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Radical Reactivity: Nucleophilic Radicals01:16

Radical Reactivity: Nucleophilic Radicals

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Radicals adjacent to electron-donating groups are called nucleophilic radicals. These radicals readily react with electrophilic alkenes. The SOMO–LUMO interactions are the driving force for the reaction, where the high-energy SOMO of the electron-rich, nucleophilic radicals interacts with the low-energy LUMO of the electron-deficient, electrophilic alkenes. Such SOMO–LUMO interactions are the basis of reactive radical traps, affecting the selectivity in radical reactions. For...
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Radicals, the highly reactive species, gain stability by undergoing three different reactions. The first reaction involves a radical-radical coupling, in which a radical combines with another radical, forming a spin‐paired molecule. The second reaction is between a radical and a spin‐paired molecule, generating a new radical and a new spin‐paired molecule. The third reaction is radical decomposition in a unimolecular reaction, forming a new radical and a spin‐paired...
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In a radical reaction, the concentration of starting materials governs the selectivity of a radical. For example, the reaction between an alkyl halide and an alkene, in the presence of tin hydride and AIBN, begins with the generation of a tin radical. The generated radical then abstracts halogen from the alkyl halide, producing an alkyl radical. This alkyl radical can either react with tin hydride, yielding an alkane, or add to an alkene, generating a nitrile-stabilized radical, eventually...
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Radicals adjacent to electron‐withdrawing groups are called electrophilic radicals. These radicals readily react with nucleophilic alkenes. For example, the malonate radical, in which the radical center is flanked by two electron‐withdrawing groups, reacts readily with butyl vinyl ether, which consists of an electron‐donating oxygen substituent. The reaction between electrophilic malonate radical and nucleophilic vinyl ether is favored because the radical has a...
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A Radical-Assisted Approach to High-Entropy Alloy Nanoparticle Electrocatalysts under Ambient Conditions.

Xu Li1,2, Jianyun Cao1, Guoliang Chen3,4

  • 1Yunnan Key Laboratory of Electromagnetic Materials and Devices, National Center for International Research on Photoelectric and Energy Materials, School of Materials and Energy, Yunnan University, Kunming 650091, P. R. China.

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|February 21, 2025
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Summary

We developed a simple wet chemical method to synthesize high-entropy alloy (HEA) nanoparticles using UV-irradiated isopropyl alcohol. These HEA nanoparticles show excellent performance for the hydrogen evolution reaction (HER) across all pH levels.

Keywords:
electrocatalysishigh-entropy alloyhydrogen evolution reactionnanoparticleswet chemical synthesis

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Area of Science:

  • Materials Science
  • Nanotechnology
  • Electrochemistry

Background:

  • High-entropy alloy (HEA) nanoparticles are emerging as potent catalysts.
  • Existing synthesis methods for HEA nanoparticles often lack simplicity and struggle to correlate structure with catalytic properties.

Purpose of the Study:

  • To develop a facile and robust wet chemical method for synthesizing HEA nanoparticles under ambient conditions.
  • To investigate the catalytic activity of synthesized HEA nanoparticles for the hydrogen evolution reaction (HER).

Main Methods:

  • Utilized UV irradiation of isopropyl alcohol to generate highly reductive carbon-centered radicals.
  • Employed these radicals to synthesize multi-element HEA nanoparticles (five to seven elements) via reduction of diverse metal ions.
  • Characterized HEA nanoparticles using electron paramagnetic resonance spectroscopy and tested their HER performance on a reduced electrochemical graphene oxide (rEGO) support.
  • Performed density functional theory (DFT) calculations to understand the structure-activity relationship.

Main Results:

  • Successfully synthesized HEA nanoparticles using a simple wet chemical approach under ambient conditions.
  • The PtPdIrRhAuAgCu HEA nanoparticles on rEGO (PtPdIrRhAuAgCu-rEGO) exhibited superior HER activity across the entire pH range.
  • Achieved very low overpotentials (11 mV in 1 M KOH, 30 mV in PBS, 31 mV in 0.5 M H2SO4) for -10 mA cm-2 current density, outperforming commercial Pt/C.

Conclusions:

  • The developed wet chemical method provides a simple and effective route for HEA nanoparticle synthesis.
  • PtPdIrRhAuAgCu-rEGO demonstrates exceptional catalytic activity for HER, making it a promising alternative to platinum-based catalysts.
  • DFT calculations suggest a correlation between HER activity and the d-band centers of nearest atoms in the HEA's face-centered cubic hollow site.