Trifunctional electrocatalysts of single transition metal atom doped g-C4N3 with high performance for OER, ORR and HER

With the rapid development of renewable energy technologies, the quest for efficient and cost-effective trifunctional catalysts capable of simultaneously driving the Hydrogen Evolution Reaction (HER), Oxygen Reduction Reaction (ORR), and Oxygen Evolution Reactions (OER) has become a focal point of research. In this study, we employed first-principles calculations to investigate the catalytic activities of the synthetic material g-C4N3 as an electrocatalyst for HER, OER, and ORR by incorporating various transition metal atoms into the numerous 3 N vacancies (TM@g-C4N3) naturally occurring in its primitive structure. Our calculations reveal that Cu@g-C4N3 holds promise as a trifunctional electrocatalyst, exhibiting low OER/ORR overpotentials (ηOER = ηORR = 0.44 V) and a |ΔG∗H| value of only 0.08 eV. Furthermore, Ni@g-C4N3_S1N2 exhibits a lower OER overpotential (ηOER = 0.34 V). Bader charge analysis, charge density difference calculations, and D-band center investigations confirm that the catalytic performance is fundamentally rooted in the electronic properties of these materials. Thus, g-C4N3 embedded with transition metal atoms shows promise as an efficient electrocatalyst for OER/ORR/HER, with implications for the development of high-efficiency trifunctional electrocatalysts.