Actinide chalcogenides with their rich structural chemistry offer a unique means to study bonding between actinides and soft chalcogenides and its effect on 5f electrons properties. However, due to actinide oxophilicity, synthesis of new and pure actinide chalcogenides is challenging. In this presentation, we will discuss a novel synthetic strategy for in situ oxide to chalcogenide conversion of transuranium oxides using boron chalcogenide mixture that previously was successfully applied to thorium and uranium. In the reaction mixture boron acts as “oxygen sponge” that results in the substitution of oxide to chalcogenide and the formation of thermodynamically stable B2O3. We demonstrate how flux-assisted synthesis of new layered compounds, NaCuThS3, NaCuThSe3, NaCuUS3, NaCuUSe3, and NaCuNpS3, depends on steric and thermodynamic factors. We also will show the difference between uranium and neptunium chalcogenide chemistry on the example of post-synthetic modification, single-crystal-to-single-crystal interlayer water uptake.

Layered NaCuNpS3: Transuranium oxide to chalcogenide conversion

ACS Spring 2022

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