Photochemical oxidation of dissolved elemental mercury by carbonate radicals in water
Abstract
In this study, photochemical oxidation of dissolved elemental mercury, Hg(0), affects mercury chemical speciation and its transfer at the water-air interface in the aquatic environment. The mechanisms and factors that control Hg(0) photooxidation, however, are not completely understood, especially concerning the role of dissolved organic matter (DOM) and carbonate (CO32-) in natural freshwaters. Here, we evaluate Hg(0) photooxidation rates affected by reactive ionic species (e.g., DOM, CO32-, and NO3–) and free radicals in creek water and a phosphate buffer solution (pH 8) under simulated solar irradiation. The Hg(0) photooxidation rate (k = 1.44 h-1) is much higher in the presence of both CO32- and NO3- than in the presence of CO32-, NO3-, or DOM alone (k = 0.1–0.17 h-1). Using scavengers and enhancers for singlet oxygen (1O2) and hydroxyl (HO•) radicals, as well as electron paramagnetic resonance spectroscopy, we found that carbonate radicals (CO3•-) primarily drive Hg(0) photooxidation. The addition of DOM to the solution of CO32- and NO3- decreased the oxidation rate by half. This study identifies an unrecognized pathway of Hg(0) photooxidation by CO3•- radicals and the inhibitory effect of DOM, which could be important in assessing Hg transformation and the fate of Hg in water containing carbonatemore »
- Authors:
-
- Zhejiang Univ. of Technology, Hangzhou (China); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Zhejiang Univ. of Technology, Hangzhou (China)
- Publication Date:
- Research Org.:
- Univ. of Michigan, Ann Arbor, MI (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1239560
- Grant/Contract Number:
- SC0007042
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Environmental Science & Technology Letters (Online)
- Additional Journal Information:
- Journal Name: Environmental Science & Technology Letters (Online); Journal Volume: 1; Journal Issue: 12; Journal ID: ISSN 2328-8930
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES
Citation Formats
He, Feng, Gu, Baohua, Zhao, Weirong, and Liang, Liyuan. Photochemical oxidation of dissolved elemental mercury by carbonate radicals in water. United States: N. p., 2014.
Web. doi:10.1021/ez500322f.
He, Feng, Gu, Baohua, Zhao, Weirong, & Liang, Liyuan. Photochemical oxidation of dissolved elemental mercury by carbonate radicals in water. United States. https://doi.org/10.1021/ez500322f
He, Feng, Gu, Baohua, Zhao, Weirong, and Liang, Liyuan. Tue .
"Photochemical oxidation of dissolved elemental mercury by carbonate radicals in water". United States. https://doi.org/10.1021/ez500322f. https://www.osti.gov/servlets/purl/1239560.
@article{osti_1239560,
title = {Photochemical oxidation of dissolved elemental mercury by carbonate radicals in water},
author = {He, Feng and Gu, Baohua and Zhao, Weirong and Liang, Liyuan},
abstractNote = {In this study, photochemical oxidation of dissolved elemental mercury, Hg(0), affects mercury chemical speciation and its transfer at the water-air interface in the aquatic environment. The mechanisms and factors that control Hg(0) photooxidation, however, are not completely understood, especially concerning the role of dissolved organic matter (DOM) and carbonate (CO32-) in natural freshwaters. Here, we evaluate Hg(0) photooxidation rates affected by reactive ionic species (e.g., DOM, CO32-, and NO3–) and free radicals in creek water and a phosphate buffer solution (pH 8) under simulated solar irradiation. The Hg(0) photooxidation rate (k = 1.44 h-1) is much higher in the presence of both CO32- and NO3- than in the presence of CO32-, NO3-, or DOM alone (k = 0.1–0.17 h-1). Using scavengers and enhancers for singlet oxygen (1O2) and hydroxyl (HO•) radicals, as well as electron paramagnetic resonance spectroscopy, we found that carbonate radicals (CO3•-) primarily drive Hg(0) photooxidation. The addition of DOM to the solution of CO32- and NO3- decreased the oxidation rate by half. This study identifies an unrecognized pathway of Hg(0) photooxidation by CO3•- radicals and the inhibitory effect of DOM, which could be important in assessing Hg transformation and the fate of Hg in water containing carbonate such as hard water and seawater.},
doi = {10.1021/ez500322f},
journal = {Environmental Science & Technology Letters (Online)},
number = 12,
volume = 1,
place = {United States},
year = {Tue Nov 11 00:00:00 EST 2014},
month = {Tue Nov 11 00:00:00 EST 2014}
}
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Works referenced in this record:
Photooxidation of Hg(0) in Artificial and Natural Waters
journal, April 2001
- Lalonde, Janick D.; Amyot, Marc; Kraepiel, Anne M. L.
- Environmental Science & Technology, Vol. 35, Issue 7
Effect of solar radiation on the formation of dissolved gaseous mercury in temperate lakes
journal, March 1997
- Amyot, Marl; Mierle, Greg; Lean, David
- Geochimica et Cosmochimica Acta, Vol. 61, Issue 5
Biological and photochemical production of dissolved gaseous mercury in a boreal lake
journal, November 2004
- Poulain, A. J.; Amyot, M.; Findlay, D.
- Limnology and Oceanography, Vol. 49, Issue 6
Photochemical Redox Reactions of Mercury
book, December 2006
- Zhang, Hong
- Recent Developments in Mercury Science
Mass-Dependent and -Independent Fractionation of Hg Isotopes by Photoreduction in Aquatic Systems
journal, October 2007
- Bergquist, B. A.; Blum, J. D.
- Science, Vol. 318, Issue 5849
Mercury isotope fractionation during photoreduction in natural water is controlled by its Hg/DOC ratio
journal, November 2009
- Zheng, Wang; Hintelmann, Holger
- Geochimica et Cosmochimica Acta, Vol. 73, Issue 22
Photoreactions of Mercury in Surface Ocean Water: Gross Reaction Kinetics and Possible Pathways
journal, January 2010
- Qureshi, Asif; O’Driscoll, Nelson J.; MacLeod, Matthew
- Environmental Science & Technology, Vol. 44, Issue 2
Mercury dynamics in a small Northern Minnesota lake: water to air exchange and photoreactions of mercury
journal, November 2004
- Hines, Neal A.; Brezonik, Patrick L.
- Marine Chemistry, Vol. 90, Issue 1-4
Mercury photolytic transformation affected by low-molecular-weight natural organics in water
journal, February 2012
- He, Feng; Zheng, Wang; Liang, Liyuan
- Science of The Total Environment, Vol. 416
Dark Oxidation of Dissolved and Liquid Elemental Mercury in Aquatic Environments
journal, January 2005
- Amyot, Marc; Morel, François M. M.; Ariya, Parisa A.
- Environmental Science & Technology, Vol. 39, Issue 1
Diel variations in photoinduced oxidation of Hg0 in freshwater
journal, May 2005
- Garcia, Edenise; Poulain, Alexandre J.; Amyot, Marc
- Chemosphere, Vol. 59, Issue 7
Stimulation of elemental mercury oxidation in the presence of chloride ion in aquatic environments
journal, March 1996
- Yamamoto, Megumi
- Chemosphere, Vol. 32, Issue 6
The evasion and spatial/temporal distribution of mercury species in Long Island Sound, CT-NY
journal, February 2001
- Rolfhus, Kristofer R.; Fitzgerald, William F.
- Geochimica et Cosmochimica Acta, Vol. 65, Issue 3
Importance of elemental mercury in lake sediments
journal, February 2009
- Bouffard, Ariane; Amyot, Marc
- Chemosphere, Vol. 74, Issue 8
History of mercury use and environmental contamination at the Oak Ridge Y-12 Plant
journal, January 2011
- Brooks, Scott C.; Southworth, George R.
- Environmental Pollution, Vol. 159, Issue 1
Photoinduced Oxidation of Hg 0 (aq) in the Waters from the St. Lawrence Estuary
journal, January 2004
- Lalonde, Janick D.; Amyot, Marc; Orvoine, Jord
- Environmental Science & Technology, Vol. 38, Issue 2
Photochemical Formation of Hydroxyl Radical by Constituents of Natural Waters
journal, October 1998
- Vaughan, Pamela P.; Blough, Neil V.
- Environmental Science & Technology, Vol. 32, Issue 19
Nitrate-induced photooxidation of trace organic chemicals in water
journal, May 1987
- Zepp, Richard G.; Hoigne, Juerg.; Bader, Heinz.
- Environmental Science & Technology, Vol. 21, Issue 5
Photosensitizer Method to Determine Rate Constants for the Reaction of Carbonate Radical with Organic Compounds
journal, December 2005
- Canonica, Silvio; Kohn, Tamar; Mac, Marek
- Environmental Science & Technology, Vol. 39, Issue 23
The role of carbonate radical in limiting the persistence of sulfur-containing chemicals in sunlit natural waters
journal, December 2000
- Huang, Jiping; Mabury, Scott A.
- Chemosphere, Vol. 41, Issue 11
Roles of dissolved organic matter in the speciation of mercury and methylmercury in a contaminated ecosystem in Oak Ridge, Tennessee
journal, January 2010
- Dong, Wenming; Liang, Liyuan; Brooks, Scott
- Environmental Chemistry, Vol. 7, Issue 1
A new method for the investigation of mercury redox chemistry in natural waters utilizing deflatable Teflon® bags and additions of isotopically labeled mercury
journal, February 2006
- Whalin, Lindsay M.; Mason, Robert P.
- Analytica Chimica Acta, Vol. 558, Issue 1-2
Mercury reduction and complexation by natural organic matter in anoxic environments
journal, January 2011
- Gu, B.; Bian, Y.; Miller, C. L.
- Proceedings of the National Academy of Sciences, Vol. 108, Issue 4
Mercury Reduction and Oxidation by Reduced Natural Organic Matter in Anoxic Environments
journal, November 2011
- Zheng, Wang; Liang, Liyuan; Gu, Baohua
- Environmental Science & Technology, Vol. 46, Issue 1
Why Dissolved Organic Matter Enhances Photodegradation of Methylmercury
journal, August 2014
- Qian, Yun; Yin, Xiangping; Lin, Hui
- Environmental Science & Technology Letters, Vol. 1, Issue 10
Apparent rates of production and loss of dissolved gaseous mercury (DGM) in a southern reservoir lake (Tennessee, USA)
journal, March 2008
- Zhang, Hong; Dill, Christopher
- Science of The Total Environment, Vol. 392, Issue 2-3
Unexpected Effects of Gene Deletion on Interactions of Mercury with the Methylation-Deficient Mutant Δ hgcAB
journal, April 2014
- Lin, Hui; Hurt, Richard A.; Johs, Alexander
- Environmental Science & Technology Letters, Vol. 1, Issue 5
Oxidation and methylation of dissolved elemental mercury by anaerobic bacteria
journal, August 2013
- Hu, Haiyan; Lin, Hui; Zheng, Wang
- Nature Geoscience, Vol. 6, Issue 9
Chromophore-assisted laser inactivation of proteins is mediated by the photogeneration of free radicals.
journal, March 1994
- Liao, J. C.; Roider, J.; Jay, D. G.
- Proceedings of the National Academy of Sciences, Vol. 91, Issue 7
Photolytic degradation of methylmercury enhanced by binding to natural organic ligands
journal, June 2010
- Zhang, Tong; Hsu-Kim, Heileen
- Nature Geoscience, Vol. 3, Issue 7
Binding Constants of Mercury and Dissolved Organic Matter Determined by a Modified Ion Exchange Technique
journal, April 2011
- Dong, Wenming; Bian, Yongrong; Liang, Liyuan
- Environmental Science & Technology, Vol. 45, Issue 8
Application of the EPR spin-trapping technique for the investigation of the reactions of carbonate, bicarbonate, and phosphate anions with hydroxyl radicals generated by the photolysis of H2O2
journal, December 1992
- Kochany, Jan; Lipczynska-Kochany, Ewa
- Chemosphere, Vol. 25, Issue 12
Generation of Hydroxyl Radicals from Metal-Loaded Humic Acids
journal, June 1999
- Paciolla, Mark D.; Davies, Geoffrey; Jansen, Susan A.
- Environmental Science & Technology, Vol. 33, Issue 11
Hydroxyl Radical Production via the Photo-Fenton Reaction in the Presence of Fulvic Acid
journal, March 2003
- Southworth, Barbara A.; Voelker, Bettina M.
- Environmental Science & Technology, Vol. 37, Issue 6
Sources and Sinks of Hydroxyl Radicals upon Irradiation of Natural Water Samples
journal, May 2006
- Vione, Davide; Falletti, Gianpaolo; Maurino, Valter
- Environmental Science & Technology, Vol. 40, Issue 12
Rate Constants for Reactions of Inorganic Radicals in Aqueous Solution
journal, July 1988
- Neta, P.; Huie, Robert E.; Ross, Alberta B.
- Journal of Physical and Chemical Reference Data, Vol. 17, Issue 3
Collisional Deactivation of O 2 ( 1 Δ g ) by Solvent Molecules. Comparative Experiments with 16 O 2 and 18 O 2
journal, June 1992
- Schmidt, Reinhard; Afshari, Ebrahim
- Berichte der Bunsengesellschaft für physikalische Chemie, Vol. 96, Issue 6
Theoretical and Experimental Studies of the Spin Trapping of Inorganic Radicals by 5,5-Dimethyl-1-Pyrroline N -Oxide (DMPO). 2. Carbonate Radical Anion
journal, December 2006
- Villamena, Frederick A.; Locigno, Edward J.; Rockenbauer, Antal
- The Journal of Physical Chemistry A, Vol. 111, Issue 2
Reduction of mercuric chloride by hydrated electrons and reducing radicals in aqueous solutions. Formation and reactions of mercury chloride (HgCl)
journal, March 1973
- Nazhat, N. B.; Asmus, K. D.
- The Journal of Physical Chemistry, Vol. 77, Issue 5
Mercury in the Atlantic Ocean: factors controlling air–sea exchange of mercury and its distribution in the upper waters
journal, January 2001
- Mason, R. P.; Lawson, N. M.; Sheu, G. -R.
- Deep Sea Research Part II: Topical Studies in Oceanography, Vol. 48, Issue 13
Works referencing / citing this record:
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- Zhang, Jingqi; Chao, Jingbo; Tang, Yang
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