In Reply Refer To:

AFHC/DEQ/016835

Water Docket, EPA Docket Center

Environmental Protection Agency

Mailcode 4101T

1200 Pennsylvania Avenue, NW

Washington, DC

Re: EPA DOCKET CONTROL NUMBER OW-2003-0080

The U.S. Fish and Wildlife Service appreciates the opportunity to submit
the following comments to the U.S. Environmental Protection Agency
regarding the Draft Ambient Aquatic Life Water Quality Criteria for
Nonylphenol (EPA DOCKET CONTROL NUMBER OW-2003-0080).

# BACKGROUND

Nonylphenol is an organic chemical with known endocrine disrupting
capabilities that is largely used as a chemical intermediate in the
production of nonylphenol ethoxylate (NPE) nonionic surfactants. The
domestic production of nonylphenol reached 230 pounds in 1998 and is
estimated to grow by 2% each year. Because of its solubility in water,
persistence in water and sediments, and demonstrated ability to
bioaccumulate in aquatic organisms, concern has been raised for biota
inhabiting both freshwater and saltwater habitats. To date, water
quality monitoring programs have identified concentrations of
nonylphenol in water or sediments that exceed levels found to produce
effects in biota in areas associated with industrial activity and sewage
outflow (Bennie 1999). While nonylphenol is considered alone in these
criteria, it is often found in conjunction with other alkylphenol
ethoxylates as a function of NPE degradation.

# COMMENTS

While the Agency's Office of Water appears to have performed a generally
thorough review of the literature pertaining to the bioaccumulative
ability and effects of nonylphenol to aquatic organisms, there are a
number of relevant studies that were either overlooked in this process
or published after the analysis was completed. Citations for these
studies are listed at the end of this correspondence.

Of particular concern are two investigations conducted by Nice et al.
(2000 and 2003) in which effects were detected in aquatic organisms at
exposure levels below the final criteria concentrations. In the 2000
study, concentrations of nonylphenol as low as

2

0.1 ug/L, an order of magnitude below the saltwater criteria, resulted
in alterations in development of Pacific oyster (*Crassostrea gigas*)
over a 72-hour exposure period. However, more dramatic effects were
observed in the 2003 study, in which a single

48-hour exposure of Pacific oyster larvae to 1 ug/L nonylphenol resulted
in skewed sex ratios and almost 20% hermaphroditism. (Baseline
hermaphroditism in oviparous oysters generally does not exceed 1%.)
Also, effects persisted to the next generation with extremely low
survivorship of progeny in which at least one parent was exposed to the
single pulse of nonylphenol. The authors suggest that nonylphenol may be
accumulated in the larval oyster and later transferred to developing
gametes, a scenario documented to occur in fish for other lipophilic
chemicals.

# RECOMMENDATIONS

The Service asks that before rendering a final Aquatic Life Water
Quality Criteria for nonylphenol that a new literature search is
completed to capture all recent publications and that all studies
referenced in this letter are considered and reviewed in the subsequent
analysis. In addition, there appears to be an increasing number of
studies describing endocrine disrupting effects of nonylphenol at low
levels of exposure, including the reproductive impairment exhibited by
Nice et al. In light of this new data, the Service asks that the EPA
reconsider studies currently addressed in the Draft Criteria that reveal
possible endocrine effects at levels below the draft criteria value
(e.g., alterations in Sertoli cell number and morphology,
Miles-Richardson et al., 1999; reduction in vitellogenin and embryo
survival, Schwaiger et al., 2002; growth reduction possibly due to
precocious sexual development, Ashfield et al., 1998). While long-term
or population effects may be difficult to surmise from these studies
individually, taken together they suggest a pattern of endocrine
function alteration in aquatic species exposed to nonylphenol. Given the
high degree of variation in interspecific chemical sensitivity and the
lack of consideration of multi-stressor scenarios and chemical mixtures
such as would be experienced in natural settings (including additive or
synergistic effects of other NPE breakdown products), the Service
believes that consideration of these low-level effects is essential in
the protection of aquatic and aquatic-dependent species, and in EPA's
fulfillment of its responsibility to protect threatened and endangered
species as described in Section 7(a)(1) of the Endangered Species Act.

Thank you for the opportunity to comment on the nonylphenol Aquatic Life
Water Quality Criteria. We look forward to working closely with you on
this and future document reviews related to the development of water
quality criteria. If you have any questions or require additional
information, please contact Nancy Golden, Division of Environmental
Quality at (703) 358-2148.

Sincerely,

Everett Wilson, Chief

Division of Environmental Quality

(signed copy to follow via mail)

cc: DEQ Surname 322

FWS/DEQ:NGolden:cv:4/5/04 file:
/media/pszemraj/PeterTrove/project-files/DATA/ms-word-files/big-DOC/328737.doc

**Literature not reviewed in draft criteria document:**

Arsenault, JTM, WL Fairchild, DL MacLatchy, L Burridge, K Haya, and SB
Brown. 2004. Effects of water-borne 4-nonylphenol and 17-estradiol
exposures during parr-smolt transformation on growth and plasma IGF-I of
Atlantic salmon (*Salmo salar* L.). Aquatic Toxicology 66:255-265.

Arukwe, A, BM Nilsen, K Berg, and A Goksoyr. 1999. Immunohistochemical
analysis of the vitellogenin response in the liver Atlantic salmon
exposed to environmental oestrogens. Biomarkers 4:373-380.

Beechman RK. 1999. Effect of the endocrine disrupter nonylphenol on the
marine copepod *Tisbe battagliai*. The Science of the Total Environment
233:33-46.

Brown, RJ, M Conradi, and MH Depledge. 1999. Long-term exposure to
4-nonylphenol affects sexual differentiation and growth of the amphipod
*Corophium volutator* (Pallas, 1766). The Science of the Total
Environment 233:77-88.

Christensen LJ, Korsgaard B, and P Bjerregaard. 1999. The effect of
4-nonylphenol on the synthesis of vitellogenin in the flounder
*Platichthys flesus*. Aquatic Toxicology 211-219.

Hecht, S and BL Boese. 2002. Sensitivity of an infaunal amphipod,
*Eohaustorius estuarius*, to acute waterborne exposures of
4-nonylphenol: evidence of a toxic hangover. Environmental Toxicology
and Chemistry 21:816--819.

Hecht, SA, JS Gunnarsson, BL Boese, JO Lamberson, C Schaffner, W Giger,
and PC Jepson. 2004. Influences of sedimentary organic matter quality on
the bioaccumulation of 4-nonylphenol by estuarine amphipods.
Environmental Toxicology and Chemistry 23:865-873.

Hoyt, PR, MJ Doktycz, KL Beattie, MS Greeley Jr. 2003. DNA microarrays
detect 4-nonylphenol-induced alterations in gene expression during
zebrafish early development. Ecotoxicology 12:469-74.

Moore, A, AP Scott, N Lowera, I Katsiadaki, and L Greenwood. 2003. The
effects of 4-nonylphenol and atrazine on Atlantic salmon (*Salmo salar*
L) smolts. Aquaculture 222:253--263.

Nice, HE, MC Thorndyke D. Morritt, S. Steele, and M. Crane. 2000.
Development of *Crassostrea gigas* larvae is affected by 4-nonylphenol.
Marine Pollution Bulletin 40:491-496.

Nice, HE, D Morritt, M Crane, and M Thorndyke. 2003. Long-term and
transgenerational effects of nonylphenol exposure at a key stage in the
development of *Crassostrea gigas*. Possible endocrine disruption?
Marine Ecology Progress Series 256:293-300. Current literature not
reviewed in draft criteria document.

Rice, CP, I Schmitz-Afonso, JE Loyo-Rosales, E Link, R Thoma, L Fay, D
Altfater, and MJ Camp. 2003. Alkylphenol and alkylphenol-ethoxylates in
carp, water, and sediment from the Cuyahoga River, Ohio. Environmental
Science and Technology 37:3747-3754.

Uguz, C, M Iscan, A Ergüven, B Isgor, and I Togan. 2003. The
bioaccumulation of nonylphenol and its adverse effect on the liver of
rainbow trout (*Onchorynchus mykiss*). Environmental Research
92:262--270.

Zhang, L, and KN Baer. 2001. The effects of 4-nonylphenol on
reproduction and embryo development in Daphia magna. Toxicologist
60:163.

# Other literature cited

Ashfield LA, TG Pottinger, and JP Sumpter. 1998. Exposure of female
juvenile rainbow trout to alkylphenolic compounds results in
modifications to growth and ovosomatic index. Environmental Toxicology
and Chemistry 17:679-686.

Bennie DT. 1999. Review of the environmental occurrence of alkylphenols
and alkylphenol ethoxylates. Water Quality Research Journal of Canada
34:79-122.

Miles-Richardson SR, SL Pierens, KM Nichols, VJ Kramer, EM Snyder, SA
Snyder, JA Render, SD Fitzgerald, and JP Giesy. 1999. Effects of
waterborne exposure to 4-nonylphenol and nonylphenol ethoxylate on
secondary sex characteristics and gonads of fathead minnows (*Pimephales
promelas*). Environmental Research (Series A) 80:S122-S137.

Schwaiger J, U Mallow, H Ferling, S Knoeer, T Braunbeck, W Kalbfus, and
RD Negele. 2002. How estrogenic is nonylphenol: A transgenerational
study using rainbow trout (*Oncorhynchus mykiss*) as a test organism.
Aquatic Toxicology 59:177-189.