This talk presents the rational molecular design of next-generation redox-active sorbents for the capture of carbon dioxide from dilute sources such as air. We discuss the electrochemical generation of organic nucleophiles (C and O-nucleophiles), with a focus on chemical species known to rapidly capture CO₂ under cathodic conditions, and that release the bound CO₂ under anodic conditions. We first introduce the thermodynamics of redox-reactive CO₂-binder chemical space for electrochemical reactive capture and release of CO₂ by electrochemically-generated nucleophiles. We then use this thermodynamic understanding to guide the synthetic development of new robust redox-reactive media for the capture of CO₂ from dilute sources that take advantage of the beneficial bulk properties of ionic liquids and the well-established redox chemistries of reduced quinones.