Pathways toward Operando Recoverable CO2 Electrolyzers

Abstract

Electrochemical CO2 conversion is approaching industrially relevant performance, yet its practical deployment is constrained by insufficient stability under realistic operating conditions. We reframe stability as a dynamic, system-wide property rather than a fixed device performance, and establish a unified multi-scale framework linking degradation pathways, detection, and corrective strategies across hierarchical levels from the active site to full-stack operation. We identify the limitations of constant-condition testing, which often misclassifies quasi-stable operation as industrial stable, and propose new measurement concepts that bridge laboratory diagnostics with real-world operating stresses. Through analyzing reversible failure modes including catalyst degradation, salt precipitation, and flooding, we organize recovery strategies that can be integrated into operational cycles for performance restoration. Building on this foundation, we chart a progression from intrinsic stability enhancement, to adaptive dynamic regulation, to fully operando recovery, in which autonomous systems are capable of operando performance restoration without interrupting production. These pathways define a research agenda for cross-disciplinary advances that could transform CO2 electrolysis from a fragile laboratory demonstration into a self-maintaining, commercially viable technology.