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Spin–Spin Coupling: One-Bond Coupling01:17

Spin–Spin Coupling: One-Bond Coupling

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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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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.
The central atom need not be NMR-active because its electrons are affected by the electron polarization of the spin-active atoms. However, spin information is transmitted less effectively than in one-bond coupling, and 2J values are usually weaker than 1J values. The energy of...
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Cationic Chain-Growth Polymerization: Mechanism00:57

Cationic Chain-Growth Polymerization: Mechanism

2.7K
The cationic polymerization mechanism consists of three steps: initiation, propagation, and termination. In the initiation step of the polymerization process, the π bond of a monomer gets protonated by the Lewis acid catalyst, which is formed from boron trifluoride and water. The protonation of the π bond generates a carbocation stabilized by the electron‐donating group. In the propagation step, the π bond of the second monomer acts as a nucleophile and attacks the...
2.7K
Thermal and Photochemical Electrocyclic Reactions: Overview01:26

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2.9K
Electrocyclic reactions are reversible reactions. They involve an intramolecular cyclization or ring-opening of a conjugated polyene. Shown below are two examples of electrocyclic reactions. In the first reaction, the formation of the cyclic product is favored. In contrast, in the second reaction, ring-opening is favored due to the high ring strain associated with cyclobutene formation.
2.9K
Spin–Spin Coupling Constant: Overview01:08

Spin–Spin Coupling Constant: Overview

1.4K
In bromoethane, the three methyl protons are coupled to the two methylene protons that are three bonds away. In accordance with the n+1 rule, the signal from the methyl protons is split into three peaks with 1:2:1 relative intensities. The methylene protons appear as a quartet, with the relative intensities of 1:3:3:1.
Qualitatively, any spin plus-half nucleus polarizes the spins of its electrons to the minus-half state. Consequently, the paired electron in the hydrogen–carbon bond must...
1.4K
Spin–Spin Coupling: Three-Bond Coupling (Vicinal Coupling)01:22

Spin–Spin Coupling: Three-Bond Coupling (Vicinal Coupling)

1.4K
Vicinal or three-bond coupling is commonly observed between protons attached to adjacent carbons. Here, nuclear spin information is primarily transferred via electron spin interactions between adjacent C‑H bond orbitals. This generally favors the antiparallel arrangement of spins, so 3J values are usually positive.
The extent of coupling depends on the C‑C bond length, the two H‑C‑C angles, any electron-withdrawing substituents, and the dihedral angle between the involved orbitals. The...
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A thermal- and light-induced switchable one-dimensional rare loop-like spin crossover coordination polymer.

Wenlong Lan1, Francisco Javier Valverde-Muñoz2, Yong Dou1

  • 1College of Chemical and Chemical Engineering, Shandong University of Technology, Zibo 255049, PR China. dpzhang73@126.com.

Dalton Transactions (Cambridge, England : 2003)
|November 7, 2019
PubMed
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Two new iron coordination polymers were synthesized. Complex 2 exhibits spin crossover (SCO) behavior and light-induced effects, highlighting the synergy between ligand field and hydrogen bonding for SCO system design.

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Synthesis of Cyclic Polymers and Characterization of Their Diffusive Motion in the Melt State at the Single Molecule Level
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Area of Science:

  • Coordination Chemistry
  • Materials Science
  • Magnetochemistry

Background:

  • One-dimensional coordination polymers (1D-CPs) are of interest for their unique properties.
  • Spin crossover (SCO) materials exhibit a change in spin state in response to external stimuli.
  • Understanding the factors influencing SCO is crucial for designing advanced materials.

Purpose of the Study:

  • To synthesize and characterize novel isostructural 1D-CPs using Fe(II) ions and a V-shaped ligand.
  • To investigate the spin crossover properties and light-induced effects in these new coordination systems.
  • To elucidate the role of ligand field and intermolecular interactions in controlling SCO behavior.

Main Methods:

  • Self-assembly of Fe(II) and pseudohalide ions with N,N'-dipyridin-4-ylisophthalamide (DPIP) ligand.
  • Characterization using elemental analysis, IR spectroscopy, TGA, and X-ray diffraction (single crystal and powder).
  • Magnetic studies to determine spin crossover transitions, thermal hysteresis, and light-induced excited spin state trapping (LIESST).

Main Results:

  • Two loop-like isostructural 1D-CPs, {Fe(DPIP)2(NCSe)2}n·4DMF (1) and {Fe(DPIP)2(NCSe)2}n·4DMF (2), were successfully synthesized.
  • Complex 2 displayed complete thermally induced SCO centered at 120 K with a 5 K hysteresis loop and LIESST at 65 K.
  • Complex 1 (X=S) and the desolvated form of complex 2 remained high spin across all temperatures, indicating the importance of specific interactions for SCO.

Conclusions:

  • The synergistic effects between the intramolecular coordination bond and intermolecular hydrogen bonding are critical for achieving SCO in complex 2.
  • These findings offer valuable insights for designing new 1D SCO materials by rationally controlling cooperative effects.
  • The study demonstrates a pathway to fine-tune SCO properties through molecular design and supramolecular interactions.