Ultrastable and Moisture-Adaptive Ozone Decomposition over FeOOH@NiFe-LDH via Interfacial Ni–O–Fe Bonds

Catalytic decomposition is regarded as a promising strategy for eliminating residual ozone (O3) in ambient environments. However, most catalysts suffer from rapid deactivation under humid conditions due to competitive H2O adsorption and accumulation of peroxide intermediates (O22-). Here, we report a moisture-adaptive FeOOH@NiFe layered double hydroxide (LDH) catalyst that enables efficient and stable O3 decomposition by interfacial Ni-O-Fe bond engineering. Unlike conventional vacancy-dominated mechanisms, the FeOOH@NiFe-LDH catalyst actively utilizes water as a cooperative reactant through adaptive surface reconstruction into Ni(Fe)OOH species during reaction. In situ spectroscopy combined with density functional theory calculations reveal that interfacial electronic coupling between FeOOH and NiFe-LDH promotes synergistic activation of O3 and H2O, lowers reaction energy barriers, and suppresses the accumulation of deactivating O22-. As a result, FeOOH@NiFe-LDH achieves nearly complete O3 conversion at a high space velocity (1200 L g-1 h-1) across a wide humidity range and retains 100% efficiency even after more than 140 h of reaction. Importantly, the catalyst preserves its activity upon kilogram-scale synthesis and demonstrates rapid O3 removal in a 30 m3 environmental chamber. This work establishes an interfacial, moisture-adaptive catalytic paradigm for O3 abatement and provides practical design principles for air pollution control under realistic humid conditions.