Computational studies on transition metal and nitrogen atoms co-doped fullerene as an efficient electrocatalyst for nitrate reduction to ammonia

Persistent accumulation of nitrate in water causes an imbalance in the nitrogen cycle in the earth, posing a serious risk to human health and the ecosystem. The technique for electro catalyzing nitrate reduction has become widely employed due to the rapid development of efficient catalysts. Transition metal (TM)-based catalysts are highly sought due to their low cost and excellent catalytic activity. TM and nitrogen co-doped fullerene (TMN-C₆₀) were constructed and investigated for nitrate reduction reaction (NO₃RR) using DFT and AIMD. FeN-C₆₀ has been discovered to have a low limiting potential of − 0.56 V based on typical hydrogen electrode model, making it a potential candidate for NO₃RR. The analysis of PDOS demonstrates the considerable pd hybridization and the interactions between dopants and C₆₀. FeN-C₆₀ is stable over 400 K, confirming its sustainability in the electrocatalysis. Periodic spin-polarized DFT calculations were carried out using the DMol³ package, utilizing the GGA-PBE functional and DND basis set. The DSPP technique and Grimme correction were applied to address core electrons and accurately correct dispersion force, respectively. Thermal smearing was set to 5.0 × 10⁻³ Ha. AIMD simulations were implemented using NVT ensemble at 400 K. The total simulation time of 10 ps with 1 fs time step was used.