Iron plays a central role in the two major processes that convert nitrogen in the atmosphere to fertilizers needed for the food on our plates. The enzyme nitrogenase uses an iron-sulfur cluster, while the Haber-Bosch process uses a solid iron catalyst. Despite intense research, the catalytic mechanisms are not understood at an atomic level of detail. We will discuss how advances in the synthesis of low-coordinate iron coordination compounds have led to new insights into both processes. These have included the first iron complexes with in which the nitrogen-nitrogen bond of N2 is broken, as well as biomimetic systems. These new research results help chemists to understand elementary steps in the conversion of N2 to ammonia, and the talk will highlight parallels between solution, enzyme, and surface chemistry.