Quantification of redox thermodynamics shifts within coacervates Edited by Catherine Murphy, University of Illinois at Urbana-Champaign, Urbana, IL; received August 7, 2025; accepted October 16, 2025 Significance The earliest enzymes are thought to have formed through the assembly of macromolecules into disordered, secondary phases known as coacervates. While these phases are believed to have played a role in early catalysis, the underlying mechanisms remain poorly understood.