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Area of Science:

  • Environmental Chemistry
  • Photochemistry
  • Organic Geochemistry

Background:

  • Dissolved organic matter (DOM) plays a crucial role in aquatic ecosystems.
  • Carbon monoxide (CO) is a significant photoproduct of DOM.
  • Understanding the photochemical pathways of DOM is essential for environmental studies.

Purpose of the Study:

  • To investigate the chemical controls on carbon monoxide (CO) photoproduction from humic substances (HSs) and pure monomeric aromatics.
  • To determine the role of aromaticity and substituent groups in CO photoproduction.
  • To elucidate the primary chromophores and photoreactants in DOM responsible for CO generation.

Main Methods:

  • Irradiation of aqueous solutions of humic substances (HSs) and pure monomeric aromatics.
  • Isolation of diverse HS fractions (humic, fulvic, hydrophobic, hydrophilic) from various aquatic environments (lakes, rivers, marsh, ocean).
  • Measurement of HS absorption coefficients, photoreactivities (bleaching, CO production), and CO photoproduction efficiency.

Main Results:

  • HS absorption coefficients and photoreactivities strongly correlated with HS aromaticity (r2 > 0.90).
  • Aromatic moieties were identified as the principal chromophores and photoreactants in HS and DOM.
  • Carbonyl carbon content did not correlate with CO photoproduction.
  • CO photoproduction efficiency of monomeric aromatics varied with ring substituents; electron-donating groups increased, while electron-withdrawing groups decreased efficiency.
  • Aromatic CO photoproduction efficiency spanned three orders of magnitude.

Conclusions:

  • Aromaticity is a critical factor controlling CO photoproduction from DOM.
  • Aromatic moieties, not carbonyl groups, are quantitatively important in CO photoproduction.
  • Variations in the apparent quantum yields of CO from natural DOM are likely related to the chemistry of aromatic substituent groups.