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With the coordination geometry of Dy III being relatively fixed, oxygen and sulfur atoms were used to replace one porphyrin pyrrole nitrogen atom of sandwich complex [(Bu) 4 N][Dy III (Pc)(TBPP)] [Pc = dianion of phthalocyanine, TBPP = 5,10,15,20-tetrakis[(4- tert -butyl)phenyl]porphyrin]. The energy barrier of the compounds was enhanced three times, with the order of Dy III (Pc)(STBPP) &gt; Dy III (Pc)(OTBPP) &gt; [(Bu) 4 N][Dy III (Pc)(TBPP)] [STBPP = monoanion of 5,10,15,20-(4- tert -butyl)phenyl-21-thiaporphyrin, OTBPP = monoanion of 5,10,15,20-(4- tert -butyl)phenyl-21-oxaporphyrin]. Theoretical calculations offer reasonable explanations of such a significant enhancement. The energy barrier of 194 K for Dy III (Pc)(STBPP) represents the highest one among all the bis(tetrapyrrole) dysprosium SMMs, providing a strategy to rationally enhance the anisotropy and energy barrier via atom replacement.

Rational enhancement of the energy barrier of bis(tetrapyrrole) dysprosium SMMs via replacing atom of porphyrin core