Heavy Metal Contamination in Water and Fishery Resources in Manila Bay Aquaculture Farms

The Philippine Journal of Fisheries 24(2): 74-97 July - December 2017
DOI: 10.31398/tpjf/24.2.2016A0014
HEAVY METAL CONTAMINATION IN WATER

AND FISHERY RESOURCES IN MANILA
BAY AQUACULTURE FARMS

Perelonia, Karl Bryan S., Abendanio, Camille C., Raña, Joan A.*, Opinion,
April Grace R., Villeza, Jordan T., and Cambia, Flordeliza D.
Fisheries Post Harvest Research and Development Division,

National Fisheries Research and Development Institute, Quezon City, Philippines 1103
ABSTRACT
Heavy metals (HM) are high-atomic weight elements hazardous at very low concentrations. Despite the
health risk HM contamination brings, studies conducted were only confined to the offshore and marine por-
tions of the bay. Hence, this study was conducted to establish baseline information and compare the spatial
and seasonal distribution of heavy metal contamination in water and fishery resources in aquaculture farms
and coastal areas in Manila Bay. Water and major aquaculture commodities were collected in November
2014, February 2015 and April 2015 and were analyzed for lead (Pb), cadmium (Cd), and mercury (Hg)
using the following methods: (1) Graphite Furnace Atomizer-Atomic Absorption Spectrophotometry (GFA-
AAS) for Pb and Cd and (2) Mercury Vaporizing Unit-AAS (MVU-AAS) for Hg. Cd (Bataan, Cavite, Bu-
lacan, and Pampanga) and Hg (Cavite and Pampanga) in water were found significantly higher during the
dry season (p<0.05). In contrast, Pb in water was relatively higher during the wet season but levels were not
significantly different with those in the dry. Several sites in Bataan, Bulacan, and Cavite, exceeded DENR
regulatory limits for Pb and Hg in water by 1.35 to 1.8%. As for the fishery commodities, 2/12 milkfish
samples and 1/9 exceeded regulatory limit for Pb in finfish (0.3 mg/kg) by 1.03 to 3.57% while 1/12 milk-
fish samples and 1/13 oyster samples exceeded the limit for Hg in bivalves (0.5 mg/kg) by 0.45 to 0.75%.
Keywords: heavy metals, aquaculture, Manila Bay
74
The Philippine Journal of Fisheries 24(2): 74-97
INTRODUCTION
Heavy metals (HM) are high-atom- Furthermore, contaminated sediments
ic weight elements hazardous at very low may cause death in benthic organisms which
concentrations. These primarily include cad- implies reduced food availability for larger an-
mium (Cd), lead (Pb), and mercury (Hg) imals such as fish. Behavioural anomalies may
(Tiimub & DzifaAfua, 2013). Heavy metals also develop such as impaired locomotors
can enter the aquatic ecosystem from differ- performance resulting in increased suscep-
ent natural and anthropogenic sources such tibility to predators or structural damages,
as domestic wastewater, pesticides and inor- mainly vertebral deformities. In humans, ex-
ganic fertilizers, geologic weathering as well posure to copper, for example, inhibit skeletal
as shipping and harbor activities (Krishna et ossification, while lead cause scoliosis (Kha-
al, 2014). Heavy metal pollution creates an yatzadeh and Abbasi, 2010; Sharma et al, 2014).
immense threat owing to their persistence in
the aquatic environment and accumulation in Human consumption of contaminated
the organisms. Their entering the food chain fish and other aquatic organisms may result in
increases public health risks (Su et al, 2009). transfer and accumulation of metals in the hu-
man body posing a threat on consumer health
Fish absorbs metals through ingestion and safety. Accumulation of high amounts of
of contaminated water, sediments, suspend- heavy metals may cause high blood pressure,
ed solids, and prey organisms. Heavy metals cancerous changes, and damage to kidneys,
have also been observed to undergo bioaccu- liver, and brain. In some cases they may also
mulation and bio-magnification in the tissue lead to mental disorders and loss of brain
of aquatic organisms (Ebrahimi and Taheri- function (Martin & Griswold, 2009).
anfard, 2011). The rate of bioaccumulation of
HM in aquatic organisms depends on several Accumulation of cadmium, for ex-
factors like fish species, ability to digest the ample, affects the liver, kidney, lung, bones,
metals, feeding habits, age of fish, lipid con- placenta, brain, and the central nervous sys-
tent in the tissue, and the concentration of tem. Other damages such as reproductive and
such metal in the area (Eneji, 2011; Khayatza- development toxicity, hepatic, haematolog-
deh and Abbasi, 2010; Su et al, 2009). Heavy ical, and immunological effects in character
metals accumulate mainly in kidneys, adrenal may also result (Morais et al, 2012). Moreover,
glands, liver, lungs or gills in fish, hair and chronic lead intoxication in adults can cause
skin (Martin & Griswold, 2009). anaemia, cancer, reproductive harm in males,
and hormonal imbalance of vitamin D metab-
Heavy metals, in trace amounts, have olism (WHO, 1995). Exposure to high levels
different roles for aquatic organisms’ prop- of metallic, inorganic, or organic mercury can
er physiological functions (Khayatzadeh and permanently damage the brain, kidneys, and
Abbasi, 2010). However, water bodies with even the developing fetus (Morais et al, 2012).
a high amount of these negatively affect the
aquatic organisms. Heavy metal pollution pri- Manila Bay is known as one of the pre-
marily inhibits the growth of fish and other mier fishing grounds in the country making
aquatic organisms. It also reduces the survival fishing as the primary source of livelihood
of fish larvae, which may considerably reduce around the bay. Surrounding coastal commu-
the fish population or result in their extinction. nities are benefited by the bountiful aquatic re-
75
Heavy Metal Contamination in Water and Fishery
Resources in Manila Bay Aquaculture Farms
sources. Moreover, the once varied ecological river mouths were higher than in the water
habitats like sea grasses, corals, and mangroves inside the bay, suggesting that the contribu-
in the bay area serve as the breeding grounds tion of land-based human activities is a ma-
of fish life and also serve indirect ecological jor source of pollution. Similar results were
functions (e.g. shoreline stabilization, storm observed in the case of HM in the sediments.
barriers, and carbon storage) (PEMSEA, 2006). In the case of HM concentration in the organ-
isms’ tissues, scad (0.067 mg/kg), sardines
Aquaculture in the provinces around species (1.39 mg/kg), and crevalle (0.296 mg/
Manila Bay was first documented in 1932 kg) are among the pelagic fish that appear to
with the introduction of oyster farming in have a high bioaccumulation of metals. HM
Binakayan, Cavite (Yap, 1999), one of the most in shellfish (mussels and oysters) from Manila
productive aquaculture areas in the country. Bay, specifically from the mouth of the Pasig
Manila Bay accounts for an average of al- River, may pose a relatively significant risk to
most 50% of the national production of tiger human health since concentrations showed
prawn and oyster (PEMSEA, 2006). As report- high RQ values of 3.8 to 7 for lead (Pb).
ed by BAS (2012), the volume of aquaculture
production in Manila bay provinces (Bataan, These studies were confined to the off-
Pampanga, Bulacan, Cavite, and NCR) in 2010 shore and marine portions of the bay only.
has reached 335,985.80 MT, 3% higher than It was only lately that Dr. Marlo Mendoza
2009 production of 314,110.74 MT. However, (unpublished) obtained data concerning HM
all these resources, which are quite beneficial concentrations in freshwater and brackishwa-
to all Filipinos especially those living near the ter aquaculture species in areas surrounding
bay, are constantly under threat. Population Manila Bay. Results of monitoring conducted
expansion, rapid urbanization, uncontrolled from January to December 2008 showed that
coast, and basin development and misman- heavy metals, such as As, Cd, Cu, Mn, Ni,
agement of resources are apparent in many Zn, Pb, Cr, and Hg were present in milkfish,
areas around the bay. Products of moderniza- tilapia, prawns, green mussel, clam “paros”,
tion are considered major threats to the bay’s and oysters collected from the area. The lev-
sustainability and productivity because these els ranged from non-detectable (ND) to sev-
products result in water pollution, including eral folds higher than the standard limits set
HM pollution. by BFAR (Fisheries Administrative Order 210
Series of 2001) and US Environmental Pro-
Several studies have been conducted tection Agency, EPA (2000). Based on stan-
to assess the contamination of HM in Manila dards set by Codex Alimentarius Commis-
bay. According to Su et al (2009), HM particu- sion (CAC 206), European Union EC1881-206
larly total chromium, total lead and total cad- and US FDA Centre for Food Safety and Ap-
mium were evident in the bay waters, fish and plied Nutrition (CFSAN), however, these are
macroinvertebrates. The study of Velazquez et acceptable. These results prompted BFAR to
al (2010) showed that the total dissolved cop- conduct a verification study, which also aims
per and cadmium were labile while total dis- to generate baseline information on the possi-
solved zinc was organically bound. Elevated ble contamination of heavy metals in fish and
levels of these metals near point sources sug- fishery products from Manila bay and adja-
gest anthropogenic inputs in the bay. Results cent aquaculture areas.
of the risk assessment conducted by PEMSEA
and MBEMP TWG-RRA (2004) showed that This study aims to establish baseline
the concentrations of HM in water around information and compare the spatial and sea-
76
sonal distribution of heavy metal contamina- were variable, as sample collection is sole-
tion in water and fishery resources in aqua- ly dependent on the availability of samples.
culture farms and coastal areas in Manila Bay.
Fifty six (56) samples of aquaculture
commodities (12 milkfish, 9 tilapia, 7 crab,
METHODOLOGY 5 shrimp, 13 oyster, and 10 mussel) were
collected throughout the sampling period.
Sampling Sites and Collection of Samples Freshly harvested fish and shellfish of at least
one kilogram (1kg) per species were put sep-
Blocking strategy and sampling sites arately in an appropriately-labeled re-seal-
used in Chapter 2 was employed in this study. able polyethylene bags and placed in a tem-
Forty-seven pre-identified aquaculture farms perature-controlled cooler kept at 0 to 4°C for
were sampled each season –November 2014 transport at laboratory for analyses.
for the wet season and February and April
2015 for the dry season. River tributaries of Fish samples were cleaned and dissect-
the aquaculture farms were also sampled for ed, composited and homogenized to make up
comparison. at least 200 grams. Homogenized samples
were stored in re-sealable polyethylene bags
WATER SAMPLES and placed in the ultralow freezer (-80°C) pri-
or to analysis.
Water samples about one liter (1L) were
collected in composite for heavy metal analy- Method of Heavy Metal Analyses
ses and were placed in appropriate container,
preserved with acid, labeled and transported Water samples were analyzed for total
to the laboratory in a temperature-controlled mercury (Hg), lead (Pb), cadmium (Cd) and
cooler. Storage and preservation of collected hexavalent chromium (Cr+6). As for the fish
water samples were done according to US-En- and fishery resources, all the above-mentioned
vironmental Protection Agency (EPA), Sam- HM analyses were conducted except for the
pling and Analysis of Waters, wastewaters hexavalent chromium. The method used for
soils and Wastes (2009). both water and fish was the closed vessel-mi-
crowave-assisted-acid digestion adopting the
Eighty one (81) water samples (35 method of the manufacturer, followed by an-
pond, 35 water source, 2 pen, and 9 coastal alytical determinations of metals using the
area) were collected during the wet season following instruments: (1) Graphite Furnace
(November 2014), while 82 water samples Atomizer-Atomic Absorption Spectrophotom-
(35 pond, 35 water source, 3 pen, and 9 coast- eter (GFA-AAS) for Pb and Cd and (2) Mercu-
al area) were collected during the dry season ry Vaporizing Unit AAS (MVU-AAS) for Hg.
(February and April 2015). The reference methods used for the analysis
of heavy metals in water were US-EPA 3015a,
FISH SAMPLES 2007(Cd, Hg, and Pb) and US-EPA 7196a 1992,
(hexavalent chromium) and for fish samples,
Six kinds of farmed fishery resources modified AOAC 2013.06 was used.
were collected from the aquaculture farms
for the study – tilapia, milkfish, shrimp, crab, To ensure the accuracy and reliability
mussel, and oyster. However, sample spe- of analytical results, the laboratory performed
cies and number of samples collected per site quality assurance and quality control schemes
77
(e.g. mid-standards, recovery of fortified sam- LEAD

ples, and method/reagent blanks) and other
performance characteristics for method vali- Table 4.1 summarizes the values of
dation (e.g. repeatability, reproducibility and lead concentration obtained for the both sam-
accuracy using Certified Reference Materials). pling periods, while its spatial distribution in
aquaculture farms are presented in Figure 4.1.
Statistical Analyses
Lead levels in the aquaculture farms
The levels of HM in the aquaculture for the both sampling season were found
farms and water sources during the wet and to be variable, with values ranging from
dry seasons were compared using t-test, as ND to 0.0759 mg/L. The highest concentra-
well as its seasonal variations. On the other tion was observed in a pond water sample
hand, HM in the fishery commodities collect- from Southern Bataan (November 2014).
ed during the wet and dry seasons were com-
pared using Analysis of Variance (ANOVA). During wet season, levels of lead
All statistical analyses were carried out using ranged from ND to 0.0759 mg/L, with three
SPSS version 20. sampling sites (one in Northern Bataan and
two in Southern Bataan) exceeding DENR
regulatory limit of 0.05 mg/L, and were found
RESULTS relatively higher compared to the dry sea-
son, with levels of Lead ranging from ND to
Levels of Heavy Metals in Water 0.0251 mg/L and all sites conforming with
the limit. However, there was no significant
Levels of heavy metals in the aquacul- difference in the levels of lead in the dif-
ture farms varied among the different blocks. ferent blocks in both sampling periods (p >
The following are the ranges of the levels list- 0.05, refer to Table 4.2). In addition, statistical
ed from the most abundant to the least: lead analysis showed that lead concentration in
(ND to 0.0759 mg/L); cadmium (ND - 0.0028 aquaculture farm (pond, pen and coastal wa-
mg/L); mercury (ND to 0.0065 mg/L); and ters) and their respective water sources had
hexavalent chromium (ND). no significant difference (p>0.05), as shown
Table 4.1. Lead concentrations in aquaculture farms for wet (November 2014) and dry season (February and
April 2015.
Mean Lead Concentration Lead Concentration Range

BLOCK
(ppm, mg/L ) (ppm, mg/L )
Block 1 (Eastern Bulacan) 0.0143 0.0022 – 0.0251
Block 2 (Western Bulacan) 0.0085 0.0014 – 0.0185
Block 3 (Northern Bataan) 0.0129 ND – 0.0502
Block 4 (Southern Bataan) 0.0232 0.0035 – 0.0759
Block 5 (Cavite) 0.0089 ND – 0.0178
Block 7 (Pampanga) 0.0078 ND – 0.0308
78
Figure 4.1. Levels of lead in coastal areas/fish pens, ponds, and water sourcesin November 2014 (A) and April
2015 (B).
79
Table 4.2. Seasonal comparison of heavy metal concentration in aquaculture farms.
Sampling Cd, mg/L Hg, mg/L Pb, mg/L

Sites Wet Dry Wet Dry Wet Dry
B1 0.00016 0.00020 0.00010 0.00100 0.0092 0.00844
P = 0.681 P = 0.298 P = 0.863
Significance, α0.05 Not Significant Not Significant Not Significant
B2 0.00016 0.00076 0.0007 0.0007 0.0075 0.0077
P = 0.098 P = 0.172 P = 0.927
B3 0.00007 0.00027 0.0004 0.0006 0.01746 0.0061
P = 0.004 P = 0.529 P = 0.249
Significance, α0.05 Significant Not Significant Not Significant
B4 0.00042 0.00088 0.0012 0.0005 0.02953 0.0097
P = 0.009 P = 0.342 P = 0.069
Significance, α0.05 Significant Not Significant Not Significant
B5 0.0002 0.0012 0.00004 0.00374 0.0098 0.0088
P = 0.012 P = 0.000 P = 0.773
Significance, α0.05 Significant Significant Not Significant
B7 0.0003 1.4934 0.0001 0.0012 0.0096 0.006
P = 0.016 P = 0.000 P = 0.394
Significance, α0.05 Significant Significant Not Significant
in Table 4.3. This indicates that neither the Bulacan, Eastern Bulacan, and Northern Bata-
aquaculture farm nor the water source affect- an. Those in Southern Bataan, on the other
ed the level of lead in the other. hand, pling sites passed the DENR regulatory
limit of 0.01 mg/L for cadmium in water.
CADMIUM
T-test results showed that cadmium
Reflected in Figure 4.2 are the levels levels in the aquaculture farms in Northern
of cadmium in the different sampling sites Bataan with an average cadmium concen-
during the wet and the dry seasons. On the tration of 0.00017 mg/L, were significantly
other hand, Table 4.4 shows the cadmium con- higher (p<0.05) than the water source (mean =
centrations obtained throughout the sampling 0.00015 µg/ml)during wet season, as indicat-
period. ed in Table 4.3.
Cadmium levels during the dry season MERCURY

(range of ND - 0.0028 mg/L) were significant-
ly higher (p<0.05) compared to the wet sea- Levels of mercury in the aquaculture
son were comparable with all the blocks. All farms during the wet and dry seasons are
sam-(range of ND - 0.0023 mg/L). Cadmium presented in Figure 4.3. On the other hand,
concentrations in Cavite and Pampanga were Table 4.5 shows the mercury concentrations
significantly higher (p<0.01) than in Western obtained throughout the sampling period.
80
Table 4.3. Comparison of concentrations of heavy metal in pond collected from different sites of Manila Bay
during wet and dry seasons.
WET
Sites Pond River Pond River Pond River
B1 0.0002 0.0002 0.0012 0.0011 0.0101 0.0096
P = 0.802 P = 0.215 P = 0.652
B2 0.0008 0.0011 N.D. N.D. 0.0077 0.0033
P = 0.0574 P = 0.151
No variance
Significance, α0.05 Not Significant Not Significant
B3 0.0001 0.00001 0.0003 0.0002 0.0175 0.0004
P = 0.018 P = 0.449 P = 0.044
Significance, α0.05 Significant Not Significant Significant
B4 0.0004 0.0003 0.0012 0.0002 0.0295 0.0352
P = 0.578 P = 0.142 P = 0.739
B5 0.0002 0.0002 0.00004 0.00012 0.0098 0.0036
P = 0.423 P = 0.545 P = 0.125
B7 0.0003 0.0009 0.0001 0.00006 0.0096 0.00155
P = 0.105 P = 0.337 P = 0.224
DRY
Sites Pond River Pond River Pond River
B1 0.0002 0.0002 0.0012 0.0011 0.0101 0.0096
P = 0.539 P = 0.619 P = 0.915
B2 0.0002 0.00005 0.0007 0.0002 0.0075 0.0064
P = 0.487 P = 0.667 P = 0.579
B3 0.0003 0.0003 0.0006 0.0004 0.0064 0.0064
P = 0.562 P = 0.200 P = 0.835
B4 0.0009 0.0009 0.0005 0.00003 0.0098 0.0079
P = 0.906 P = 0.378 P = 0.388
B5 0.0012 0.0011 0.0037 0.0031 0.0088 0.0046
P = 0.857 P = 0.164 P = 0.341
B7 0.0015 0.0012 0.0012 0.00043 0.006 0.0051
P = 0.643 P = 0.006 P = 0.565
Significance, α0.05 Not Significant Significant Not Significant
81
Table 4.4. Cadmium concentrations in aquaculture farms for wet (November 2014) and dry season (February
and April 2015.
Mean Cadmium Cadmium Concentration

BLOCK
Concentration (ppm, mg/L ) Range (ppm, mg/L )
Block 1 (Eastern Bulacan) 0.0003 0.00004 – 0.00050
Block 2 (Western Bulacan) 0.0007 ND – 0.0027
Block 4 (Southern Bataan) 0.0006 0.0002 – 0.0011
Block 5 (Cavite) 0.0008 0.0001 – 0.0019
Mercury levels during the dry season cury levels in the aquafarm than its water
(range of ND - 0.0065 mg/L) were higher than source, as indicated in Table 4.3.
in the wet season (range of ND - 0.0037 mg/L).
Significantly higher mercury levels during the
dry season were observed in Cavite and Pam- Levels of Heavy Metals in Fish and Fishery
panga (p<0.05). Resources
Three out of 46 sampling sites, all noted Heavy metals in fish and fishery re-
in Southern Bataan during the wet season ex- sources had no significant difference (p>0.05)
ceeded DENR regulatory limit of 0.002 mg/L during the wet (November) and dry (Febru-
for mercury in water. For the dry season, 14 ary and April) seasons except for lead in crab
out of 47 sites – three from Eastern Bulacan, (refer to Table 4.6). The following are the rang-
one in Western Bulacan, Northern Bataan, and es and mean values of heavy metals in aqua-
Southern Bataan, and eight in Cavite – failed culture commodities collected arranged in
to meet the DENR regulatory limit. descending order: lead (ND - 1.0723 mg/kg;
0.1463 mg/kg); cadmium (ND - 0.5526 mg/kg;
T-test results showed that only Pam- 0.0606 mg/kg); and mercury (ND - 1.1063 mg/
panga had significantly higher (p<0.05) mer kg; 0.0567 mg/kg).
Table 4.5. Mercury concentrations in aquaculture farms for wet (November 2014) and dry season (February
and April 2015.
Mean Mercury Concentration Mercury Concentration Range

BLOCK
(ppm, mg/L ) (ppm, mg/L )
Block 1 (Eastern Bulacan) 0.0008 ND – 0.0034
Block 2 (Western Bulacan) 0.0004 ND – 0.0022
Block 4 (Southern Bataan) 0.0010 ND – 0.0037
Block 5 (Cavite) 0.0022 ND – 0.0065
82
Figure 4.2. Levels of cadmium in coastal areas/fish pens, ponds, and water sourcesin November 2014 (A) and
April 2015 (B).
83
Figure 4.3. Levels of mercury in coastal areas/fish pens, ponds, and water sourcesin November 2014 (A) and
April 2015 (B).
84
Table 4.6. Seasonal comparison of heavy metal concentrations in crab.

HEAVY METAL CONCENTRATIONS (ppm, mg/kg)
SEASON
Cd Hg Pb
Wet 0.0174 0.0122 0.0609
Dry 0.0191 0.0581 0.2640
P = 0.997 P = 0.570 P = 0.030
Significance, α0.05 Not Significant Not Significant Significant
Table 4.7. Seasonal comparison of heavy metal concentrations in milkfish.

SEASON
Cd Hg Pb
Wet 0.0159 0.1568 0.1986
Dry 0.0105 0.0269 0.1384
P = 0.068 P = 0.699 P = 0.788
Table 4.8. Seasonal comparison of heavy metal concentrations in mussel.

SEASON
Cd Hg Pb
Wet 0.0269 0.0179 0.1781
Dry 0.0384 0.0844 0.2079
P = 0.546 P = 0.534 P = 0.761
Table 4.9. Seasonal comparison of heavy metal concentrations in oyster.

SEASON
Cd Hg Pb
Wet 0.0804 0.5590 0.1203
Dry 0.2044 0.2249 0.1515
P = 0.153 P = 0.449 P = 0.663
Table 4.10. Seasonal comparison of heavy metal concentrations in shrimp.

SEASON
Cd Hg Pb
Wet 0.0158 0.0076 0.0914
Dry 0.0091 0.0091 0.1652
P = 0.327 P = 0.810 P = 0.654
85
Table 4.11. Seasonal comparison of heavy metal concentrations in tilapia.

SEASON
Cd Hg Pb
Wet 0.0122 0.1021 0.1242
Dry 0.0121 0.0637 0.2223
P = 0.978 P = 0.776 P = 0.205
LEAD values noted in Cavite. All oyster and mus-

sel samples collected had lead concentrations
Results for lead concentration in aqua- within the regulatory limit of 1.5 mg/kg (EC
culture commodities collected are reflected 1881/2006).
in Figure 4.4. Lead concentrations in samples
collected in the wet season ranged from ND CADMIUM
to 1.0723 mg/kg, with the highest noted in a
milkfish sample from Eastern Bulacan, while Cadmium levels in aquaculture com-
dry season lead concentrations ranged from modities collected during the wet and the dry
ND to 0.3953 mg/kg, the highest noted in a seasons are presented in Figure 4.5. Cadmi-
mussel sample from Cavite. um concentrations in the dry season (range of
0.0034 - 0.5526 mg/kg) were relatively higher
Lead concentrations in milkfish sam- compared to cadmium concentrations in wet
ples ranged from ND to 1.0723 mg/kg, high- season (range of ND - 0.1283 mg/kg). Highest
est in a sample collected in Eastern Bulacan, concentrations for both seasons were noted in
while lead levels in tilapia samples ranged oyster samples from Western Bulacan.
from ND to 0.3087 mg/kg, highest in sample
from Pampanga. Two out of twelve milkfish Cadmium in milkfish samples ranged
samples, collected from Eastern Bulacan (wet from ND to 0.0178 mg/kg, the highest concen-
season) and Pampanga (dry season), and one tration noted in a sample collected from Pam-
out of nine tilapia samples, collected from panga, while the levels in tilapia ranged from
Pampanga (dry), failed to meet the regulatory ND to 0.0191 mg/kg, the highest observed in a
limit of 0.3 mg/kg (EC 1881/2006). sample from Northern Bataan. All finfish sam-
ples had levels within the regulatory limit of
Crab samples had lead concentrations 0.05 mg/kg (EC 1881/2006).
ranging from ND to 0.2688 mg/kg, highest in
sample collected from Cavite while shrimp Crab and shrimp samples had cad-
samples had lead levels that ranged from ND mium concentrations ranging from 0.0047 to
to 0.3065 mg/kg, highest in sample collected 0.0392 mg/kg and 0.0034 to 0.0158 mg/kg, re-
from Pampanga. Lead concentrations in all spectively. The highest levels in both species
the crustacean samples were within the regu- were noted in samples collected from Pam-
latory limit of 0.5 mg/kg (EC 1881/2006). panga. Cadmium concentrations in crusta-
cean samples were within the regulatory limit
Lead in oyster and mussel samples of 0.5 mg/kg (EC 1881/2006).
ranged from ND to 0.3147 mg/kg and 0.0726
to 0.3953 mg/kg, respectively, both maximum Cadmium levels in oyster samples,
86
1.5
Bivalves (1.5) A
1.2
0.9
Lead (µg/g)
0.6
Crustacean (0.5)
Finfish (0.3)
0.3
0.0
0 1
Eastern 2
Western 3 4
Southern 5
Cavite 6
Pampanga
Northern
Bulacan Bulacan Bataan Bataan
1.5
Bivalves (1.5) B
1.2
0.9
Lead (µg/g)
0.6
Crustacean (0.5)
Finfish (0.3)
0.3
0.0
0 1 2 3 4 5 6
Eastern Western Northern Southern Cavite Pampanga
Figure 4.4. Lead levels in aquaculture commodities collected in wet season (A) and in the dry season (B).
Milkfish (MF) Tilapia (TI) Crab (CR) Shrimp (SH) Oyster (OY) Mussel (MU)
87
1.0
Bivalves (1.0) A
0.8
Cadmium (µg/g)
Crustacean (0.5)
0.5
0.3
Finfish (0.05)
0.0
0 1 2 3 4 5 6
1.0
Bivalves (1.0) B
0.8
Cadmium (µg/g)
Crustacean (0.5)
0.5
0.3
Finfish (0.05)
0.0
0 1 2 3 4 5 6
Figure 4.5. Cadmium levels in aquaculture commodities collected in the wet season (A) and in the dry season (B).
88
ranging from 0.0500 to 0.5526 mg/kg, were son) failed to meet the regulatory limit of 0.5
highest in a sample collected in Western Bu- mg/kg (EC 1881/2006).
lacan. Oyster had higher levels than mussels
whose range was from 0.0077 to 0.0769 mg/kg,
and highest in a sample from Northern Bata- Method Validation
an. All bivalve samples had cadmium concen-
trations within the regulatory limit of 1.0 mg/ The methods for the determination of
kg (EC 1881/2006). total cadmium (Cd), lead (Pb), and mercury
(Hg) were validated by using spiked con-
MERCURY centrations of 1 µg/L Cd, 5 µg/L Pb, and 0.1
µg Hg in different fishery resources such as
Mercury in aquaculture commodities finfish (n=9), crustaceans (n=7), and mollusk
collected in the wet and the dry seasons are (n=9). Validation were also done in certified
presented in Figure 4.6. As shown, the wet reference material (CRM) sample, DORM-3
season samples had mercury levels ranging (NRC-CNRC Fish Protein Certified Refer-
from ND to 1.1063 mg/kg, while dry season ence Material for Trace Metals) with certi-
samples had levels ranging from ND to 0.1271 fied values of 0.290±.020 mg/kg for cadmium,
mg/kg. Maximum mercury concentrations 0.395±0.050 mg/kg for lead, and 0.382±0.060
were noted in oyster (wet) and mussel (dry) mg/kg for mercury. The calculations for the
samples both collected from Eastern Bulacan. method detection limit (MDL) and limit of
quantification (LOQ) were based on signal-to-
Milkfish samples had mercury levels noise ratio since the analytical procedure ex-
ranging from ND to 0.6662 mg/kg, highest hibited a baseline noise. The determination of
in a sample collected from Pampanga, while method MDL and LOQ was done by compar-
tilapia samples had mercury concentrations ing the measured signal of the spiked blank
ranging from ND to 0.2930 mg/kg, highest in sample with those of the signal of the blank
sample collected from Eastern Bulacan. One sample alone. Results of the method valida-
out of twelve milkfish samples (collected from tion are summarized in Table 4.12.
Pampanga, wet season) failed to meet the reg-
ulatory limit of 0.5 mg/kg (EC 1881/2006).
DISCUSSION
Mercury in crab samples ranged from
ND to 0.1257 mg/kg, highest in a sample col- Spatial and Seasonal Distribution of Heavy
lected from Western Bulacan, while those in Metals in Water
shrimp ranged from ND to 0.0846 mg/kg,
highest in a sample collected from Northern Heavy metals are known to exist in
Bataan. All crustacean samples had mercury trace amounts in the environment. These are
levels within the regulatory limit of 0.5 mg/kg naturally harmless (Shremati & Varma, 2010).
(EC 1881/2006). However, continuous urbanization and in-
dustrialization along with the increase in
Oyster and mussel samples had mercu- population and different anthropogenic activ-
ry concentrations ranging from ND to 1.1063 ities result in the increment of these (Oluyemi
mg/kg and ND to 0.1271 mg/kg, respectively. et al, 2008) to alarming levels necessitat-
Maximum values in both were noted in East- ing that regulatory standards are to be set.
ern Bulacan. One out of thirteen oyster sam-
ples (collected from Eastern Bulacan, wet sea- Rainfall causes urban runoff, a non-
89
1.2
A
0.9
Mercury (µg/g)
N N
0.6
D D
Finfish, Crustacean, Bivalves (0.5)
0.3
0.0
0 1
Eastern 2
Western 3 4
Southern 5
Cavite 6
Pampanga
Northern
1.2
B
0.9
Mercury (µg/g)
0.6
Finfish, Crustacean, Bivalves (0.5)
0.3
0
0 1 2 3 4 5 6
Figure 4.6. Mercury levels in aquaculture commodities collected in the wet season (A) and in the dry season (B).
90
Table 4.12. Summary of the method validation results for total cadmium, lead, and mercury.
Performance Characteristics and CADMIUM: LEAD: MERCURY:

its Accepted Criteria Microwave digestion followed Microwave digestion followed Microwave digestion followed
by Graphite Furnace by Graphite Furnace by Mercury Vapor Unit
MDL * 0.0011 (Fish) 0.0334 (Fish) 0.0353(Fish)

0.0033 (Mollusk) 0.0480 (Mollusk) 0.0291 (Bivalves)
0.0034 (Crustaceans) 0.0205 (Crustaceans)
LOQ ¥ 0.0036 (Fish) 0.1114 (Fish) 0.1176 (Fish)

0.0109 (Mollusk) 0.1598 (Mollusk) 0.971 (Bivalves/ Mollusk)
0.0113 (Crustaceans) 0.0683 (Crustaceans)
Mean Concentration δ 0.0001±0.00002 0.0005±0.00007
Mean % RSD α 1.68% 12.98%
Accuracy: Spike 87.49% 77.06% 76.7-113.4%

% Recovery (40-120% for Pb and 78.46-101.77% 72.06-81.17%
Cd; 80-110 for Hg) β
Accuracy: CRM 100.10% 98.47% 80.47-116.62% (Day 1)

% Recovery (80 -110%) β 92.81-106.65% 88.39-110.73% 88.38-125.84% (Day2)
All concentrations are expressed as µg/g total cadmium, lead and mercury
* MDL is calculated as 3 X standard deviation
¥ LOQ is calculated as 3.33 X LOD
δ Mean concentration is the average concentration of the number of samples analyzed
α % Relative standard deviation, calculated as: (standard deviation divided by mean concentration) X 100
β % Recovery is calculated as: (difference of concentration of the spiked and unspiked samples divided
by the theoretical concentration) X 100; reported % recovery range corresponds to number of samples analyzed.
point source of pollution, that carries sever- only in the atmosphere but also in the soil,
al contaminants, including heavy metals (US which in turn gets washed off into river sys-
EPA, 2016), draining into river systems and tems (Buat-Ménard et al, 1987; Hutton et al,
enters aquaculture farms through water ex- 1987). Quarrying and coal combustion, two of
change activities (Srivanasa et al, 2007). It is the anthropogenic activities that emit cadmi-
known that water exchange activity in ponds um, are practiced in the province following the
is more frequent during the wet season since 1991 eruption of Mount Pinatubo as reported
water levels in river tributaries or water sourc- by the Greenpeace Southeast Asia and Orejas
es increases with rainfall, thus more water is in 2014. Some aquaculture farmers do not ob-
available for the farmers (Yoo& Boyd, 1994). serve proper buffer zone nor monitor water
This only means that rainfall results in an in- quality; they had the highest population of
crease in heavy metal concentration in pond chicken and wild birds among the provinces,
water due to the continuous influx of water. and used chicken manure and urea as fertil-
This is evident in the high concentrations of izers, as reported in the previous study con-
lead during the wet season where rainfall is ducted by the group, “Review of Aquaculture
greater. Practice and Anthropogenic Activities in Manila
Bay Aquaculture Farms.” Inorganic fertilizers
Contrary to the case of lead, cadmium such as urea as well as chicken manure may
and mercury concentrations were found high- contain trace metals such as cadmium, which
er during the dry season. This can be attribut- are deposited in pond sediment (Benson et
ed to slow water exchange owing to the limit- al, 2014; Boyd & Masaut, 1999). Buffer zones
ed supply from water sources, and/or due to filter out wastes, fertilizers, pesticide runoffs,
an increase in temperature, which increases and other contaminants (chemical and micro-
the evaporation rate. In a study by Nartey et biological) from entering the ponds (DeFries,
al (2011), mercury concentrations in the river Karanth, & Pareeth, 2010). The lack of these
increased with increased evaporation rate of may result in higher contamination of the
surface water. Cadmium, on the other hand, pond.
is a very soluble heavy metal easily leached
from the sediments and dissolved in water Mercury was found highest in Cavite
(Rajan et al, 2013). where the population is highest among the
provinces sampled (NSO, 2010). Mercury is
Aside from the observed seasonal dis- primarily used in dental amalgams, fluores-
tribution of heavy metal contamination in cent lights, thermometers, electric switches,
aquaculture farms, spatial distribution was batteries, insecticide, disinfectant, rat poi-
also observed. Cadmium was found highest sons, and even in skin ointments (The Co-
in Pampanga, where farming, fishing, man- lumbia Electronic Encyclopedia, 2012). Since
ufacturing, handicrafts, poultry and swine, the province has the highest population, it
food processing industries, as well as ceram- is safe to assume that production as well as
ics and metalworking are the main sources usage of above-mentioned products is high-
of livelihood (pampanga.gov.ph). Wetlands, est in the province and so is mercury emis-
swamplands, agricultural lands, clay, grav- sion. Aside from anthropogenic activities al-
el, sand, and copper are the natural resourc- ready discussed, mining and quarrying, huge
es there (alviera.ph). Pampanga is adjacent contributors to mercury contamination, are
to Zambales, which houses Mount Pinatubo, major components of production land-use
an active volcano. Volcanic action is known in the province (cavite.gov.ph). Mercury is
as one of the natural sources of cadmium not discharged into the air (gets deposited into
92
the ground through precipitation) or water valves, which was observed to be higher com-
through point sources (Lindberg et al, 1987). pared to the other aquaculture commodities
This in turn gets into aquaculture farms by analyzed, may be attributed to their feeding
way of river systems. In addition, aquaculture habit of filter feeding (Garrido-Handog, 1990;
farmers in Cavite bypass residual waste re- Aypa, 1990). Filter feeders siphon the water in
moval and water flushing – two activities that which they are suspended through filters that
reduce contamination in the pond – during retain suspended matter, like phytoplanktons
pond preparation as reported in the previous (Barker Jørgensen, 1990). This siphoning and
study conducted by the group entitled, “Re- filtration processes cause heavy metals in the
view of Aquaculture Practice and Anthropogenic water column to pass through the organism,
Activities in Manila Bay Aquaculture Farms.” ultimately to get deposited in different cel-
lular compartments (Rodríguez de la Rúa et
Lead, which is known to come from al, 2005). Oysters and mussels were collected
gasoline, batteries, ammunition, paint, ceram- from coastal areas. It is known that all efflu-
ics, and even in cosmetics (US EPA, 2015) was ents, treated and untreated, flow to the bay as
found highest in Bataan, where oil and gas- the bay is the catch basin for all water systems
oline companies, refineries, and feed mills in Manila Bay. As shown in the results on the
are the major industry sectors. The province, heavy metals in water, although inconsistent,
which will soon be considered a special de- concentration of heavy metals came out to be
fense economic zone, has also been manufac- high in coastal areas. This implies that higher
turing ammunition for nearly 60 years (Rive- heavy metal concentration in the water col-
ra, 2015). Aquaculture farmers in the province umn causes a higher contamination in aqua-
use urea, an inorganic fertilizer that may culture commodities.
contribute to the concentration of lead in the
water. In a study by Benson et al in 2013, lead Heavy metals in aquaculture commod-
concentration was found highest among the ities were found higher during the dry season
other trace elements in the urea fertilizer. than the wet season. Milkfish, tilapia, shrimp,
and crab feeding habits depend on tempera-
Heavy Metals Concentration in Fish and ture; as temperature increases, feeding fre-
Fishery Resources quency also increases (FAO2, 2011; Garcia,
1990; Greenfield et al, 2005; Benitez, 1984) and
Aquaculture commodities such as so does their heavy metal uptake.
milkfish, tilapia, shrimp, crab, mussel, and
oyster differ in several ways – size, produc-
tion cycle, feeding habit, etc. It is only logical CONCLUSION
to assume that the uptake of heavy metals
in the above-mentioned commodities differ Lead was found higher during the wet
from species to species. In fact, findings in season while cadmium and mercury, during
a study by Su et al (2009) suggest that accu- the dry season. The following are the sites
mulation of heavy metals in aquatic organ- that failed to meet DENR regulatory limits for
isms is species-dependent. In the present heavy metals in water in wet season: Northern
study, heavy metal accumulation in aqua- Bataan (1) and Southern Bataan (2) for lead
culture commodities is as follows: oyster > (0.05 µg/mL); Northern Bataan (3) for mercu-
mussel >tilapia > shrimp > crab > milkfish. ry (0.002 µg/mL); while the following are the
sites that failed DENR regulatory limits in
Heavy metal contamination in bi- the dry season: Eastern Bulacan (3), Western
93
Bulacan (1), Northern Bataan (1), Southern associated with the use of chemicals
Bataan (1), and Cavite (8) for mercury (0.002 in pond aquaculture. Aquacultural
µg/mL). Cadmium was found highest in Pam- Engineering, 20 (1999), 113-132.
panga, while mercury and lead in Cavite and
Bataan, respectively. Two out twelve milkfish Bureau of Agricultural Statistics (BAS). (2010).
samples and one out of nine tilapia samples
failed to meet the regulatory limit for lead in Chang, K. H., Amano, A., Miller, T. W., Isobe
finfish (0.3µg/g) while one out of twelve milk- T., Maneja, R., Siringan, F.P., Imai, H.,
fish samples and one out of thirteen oyster sam- and S. Nakano. (2009). Pollution study
ples exceeded the limit for mercury in finfish in manila bay: Eutrophication and its
(0.5 µg/g) and bivalves (0.5 µg/g), respectively. impact on plankton community. In-
terdisciplinary Studies on Environ-
mental Research in Asia, 261-267.
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The Philippine Journal of Fisheries 24(2): 74-97 July - December 2017

HEAVY METAL CONTAMINATION IN WATER

BAY AQUACULTURE FARMS

Fisheries Post Harvest Research and Development Division,

Keywords: heavy metals, aquaculture, Manila Bay

(e.g. mid-standards, recovery of fortified sam- LEAD

Mean Lead Concentration Lead Concentration Range

Table 4.2. Seasonal comparison of heavy metal concentration in aquaculture farms.

Sampling Cd, mg/L Hg, mg/L Pb, mg/L

Cadmium levels during the dry season MERCURY

Mean Cadmium Cadmium Concentration

Mean Mercury Concentration Mercury Concentration Range

Table 4.6. Seasonal comparison of heavy metal concentrations in crab.

Table 4.7. Seasonal comparison of heavy metal concentrations in milkfish.

Table 4.8. Seasonal comparison of heavy metal concentrations in mussel.

Table 4.9. Seasonal comparison of heavy metal concentrations in oyster.

Table 4.10. Seasonal comparison of heavy metal concentrations in shrimp.

Table 4.11. Seasonal comparison of heavy metal concentrations in tilapia.

LEAD values noted in Cavite. All oyster and mus-

Performance Characteristics and CADMIUM: LEAD: MERCURY:

MDL * 0.0011 (Fish) 0.0334 (Fish) 0.0353(Fish)

LOQ ¥ 0.0036 (Fish) 0.1114 (Fish) 0.1176 (Fish)

Mean Concentration δ 0.0001±0.00002 0.0005±0.00007

Mean % RSD α 1.68% 12.98%

Accuracy: Spike 87.49% 77.06% 76.7-113.4%

Accuracy: CRM 100.10% 98.47% 80.47-116.62% (Day 1)

Nonpoint Source Pollution. Retrieved Bay, Philippines. Marine Pollution

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