Lithiated graphitic carbon nitride (C3N4) was fabricated by electrochemical and solid-state reactions. The addition of Li to C3N4 results in a reaction between the Li and the graphite-like C3N species in C3N4. This irreversible reaction leads to the formation of Li-CHNR and Li-NCR2 species, which are detrimental to anode properties. Suitable nitrogen-doped carbon structures for anode applications are predicted to need high concentrations of pyridinic C–N–C terminal bonds and low concentrations of quaternary C3N species to boost electronic conductivity and reversibly cycle Li ions.

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