"Tail" tuning of iron(II) spin crossover temperature by 100 K

Inorganic Chemistry
Humphrey L C FelthamSally Brooker

Abstract

Two new Rdpt ligands featuring long "tails", padpt (N-4H-1,2,4-triazole-3,5-di(2-pyridyl)palmitamide) and hpdpt (4-(4-heptadecafluoroctylphenyl)-3,5-bis(2-pyridyl)-4H-1,2,4-triazole), were made and reacted with [Fe(II)(py)4(NCS)2] to give pinkish-red [Fe(II)(padpt)2(SCN)2] (1) and purple-red [Fe(II)(hpdpt)2(SCN)2] (2) as solvent-free crystals. Magnetic measurements reveal that both 1 and 2 exhibit complete and reproducible spin crossovers, with a far lower T1/2 for the amide-alkyl tailed 1 (182 K) than for the fluorocarbon tailed 2 (248 K), which in turn is far lower than the T1/2 of 290 K previously reported for the nonamide-alkyl tailed analogue [Fe(II)(C16dpt)2(SCN)2]·(2)/3H2O (3). Structure determinations for 1 and 2 in both the high spin (HS) and low spin (LS) states confirm the expected trans-NCS conformation and reveal that (a) the "tails" interdigitate and (b) the LS forms are less distorted than the HS forms (Σ = 58-70° vs 47-54°). DSC and Raman spectroscopy confirmed the high tail-dependence of the SCO events in 1 and 2, as well as in 3, with the Raman data giving T1/2 values of 190, 243, and 285 K, respectively. Bright orange single crystals of the solvatomorph [Fe(II)(hpdpt)2(SCN)2]·MeOH·H2O (2solv) were also struct...Continue Reading

References

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Citations

Dec 25, 2015·Inorganic Chemistry·Fuxing ShenOsamu Sato
Apr 25, 2015·Chemical Society Reviews·Sally Brooker
May 29, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Fabrice N H KarabulutSally Brooker
Aug 21, 2018·Chemical Society Reviews·Ross W HogueSally Brooker
May 30, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Sandhya SinghSally Brooker
Jun 25, 2020·Chemistry : a European Journal·Zhi-Guo GuHui-Shu Lu
Jul 1, 2018·ChemPlusChem·Humphrey L C FelthamSally Brooker
Apr 23, 2021·Chemical Communications : Chem Comm·Iurii GaladzhunMalcolm A Halcrow
Jul 27, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Yunnan GuoYann Garcia
Nov 8, 2017·Inorganic Chemistry·Santiago Rodríguez-Jiménez, Sally Brooker
May 17, 2018·Inorganic Chemistry·Santiago Rodríguez-JiménezSally Brooker
Mar 7, 2018·Langmuir : the ACS Journal of Surfaces and Colloids·Francesco BorgattiMassimiliano Cavallini

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