Pollutant‐Powered Oxygen Activation by Enzyme‐Inspired Self‐Sustaining Catalytic Membranes for Water Purification

Abstract Conventional catalytic water purification remains energy‐ and chemical‐intensive due to reliance on external stimuli for oxidant activation. Here, we present a self‐sustaining catalytic membrane (TMF‐CM) incorporating Ti‐doped Mn 3 O 4 /Fe 3 O 4 catalysts with engineered oxygen vacancies, which harness pollutants as electron donors to drive enzyme‐mimetic redox cycles. Through nanoconfinement within ceramic membrane pores, dissolved oxygen is autonomously activated by electrons derived from contaminants, enabling continuous regeneration of active sites without chemical additives. Mechanistic investigations, supported by spectroscopic and computational evidence, reveal that high‐valent metal–oxo intermediates mediate contaminant oxidation while concurrently restoring oxygen vacancies, thereby sustaining catalytic cycles. During 10‐day continuous testing in real wastewater, the TMF‐CM system achieved over 90.1% contaminant removal and exhibited self‐cleaning capability. This autonomous catalytic paradigm leverages the inherent chemical energy of wastewater, eliminating chemical additives and cutting energy consumption by 70%–98% compared to UV‐ or electrochemical‐based systems. By integrating molecular oxygen activation with circular electron transfer, we establish a sustainable oxidation strategy that extends beyond conventional water treatment paradigms.