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MMM 2022

November 07, 2022

Minneapolis, United States

Magnetic Coupling of Divalent Metal Centers in Post Synthetic Metal Exchanged Bimetallic DUT 49 MOFs by EPR interrogations

Metal-organic frameworks (MOFs) are a novel and the most prominent class of microporous materials for the applications such as gas storage and separation, catalysis, heat storage and liquid purification, owing to their unique structural diversity and tunability. 1 In the current scenario, understanding the magnetic properties of MOFs has started to be explored in the field of molecular magnetism, 2,3 and the electron paramagnetic resonance (EPR) spectroscopy is one of the inevitable tools to investigate the magnetic exchange interactions between spin centers to understand the local structure of the MOF materials 1,4,5.
Herein, EPR measurements at X- (9.4 GHz), Q- (34 GHz) and W-band (94 GHz) on paddlewheel (PW) type post-synthetic metal exchanged DUT-49(M, M): M-Zn, Mn, Cu MOFs were investigated. Temperature-dependent X-band measurements were recorded from T = 7 K to T = 170 K on DUT-49(Cu), DUT-49(Mn) and bimetallic DUT-49(CuZn) and DUT-49(CuMn) MOFs. Moreover, an EPR signal intensity of the magnetically coupled metal ion pairs in the PW units, which is proportional to the magnetic susceptibility, was extracted from the temperature-dependent X-band EPR data for all MOFs. The sign of the isotropic coupling constant (2J = -239 cm-1) determined via Bleaney Blowers susceptibility fit confirms the excited S= 1 state antiferromagnetic interaction above T = 60 K of DUT-49(Cu) within the paddlewheel. Also, other DUT-49(M, M) MOFs are expected to have antiferromagnetic interaction within the paddle wheel (see Table). X-band measurements at T =160 K confirm the excited spin states (SCuCu = 1, SCuMn = 3, and SMnMn = 5) of the antiferromagnetically (AFM) coupled ions of the PW units for the DUT-49(Cu), DUT-49(CuMn) and DUT-49(Mn) MOFs, respectively. While signals observed from DUT-49(CuMn) and DUT-49(CuZn) MOFs at T = 7 K could be due to the low spin states of the coupled paramagnetic ions within the PW and corresponds to the SCuMn = 2 and SCuZn = 1/2 spin states, respectively.

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