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¹H NMR: Long-Range Coupling01:27

¹H NMR: Long-Range Coupling

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The coupling interactions of nuclei across four or more bonds are usually weak, with J values less than 1 Hz. While these are usually not observed in spectra, the presence of multiple bonds along the coupling pathway can result in observable long-range coupling.
In alkenes, spin information is communicated via σ–π overlap, as seen in allylic (four-bond) and homoallylic (five-bond) couplings. These coupling interactions are stronger when the σ bond is parallel to the alkene...
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π Electron Effects on Chemical Shift: Overview01:27

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An applied magnetic field causes loosely bound π-electrons in organic molecules to circulate, producing a local or induced diamagnetic field over a large spatial volume. As the molecules tumble in solution, the field generated by π-electrons in spherical substituents results in a zero net field. However, the net field generated by π-electrons in non-spherical substituents is not zero. The effect of this induced field depends on the orientation of the molecule with respect to B0,...
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Reduction of Alkenes: Catalytic Hydrogenation02:13

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Alkenes undergo reduction by the addition of molecular hydrogen to give alkanes. Because the process generally occurs in the presence of a transition-metal catalyst, the reaction is called catalytic hydrogenation.
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
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Catalysis02:50

Catalysis

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The presence of a catalyst affects the rate of a chemical reaction. A catalyst is a substance that can increase the reaction rate without being consumed during the process. A basic comprehension of a catalysts’ role during chemical reactions can be understood from the concept of reaction mechanisms and energy diagrams.
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π Molecular Orbitals of 1,3-Butadiene01:24

π Molecular Orbitals of 1,3-Butadiene

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Conjugated dienes have lower heats of hydrogenation than cumulated and isolated dienes, making them more stable. The enhanced stabilization of conjugated systems can be understood from their π molecular orbitals.
The simplest conjugated diene is 1,3-butadiene: a four-carbon system where each carbon is sp2-hybridized and has an unhybridized p orbital that contains an unpaired electron. According to molecular orbital theory, atomic orbitals combine to form molecular orbitals such that the...
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Reduction of Alkenes: Asymmetric Catalytic Hydrogenation

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Catalytic hydrogenation of alkenes is a transition-metal catalyzed reduction of the double bond using molecular hydrogen to give alkanes. The mode of hydrogen addition follows syn stereochemistry.
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
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Updated: May 9, 2025

Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
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Beyond Second Coordination Shell: Long-Range π-Electrons Delocalization Engineering in Single-Atom Catalysts for CO2

Lingxiao Wang1,2, Shengquan Fu2, Ran Shi2

  • 1College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, Guangdong, 518060, China.

Angewandte Chemie (International Ed. in English)
|April 30, 2025
PubMed
Summary

Researchers engineered nickel catalysts by precisely controlling charge delocalization. This significantly boosted CO electrocatalysis efficiency and selectivity, paving the way for advanced catalyst design.

Keywords:
CO2 electroreductionLong‐range  charge delocalizationNickel tetraphenylporphyrinSecond‐beyond coordination shellSingle‐atom catalysts

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Long-range charge delocalization impacts single-atom active sites.
  • Systematic modulation of these sites for catalysis is underexplored.

Purpose of the Study:

  • To engineer nickel tetraphenylporphyrin (NiTPP) precursors.
  • To modulate π-electron delocalization in extended coordination environments.
  • To enhance multielectron catalytic processes.

Main Methods:

  • Site-specific cleavage of carbon-carbon single bonds at β-carbon sites of NiTPP.
  • Preservation of the Ni-centered first and second coordination shells.
  • Experimental and theoretical analyses.

Main Results:

  • A 29-fold enhancement in CO faradaic efficiency at -1.4 V versus RHE.
  • Maintained 98.3% CO selectivity at 500 mA cm⁻² in a flow cell.
  • Electron-enriched Ni sites facilitate stabilization of the *COOH intermediate.

Conclusions:

  • Deliberate engineering of higher coordination shells offers a new paradigm for catalyst design.
  • Precise regulation of charge delocalization enhances catalytic performance.
  • Developed Ni-N4 catalyst shows significant improvements for CO electrocatalysis.