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Amine compounds can greatly enhance the thermal stability of the insulating paper used in paper-oil insulation. Many research documents focus on paper's excellent thermal stability, but less attention has been paid to the effect of oil on paper's degradation. In this research paper, we study the influence of different amine compounds on the thermal stability of both paper and oil, and a mechanism for the influence on paper-oil insulation as well as an optimal formula are proposed. First, six groups of paper were modified with different proportions of dicyandiamide (DICY), melamine, and polyacrylamide (PAM). Then, an accelerated thermal aging test at 130 °C was conducted for 30 days and the thermal aging characteristics of the oil-modified paper insulation were measured. The results showed that the thermal stability of the insulation paper modified with the amine compounds was remarkably improved, and P2 (2.25 wt % melamine, 0.75 wt % DICY, and 0.2 wt % PAM) presented the best anti-aging properties. However, certain properties of oil were influenced, such as acid value, and it was found that the ammonia produced by the amine stabilizers increased the copper compound content, which led to the deterioration of the insulating oil. Moreover, using a front-line orbital energy analysis by molecule modeling, it was determined that melamine was the core thermal stabilizer for the paper among the three amine compounds used in P2. [ABSTRACT FROM AUTHOR]