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Related Concept Videos

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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Photochemical Electrocyclic Reactions: Stereochemistry01:26

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The absorption of UV–visible light by conjugated systems causes the promotion of an electron from the ground state to the excited state. Consequently, photochemical electrocyclic reactions proceed via the excited-state HOMO rather than the ground-state HOMO. Since the ground- and excited-state HOMOs have different symmetries, the stereochemical outcome of electrocyclic reactions depends on the mode of activation; i.e., thermal or photochemical.
Selection Rules: Photochemical Activation
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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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Valence Bond Theory02:42

Valence Bond Theory

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Coordination compounds and complexes exhibit different colors, geometries, and magnetic behavior, depending on the metal atom/ion and ligands from which they are composed. In an attempt to explain the bonding and structure of coordination complexes, Linus Pauling proposed the valence bond theory, or VBT, using the concepts of hybridization and the overlapping of the atomic orbitals. According to VBT, the central metal atom or ion (Lewis acid) hybridizes to provide empty orbitals of suitable...
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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.
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Ideally, an unpaired electron shows a single peak in the EPR spectrum due to the transition between the two spin energy states. However, coupling interactions can occur between the spins of the unpaired electron and any neighboring spin-active nuclei. This hyperfine coupling results in hyperfine splitting, where the EPR signal is split into multiplets. The signals split into 2nI + 1 peaks, where n is the number of equivalent nuclei and I is the nuclear spin. These splitting patterns provide...
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Spontaneous-Spin-Polarized 2D π-d Conjugated Frameworks Towards Enhanced Oxygen Evolution Kinetics.

Won Seok Lee1, Hiroaki Maeda2, Yen-Ting Kuo3

  • 1Research Center for Energy and Environmental Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.

Small (Weinheim an Der Bergstrasse, Germany)
|May 28, 2024
PubMed
Summary

Developing affordable electrocatalysts for green hydrogen is crucial. This study introduces a novel nickel-iron framework that enhances oxygen evolution reaction kinetics through spontaneous spin-polarization, offering a sustainable alternative for water electrolyzers.

Keywords:
bimetallic p‐d conjugationcoordination frameworkselectrocatalystsoxygen evolution reactionspin‐polarization

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Sustainable Energy

Background:

  • High-performance electrocatalysts are essential for efficient water electrolysis and green hydrogen production.
  • Current catalysts often rely on expensive precious metals, driving the need for sustainable alternatives.
  • Designing earth-abundant electrocatalysts that enhance oxygen evolution reaction (OER) kinetics is a key challenge.

Purpose of the Study:

  • To develop a sustainable-element-based electrocatalyst for improved oxygen evolution reaction (OER) kinetics.
  • To investigate the potential of 2D π-d conjugated frameworks with nickel and iron for water electrolysis.
  • To explore the role of spontaneous spin-polarization in enhancing electrocatalytic activity.

Main Methods:

  • Synthesis and characterization of bimetallic NiFex:y-benzenehexathiol (BHT) frameworks.
  • Electrochemical evaluation of OER activity, including specific current density and overpotential measurements.
  • Density functional theory (DFT) calculations to understand the electronic properties and mechanism of spin-polarization.

Main Results:

  • The NiFe1:4-BHT framework demonstrated superior OER activity, achieving a specific current density of 140 A g-1 at 350 mV overpotential.
  • This performance is competitive with state-of-the-art non-precious metal catalysts and comparable to RuO2 and IrO2.
  • DFT calculations confirmed that Ni incorporation induces a spontaneous-spin-polarized state, enhancing OER kinetics without external magnetic fields.

Conclusions:

  • Rational design of 2D π-d conjugated frameworks offers a powerful strategy for creating high-performance electrocatalysts from abundant elements.
  • The spontaneous-spin-polarized NiFe1:4-BHT framework presents a promising, cost-effective solution for efficient water electrolysis.
  • This approach paves the way for developing advanced electrocatalysts for next-generation energy devices and green hydrogen production.