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

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 Al₂O₃ 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.