BSc (Hons) Environmental Science: Dissertation

8/14/2019 BSc (Hons) Environmental Science: Dissertation

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NOTTINGHAM TRENT UNIVERSITY

A COMPARISON OF THE HEAVY-METAL LOADING BETWEEN A GRAZED AND

UNGRAZED SALTMARSH IN MORECAMBE BAY

by

ANTHONY McKEOWN


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ABSTRACT

Heavy-metals pose a risk to organisms and are substantially more prevalent in the

environment as a result of anthropogenic activities. Morecambe Bay, UK is a European

Marine site with established estuarine saltmarshes and a history of metalliferous mining

in watersheds draining into the bay. The 63m sediment fraction of two separate areas

of saltmarsh, grazed and ungrazed, in the Ulverston Channel draining into the north of

Morecambe Bay were analysed for their residual fraction of copper, zinc and lead to a

depth of 22.86cm by digestion in aqua regia and analysis by inductively-coupled plasma

optical emission spectroscopy (ICP-OES). Soil parameters such as pH, Electrical

Conductivity (EC), moisture content (%) and organic matter (%) were also determined

and with the exception of pH, significant differences between sites were found in all.

Despite physicochemical conditions at the ungrazed site seeming more favourable to

l i i ifi diff i h i f h l


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ACKNOWLEDGMENTS

I would firstly like to thank my tutor and chief supervisor Dr. Nicholas Ray of

Nottingham Trent University for his guidance and support throughout not only my

project but also the academic years preceding and surrounding it. I would like to also

thank, in alphabetical order: Dr. Benjamin Clutterbuck; Dr. Mike Coffey; Dr. Kirsty

Mitchell; Nigel Mould; and Sheralyn Smith, all of Nottingham Trent University, for their

assistance in the laboratory work and data analysis I undertook. Often these people

went above and beyond the call of duty for me and it is very much appreciated. A

special thank you must be extended to Neil Forbes, Ranger Supervisor at the National

Trust, and Nicola Evans of Natural England, for granting permission to conduct the work

on the saltmarshes, which are protected habitats under EU legislation. I must express

my gratitude to Will and Victoria Case of Plumpton Cottage Farm, who authorised the

li f Pl M h hi h i d b h i f il A h k f i d


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What would the world be, once bereft

Of wet and wilderness? Let them be left,

Oh let them be left, wilderness and wet;

Long live the weeds and wilderness yet.


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TABLE OF CONTENTS

Abstract .............................................................................................................................................................. 2

Acknowledgments .............................................................. ................................................................. ........... 3

1 Introduction ............................................................................................................ ............................... 10

1.1 Pollution of coastal wetlands ....................................................... .......................................... 10

1.1.1 History of anthropogenic pollution ............................................................................. 11

1.1.2 Contemporary pollution issues...................................................... ............................... 12

1.2 Heavy-metals ...................................................................................... .......................................... 13

1.2.1 The role of metals in biological functions ........................................................ ......... 13

1.2.2 Metal toxicity........................ ................................................................. ............................... 14


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1.3.7 Heavy metals in saltmarsh ............................................................... ............................... 32

1.3.8 Saltmarsh extent and locations in the UK ........................................................ ......... 36

1.4 Aims and objectives ............................................................... .................................................... 37

1.4.1 Hypotheses ................................................. ................................................................. ......... 37

Hypothesis #1 .................................................. ................................................................. .................... 37

Hypothesis #2 .................................................. ................................................................. .................... 38

Hypothesis #3 .................................................. ................................................................. .................... 38

Hypothesis #4 .................................................. ................................................................. .................... 38

1.4.2 Metal profiles ................................................................................................... .................... 38

1.5 Morecambe Bay ................................................. ................................................................. ......... 38

1.5.1 Geology and geography of Morecambe Bay ............................................................. 39


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Brackenhurst Campus laboratory (The Bramley Building) .................................... ............ 55

Clifton Campus laboratory (Rosalind Franklin Building) .................................................... 56

2.4 Inductively Coupled Plasma Optical Emission Spectroscopy (ICP-OES) ........... 56

2.5 Statistical techniques ............................................................. .................................................... 57

2.6

Geographical Information Systems (GIS) ........................................... ............................... 58

3 Results ...................................................... ................................................................. ............................... 59

3.1 Heavy-metals ...................................................................................... .......................................... 59

3.1.1 Plumpton saltmarsh (SD324801) ................................................................................ 60

3.1.2 Plumpton Hall saltmarsh (SD314786) .............................................................. ......... 61

3.2 Soil parameters ............................................................. ............................................................... 62

3.2.1 Plumpton saltmarsh (SD324801) ................................................................................ 62


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3.4.2 Plumpton Marsh (SD324801) ................................................................... .................... 71

3.4.3 Plumpton Hall Marsh (SD314786) .................................................................. ............ 72

3.5 Regression Analysis .............................. ................................................................. .................... 72

3.5.1 Pooled data ........................... ................................................................. ............................... 72

pH.......................................................................................................... ..................................................... 72

Moisture Content............................................. ................................................................. .................... 73

Organic matter................................................................................. ..................................................... 74

3.5.2 Individual ......................................... ................................................................. .................... 74

Organic Matter................................................................................. ..................................................... 74

3.6 Multiple regression ............................... ................................................................. .................... 75

3.7 GIS Interpolation .......................................................... ............................................................... 75


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4.3 Limitations ........................................................... ................................................................. ......... 85

4.4 Improvements to the study ........................................................... .......................................... 85

5 Conclusion .................................................................... .............................................................. ............ 85

6 Reference List .............................................................. ................................................................. ......... 86

7

Appendix 1: Mines in Cumbria .................................................................................................... 111

8 Appendix 2: Inventory of Equipment Used ........................... ................................................. 113

9 Appendix 3: Raw Primary Data ................................................................................................... 114

9.1 Plumpton Marsh ................................................................................................................. ...... 114

9.1.1 pH and Electrical Conductivity (Siemens/cm) ................................................. 114

9.1.2 Moisture Content (%) and Loss On Ignition (%) ................................................ 115

9.2 Plumpton Hall ..................................................... ................................................................. ...... 116


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1 INTRODUCTIONThe pervasiveness of heavy-metals in the environment is of major concern due to their

perturbation of biochemical processes, their potential for bioaccumulation in food-webs

and the threat they pose to life (van Malderen, Hoornaert & van Grieken 1996). Coastal

wetland1areas such as saltmarsh are depositional environments for suspended organic

and particulate matter, which heavy-metals preferentially bind to (Callaway et al.1998;

Spencer, Cundy & Croudace 2003). Those located in or connected to areas with a history

of anthropogenic activity can be particularly enriched compared to background levels

(Bromberg Gedan, Silliman & Bertness 2009). Saltmarsh extent has been declining

worldwide for centuries, primarily due to their location in areas desirable for human

settlement (Doody 2008; Weis & Butler 2009). Global mean sea-level (MSL) is predicted

to rise over the current century (IPCC 2007a). Any restriction on the ability of saltmarsh


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al.1997; Millennium Ecosystem Assessment, 2005). Wetlands face numerous threats

and are suffering a decline in their global extent as a result (Bromberg Gedan, Silliman &Bertness 2009; Silliman, Grosholz & Bertness (eds.) 2009). Although an accurate figure

is difficult to identify, the OECD (1996) estimate 50% of global wetlands have been lost

since 1900.

Coastlines are dynamic and subject to natural processes which modify them physically,

chemically and biologically on varying spatial and temporal scales (Williams, Dodd &

Gohn 1991). Due to inadequate knowledge of their nature humans disturb these

processes both directly and indirectly, placing multiple, intense and often competing

pressures on the coastline and associated habitats (Kay & Alder 2005). Removal or

addition of material through dredging and land reclamation are amongst the most

conspicuous direct impacts but of equal concern are the insidious effects of various


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development through the Iron and Bronze Ages (Photos, 1989) and GRIP2ice-core

analysis indicates that effluents resulting from smelting by the civilizations of ancientGreece, Rome and medieval China were hemispheric rather than localised (Hong et al.

1996). The advent of the Industrial Revolution coupled with an increasing human

population led to a substantial rise in resource use and pollution in many guises

becoming a more serious, global problem (Candelone et al.1995; Nriagu 1996; Jrup

2003).

1.1.2 Contemporary pollution issues

Heavy-metals are amongst a suite of pollutants of major concern due to their capacity toseriously damage the health of many organisms, ecosystems and habitats (Table 1).

Table 1Anthropogenic pollutants of chief concern (adapted from Pierzynski et al., (2000))

Pollutant Examples

Compartment Impacted

ImpactsWater


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Certain metals are therefore known biochemically as trace or essentialelements and

regarded as such when (a) they are present in all living tissues within a zoological

family; (b) depletion or removal causes deficiency symptoms which cease when supply

is returned; and (c) deficiency symptoms can be ascribed to a distinct biochemical

defect (Frstner & Wittman 1981). Certain metals are understood to be vital for

optimum human development (Table 2).

Table 2 Essential metals and respective concentrations for human beings (expressed in mg/70kg bodyweight) (adapted from Frstner & Wittman, 1981, after Vahrenkampf, 1973).

Period

Group

IA IIA VIB VIIB VIII IB IIB

311Na

70,000

12Mg

40,000

419K

250,000

20Ca

1,700,000

25Mn

30

26Fe

7,000

27Co

1

29Cu

150

30Zn

3,000


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similar metalloids with no identifiable biological function, known as non-essential

elements, can be deleterious even in small quantities. Wood (1974) proposed a

classification of elements based on three criteria (Table 3).

Table 3 Classification of elements according to toxicity and availability. Essential elements that canbecome toxic are highlighted in bold (adapted from Wood, 1974).

Noncritical

Toxic but very insoluble or

very rare

Very toxic and relatively

accessible

Sodium (Na) Carbon (C)

Fluorine (F) Potassium (K)

Phosphorous (P) Lithium (Li)

Magnesium (Mg) Iron (Fe)

Rubidium (Rb) Calcium (Ca)

Sulphur (S) Strontium (Sr)

Hydrogen (H) Chlorine (Cl)

Aluminium (Al) Oxygen (O)

Bromine (Br) Silicon (Si)

Nitrogen (N)

Titanium (Ti) Gallium (Ga)

Hafnium (Hf) Lanthanum (La)

Zircon (Zr) Osmium (Os)

Tungsten (W) Rhodium (Rh)

Niobium (Nb) Iridium (Ir)

Tantalum (Ta) Ruthenium (Ru)

Rhenium (Re) Barium (Ba)

Beryllium (Be) Arsenic (As)

Gold (Au) Cobalt (Co)

Selenium (Se) Mercury (Hg)

Nickel (Ni) Tellurium (Te)

Thallium (Tl) Copper (Cu)

Palladium (Pd) Lead (Pb)

Zinc (Zn) Silver (Ag)

Antimony (Sb) Tin (Sn)

Cadmium (Cd) Bismuth (Bi)

Platinum (Pt)


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aeolian and fluvial transportation provides parent material to terrestrial and marine

landscapes (Thornton 1981). Hydrolytic weathering mobilises hydronium (H3O+) which

can penetrate mineral crystal lattices, create a charge imbalance and break

metaloxygen bonds, removing them from rocks in solution. Weaker bonds disassociate

more readily. Liberation of lithospheric metals is the primary natural source but others

include volcanic eruptions and outgassings (Bagnato et al.2007), animal excretion

(including humans) (Nicholson et al.2003) and forest fires. Natural sources contribute

to the background level of heavy-metals in environmental compartments, which vary

spatially according to local geology (Frstner & Wittman 1981; Pierzynski, Sims & Vance

2000; ICMM 2007). Organisms have evolved within background level ranges which are

usually low enough not to warrant concern. Occasionally surface or near-surface

mineralization results in localized zones of contamination. Organisms may adapt to this

(Posthuma & van Straalen 1993) or the area may become reduced in or devoid of life.


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Figure 1.1Global production and emissions of selected heavy-metals 1850-1990 (Jrup 2003).

Since increased metal consumption is one of the best indicators of material progress

(Krech, McNeill & Merchant (eds.) 2004) this general trend is likely to reflect most


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Mining and smelting of metal-bearing ores releases heavy-metals as atmospheric

particulates as well as leaching metals into the aqueous phase (Jennings et al.2008) via

acid mine drainage (AMD). The degree of mineralisation of the tailings and surrounding

geochemical conditions determine the intensity of metal pollution around mines

(Navarro et al.2008). Dissolved metals resulting from AMD can threaten marine

organisms many years after the closure of nearby mines (Grout & Levings 2001)

(Johnston et al.2008).

Since 1990 emissions of many heavy-metals in European countries have reduced

significantly due to recognition of their harmful effects and subsequent legislation to

lessen their impacts (Travnikov et al. 2012). The ban on leaded petrol in many

developed countries has profoundly lowered concentrations found in the environment

(Landrigan 2002).


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occurs when particles are removed from the atmosphere by falling hydrometeors

constituting precipitation.

On the ground surface run-off can transport heavy-metals between compartments.

Precipitation can leach them into water-tables or wash them from impermeable

surfaces into drainage systems. Transport-related substances in particular take this

route as they form part of the particulate dust found in urbanised areas (Legret &

Pagato 1999) (Turer, Maynard & Sansalone 2001).

1.2.5 Heavy-metal behaviour in environmental compartmentsThe behaviour of heavy-metals in compartments varies according to their speciation

and the physicochemical conditions found there, influenced by biotic and abiotic factors

(Brown Jr. et al. 1999). pH is the master variable and metal availability generally


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(Fest et al.2008) and humic colloids in suspension the majority eventually settle to

become incorporated into sediments.

Soil

Soil is a reservoir for heavy-metals and pollution can be long-lasting due to the

relatively strong adsorption of metals to organic matter and clay (Alloway & Ayres

1993; Franklin & Jones 1994; Pierzynski, Sims & Vance 2000; Nicholson et al., 2003;

Zimmerman & Weindorf, 2010). Clays, especially those containing aluminium, are

anionic and able to adsorb hydrated metal cations (Mn+):

Metals are thus held in the soil and prevented from leaching out. They can be released

slowly by cation exchange whereby different ions in the soil displace them from the clay

surface and into the aqueous phase:


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decomposed fragments of plants and soil organisms. The latter is a complex mixture of

amorphous and colloidal substances highly-modified from the original organic tissues

and containing highly-polymerised compounds (Winfield 1995). Cellulose material

broken down to a resistant state of decomposition leaves long protein molecules. Lone

electron pairs on the nitrogen atoms of these molecules are donated into empty orbital

shells of metal cations to form a ring-like structure known as a chelate. These

organomineral complexes restrict the solubility and mobility of metals in soil (Tapia et

al.2010). Complexes with di- and polyvalent metals exhibit the highest stability and

stability generally follows the order Cu > Fe = Al > Mn = Co > Zn. Generally, organic

matter levels will correlate positively with total metal concentrations in soils (Otte et al.

1993). The influence of organic matter (solid and dissolved) on heavy-metal behaviour

is particularly strong in sandy soils such as is found in saltmarshes (Fest et al.2008).


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Typical concentrations of heavy-metals in the soils of England and Wales are presented

in Table 6.

Table 6 Typical concentrations (mg kg-1dry matter) of heavy-metals in the soils of England and Wales (EA, 2010)

Metal 10thPercentile Median 90thPercentile Arithmetic mean

Copper 9 18 37 23

Zinc 38 82 147 97

Cadmium 0.2 0.7 1.4 0.8

Lead 20 40 131 74

1.2.6 Heavy-metals in estuarine systems

Firm evidence exists for the capacity of wetlands to store and accumulate heavy-metals

(Valiela & Teal 1974; Windom 1977). Estuaries are open systems linking different

environmental compartments and transferring energy and material between


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2005; Siddique & Aktar 2012). Most heavy-metals are found bound to sulphides in the

anoxic zone (Weis & Weis 2004). Changes in physicochemical conditions such as an

increase in soil acidity or a reduction in organic matter can mobilise metals in the

residual fraction (Vega et al.2009). Numerous sediment quality guidelines (SQGs) have

been devised worldwide and the values for Cu, Zn & Pb in some of the most popularly

cited are presented in Table 7 & 8.

Table 7 Sediment Quality Guidelines of various countries and respective concentrations.

Guidelines Cu Zn Pb References

Ontario GuidelinesLEL 16 120 31

Fletcher et al.(2008)SEL 110 820 250

Hong Kong ISQVsISQV-Low 65 200 75

(Bai et al.2012)ISQV-High 270 410 218

Sediment Quality Criteria of China Class I 35 150 60 (Bai et al. 2012)Class II 100 350 130

LEL: lowest effect level; SEL: severe effect level; ISQV: interim sediment quality value.

Table 8Screening Quick Reference Table (SQuiRT) for heavy-metal concentrations in marine sediment mg kg-1(Buchman 2008)

acee

tThreshold

ff l

Effect Probable

ff l

Effects Range

d ( )

Apparent Effects Threshold

( )


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in a steady decline worldwide but recent recognition of the many EG&S they provide has

led to a reappraisal of their worth and subsequent protection under EU legislation6

(Costanza et al. 1997; English Nature 2000; Jones et al.2011). Despite a long history of

study (Chapman, 1939; Chapman, 1940) debate still surrounds many of the processes

governing saltmarsh establishment, development and ecology which has implications

for the decision-making processes of management plans aimed at protecting and

restoring this precious habitat.

1.3.1 Saltmarsh establishment and succession

Saltmarsh formation varies between locations but is generally regulated by four

physical factors: tidal regime, sediment supply, wind-wave climate and relative sea-level

fluctuations (JNCC, 2004; Jones et al.2010). Essentially, in sheltered conditions fine

sediments suspended within tidal waters settle onto a variety of substrates and


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littoral zone and beyond where it provides food for microorganisms and detritivores

and forms the basis of food-webs important to humans (Valiela, 1975; Odum 1988).

Spartina anglicais a particularly well adapted halophyte. It has deeply recessed

respiratory pores to reduce water loss and glands to secrete salt as well as thick,

leathery leaves which protect against tidal scour by water-borne silt. It also has an

elaborate root system. Fine surface roots bind the mud and long thick roots with air

channels hold it firmly within it (Colebourn 1984). Fauna diversity in saltmarshes is also

low and the most ubiquitous animal found is birds (Packham & Willis 1997). Other

animal visitors may include mink, water voles and other rodents from the land as well

as aquatic creatures such as seals and dolphins at high tide (Adam 1990).

1.3.3 Subsurface hydrology and chemistry

The chemistry of saltmarsh is complex and varies between sites but a number of general


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materials within inundating waters (Weis & Butler 2009). The rate of clay accretion can

thus affect the rate of vegetation succession (van Wijnen & Bakker 1997).

Table 9 Comparison of physical characteristics between tidal freshwater marshes and salt marshes (adapted fromOdum, 1988).

Tidal freshwater marsh Saltmarsh

LocationHead of the estuary (above theoligohaline zone)

Mid and lower estuary

Geographical distributionWorldwide, usually associated withrivers

Worldwide, not always associatedwith rivers

Salinity Annual average below 0.5 ppt Annual average 18.0 - 35.0 ppt

Tidal range

Ocean-derived lunar tide, oftengreater amplitude than nearby saltmarshes

Ocean-derived lunar tide

SedimentsSilt-clay, high organic content, low-moderate root and peat content

More sand, lower organic content,higher peat and root content

Streambank morphologyLow gradient, little undercutting Steeper gradient, more

undercutting

Stream channel Low sinuosity Moderate to high sinuosity


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(Silliman, Grosholz & Bertness (eds.) 2009). Attempts to control mosquito populations

led to the infilling of creeks and pans as well as the use of pesticides on many

saltmarshes in the USA (Bromberg Gedan, Silliman & Bertness 2009) (Weis & Butler

2009). In south-east England saltmarshes have been declining continuously at a rate of

approximately 40 ha a-1for the past 50 years (Hughes & Paramor 2004).

Table 10Recent saltmarsh loss at sites in south-east England (adapted from French and Burningham, 2003)Location Net saltmarsh loss in hectares and (%) 1973-98

Orwell estuary (Suffolk) 46 ha (46%)Stour Estuary (Suffolk/Essex) 157 ha (59%)Hamford Water (Essex) 255 ha (29%)Blackwater estuary (Essex) 197 ha (22%)Dengie (Essex open coast) 64 ha (14%)Crouch estuary (Essex) 159 ha (34%)

The reasons are largely unknown and research can be complicated by a number of

factors. Isostatic rebound is thought to be exacerbating rising MSL by causing a relative

sea-level (RSL) rise (Jones et al.2011) at a rate above which saltmarsh can keep pace


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Coastal squeeze describes the inability of saltmarsh to migrate landward due to physical

barriers. It has been blamed for saltmarsh loss in areas where land is protected by sea-

walls. Provided they receive a sufficient supply of sediment saltmarsh can extend

seaward and thus the claim that coastal squeeze is primarily to blame for losses in these

areas is refuted by some researchers. Invertebrate infauna is suggested to impede plant

colonisation through bioturbation, herbivory and seed consumption (Hughes & Paramor

2004). Conversely, Morris et al.(2004) assert that the presence of such infauna is

essential for healthy mudflat ecology with bioturbation providing adequate oxygenation

for other organisms which in turn provide sustenance for indigenous and migratory

birds.

Saltmarshes vulnerability to pollution stems from their location in or near estuaries and

coastlines and the various inputs to these areas from coastal waters, local run-off,


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In Europe, grazing by livestock is one of the oldest traditions and this has a major effect

on the ecology and geomorphology of the saltmarshes (Jensen, 1985; Silliman, Grosholz

& Bertness (eds.) 2009). Six main impacts arise from grazing: defoliation of plants;

removal of plant material; treading and pawing deposition of faeces; deposition of urine;

and uprooting plants, which are growing in soft sediments (Jensen et al.1985). In

ungrazed areas natural succession dictates the changes in vegetational communities

(Bos et al.2005). Reimold et al.(1975) found aerial plant production and fiddler crab

numbers to be reduced in a grazed saltmarsh community compared to ungrazed and

formerly grazed areas, suggesting that the lower biomass production has an effect on

detritivore populations. Abandoning grazing in an area can result in a loss of

biodiversity but both biomass and litter production can increase due to the vigour of the

domineering species (Bos et al.2005; Silliman, Grosholz & Bertness (eds.) 2009).


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and the capacity of species such as Phragmites australisfor the phytoremediation of

contaminated areas has been recognized by several studies (Weis & Weis 2004;

Windom et al.2001). The potential for heavy-metal translocation via uptake and release

by plants or erosion and remobilisation of contaminated sediments is of more concern

than any effects on the plants themselves (Burd 1995).

Emmerson et al.(1997) used multivariate statistical techniques to assess the spatial

distribution of heavy-metals at various locations in the Blackwater Estuary, Essex. A

general seaward decrease in heavy-metal concentrations was found, suggesting that

heavy-metals derived from local anthropogenic sources higher up the estuary. Elevated

levels were found in one lower estuary location which was not comparable with a site a

similar distance from the nearest urban area. The former area is an enhanced

depositional environment with extensive mudflats and saltmarshes. Where dilution and


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heavy-metals in summer. The opposite was found for soils densely colonised by S.

maritima, which showed a decrease in pH and concomitant increase in heavy-metal

concentrations. This was attributed to an increase in soil aeration and subsequent

oxidation of metal sulphides such as Acid Volatile Sulphate (AVS) and pyrite. Burke et al.

(2000) compared the release of metals by two saltmarsh grasses in field and laboratory

conditions. They found that Spartina alternifloraboth accumulated and released

significantly more metals than Phragmites australis. This could have repercussions for

restoration schemes within contaminated areas, with S.alterniflorapossibly liberating

sediment-bound heavy-metals and making them available to detritivores and food-webs

surrounding them. Salinity can also affect the accumulation of metals in vegetation and a

positive correlation has been shown to exist between salinity and translocation to the

shoots of certain saltmarsh plants. Fitzgerald et al. (2003) suggest the inclusion of such

considerations when choosing species for biomonitoring purposes. MacLeod et al.


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between 1989-1992 could be attributed to the erosion and subsequent redistribution of

saltmarsh sediment within the monitoring area. Their hypothesis was supported by a

subsequent reduction in levels which paralleled the abatement of saltmarsh erosion by

the mid-1990s. The concentrations of heavy-metals found in saltmarsh sediments

depends on a number of factors and shows the wide range found worldwide (Table 12).

Table 12Average Cu, Zn and Pb concentrations (g g-1) in bulk sediments of saltmarshes around the world

Marsh Site (Location) Cu Zn Pb Reference

(New York)12-600 25-500 25-700

Cochran, et al.(1979, cited in (Weis,Callaway & Gersberg 2001))

Rhode Island 6-150 19-225 12-200 Bricker et al.(1993

Oneonta Slough (Tijuana Estuary,USA) 26.3 107.1 36.1 Weis, et al. (2001)

(Medway Estuary Kent, UK) 23-52 61-202 20-126 (Spencer & MacLeod 2002)

Hortas (Tagus Estuary, Portugal) 27.6 167.6 65.2 Frana, et al.(2005)

S. Joo da Talha (Tagus Estuary,Portugal)

89.1 427.4 126.9Frana, et al.(2005)


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Little Oakley 20 108 55 (O'Reilly Wiese, Bubb & Lester 1995)

Dengie 20 77 36 (O'Reilly Wiese, Bubb & Lester 1995)

Although heavy-metals can be fixed in saltmarsh sediments for extended time periods, a

change in conditions could cause established saltmarshes to erode and remobilise

sediments-bound metals back into the environment (EA 2007).

1.3.8 Saltmarsh extent and locations in the UK

Saltmarsh in the UK is widely distributed (EA, 2007). Of the 34,000 hectares in England

(Phelan, Shaw & Baylis 2011) the vast majority are found within five predominantly

estuarine areas (Figure 1.3).


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1.4 Aims and objectives

The aims of this study were to:

ascertain the magnitude and horizontal spatial distribution of copper, zinc and lead

in the sediment of two estuarine saltmarshes within the Morecambe Bay European

Marine Site;

compare the concentrations of copper, zinc and lead and physicochemical

conditions between a grazed and ungrazed site;

investigate whether they act as a sink for heavy-metals deriving from contemporary

and historic pollution sources in the area.

Although extensive literature relating to heavy-metals in saltmarshes exists, no papers

could be found pertaining to the differences in their loadings between grazed and


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H1 The average concentrations of all heavy-metals at Plumpton Hall will be significantly higher than at

Plumpton.

Hypothesis #2

H0 Organic matter levels at Plumpton Hall will not be significantly higher than at Plumpton.

H1 Organic matter levels at Plumpton Hall will be significantly higher than at Plumpton.

Hypothesis #3

H0 There will not be a significant positive relationship between organic matter and all heavy-metals.

H1 There will be a significant positive relationship between organic matter and all heavy-metals.

Hypothesis #4

H0 There will not be a significant negative relationship between pH and all heavy-metals.

H1 There will be a significant negative correlation between pH and all heavy-metals.

1.4.2 Metal profiles

Three heavy-metals were the focus of this study: copper, zinc and lead. All have known

potential for harmful effects on organisms in elevated concentrations (Hogan 2011;


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Figure 1.4 The location of Morecambe Bay on the north-western coastline of England. Note: thelandmasses of Eire and Northern Ireland have been omitted. Created using ESRI ArcMap10.0.

The confluence of five rivers draining into the bay coupled with a macrotidal regime

creates the largest continuous area of sandflats and mudflats in the UK, representing

approximately 12% of the UKsintertidal area (Annan 2001; Oceana 2012). These


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releases aqueous copper which can precipitate into secondary minerals or be

transported downstream (Kimball et al. 2009). The general reaction is

Sediment cores of Coniston Water taken by Davison et al. (1985) show a clear record of

mining activity, with raised levels of copper and iron found. Tipping et al.(1997) also

found highly-enriched levels of copper and zinc in the sediment of Coniston Water

compared to Blelham Tarn, which drained areas unaffected by mining activities.

Maberly et al. (2011) conducted the first systematic survey of heavy-metals in the water

bodies of Cumbria. Elevated copper concentrations were found in Coniston Water

suggesting that tailings from Coniston Copper Mine are still discharging metals into the

local hydrological cycle.


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Figure 1.11Pb concentrations (g g-1) at different locations with the catchment areas draining into the


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reduced values compared to most sites within the dataset. Similarly site 4718 down the

estuary from Plumpton Hall generally showed a lower concentration of each metal than

others in the dataset. These particular sites may provide the closest comparable site to

the study area and to Plumpton particularly due to its sheltered location.

1.5.4 Pollution in Morecambe Bay

Despite a long history of human habitation around Morecambe Bay it is not highly

urbanised at the coastline with fragmented human development centred on Morecambe,

Grange-over-Sands, Heysham and Barrow-in-Furness (Centrica, 2012). Active ports

exist at the former two locations and a defunct one at previously landlocked Ulverston,

which was connected to the sea by the Ulverston Canal in the late 18thcentury

(Priestley, 1831). It thrived until the advent of the railway age when demand for its use

waned drastically and it eventually fell in to disrepair. It was recently acquired by


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1.5.6 Saltmarsh in Morecambe Bay

Morecambe Bay EMS has over 5% of the UKs total saltmarsh(Gray & Scott 1987)

(Tuley, Cranbrook & Yates 1996). Forming a discontinuous fringe around the bay,

saltmarshes are particularly well established within the estuaries of the Rivers Wyre,

Lune, Kent and Leven (Pringle 1995). The mean spring tidal range of 10.5m and mean

neap tidal range of 3.4m influences the distribution of saltmarshes which are generally

only found within the upper 2.5m of the intertidal range (Gray & Scott 1987)(French &

Livesy 2000). The majority have sandy substrates and are grazed by livestock, giving

them a unique character (Gray & Scott 1987). They are classified phytogeographically as

typical west-coast (Type B) marshes by Adam (1978), who also highlighted the

difficulty of separating the effects of livestock grazing and substrate type in governing

the phytosociological relationships in many British saltmarshes. Less than 1% of


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2.1 Description of the Study Area

Plumpton (SD324801) and Plumpton Hall (SD314786) saltmarshes are located in the

Ulverston Channel draining into the north of Morecambe Bay (Figure 2.1).


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Figure 2.3Map showing the 1000 randomly generated sampling points for Plumpton Marsh

Coordinates were input into ESRI ArcMap 10.0and clipped to a polygon shapefile

relating to the surface area of each saltmarsh. This restricted the potential sampling

sites to those found on the saltmarsh surface. Sampling proceeded at the first 30

accessible points, located by inputting coordinates into a Garmin GPSmap 62.

2.2.2 Sampling procedure at each sampling point


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At each point a composite sample consisting of five increments was taken (Figure 2.5).

Figure 2.5Photograph showing the pattern of increments that were takenin a 10cm by 10cm plot ateach sampling point.

An increment consisted of one load from a 22.86cm (=1.748cm) JMC wetsampling

tube attached to a JMC Handle (Appendix 2). Increments were immediately deposited in

pre-labelled polythene bags, sealed and stored in a cool bag < 4C for transport to the

laboratory.

2.3 Laboratory procedure


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15 sampling points per marsh from the second sub-sample was prepared for acid

digestion by air-drying for seven days followed by 24h oven-drying at 105C. The

dessicated sample was then ground using a pestle and mortar, passed through a 63m

sieve and stored in fresh, pre-labelled polythene bags ready for transport to Clifton

campus.

Clifton Campus laboratory (Rosalind Franklin Building)Duplicates of homogenized sub-sample of the


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Table 16Statistics and results for each element analysed using ICP-OES

ElementWavelength

(nm)

Standards

(ppm)R2 RSD%

Detection Limit

(g ml-1)

Cu 327.393 0.2; 0.5; 1; 5; 10; 20 0.99971 0.8589428 0.001

Zn 206.2 0.2; 0.5; 1; 5; 10; 20 0.99995 1.890046977 0.002

Pb 220.353 0.2; 0.5; 1; 5; 10; 20 0.99990 1.188729783 0.003

RSD% was < 2 for all calibrations. Sample analysis precision was much more varied

with RSD% values of 2.48(Cu), 0.90(Zn) and 114.32(Pb). Duplicate analysis provided

measurements in mg l-1which were averaged and converted to mg kg-1using the

following formula.

[ ][ ]

[ ] []

2.5 Statistical techniquesStatistical analysis was conducted using Microsoft Excel and Minitab 16.2.2


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denoted by a ^ next to the variable symbol (e.g. Pb^). Regression analysis was not

possible with Cu as a variable as the dataset could not be converted to a Gaussian

distribution by either or log10 transformations and was therefore unsuitable for

parametric tests.

2.6 Geographical Information Systems (GIS)Geographical Information Systems (GIS) are increasingly used in a variety of disciplines.

GIS can visualize and represent data in different forms and the ability to input,

manipulate and spatially analyse primary data is valuable in environmental science,

particularly with respect to research into the spatial distribution of pollutants. GIS thus

provide a useful tool to assist management and remediation plans by providing

information on sources, depositional trends and mobilisation of pollutants.

Interpolation techniques and maps were used to predict and visualise the distribution

of different variables at each site.


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3 RESULTSMean values of soil parameters and heavy-metal concentrations in both marshes are

summarised in Table 17.

Table 17Results for each site. Mean standard deviation.

Variable (units) Plumpton Marsh (P) Plumpton Hall Marsh (S)

n Mean Std Dev Min Max Mean Std Dev Min Max

pH(water) 30 8.60 0.41 7.46 9.28 8.42 0.38 7.77 9.07

EC (S cm-1) 30 613 204 285 919 958 327 127 1367

Moisture Content (%) 15 27.56 3.90 22.43 35.05 35.20 9.58 21.73 59.80

LOI (%) 15 4.90 1.22 2.74 6.93 6.50+ 2.41 3.99 12.74

Cu (mg kg-1) 15 17.47 3.06 14.33 25.90 17.55 2.34 14.43 23.08

Zn (mg kg-1) 15 38.39 19.76 12.06 82.87 37.69 11.36 17.50 58.30

Pb (mg kg-1) 15 5.64 1.63 4.24 10.44 6.70 2.22 3.75 10.52

3.1 Heavy-metalsMagnitudes of heavy-metals in both marshes followed the order Zn>Cu>Pb with mean


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3.1.2 Plumpton Hall saltmarsh (SD314786)

9

7

6

5

4

3

2

1

30

29

28

27

26

25

24

23

22

21

20

19

18 1716

1514

13

12

11

10


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Electrical Conductivity

Figure 3.9Column chart with standard error bars showing the mean EC for each sampling point at Plumpton Hallsaltmarsh.

1456

975

490

1184

922

625

1120 1060 8641000

786

1306

943

1141

451

0

200

400

600

800

1000

1200

1400

1600

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15

EC(Siemenscm-1)

Sampling Point

38.96

26.57

59.80

34.46

29.59

36.3233.15

28.16 21.7333.78 31.77

40.4542.90

45.77

40

50

60

ontent(%)


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3.3 Differences3.3.1 Heavy-metals

There was no significant difference between copper concentrations at each marsh

(Mann-Whitney test, W=218.0, n=15, p=0.5614)(Figure 3.12).

Figure 3.12Bar chart with standard error bars showing the mean concentration of Cu at each sampling site (n=15).

No significant difference in zinc concentrations was found between sites (two-sample

t(22)=0.12, n=15, p=0.908)(Figure 3.13).

17.47 17.55

16.0

16.5

17.0

17.5

18.0

18.5

Cuconc.(mgkg-1)

Plumpton Plumpton Hall


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Figure 3.14Bar chart with standard error bars showing the mean concentration of Pb at each sampling site (n=15).

3.3.2 Soil parameters

No significant difference in pH was found between sites (two-sample t(57)=1.75,

p=0.086, n=30 (Figure 3.15).

5.64

6.70

4.0

4.5

5.0

5.56.0

6.5

7.0

7.5

Pbconc.(m

gkg-1)

Plumpton Plumpton Hall

8.60

8.42

8.3

8.4

8.5

8.6

8.7

8.8

pH


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Table 18 Correlations between all measured variables (pooled data).

pH EC MC LOI% Cu Zn Pb

pH 1 -0.096 -0.650*** -0.468** -0.403* -0.551** -0.364*EC 1 0.102 0.250 0.128 0.037 0.116MC% 1 0.894** 0.657** 0.496** 0.554**

LOI% 1 0.660** 0.710** 0.558**Cu 1 0.785** 0.797**Zn 1 0.776**Pb 1* Indicates significant correlation at the 0.05 level (2-tailed).** Indicates significant correlation at the 0.01 level (2-tailed).*** Indicates significant correlation at the 0.001 level (2-tailed).

Soil parameters

All heavy-metals had significant or very significant negative correlations with pH

(Figure 3.19).

y = -29.513x + 290.69

R = 0.304

50

60

70

80

90

on(mgkg-1)


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Figure 3.25Scatterplot with regression trendlines showing the significant negative relationship between pH and Zn.

A very significant positive relationship was found between pH and organic matter^ (pH

2

y = -29.513x + 290.69

R = 0.304

0

10

20

30

40

50

60

70

80

90

7.6 7.8 8 8.2 8.4 8.6 8.8 9 9.2 9.4

Zn(mgkg-1)

pH


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Figure 3.26Scatterplot with regression trendlines showing the significant positive relationship between MoistureContent (%) and Zn.

y = 0.9613x + 7.869

R = 0.246

0

10

20

30

40

50

60

70

80

90

100

0 10 20 30 40 50 60 70

Zn

(mgkg-1)

Moisture Content (%)


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Inverse Distance Weighting


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Global Polynomial Interpolation


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Kriging/CoKriging


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4 DISCUSSIONThe results suggest that concentrations of copper, zinc and lead in the sediment of

Plumpton and Plumpton Hall saltmarshes is minimal. All mean heavy-metal

concentrations were below various SGQs (Tables 7 & 8) and low when compared to

studies of other anthropogenically impacted estuaries (Tables 12 & 13). The

concentrations found for Zn and Pb were much lower than levels predicted utilising

stream sediment data in the local area (Johnson et al.2005)(Figures 1.10 1.11) and

comfortably below the bottom end of numerous sediment quality guidelines (Tables 7 &

8). No sampling points on either site had Zn or Pb concentration above their respective

SQUIRT

TEL (Figures 4.1 & 4.2).

TEL 124

60

80

100

120

on(mgkg-1)

CuZnPb


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In contrast, four sampling points at Plumpton and five at Plumpton Hall had copper

concentrations above the SQuiRTTEL of 18.7 mg kg-1(Buchman 2008) but the figure rises

to nine sampling points for Plumpton and 12 for Plumpton Hall when using the ONTARIO

LEL of 16 mg kg-1(Figure 4.3 & 4.4).

Figure 4.3 Column chart with standard error bars showing the mean concentrations of Cu at Plumptonsampling points and corresponding SQUIRT TEL concentrations.

TEL 18.7

ERL 34.0

LEL 16

0

5

10

15

20

25

30

35

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15

Concentration(mgkg-1)

Sampling Point

ERL 34.035


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points were below the 10thpercentile (20 mg kg-1). The highest zinc concentration,

82.87 mg kg-1at Plumpton Marsh (sampling point #3), was comfortably below the SQuiRT

TEL of 124 mg kg-1. Similarly for lead, the highest concentration, 10.52 mg kg-1at

Plumpton Hall Marsh (sampling point #15), was well below the SQuiRTTEL of 30.2 mg kg-

1. Copper concentrations in both marshes were low and ranged between just under the

median (18 mg kg-1) and just above the arithmetic mean (23 mg kg-1) values of typical

concentrations found in the soils of England and Wales (Table 6) (Buchman, 2008).

However, despite a relatively low mean copper concentration,

The results bear similarities with the low concentrations of heavy-metals in lower-

estuarine marshes of the Blackwater estuary, UK reported by Emmerson et al. (1997).

The marshes do not appear to be susceptible to high loads of Cu from abandoned mines

in the catchment areas draining into the Ulverston Channel. Despite an increased input


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Investigations into sediment provenance using fingerprinting techniques could

elucidate this theory (Rotman et al. 2008).

4.1.1 Organic matter

In both saltmarshes organic matter was relatively low with mean values of 4.9% and

6.5% for Plumpton and Plumpton Hall respectively. This is higher than the mean value

of 3.2% for saltmarsh sediments of the Karnafully River coast, India (Siddique & Aktar,

2012) but lower than values reported by other studies. Organic matter in sediments of

the Tijuana Estuary, California ranged between 8.7% and 13.8% (Weis, Callaway &

Gersberg 2001) and (Leendertse, Scholten & van der Wal 1996) found levels of 9.6-

14.8% in Delfzijl and 14.3-16.2% in Marsdiep saltmarsh sediments. The organic matter

levels may contribute to the higher EC at Plumpton Hall due to the high CEC of organic

matter (Fest et al.1994). The significant positive relationships between all heavy-

metals and moisture content could relate to dissolved organic matter within the water


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Hypothesis #2

H0 Organic matter levels at Plumpton Hall will not be significantly higher than at Plumpton.

Statistical analysis provided evidence to reject the null hypothesis. As expected, organic

matter at Plumpton Hall was significantly higher than at Plumpton. It is likely that sheep

grazing over many years at Plumpton has affected species composition and resulted in

an abundance of low-lying swards of grasses with corresponding reduction in NPP

detritus production (Jensen et al., 1985) (Robinson 1987)(Bos et al., 2005). This leads to

a reduced incorporation of decaying biomass into the saltmarsh sediment (Silliman,

Grosholz & Bertness (eds.) 2009). The higher levels of organic matter did not

correspond to an increased loading of any heavy-metal at Plumpton Hall marsh despite

the apparently favourable conditions for their retention.

Hypothesis #3

H0 There will not be a significant positive relationship between organic matter and all heavy-metals.


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Hypothesis #4

H0 There will not be a significant negative correlation between pH and all heavy-metals.

Statistical analysis showed pH to have a significant relationship with all heavy-metal

concentrations and there is therefore sufficient evidence to reject the null hypothesis.

pH is the factor that mostly strongly influences the adsorption, retention and mobility of

heavy-metals in various compartments (Calmano, Hong & Frstner 1993; Pierzynski,Sims & Vance 2000; de Matos et al.2001; Bhargava et al. 2012). The mobility of copper ,

zinc and lead all increase with decreasing pH (Kumpiene, Lagerkvist & Maurice 2008)

The alkalinity of both marshes is likely to restrict the mobility of heavy-metals within

the saltmarsh sediment and soil.

4.2 AssumptionsThe theoretical foundation dictated that elevated levels of heavy-metals can be found in


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4.3 LimitationsDespite the measures taken to homogenise each sample the imperfections in each

technique and the inherent heterogeneity of the sediment leads to fundamental error

(FE) which cannot be controlled. Assumptions are made that digestion of each sample is

complete and comparable. Samples were not collected or digested in an oxygen-free

environment and metal sulphides may have been oxidised during storage.

The unique conditions of the study area mean that the generalisability of the study is

low. The results would be difficult to extrapolate in situations anywhere outside or even

within Morecambe Bay.

4.4 Improvements to the studyIncreasing the sample size to minimum of 30 for each site would increase the accuracy


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1.1 Recommendations for further research

There are numerous options for future research. This study looked at homogenized

surface samples down to 22.86 cm. Depending on the accretion rate at each site this can

represent anything in the order of tens to hundreds of years of particulate deposition.

Looking at changes in concentrations with incremental depth would enable

chronological depositional trends to be investigated and may reveal horizons related to

periods when deposition was elevated. Including marshes higher up the estuary would

provide further data to help explain the low concentrations of all metals found at both

sites.

The pseudototal provided by aqua regia digestion is less useful in assessing risk to biota

(Spencer & MacLeod 2002). Undertaking a sequential extraction to analyse the labile

fraction can aid research into the uptake of heavy-metals by plants and potential


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