In this experiment, C
3N
5 was synthesized by pyrolysis of 3-amino-1,2,4 triazole material, and then 1% Co-C
3N
5, 3% Co-C
3N
5, 5% Co-C
3N
5, 7% Co-C
3N
5, and 9% Co-C
3N
5 were synthesized by varying the mass ratio of cobalt chloride to C
3N
5 by stirring and ultrasonic shaking. SEM, XPS, and XRD tests were performed on the synthesized materials. The experimental results showed that Co atoms were successfully doped into C
3N
5. The electrocatalytic reduction experiments were performed to evaluate their NH
3 yields and electrochemical properties. The results showed that the ammonia yield obtained by the electrolysis of the 9% Co-C
3N
5 catalyst as the working electrode in a mixed electrolytic solution of 0.1 mol/L KNO
3 and 0.1 mol/L KOH for 1 h at a potential of −1.0 V vs. RHE was 0.633 ± 0.02 mmol∙h
−1∙mg
cat−1, and the Faraday efficiency was 65.98 ± 2.14%; under the same experimental conditions, the ammonia production rate and Faraday efficiency of the C
3N
5 catalyst were 0.049 mmol∙h
−1∙mg
cat−1 and 16.41%, respectively, and the ammonia production rate of the C
3N
5 catalyst was nearly 13-fold worse than the 9% Co-C
3N
5, which suggests that Co can improve the Faraday efficiency and ammonia yield of the electrocatalytic reduction of NO
3−. This is due to the strong synergistic effect between the cobalt and C
3N
5 components, with C
3N
5 providing abundant and homogeneous sites for nitrogen coordination and the Co-N species present in the material being highly efficient active sites. The slight change in current density after five trials of 9% Co-C
3N
5 and the decrease in ammonia yield by about 12% in five repetitions of the experiment indicate that 9% Co-C
3N
5 can be recycled and work stably in electrocatalytic reactions and has good application prospects.
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