Proton-coupled electron transfer (PCET) underlies many of nature's most demanding redox processes and has emerged as a central principle in synthetic catalysis, enabling the activation of strong and otherwise inert X─H bonds (X = N, O, C) under mild conditions.[1-3] By coupling electron and proton motion, PCET lowers activation barriers and avoids high-energy ionic intermediates, thereby imparting control and selectivity in transformations ranging from enzymatic reactions to photoredox...