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MnO, as a promising anode for lithium-ion batteries, is easy to form high-valence manganese oxides during the battery operation, causing a continuous capacity increase and hindering practical applications. Herein, an effective approach for regulating the electrochemical capacity trend is presented with the guide of the thermodynamic calculations. According to the calculated Ellingham diagrams, the potential metals (Me = Fe, Sn, Co, Ni, and Cu) were selected to synthesize the Me–MnO composite anode materials. The cycling test results indicate that the selected metals show the abilities to inhibit the further oxidation of Mn2+ and regulate the capacity in the order of Fe < Sn < Co < Ni < Cu. The mechanism of the electrochemical reaction sequence is clarified based on the thermodynamic properties. This approach provides a rational design of electrode materials for improved performance via a hybrid electrochemistry-thermodynamics analysis.

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