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A thermodynamically based method to quantify true sorption hysteresis.

Michael Sander1, Yuefeng Lu, Joseph J Pignatello

  • 1Department of Chemical Engineering, Environmental Engineering Program, Yale University, New Haven, CT 06520-8286, USA.

Journal of Environmental Quality
|May 13, 2005
PubMed
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A new Thermodynamic Index of Irreversibility (TII) quantifies soil contaminant sorption hysteresis. This index measures the energy difference between real and hypothetical reversible desorption, offering a model-independent way to assess contaminant fate.

Area of Science:

  • Environmental Chemistry
  • Soil Science
  • Chemical Engineering

Background:

  • Sorption of organic chemicals to soils and sediments frequently exhibits true hysteresis, a phenomenon crucial for understanding contaminant fate.
  • Existing hysteresis indices are often empirical and model-dependent, limiting their broad applicability.
  • True sorption hysteresis is linked to irreversible changes in the solid matrix during sorption-desorption cycles.

Purpose of the Study:

  • To propose and validate a new, model-independent method for quantifying true sorption hysteresis in soils.
  • To introduce the Thermodynamic Index of Irreversibility (TII) as a measure of hysteresis based on free energy differences.
  • To assess the concentration dependency of hysteresis in organic-rich soils and coal.

Main Methods:

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  • Developed the Thermodynamic Index of Irreversibility (TII) based on the free energy difference between actual desorption and hypothetical reversible desorption.
  • Eliminated common experimental artifacts that can cause artificial hysteresis.
  • Applied the TII to the sorption of 1,4-dichlorobenzene (DCB) to Pahokee peat, Amherst soil, and Beulah-Zap lignite.

Main Results:

  • The TII effectively quantifies hysteresis without requiring assumptions about solid properties or specific equilibrium models.
  • Significant hysteresis was observed in Pahokee peat and Beulah-Zap lignite, confirming the TII's applicability.
  • The TII demonstrated concentration-dependent behavior, decreasing with concentration in peat but increasing in lignite.

Conclusions:

  • The Thermodynamic Index of Irreversibility (TII) provides a robust, thermodynamic basis for quantifying true sorption hysteresis.
  • The TII is a valuable tool for assessing contaminant fate and transport in soils and sediments.
  • Hysteresis quantification is dependent on the sorbate-sorbent combination and concentration, highlighting the complexity of contaminant interactions.