%0 Journal Article %T Designing electrochemically reversible H2 oxidation and production catalysts %J - %D 2018 %R https://doi.org/10.1038/s41570-018-0032-8 %X The most energy-efficient electrocatalysts mediate forward and reverse reactions at high rates with minimal overpotential requirements. Such electrocatalytic reversibility is commonly observed for redox enzymes and is an attribute that we have sought to bestow on synthetic molecules to realize highly active and robust catalysts for applications in renewable energy. The recent development of the first synthetic molecular catalysts that reversibly mediate H2£¿£¿£¿2£¿H+£¿+£¿2e£¿ exploits an enzyme-inspired outer coordination sphere that works in concert with both first and second coordination spheres. In this Perspective, we discuss a series of molecular Ni catalysts for H2 production and oxidation that exhibit electrochemical reversibility. Study of these catalysts allows us to identify important first, second and outer coordination sphere features necessary for efficient conversions of H2 and provides direction for the rational design of electrocatalysts that operate on other small molecules %U https://www.nature.com/articles/s41570-018-0032-8