Ion sieving in graphene oxide membrane enables efficient actinides/lanthanides separation.

Separation of actinides from lanthanides is of great importance for the safe management of nuclear waste and sustainable development of nuclear energy, but it represents a huge challenge due to the chemical complexity of these f-elements. Herein, we report an efficient separation strategy based on ion sieving in graphene oxide membrane. In the presence of a strong oxidizing reagent, the actinides (U, Np, Pu, Am) in a nitric acid solution exist in the high valent and linear dioxo form of actinyl ions while the lanthanides (Ce, Nd, Eu, Gd, etc.) remain as trivalent/tetravalent spheric ions. A task-specific graphene oxide membrane with an interlayer nanochannel spacing between the sizes of hydrated actinyl ions and lanthanides ions is tailored and used as an ionic cut-off filter, which blocks the larger and linear actinyl ions but allows the smaller and spheric lanthanides ions to penetrate through, affording lanthanides/actinides separation factors up to ~400. This work realizes the group separation of actinides from lanthanides under highly acidic conditions by a simple ion sieving strategy and highlights the great potential of utilizing graphene oxide membrane for nuclear waste treatment.