Significance of density functional theory (DFT) calculations for electrocatalysis of N 2 and CO 2 reduction reactions.

Density functional theory (DFT) based computational methods have shown great significance in developing high-performance electrocatalysts. In this perspective, we briefly summarized the state-of-the-art research progress of electrocatalysts for the nitrogen reduction reaction (NRR) and CO 2 reduction reaction (CO 2 RR), which are important processes for the conversion of common molecules into value-added products. With the help of DFT calculations, various modulation strategies are employed to improve the catalytic activity and performance of NRR and CO 2 RR electrocatalysts. DFT calculations are performed to confirm the surface catalytic sites, evaluate the catalytic activity, reveal the possible reaction mechanisms, and design novel structures with high catalytic performance. By discussing the currently applied computational methods and conditions during the calculations, we outlined our concerns on the prospects and future challenges of DFT calculations in electrocatalysis studies.