Persulfate persistence under thermal activation conditions

Richard Johnson, Paul Tratnyek, Reid O Brien Johnson

Research output: Contribution to journalArticle

215 Citations (Scopus)

Abstract

Contaminant destruction with in situ chemical oxidation (ISCO) using persulfate (peroxydisulfate, S2O8 2-) can be enhanced by activation, which increases the rate of persulfate decomposition to sulfate radicals (SO4 •-). This step initiates a chain of radical reactions involving species (including SO4 •- and OH) that oxidize contaminants more rapidly than persulfate does directly. Among current activation methods, thermal activation is the least well studied. Combining new data for environmentally relevant conditions with previously published data, we have computed three sets of Arrhenius parameters (In A and Eact) that describe the rate of persulfate decomposition in homogeneous solutions over a wide range of temperature and pH. The addition of soil increases the decomposition rate of persulfate due to reactions with organic matter and possibly mineral surfaces, but the kinetics are still pseudo-first-order in persulfate and conform to the Arrhenius model. A series of respike experiments with soil at 70°C demonstrate that once the oxidant demand is met, reaction rates return to values near those observed in the homogeneous solution case. However, even after the oxidant demand is met, the relatively short lifetime of the persulfate at elevated temperatures (e.g., >50°C) will limit the delivery time over which persulfate can be effective.

Original languageEnglish (US)
Pages (from-to)9350-9356
Number of pages7
JournalEnvironmental Science and Technology
Volume42
Issue number24
DOIs
StatePublished - Dec 15 2008

Fingerprint

persistence
Chemical activation
decomposition
Decomposition
Oxidants
oxidant
Impurities
Soils
pollutant
Biological materials
reaction rate
Reaction rates
Minerals
soil
temperature
sulfate
oxidation
organic matter
kinetics
Oxidation

ASJC Scopus subject areas

  • Chemistry(all)
  • Environmental Chemistry

Cite this

Persulfate persistence under thermal activation conditions. / Johnson, Richard; Tratnyek, Paul; Johnson, Reid O Brien.

In: Environmental Science and Technology, Vol. 42, No. 24, 15.12.2008, p. 9350-9356.

Research output: Contribution to journalArticle

@article{7b26041836f64774b49989d3c88a88b3,
title = "Persulfate persistence under thermal activation conditions",
abstract = "Contaminant destruction with in situ chemical oxidation (ISCO) using persulfate (peroxydisulfate, S2O8 2-) can be enhanced by activation, which increases the rate of persulfate decomposition to sulfate radicals (SO4 •-). This step initiates a chain of radical reactions involving species (including SO4 •- and OH•) that oxidize contaminants more rapidly than persulfate does directly. Among current activation methods, thermal activation is the least well studied. Combining new data for environmentally relevant conditions with previously published data, we have computed three sets of Arrhenius parameters (In A and Eact) that describe the rate of persulfate decomposition in homogeneous solutions over a wide range of temperature and pH. The addition of soil increases the decomposition rate of persulfate due to reactions with organic matter and possibly mineral surfaces, but the kinetics are still pseudo-first-order in persulfate and conform to the Arrhenius model. A series of respike experiments with soil at 70°C demonstrate that once the oxidant demand is met, reaction rates return to values near those observed in the homogeneous solution case. However, even after the oxidant demand is met, the relatively short lifetime of the persulfate at elevated temperatures (e.g., >50°C) will limit the delivery time over which persulfate can be effective.",
author = "Richard Johnson and Paul Tratnyek and Johnson, {Reid O Brien}",
year = "2008",
month = "12",
day = "15",
doi = "10.1021/es8019462",
language = "English (US)",
volume = "42",
pages = "9350--9356",
journal = "Environmental Science & Technology",
issn = "0013-936X",
publisher = "American Chemical Society",
number = "24",

}

TY - JOUR

T1 - Persulfate persistence under thermal activation conditions

AU - Johnson, Richard

AU - Tratnyek, Paul

AU - Johnson, Reid O Brien

PY - 2008/12/15

Y1 - 2008/12/15

N2 - Contaminant destruction with in situ chemical oxidation (ISCO) using persulfate (peroxydisulfate, S2O8 2-) can be enhanced by activation, which increases the rate of persulfate decomposition to sulfate radicals (SO4 •-). This step initiates a chain of radical reactions involving species (including SO4 •- and OH•) that oxidize contaminants more rapidly than persulfate does directly. Among current activation methods, thermal activation is the least well studied. Combining new data for environmentally relevant conditions with previously published data, we have computed three sets of Arrhenius parameters (In A and Eact) that describe the rate of persulfate decomposition in homogeneous solutions over a wide range of temperature and pH. The addition of soil increases the decomposition rate of persulfate due to reactions with organic matter and possibly mineral surfaces, but the kinetics are still pseudo-first-order in persulfate and conform to the Arrhenius model. A series of respike experiments with soil at 70°C demonstrate that once the oxidant demand is met, reaction rates return to values near those observed in the homogeneous solution case. However, even after the oxidant demand is met, the relatively short lifetime of the persulfate at elevated temperatures (e.g., >50°C) will limit the delivery time over which persulfate can be effective.

AB - Contaminant destruction with in situ chemical oxidation (ISCO) using persulfate (peroxydisulfate, S2O8 2-) can be enhanced by activation, which increases the rate of persulfate decomposition to sulfate radicals (SO4 •-). This step initiates a chain of radical reactions involving species (including SO4 •- and OH•) that oxidize contaminants more rapidly than persulfate does directly. Among current activation methods, thermal activation is the least well studied. Combining new data for environmentally relevant conditions with previously published data, we have computed three sets of Arrhenius parameters (In A and Eact) that describe the rate of persulfate decomposition in homogeneous solutions over a wide range of temperature and pH. The addition of soil increases the decomposition rate of persulfate due to reactions with organic matter and possibly mineral surfaces, but the kinetics are still pseudo-first-order in persulfate and conform to the Arrhenius model. A series of respike experiments with soil at 70°C demonstrate that once the oxidant demand is met, reaction rates return to values near those observed in the homogeneous solution case. However, even after the oxidant demand is met, the relatively short lifetime of the persulfate at elevated temperatures (e.g., >50°C) will limit the delivery time over which persulfate can be effective.

UR - http://www.scopus.com/inward/record.url?scp=58149145761&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=58149145761&partnerID=8YFLogxK

U2 - 10.1021/es8019462

DO - 10.1021/es8019462

M3 - Article

C2 - 19174915

AN - SCOPUS:58149145761

VL - 42

SP - 9350

EP - 9356

JO - Environmental Science & Technology

JF - Environmental Science & Technology

SN - 0013-936X

IS - 24

ER -