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Radical Oxidation of Allylic and Benzylic Alcohols01:21

Radical Oxidation of Allylic and Benzylic Alcohols

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Activated manganese(IV) oxide can selectively oxidize allylic and benzylic alcohols via a radical intermediate mechanism. Primary allylic alcohols are oxidized to aldehydes, while secondary allylic alcohols yield ketones. The redox reaction of potassium permanganate with an Mn(II) salt such as manganese sulfate (under either alkaline or acidic conditions), followed by thorough drying, yields the oxidizing agent: activated MnO2. While MnO2 is insoluble in the solvents used for the reaction, the...
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Microbial activity plays a pivotal role in the biogeochemical cycling of iron and manganese, especially at the redox gradients characteristic of stratified aquatic environments. These cycles are driven by microbial transformations between oxidized and reduced forms of the metals, allowing organisms to exploit them for metabolic energy and structural purposes.Iron Cycling Across Redox GradientsIn neutral, oxygen-rich surface waters, iron is predominantly found in its oxidized, insoluble ferric...
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Few compounds act as strong acids. A far greater number of compounds behave as weak acids and only partially react with water, leaving a large majority of dissolved molecules in their original form and generating a relatively small amount of hydronium ions. Weak acids are commonly encountered in nature, being the substances partly responsible for the tangy taste of citrus fruits, the stinging sensation of insect bites, and the unpleasant smells associated with body odor. A familiar example of a...
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The degradation of metals due to natural electrochemical processes is known as corrosion. Rust formation on iron, tarnishing of silver, and the blue-green patina that develops on copper are examples of corrosion. Corrosion involves the oxidation of metals. Sometimes it is protective, such as the oxidation of copper or aluminum, wherein a protective layer of metal oxide or its derivatives forms on the surface, protecting the underlying metal from further oxidation. In other cases, corrosion is...
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A functionally stable manganese oxide oxygen evolution catalyst in acid.

Michael Huynh1, D Kwabena Bediako, Daniel G Nocera

  • 1Department of Chemistry and Chemical Biology, Harvard University , Cambridge, Massachusetts 02138, United States.

Journal of the American Chemical Society
|March 28, 2014
PubMed
Summary
This summary is machine-generated.

Manganese oxide (MnOx) acts as a stable oxygen evolution reaction (OER) catalyst through self-healing. This process, driven by MnOx redeposition, enables non-noble metal catalysts to function in acidic conditions.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • First-row metals are crucial for developing cost-effective oxygen evolution reaction (OER) catalysts.
  • Manganese oxide (MnOx) is a promising non-noble metal catalyst candidate for OER.

Purpose of the Study:

  • To comprehensively characterize MnOx electrochemistry across a wide pH range.
  • To elucidate the OER mechanism and self-healing properties of MnOx.
  • To establish conditions for stable MnOx OER catalysis, including in acidic media.

Main Methods:

  • Electrochemical characterization of MnOx over acidic, neutral, and alkaline pH.
  • Kinetic analysis including Tafel slopes and proton concentration dependence.
  • Investigation of MnOx electrodeposition and dissolution mechanisms.

Main Results:

  • MnOx exhibits functional stability as an OER catalyst due to self-healing via redeposition.
  • Two competing OER mechanisms were identified: PCET (alkaline) and Mn(3+) disproportionation (acidic).
  • Kinetic analysis revealed distinct rate laws for OER and MnOx electrodeposition across pH.

Conclusions:

  • Self-healing via MnOx redeposition offsets dissolution, ensuring catalyst stability.
  • The interplay between OER kinetics and deposition kinetics defines MnOx stability regions.
  • Non-noble metal oxides like MnOx can be operated as stable OER catalysts in acidic media by leveraging self-healing.