The activation of molecular nitrogen toward reduction is key to the efficient synthesis of valuable ammonia-based agricultural fertilizers. With this in mind, we have explored the electrocatalytic reduction and oxidation of N₂ with a range of materials, including Re, Ni, and Fe metals predicted to have high nitrogen reduction activity via DFT calculations. The activity of these electrocatalytic materials toward nitrogen reduction and oxidation was evaluated under a range pressures (1-50 bar) and under a range of electrolyte conditions, including various pH levels, solvents (H₂O, ethanol, THF), and supporting electrolyte salts (Li⁺, Na⁺, K⁺) to understand and minimize the loss of Faradaic efficiency for nitrogen due to concurrent hydrogen evolution. Our experimental results were compared to computationally predicted nitrogen reduction electrocatalytic activities in order to understand the mechanism of N₂ activation as well as improve computational methods for further theory-based hypothesis generation and catalyst selection.