“…The basic component of the insulating paper sample used in our work is cellulose, a molecular chain containing multiple hydroxyl and aldehyde groups. The oxygen atoms of hydroxyl and aldehyde groups have strong electronegativity, consequently, it has high affinity for negative charges and tends to attract negative ions in insulating oil. ,, According to Koopmans’ theorem, the electron affinity energy can be approximately represented with the lowest unoccupied molecular orbital energy ( E LOMO ). , The partial density of states (PDOS) of the oil–paper interface structure is calculated by the Perdew–Burke–Ernzerhof (PBE) functional (details are given in the Supporting Information), as shown in Figure a,b, E LOMO of insulating paper is 20% lower than that of insulating oil, which means that insulating paper is more likely to become an electron acceptor in the oil–paper insulation system.…”