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Spin–Spin Coupling: Two-Bond Coupling (Geminal Coupling)01:20

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Two NMR-active nuclei bonded to a central atom can be involved in geminal or two-bond coupling. Geminal coupling is commonly seen between diastereotopic protons in chiral molecules and unsymmetrical alkenes, among others.
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Crystal Field Theory
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Coupling interactions are strongest between NMR-active nuclei bonded to each other, where spin information can be transmitted directly through the pair of bonding electrons. While nuclei polarize their electrons to the opposite spins, the bonding electron pair has opposite spins. Configurations with antiparallel nuclear spins are expected to be lower in energy. When coupling makes antiparallel states more favorable, J is considered to have a positive value. The one-bond coupling constant, 1J,...
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Halogen-Driven Single-Crystal to Single-Crystal Transformation Engineering the Cluster-based Spin Crossover

Guang Yang1, Ze-Yu Ruan1, Yan-Cong Chen1

  • 1Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, IGCME, Guangdong Basic Research Center of Excellence for Functional Molecular Engineering, Sun Yat-Sen University, Guangzhou, 510275, P. R. China.

Angewandte Chemie (International Ed. in English)
|October 11, 2024
PubMed
Summary
This summary is machine-generated.

We report a novel cluster-based spin crossover (SCO) metal-organic framework (MOF) with a rare topology. This MOF can be transformed into new frameworks with modified SCO properties through stepwise single-crystal transformations.

Keywords:
clusterironmetal–organic frameworksingle-crystal to single-crystal transformationspin crossover

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Area of Science:

  • Materials Science
  • Coordination Chemistry
  • Supramolecular Chemistry

Background:

  • Cluster-based spin crossover (SCO) frameworks are emerging smart metal-organic frameworks (MOFs).
  • These materials exhibit unique bistable properties due to diverse structures and topologies.
  • Developing new SCO MOFs with tunable properties is crucial for advanced applications.

Purpose of the Study:

  • To report a novel cluster-based SCO framework with an exceptionally rare 3,4,6-T108 topology.
  • To demonstrate the feasibility of post-synthetic modification (PSM) via single-crystal to single-crystal (SCSC) transformations.
  • To investigate the influence of these transformations on the SCO behavior.

Main Methods:

  • Synthesis of a new cluster-based SCO framework [Fe3{Ag4(CN)6(H2O)}2(TPBA)3](ClO4)2·7DMF (1).
  • Utilized reticular chemistry principles for post-synthetic modification (PSM).
  • Performed successive single-crystal to single-crystal (SCSC) transformations to alter framework topology and composition.

Main Results:

  • The synthesized framework (1) features a 3,4,6-T108 topology with n-fold Borromean entangled networks.
  • Achieved the first SCSC transformation of a 3,4,6-T108 topology MOF to urk topology frameworks (2_X, X=Cl, Br, I).
  • Demonstrated successive SCSC transformations (2_Cl → 2_Br → 2_I) and observed modified SCO behaviors driven by halogen substitution.

Conclusions:

  • The study presents new strategies for designing cluster-based SCO MOFs.
  • Successfully demonstrated SCSC transformations for creating novel MOF topologies and functionalities.
  • The findings pave the way for developing advanced smart functional porous materials.