Dual-Pathway Catalytic Proton Exchange in Water Distillation Enables Record Detritiation of Tritiated Water

-MIL-101(Cr), which achieves a record separation efficiency of 42.5 theoretical plates per meter. This corresponds to a 134-fold improvement over the best reported packing and a 6 orders of magnitude enhancement over commercial packings at an industrially relevant packed height of 10 m. The exceptional performance originates from a dual-pathway catalytic proton exchange mechanism, in which Cr-oxo clusters and amino-functionalized organic ligands provide parallel proton-transfer pathways through hydrogen-bond networks of water molecules. These dual pathways markedly strengthen liquid-solid isotope exchange and enable an efficient and continuous vapor-liquid-solid triphasic distillation process beyond the limits of conventional biphasic operation. This work provides a promising strategy for advancing detritiation technologies and mitigating tritium releases from the nuclear industry.