Our work on the photoredox-catalyzed oxidation of anions to generate electrophilic radicals is published in The Journal of Organic Chemistry! This work generates 1,3-dicarbonyl and amidyl radicals by a stepwise proton-coupled electron transfer process for the functionalization of alkenes. The result is a highly atom-economical process for hydro-, amido-, and dialkylation of alkenes. We used experimental and computational mechanistic experiments to understand the role of the catalyst as an electron shuttle between starting material and product molecules.