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Roxarsone and it metabolites in organic fertilizer lead to human exposure to arsenic

(09.02.2014)


Background:
Chemical structure of Roxarsone
Chemical structure of Roxarsone
Roxarsone (3-nitro-4-hydroxyphenylarsonic acid) is an organoarsenic feed additive to promote growth, control intestinal parasites and improve feed efficiency in animal production. First approved as animal feed additives in the 1940s, roxarsone and three other very similar arsenic-containing compounds remain legal for use in U.S. chicken, turkey, and swine production. They were never approved as safe for animal feed in the European Union, Japan, and many other countries. In 2006, approximately one million kilograms of roxarsone were produced in the U.S. The toxicity of roxarsone is low but it can be degraded into higher toxic metabolites soon after being excreted by the fed animals or after the animal manure enters environment or when the animal manure is composted. The use of roxarsone as a feed additive had been banned by the European Union in 1999 and the sales of roxarsone also had been suspended by the United States in 2011. However, the voluntary suspension does not preempt Pfizer from selling roxarsone in the future, as FDA has not withdrawn its approval to market the drug in the U.S, and also roxarsone was approved for use in 14 other countries including China.

The new study:
A new study from chinese researchers now shows that more than 96% of roxarsone added in chicken feed was degraded and converted to higher toxic As forms such as arsenite, mono- methylarsonic acid, dimethylarsinic acid, arsenate, 4-hydroxyphenylarsonic acid and other unknown As species. Arsenite and arsenate could be found in roots of vegetables grown in  soil amended with chicken manure,  but only arsenite transported up to shoots. Chicken manure bearing roxarsone and its metabolites increased the arsenic plant uptake by 33–175% for  arsenite, by 28%∼seven times of arsenate in vegetable roots and by 68–175% of arsenite in edible vegetable shoots. Arsenite, the most toxic As form, was the major extractable As species in vegetables accounted for 79–98%. The results reflected that the toxic element As could come into human body via the way: roxarsone in feed → animal → animal manure → soil → crop. It follows, that regarding food security not only chicken meat should be watched carefully but also vegetables applied with animal manure containing roxarsone and its metabolites need to be investigated with great attention.


Editor's comment:
In 2005 (see the EVISA's News below) we commented that the discussion about the human exposure resulting from the use of Roxarsone should motivate analytical scientists to study exposure routes in more detail. 9 years later, this study shows that the use of roxarsone indeed is responsible for human exposure to arsenic. Also a study published 2013 by Nachman et al. (see below) reveals that, despite the voluntarily withdrawal by Pfizer of its arsenical drug roxarsone back in 2011, similar drugs continue to quietly be used in both factory chicken and turkey meat, which may be exposing the public to elevated levels of inorganic arsenic (iAs).
Michael Sperling


The original paper:

Lianxi Huang, Lixian Yao, Zhaohuan He, Changmin Zhou, Guoliang Li, Baomei Yang, Xiancai Deng, Roxarsone and its metabolites in chicken manure significantly enhance the uptake of As species by vegetables, Chemosphere, 100 (2014) 57–62. DOI: 10.1016/j.chemosphere.2013.12.074




Related studies (newest first):

L.X. Huang, L.X. Yao, Z.H. He, C.M. Zhou, G.L. Li, B.M. Yang, Y.F. Li,  Uptake of arsenic species by turnip (Brassica rapa L.) and lettuce (Lactuca sativa L.) treated with roxarsone and its metabolites in chicken manure, Food. Addit. Contam. A, 30 (2013) 1546–1555. DOI: 10.1080/19440049.2013.812809

K.E. Nachman, P.A. Baron, G. Raber, K.A. Francesconi, A. Navas-Acien, D.C. Love, Roxarsone, inorganic arsenic, and other arsenic species in chicken: a U.S.-based market basket sample; Environ. Health Perspect., 121 (2013) 818–824. doi:10.1289/ehp.1206245.

L.X. Huang, Z.H. He, F. Zeng, L.X. Yao, C.M. Zhou, B. Guo, Simultaneous analysis of roxarsone and its metabolites by liquid chromatography-hydrodide generation-atomic fluorescence spectrometry, Chin. J. Anal. Chem., 38 (2010) 1321–1324. DOI: 10.3724/SP.J.1096.2010.01321

Ellen K. Silbergeld, Keeve Nachman, The Environmental and Public Health Risks Associated with Arsenical Use in Animal Feeds, Ann. N.Y. Acad. Sci., 1140 (2008) 346-357. doi: 10.1196/annals.1454.049

Jianjing Liu, Hongxia Yu, Haibin Song, Jing Qiu, Fengmei Sun, Ping Li, Shuming Yang, Simultaneous determination of p-arsanilic acid and roxarsone in feed by liquid chromatography-hydride generation online coupled with atomic fluorescence spectrometry, J. Environ. Monit., 10/8 (2008) 975-978. DOI: 10.1039/b803210f

Konstantinos C. Makris, Shahida Quazi, Pravin Punamiya, Dibyendu Sarkar,
Rupali Datta, Fate of Arsenic in Swine Waste from Concentrated Animal Feeding Operations, J. Environ. Qual., 37/4 (2008) 1626-1633. doi: 10.2134/jeq2007.0479

John F. Stolz, Eranda Perera, Brian Kilonzo, Brian Kail, Bryan Crable, Edward Fisher, Mrunalini Ranganathan, Lars Wormer, Partha Basu, Biotransformation of 3-Nitro-4-hydroxybenzene Arsonic Acid (Roxarsone) and Release of Inorganic Arsenic by Clostridium Species, Environ. Sci. Technol., 41/3 (2007) 818-823. DOI: 10.1021/es061802i

Irail Cortinas, Jim A. Field, Mike Kopplin, John R. Garbarino, A. Jay Gandolfi, Reyes Sierra-Alvarez, Anaerobic Biotransformation of Roxarsone and Related N-Substituted Phenylarsonic Acids, Environ. Sci. Technol., 40/9 (2006) 2951-2957. doi: 10.1021/es051981o

B.P. Jackson, J.C. Seaman, P.M. Bertsch, Fate of arsenic compounds in poultry litter upon land application, Chemosphere, 65/11 (2006) 2028-2034. doi:10.1016/j.chemosphere.2006.06.065

C.G. Rosal, G.-M. Momplaisir, E.M. Heithmar, Roxarsone and transformation products in chicken manure: Determination by capillary electrophoresis-inductively coupled plasma-mass spectrometry, Electrophoresis, 26/7-8 (2005) 1606-1614. DOI: 10.1002/elps.200406198

Rod O'Connor, Mark O'Connor, Kurt Irgolic, Justin Sabrsula, Hakan Gürleyük, R. Brunette, C. Howard, J. Garcia, J. Brien, J. Brien, J. Brien, Transformations, Air  Transport, and Human Impact of Arsenic from Poultry Litter, Environ. Forensics, 6  (2005) 83-89. DOI: 10.1080/15275920590913967

L. Cang, Y.J. Wang, D.M. Zhou,  Y.H. Dong, Heavy metals pollution in poultry and livestock feeds and manures under intensive farming in Jiangsu Province, China, J. Environ. Sci. (China), 16 (2004) 371–374. available from publisher

A.J. Bednar, J.R. Garbarino, I. Ferrer, D.W. Rutherford, R.L. Wershaw, Photodegradation of roxarsone in poultry litter leachates, Sci. Total Environ., 302/1-3 (2003) 237-245. doi:10.1016/S0048-9697(02)00322-4

J.R. Garbarino, A.J. Bednar, D.W. Rutherford, R.S. Beyer, R.L. Wershaw, Environmental Fate of Roxarsone in Poultry Litter. I. Degradation of Roxarsone during Composting, Environ. Sci. Technol., 37/8 (2003) 1509-1514. DOI: 10.1021/es026219q

B. P. Jackson, P. M. Bertsch, M. L. Cabrera, J. J. Camberato, J. C. Seaman,
and C. W. Wood, Trace Element Speciation in Poultry Litter, J. Environ. Qual., 32/2 (2003) 535-540. DOI: 10.2134/jeq2003.0535

H.D. Chapman, Z.B. Johnson, Use of antibiotics and roxarsone in broiler chickens in the USA: analysis for the years 1995–2000, Poultry. Sci., 81 (2002) 356–364. DOI: 10.1093/ps/81.3.356

B.P. Jackson, P.M. Bertsch, Determination of arsenic speciation in poultry wastes by IC-ICP-MS, Environ. Sci. Technol., 35 (2001) 4868–4873. DOI: 10.1021/es0107172

R.L. Weshaw, J.R. Garbarino, M.R. Burkhardt, Roxarsone in Natural Water Systems, in: F.D. Wilde, L.J. Britton, C.V. Miller, D.W. Kolpin, (eds.), Effects of animal feeding operations on water resources and the environment, USGS Open File Report 2000-204, 2000, 95.

Spiros A. Pergantis, Edward M. Heithmar, Thomas A. Hinners, Speciation of Arsenic Animal Feed Additives by Microbore High-performance Liquid Chromatography with Inductively Coupled Plasma Mass Spectrometry, Analyst (London), 122/10 (1997) 1063-1068. DOI: 10.1039/a702691i

John R. Dean, Les Ebdon, Michael E. Foulkes, Helen M. Crews, Robert C. Massey, Determination of the Growth Promoter, 4-Hydroxy-3-Nitrophenyl-Arsonic Acid in Chicken Tissue by Coupled High-performance Liquid Chromatography - Inductively Coupled Plasma Mass Spectrometry, J. Anal. At. Spectrom., 9/5 (1994) 615-618. DOI: 10.1039/JA9940900615


Related Information

FDA: 3-Nitro (Roxarsone) and Chicken
FDA: Questions and Answers Regarding 3-Nitro (Roxarsone)

 
Related EVISA Resources

Link Database: Use of Arsenic
Link Database: Toxicity of Roxarsone
Link Database: Environmental fate of Roxarsone
Brief summary: LC-ICP-MS - The most often used hyphenated system for speciation analysis
Brief summary: Atomic Fluorescence Spectrometry as a Detection System for Speciation Analysis
Brief summary: Speciation and Toxicity



Related EVISA News:

June 10, 2011: U.S. sales of widely used drug "Roxarsone" for chickens to be suspended
January 11, 2007: More evidence linking chicken litter and toxic arsenic
April 4, 2006: Testing finds: Arsenic added to feedstuff finds its way into chicken meat
April 27, 2005: Conflict raised in chicken arsenic debate
February 8, 2005: The use of arsenic in "poultry industry" 


last time modified: February 9, 2014



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