Spatiotemporal studies of the one dimensional coordination polymer [Fe(ebtz)2(C2H5CN)2](BF4)2. Tug of war - nitrile reorientation versus crystal lattice as tool for tuning of spin crossover properties

Chemistry : a European Journal
Robert BroniszJoachim Kusz

Abstract

Reaction of 1,2-di(tetrazol-2-yl)ethane (ebtz) with Fe(BF4)2·6H2O in different nitriles yields one dimensional coordination polymers [Fe(ebtz)2(RCN)2](BF4)2⋅nRCN (n =2 for R=-CH3  (1) and n=0 for R=-C2H5  (2),-C3H7  (3),-C3H5  (4),-CH2Cl (5)) exhibiting spin crossover (SCO). SCO in 1 and 3-5 is complete and occurs above 160 K. In 2 it is shifted to lower temperatures and is accompanied by wide hysteresis (T1/2↓=78 K, T1/2↑=123 K) and proceeds extremely slow. Isothermal (80K) time resolved single crystal X-ray diffraction studies revealed a complex nature of the HS→LS transition in 2 . Initial, slow stage is associated with shrinkage of polymeric chains and with reduction of cell volume at 77% (in relation to difference between cell volumes VHS -VLS ) whereas only 16% of iron(II) ions changed spin state. In the second stage an abrupt SCO commences, associated with breathing of crystal lattice along direction of Fe-nitrile bonds, while the nitriles reorient. HS→LS switching triggered by light (808 nm) reveals the coupling of spin state and nitrile orientation. The importance of this coupling was confirmed by studies of [Fe(ebtz)2(C2H5CN/C3H7CN)2 ](BF4)2 mixed crystals (2a, 2b), showing a shift of T1/2 to higher values and narrowi...Continue Reading

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Citations

May 11, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Izar Capel BerdiellMalcolm A Halcrow

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