The demand for lithium compensation materials is becoming urgent as energy density requirements increase. As next-generation anodes, mixed silicon and carbon (Si−C) materials are limited by low efficiency in the first cycle owing to the formation of a solid electrolyte interphase film. However, most compensation materials are water-and oxygen-sensitive and exhibit low electrochemical activity and decomposition efficiency. In this study, water-and oxygen-stable lithium oxalate (Li 2 C 2 O 4 ) was developed to enhance the capacity and cycle-life of the lithium-ion battery. Various metal oxides were screened to improve the electrochemical activity of Li 2 C 2 O 4 . Co 3 O 4 exhibited the strongest catalytic performance, and the catalytic mechanism of Co 3 O 4 on Li 2 C 2 O 4 was studied by density functional theory. Ultrasonic atomization drying was used to combine Co 3 O 4 quantum dots (Co 3 O 4 -QDs) with Li 2 C 2 O 4 for improved efficiency. The electrochemical activity of the modified Li 2 C 2 O 4 improved, and the decomposition voltage decreased from 4.65 to 4.0 V. The modified Li 2 C 2 O 4 exhibits catalytic activity, and it can be used in LiFePO 4 , which has weak catalytic activity; the decomposition efficiency in the LiFePO 4 system increased from 34.16 to 99.10%. In the Si−C//LiFePO 4 full battery system, the first cycle discharge capacity increased from 80 to 160 mA h g −1 ; the lost capacity of the first cycle was fully compensated for. Additionally, the CO 2 produced by Li 2 C 2 O 4 decomposition could inhibit the decomposition of the electrolyte, further improving the cycle performance of the battery.