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Type: Journal article
Title: Guest-Induced Multistep to Single-Step Spin-Crossover Switching in a 2-D Hofmann-Like Framework with an Amide-Appended Ligand
Author: Ahmed, M.
Arachchige, K.S.A.
Xie, Z.
Price, J.R.
Cruddas, J.
Clegg, J.K.
Powell, B.J.
Kepert, C.J.
Neville, S.M.
Citation: Inorganic Chemistry: including bioinorganic chemistry, 2022; 61(30):11667-11674
Publisher: American Chemical Society (ACS)
Issue Date: 2022
ISSN: 0020-1669
Statement of
Manan Ahmed, Kasun S. A. Arachchige, Zixi Xie, Jason R. Price, Jace Cruddas, Jack K. Clegg, Benjamin J. Powell, Cameron J. Kepert, and Suzanne M. Neville
Abstract: A detailed study of the two-dimensional (2-D) Hofmann like framework [Fe(furpy)2Pd(CN)4]·nG (furpy: N-(pyridin-4-yl)furan-2- carboxamide, G = H2O,EtOH (A·H2O,Et), and H2O (A·H2O)) is presented, including the structural and spin-crossover (SCO) implications of subtle guest modification. This 2-D framework is characterized by undulating Hofmann layers and an array of interlayer spacing environments --this is a strategic approach that we achieve by the inclusion of a ligand with multiple host−host and host−guest interaction sites. Variable temperature magnetic susceptibility studies reveal an asymmetric multistep SCO for A·H2O,Et and an abrupt single-step SCO for A·H2O with an upshift in transition temperature of ∼75 K. Single-crystal analyses show a primitive orthorhombic symmetry for A·H2O,Et characterized by a unique FeII centers the multistep SCO character is attributed to local ligand orientation. Counterintuitively, A·H2O shows a triclinic symmetry with two inequivalent FeII centers that undergo a cooperative single-step high-spin (HS)-to-low-spin (LS) transition. We conduct detailed structure−function analyses to understand how the guest ethanol influences the delicate balance between framework communication and, therefore, the local structure and spin-state transition mechanism.
Rights: © 2022 American Chemical Society
DOI: 10.1021/acs.inorgchem.2c01253
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Appears in Collections:Chemistry publications

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