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Hybrid perovskites have potential applications in several electrochemical devices such as supercapacitors, batteries, and fuel cells. Here, the thermal stabilities as a function of the length n of the CH 2 groups in [NH 3 (CH 2 )  n  NH 3 ]CdCl 4 ( n = 2, 3, and 4) crystals were considered by TGA and DTA. The structural characteristics and molecular dynamics were studied by MAS and static NMR experiments. A comparison of spin-lattice relaxation times indicated that the organic cation containing 1 H and 13 C was significantly more flexible than the inorganic anion containing 113 Cd. The flexibility of 1 H increased with an increase in the length of CH 2 in the carbon chain, resulting in a decrease in the activation energy ( E  a ) of 1 H. The E  a of 13 C a n = 3 and 4 was more flexible at high temperatures than at low temperatures. In contrast, the E  a of 13 C a n = 2 was more flexible at low temperatures. These results provide insight into the thermal stability and molecular dynamics of these crystals as a function of the length n of CH 2 groups in the carbon chain and are expected to facilitate applications.

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Physicochemical Property Investigations of Perovskite-Type Layer Crystals [NH3(CH2)nNH3]CdCl4 (n = 2, 3, and 4) as a Function of Length n of CH2