Interfacial Bonding of Fe Single‐Atom Catalysts on Ceramic Membranes for Sustainable Water Purification

ABSTRACT Catalytic membranes, which integrate molecular sieving with in situ reactive oxygen species (ROS) generation, offer a promising platform to achieve simultaneous pollutant removal and fouling mitigation. However, fabricating stable catalytic membranes remains challenging, as conventional deposition/filtration techniques often result in weak interfacial adhesion, especially on inert substrates. Here, we develop an interfacial bonding strategy to stabilize Fe single atoms on Al 2 O 3 membranes. By employing a metal‐organic framework‐derived template, N atoms from the framework bond with Al atoms of the substrate to form Al─N linkages, which subsequently coordinate with Fe to generate atomically dispersed Fe─N sites. This dual anchoring not only imparts structural stability but also tailors the electronic configuration of the Fe center to manipulate ROS generation. The resulting catalytic membranes exhibit exceeding 90% antibiotic degradation over a wide pH range of 3.37–11.03, excellent antifouling behavior for irreversible membrane resistance are only 6.6% which is nearly half of that of original ceramic membranes (11.4%), and long‐term durability in complex water matrices for maintained over 90% removal of tetracycline within 3600‐min in actual lake water. Supported by theoretical calculations, this work establishes interfacial bonding as an effective strategy for synthesizing single‐atom based catalytic membranes toward sustainable water purification.