The search for sustainable synthesis has provided insight into C–C bond formation during small molecule catalysis. In contrast, methods for breaking C–C bonds are important for industrial synthesis from crude oil. As a green alternative for top-down synthesis, we will study mild electrochemically driven C–C bond cleavage in hydrocarbons to mimic oil cracking and create future paths for upcycling difficult-to-transform plastics. We will investigate alternating potential electrochemistry for combining oxidative cleavage and reductive release of hydrocarbons and polymers at metal electrodes for green fuel and chemical synthesis that will create valuable carbon feedstocks. Additives like CO or CN– can also be introduced to intercept cracked alkyl intermediates and synthesize new bonds using the potential to control the polarity of adsorbates. This work will develop new techniques to study hydrocarbon-electrode interactions and provide fundamental insight into how dynamic applied potential methods can control adsorption, oxidation, reduction, and desorption steps for sustainable synthesis.