Photo‐induced catalytic uranium extraction via a metal–organic framework‐carbon dot heterojunction on cellulose aerogel

Abstract Metal–organic frameworks (MOF) and conventional bioadsorbents, such as UiO‐66‐NH 2 and poplar cellulose fibers (PCF), often suffer inefficient charge separation, limited uranium binding affinity, and severe biofouling, restricting their performance in seawater. Here, we report a cellulose‐based aerogel catalyst incorporated with shrimp‐derived carbon dots (SCD) and a MOF heterojunction network (SCD‐MOF@PCF) with engineered interfacial structures and a regulated coordination environment. The interfacial coupling between SCD and UiO‐66‐NH 2 enhances visible‐light harvesting, promotes charge separation, and enriches photogenerated electrons at Zr sites, strengthening uranium coordination, elongating the U–O bond, and lowering the energy barrier. Density functional theory calculations reveal a maximum adsorption energy of −6.99 eV, consistent with the experimentally observed high adsorption capacity of 899.94 mg g −1 . In natural seawater, the catalyst achieves a uranium uptake of 7.13 mg g −1 after 3 weeks. Additionally, light induces the production of reactive oxygen species, thereby mitigating biofouling, enabling sustainable and efficient uranium extraction.