A spin-crossover framework endowed with pore-adjustable behavior by slow structural dynamics

Jin-Peng Xue, Yang Hu, Bo Zhao, Zhi-Kun Liu, Jing Xie, Zi-Shuo Yao () and Jun Tao ()
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Jin-Peng Xue: Beijing Institute of Technology
Yang Hu: Beijing Institute of Technology
Bo Zhao: Beijing Institute of Technology
Zhi-Kun Liu: Beijing Institute of Technology
Jing Xie: Beijing Institute of Technology
Zi-Shuo Yao: Beijing Institute of Technology
Jun Tao: Beijing Institute of Technology

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Host-guest interactions play critical roles in achieving switchable structures and functionalities in porous materials, but design and control remain challenging. Here, we report a two-dimensional porous magnetic compound, [FeII(prentrz)2PdII(CN)4] (prentrz = (1E,2E)−3-phenyl-N-(4H-1,2,4-triazol-4-yl)prop-2-en-1-imine), which exhibits an atypical pore transformation that directly entangles with a spin state transition in response to water adsorption. In this material, the adsorption-induced, non-uniform pedal motion of the axial prentrz ligands and the crumpling/unfolding of the layer structure actuate a reversible narrow quasi-discrete pore (nqp) to large channel-type pore (lcp) change that leads to a pore rearrangement associated with simultaneous pore opening and closing. The unusual pore transformation results in programmable adsorption in which the lcp structure type must be achieved first by the long-time exposure of the nqp structure type in a steam-saturated atmosphere to accomplish the gate-opening adsorption. The structural transformation is accompanied by a variation in the spin-crossover (SCO) property of FeII, i.e., two-step SCO with a large plateau for the lcp phase and two-step SCO with no plateau for the nqp phase. The unusual adsorption-induced pore rearrangement and the related SCO property offer a way to design and control the pore structure and physical properties of dynamic frameworks.

Date: 2022
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DOI: 10.1038/s41467-022-31274-8

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