almost recess-free Ge1Sb4Te5 film surface of the confined-PCRAM cells, having an aspect ratio of 60-nm-height to 4-nm-diameter after CMP.