Mechanism-Guided Triple Defense of Solid Deposition Enabling Durable Electrochemical Cement Clinker Precursor Synthesis

Abstract Electrifying cement production offers a viable pathway to decarbonize one of the world’s most CO2-intensive industries. Electrochemical synthesis of cement clinker precursors enables low-temperature manufacturing but is constrained by solid deposition, reactor blockage, and voltage instability that limit durability. Here, we identify the dominant deposition-induced degradation pathway in a three-chamber electrochemical reactor and develop mechanism-guided mitigation strategies. The voltage rise is governed by ohmic loss from Ca(OH)2 accumulation in the middle chamber, while coupled experiments and simulations reveal that hydrodynamic heterogeneity creates low-velocity zones that promote particle retention. Guided by these insights, a synergistic triple-defense strategy integrating flow-field redesign, electrolyte regulation, and surface wettability control suppresses deposition at multiple origins. As a consequence, these coordinated interventions extend continuous reactor operation from ∼1 to ∼9 h without sacrificing Faradaic efficiency. Furthermore, the strategy was validated in a scaled-up reactor with an effective electrode area of 100 cm2, achieving stable operation for 100 h at 5 A (50 mA cm–2). This work elucidates deposition-driven degradation mechanisms and establishes general design principles for durable electrochemical reactors for industrial decarbonization.