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Reaction of uranyl dications with (2‐carboxyethyl)(phenyl)phosphinic acid (CPPA, H2L) under hydrothermal conditions gave two layered isomers (UO2)2(L)2, namely, CPP‐U1 and CPP‐U2. Both of them feature edge‐sharing uranyl dimers as structure‐building units, which are ligated by CPP ligands in different ways, thus leading different layered arrangements. With the addition of imidazole derivatives, two...
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