Measurement of hydroxyl radical activity in a soil slurry using the spin trap α-(4-pyridyl-1-oxide)-N-tert-butylnitrone

Scott G. Huling, Robert G Arnold, Raymond A. Sierka, Matthew R. Miller

Research output: Contribution to journalArticle

36 Citations (Scopus)

Abstract

The spin trap-compound α-(4-pyridy-M-oxide)N-tert-butylnitrone (4- POBN) served as a probe to estimate the activity of Fenton-derived hydroxyl radicals (·OH) in a batch suspension comprised of silica sand and crushed goethite ore. The rate of probe disappearance was used to analyze system kinetics and oxidation efficiency under heterogeneous, Fenton-driven conditions. The ·OH-(4-POBN) adduct produced by the reaction of 4-POBN with ·OH was observed via electron paramagnetic resonance to confirm the mechanism of 4-POBN transformation. The disappearance of 4-POBN with ·OH in the sand/goethite slurry amended with H2O2 (150 mM) was first-order in 4- POBN. Under the conditions of this experiments, the effective steady-state ·OH concentration ([·OH](ss)) was estimated at 1.2 x 10-15 and 6.5 x 10- 16 M, when 4-POBN was initially present at 700 and 144 μM, respectively. Observed kinetics were in qualitative agreement with a conceptual model in which H2O2 is consumed in both Fenton and non-Fenton reactions and 4-POBN competes with other slurry constituents for ·OH. Reaction of H2O2 with ·OH was an appreciable sink for ·OH, but the reaction did not contribute significantly to H2O2 depletion. Nonproductive reactions involving H2O2 (those that did not contribute to ·OH production) represented a significant source of overall reaction inefficiency, as defined.

Original languageEnglish (US)
Pages (from-to)3436-3441
Number of pages6
JournalEnvironmental Science and Technology
Volume32
Issue number21
DOIs
StatePublished - Nov 1 1998

Fingerprint

hydroxyl radical
goethite
Hydroxyl Radical
Oxides
slurry
probe
oxide
Soils
Silica sand
kinetics
Kinetics
sand
electron spin resonance
Ores
Paramagnetic resonance
Sand
soil
silica
oxidation
Oxidation

ASJC Scopus subject areas

  • Environmental Science(all)
  • Environmental Chemistry
  • Environmental Engineering

Cite this

Measurement of hydroxyl radical activity in a soil slurry using the spin trap α-(4-pyridyl-1-oxide)-N-tert-butylnitrone. / Huling, Scott G.; Arnold, Robert G; Sierka, Raymond A.; Miller, Matthew R.

In: Environmental Science and Technology, Vol. 32, No. 21, 01.11.1998, p. 3436-3441.

Research output: Contribution to journalArticle

@article{e77294dcc5cf4300b9b3b96ae5843815,
title = "Measurement of hydroxyl radical activity in a soil slurry using the spin trap α-(4-pyridyl-1-oxide)-N-tert-butylnitrone",
abstract = "The spin trap-compound α-(4-pyridy-M-oxide)N-tert-butylnitrone (4- POBN) served as a probe to estimate the activity of Fenton-derived hydroxyl radicals (·OH) in a batch suspension comprised of silica sand and crushed goethite ore. The rate of probe disappearance was used to analyze system kinetics and oxidation efficiency under heterogeneous, Fenton-driven conditions. The ·OH-(4-POBN) adduct produced by the reaction of 4-POBN with ·OH was observed via electron paramagnetic resonance to confirm the mechanism of 4-POBN transformation. The disappearance of 4-POBN with ·OH in the sand/goethite slurry amended with H2O2 (150 mM) was first-order in 4- POBN. Under the conditions of this experiments, the effective steady-state ·OH concentration ([·OH](ss)) was estimated at 1.2 x 10-15 and 6.5 x 10- 16 M, when 4-POBN was initially present at 700 and 144 μM, respectively. Observed kinetics were in qualitative agreement with a conceptual model in which H2O2 is consumed in both Fenton and non-Fenton reactions and 4-POBN competes with other slurry constituents for ·OH. Reaction of H2O2 with ·OH was an appreciable sink for ·OH, but the reaction did not contribute significantly to H2O2 depletion. Nonproductive reactions involving H2O2 (those that did not contribute to ·OH production) represented a significant source of overall reaction inefficiency, as defined.",
author = "Huling, {Scott G.} and Arnold, {Robert G} and Sierka, {Raymond A.} and Miller, {Matthew R.}",
year = "1998",
month = "11",
day = "1",
doi = "10.1021/es970876e",
language = "English (US)",
volume = "32",
pages = "3436--3441",
journal = "Environmental Science & Technology",
issn = "0013-936X",
publisher = "American Chemical Society",
number = "21",

}

TY - JOUR

T1 - Measurement of hydroxyl radical activity in a soil slurry using the spin trap α-(4-pyridyl-1-oxide)-N-tert-butylnitrone

AU - Huling, Scott G.

AU - Arnold, Robert G

AU - Sierka, Raymond A.

AU - Miller, Matthew R.

PY - 1998/11/1

Y1 - 1998/11/1

N2 - The spin trap-compound α-(4-pyridy-M-oxide)N-tert-butylnitrone (4- POBN) served as a probe to estimate the activity of Fenton-derived hydroxyl radicals (·OH) in a batch suspension comprised of silica sand and crushed goethite ore. The rate of probe disappearance was used to analyze system kinetics and oxidation efficiency under heterogeneous, Fenton-driven conditions. The ·OH-(4-POBN) adduct produced by the reaction of 4-POBN with ·OH was observed via electron paramagnetic resonance to confirm the mechanism of 4-POBN transformation. The disappearance of 4-POBN with ·OH in the sand/goethite slurry amended with H2O2 (150 mM) was first-order in 4- POBN. Under the conditions of this experiments, the effective steady-state ·OH concentration ([·OH](ss)) was estimated at 1.2 x 10-15 and 6.5 x 10- 16 M, when 4-POBN was initially present at 700 and 144 μM, respectively. Observed kinetics were in qualitative agreement with a conceptual model in which H2O2 is consumed in both Fenton and non-Fenton reactions and 4-POBN competes with other slurry constituents for ·OH. Reaction of H2O2 with ·OH was an appreciable sink for ·OH, but the reaction did not contribute significantly to H2O2 depletion. Nonproductive reactions involving H2O2 (those that did not contribute to ·OH production) represented a significant source of overall reaction inefficiency, as defined.

AB - The spin trap-compound α-(4-pyridy-M-oxide)N-tert-butylnitrone (4- POBN) served as a probe to estimate the activity of Fenton-derived hydroxyl radicals (·OH) in a batch suspension comprised of silica sand and crushed goethite ore. The rate of probe disappearance was used to analyze system kinetics and oxidation efficiency under heterogeneous, Fenton-driven conditions. The ·OH-(4-POBN) adduct produced by the reaction of 4-POBN with ·OH was observed via electron paramagnetic resonance to confirm the mechanism of 4-POBN transformation. The disappearance of 4-POBN with ·OH in the sand/goethite slurry amended with H2O2 (150 mM) was first-order in 4- POBN. Under the conditions of this experiments, the effective steady-state ·OH concentration ([·OH](ss)) was estimated at 1.2 x 10-15 and 6.5 x 10- 16 M, when 4-POBN was initially present at 700 and 144 μM, respectively. Observed kinetics were in qualitative agreement with a conceptual model in which H2O2 is consumed in both Fenton and non-Fenton reactions and 4-POBN competes with other slurry constituents for ·OH. Reaction of H2O2 with ·OH was an appreciable sink for ·OH, but the reaction did not contribute significantly to H2O2 depletion. Nonproductive reactions involving H2O2 (those that did not contribute to ·OH production) represented a significant source of overall reaction inefficiency, as defined.

UR - http://www.scopus.com/inward/record.url?scp=0032213512&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=0032213512&partnerID=8YFLogxK

U2 - 10.1021/es970876e

DO - 10.1021/es970876e

M3 - Article

AN - SCOPUS:0032213512

VL - 32

SP - 3436

EP - 3441

JO - Environmental Science & Technology

JF - Environmental Science & Technology

SN - 0013-936X

IS - 21

ER -