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As an important nuclear material, uranium is one of the most concerned elements in the nuclear fuel cycle, which could interact with many inorganic and organic ligands. Amine templates have a significant structural-oriented effect on the construction of uranyl oxalate complex. In this work, the piperazine diamine templates were used to synthesize uranyl oxalate complex and their crystal structures were resolved by single crystal diffraction, and their spectra were studied by IR, Raman, UV–vis, fluorescence, and EPR techniques. The final results show that crystal structures, properties and applications of uranyl oxalate complex have a close correlation with polyamine templates. The single crystal structure results show that the structural-oriented effect of piperazine diamine template is greatly affected by the proportion and concentration of solute in the surrounding environment. And the alkyl substituents on N atoms of amine templates are related to the tight of structures. Interestingly, 5# has a potential application as the original material for multiple reuse of fluorescent sensor materials. At present, there is no clear and in-depth study on the internal mechanism of such phenomena in solid uranyl complexes, and the specific mechanism needs to be further explored.

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