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Last Updated September 15, 2015

Northern Contaminants Program

Canadian Arctic Contaminants Assessment Report II (2003)

Volume 5: Sources, Occurrences, Trends and Pathways in the Physical Environment

Full Document

 

Executive Summary     i

Résumé     iii

 

PART I     1

 

1 Introduction     3

1.1 Findings of the abiotic studies during NCP-Phase I (1991–1996) 5

1.2 Abiotic studies during NCP-Phase II (1997–2002) 8

1.2.1 Organization of the abiotic assessment 9

1.2.1.1 Section A: Properties and sources 9

1.2.1.2 Section B: Occurrence and trends 9

1.2.1.3 Section C: Process studies and modelling 9

1.2.1.4 Section D: The interaction of climate change and contaminants 9

 

2 Summary     11

2.1 Properties and sources 11

2.1.1 Physicochemical properties of contaminants (Harner et al., Section A.1) 11

2.1.2 Usage and emissions of organochlorine pesticides (Li et al., Section A.2) 12

2.1.3 Organochlorines in Russian rivers and loadings to the Russian northern seas (Strachan et al., Section A.3) 12

2.1.4 Local sources of contaminants in the Canadian Arctic (Gregor et al., Section B.9) 13

2.2 Occurrence and trends 14

2.2.1 Polychlorinated biphenyls (PCBs) 15

2.2.1.1 Polychlorinated biphenyls in air (Blanchard et al., Section B.1) 15

2.2.1.2 Polychlorinated biphenyls in seawater (Muir et al., Section B.2) 15

2.2.2 Organochlorine pesticides 16

2.2.2.1 Organochlorine pesticides in air (Blanchard et al., Section B.1) 16

2.2.2.2 Organochlorine pesticides in seawater (Muir et al., Section B.2) 16

2.2.2.3 Hexachlorocyclohexanes in seawater (Li et al., Section C.3) 17

2.2.2.4 Summary — Organochlorine pesticides in air and seawater 18

2.2.3 Polycyclic aromatic hydrocarbons (PAHs) 18

2.2.3.1 Polycyclic aromatic hydrocarbons in air (Blanchard et al., Section B.1) 18

2.2.4 Polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs) 18

2.2.4.1 Polychlorinated dibenzo-p-dioxins/furans in air (Blanchard et al., Section B.1) 18

2.2.5 Persistent organic pollutants in marine sediments (Stern et al., Section B.3) 18

2.2.6 Persistent organic pollutants in freshwater sediments (Stern et al., Section B.3) 19

2.2.7 New persistent chemicals in the Arctic (Alaee et al., Section B.4) 20

2.2.7.1 Brominated fire retardants 21

2.2.7.2 Short-chain chlorinated paraffins (SCCPs) 21

2.2.7.3 Modern agrochemicals 21

2.2.7.4 Polychlorinated naphthalenes (PCNs) 22

2.2.7.5 Coplanar PCBs (CoPCBs) 22

2.2.7.6 Octachlorostyrene (OCS) 22

2.2.8 Mercury 22

2.2.8.1 Mercury in air (Steffen et al., Section B.5) 22

2.2.8.2 Mercury in sediments (Lockhart et al., Section B.6) 23

2.2.9 Other metals in air (Gong et al., Section B.7) 23

2.2.10 Radionuclides in the Arctic Ocean (Smith, Section B.8) 24

2.3 Process studies and modelling 25

2.3.1 Air-snow exchange of POPs (Wania and Halsall, Section C.1) 25

2.3.2 Modelling mercury in freshwater lakes (Diamond et al., Section C.2) 26

2.3.3 Modelling persistent organic pollutants in freshwater lakes (Diamond et al., Section C.2) 26

2.3.4 Modelling and mass balance of HCHs in the Arctic Ocean (Li et al., C.3) 27

2.3.5 Modelling in support of international negotiations (Wania, Section C.4) 27

2.4 The interaction of climate change and contaminants (Macdonald et al., Section D.1) 28

 

3 Conclusions and Recommendations     31

3.1 Properties and sources 31

3.1.1 Physicochemical properties of persistent organic pollutants 31

3.1.2 Usage and emissions of organochlorine pesticides 31

3.1.3 Organochlorines in Russian rivers and loadings to Russian northern seas 32

3.2 Occurrence and trends 32

3.2.1 Persistent organic pollutants in the Arctic atmosphere 32

3.2.2 Persistent organic pollutants in seawater 33

3.2.3 Persistent organic pollutants in marine and lake sediments 34

3.2.4 New persistent chemicals in the Arctic environment 35

3.2.5 Mercury in the Arctic atmosphere 35

3.2.6 Mercury in abiotic samples 36

3.2.7 Other heavy metals in Arctic air 36

3.2.8 Radionuclides — Local and long-range sources 37

3.2.9 Local sources of contamination in the Canadian Arctic 37

3.3 Process studies and modelling 38

3.3.1 Air/snow exchange of persistent organic pollutants 38

3.3.2 Mass balance and modelling of contaminants in lakes 38

3.3.3 Transport and fate of hexachlorocyclohexanes in the North American Arctic Ocean 39

3.3.4 Modelling in support of international negotiations 39

3.4 Special topic 40

3.4.1 The interaction of climate change on contaminant pathways to and within the Canadian Arctic 40

 

PART II     43

 

A Properties and Sources     45

A.1 Physicochemical properties of persistent organic pollutants 45

A.1.1 Introduction 45

A.1.2 Incentives to measure physicochemical properties 47

A.1.3 New physicochemical property data 47

A.1.4 Advances in describing chemical partitioning 47

A.1.4.1 Octanol-air partition coefficient 47

A.1.4.2 Partitioning to aerosols 47

A.1.4.3 Partitioning to soil 47

A.1.4.4 Air-water exchange 48

A.1.4.5 Partitioning to snow and ice 48

A.1.5 Reaction rates 48

A.2 Usage and emissions of organochlorine pesticides 49

A.2.1 Introduction 49

A.2.2 Hexachlorocyclohexane (HCH) 50

A.2.2.1 Global technical HCH usage 50

A.2.2.2 Technical HCH usage in China 50

A.2.2.3 Global lindane usage 52

A.2.2.4 Lindane usage in Europe 52

A.2.2.5 Lindane usage in China 52

A.2.2.6 Lindane usage in Canada 53

A.2.2.7 Lindane usage in the USA 55

A.2.2.8 Alpha-HCH emissions and their impact on the Arctic atmosphere 56

A.2.2.9 Beta-HCH emissions and their impact on the Arctic atmosphere 58

A.2.2.10 Gamma-HCH emissions and their impact on the Arctic atmosphere 59

A.2.3 Toxaphene 61

A.2.3.1 Global toxaphene usage 61

A.2.3.2 Toxaphene usage in Asian countries — The former Soviet Union and China 62

A.2.3.3 Toxaphene usage in Mexico, Central America, and Colombia 62

A.2.3.4 Toxaphene usage in Canada 62

A.2.3.5 Toxaphene production and usage in the United States 63

A.2.3.6 Toxaphene emissions and residues in the United States 64

A.2.3.7 Toxaphene in Arctic air 64

A.2.3.8 Sources of toxaphene to the Arctic 65

A.2.4 Dichlorodiphenyltrichloroethane (DDT) 65

A.2.4.1 Global DDT use 65

A.2.4.2 DDT use in China, India, and Japan 65

A.2.5 Summarized usage and emission estimates 70

A.3 Organochlorines in Russian rivers and loadings to Russian northern seas 70

A.3.1 Introduction 70

A.3.2 Verification of older Russian river water data 71

A.3.2.1 Sampling program 71

A.3.2.2 DDT, -HCH, and -HCH levels and spatial/temporal trends 72

A.3.2.3 Other chlorinated pesticides in northern Russian rivers 74

A.3.2.4 Loadings of OC pesticides into the Russian northern seas 74

A.3.3 Recent studies of organochlorines in Russian freshwater 75

 

B Occurrence and Trends     77

B.1 POPs in the atmosphere 77

B.1.1 Introduction 77

B.1.2 Data and time series analysis 77

B.1.2.1 Polychlorinated biphenyls (PCBs) 78

B.1.2.2 Organochlorine pesticides 80

B.1.2.3 Polycyclic aromatic hydrocarbons (PAHs) 87

B.1.2.4 Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) 88

B.1.2.5 Evidence of trans-Pacific transport 89

B.2 Persistent organic pollutants in seawater 92

B.2.1 Introduction 92

B.2.2 Hexachlorocyclohexanes (HCHs) 93

B.2.3 Polychlorinated biphenyls (PCBs) 95

B.2.4 Toxaphene 97

B.2.5 Other “legacy” organochlorine pesticides 98

B.2.6 Chlorinated benzenes 99

B.3 Persistent organic pollutants in marine and lake sediments 100

B.3.1 Introduction 100

B.3.2 Marine sediments 100

B.3.3 Lake sediments 104

B.3.3.1 Yukon 104

B.3.3.2 Nunavut 111

B.3.3.3 Northwest Territories (Great Slave Lake) 113

B.4 New persistent chemicals in Arctic air and water 116

B.4.1 Introduction 116

B.4.2 Polychlorinated naphthalenes and coplanar PCBs 116

B.4.2.1 Usage and sources 116

B.4.2.2 Physicochemical and toxicological properties 116

B.4.2.3 Occurrence in the environment 117

B.4.2.4 PCNs and coplanar PCBs in Arctic air 117

B.4.3 Polybrominated diphenyl ethers (PBDEs) and other brominated flame retardants 118

B.4.3.1 Usage and sources 118

B.4.3.2 Physicochemical and toxicological properties 119

B.4.3.3 Occurrence in the environment 119

B.4.3.4 Polybrominated diphenyl ethers in Arctic air 119

B.4.3.5 Other brominated flame retardants (BFRs) in Arctic air 122

B.4.4 Short-chain chlorinated paraffins (SCCPs) 122

B.4.5 Modern pesticides, other biocides, and by-products 122

B.4.5.1 Occurrence in Arctic air 122

B.4.5.2 Occurrence in Arctic water 123

B.5 Mercury in the Arctic atmosphere 124

B.5.1 Introduction. 124

B.5.2 NCP-Phase I and II programs 125

B.5.3 Continuous gaseous mercury concentration measurements 126

B.5.4 Discovery of mercury depletion events (MDEs) in the Arctic 129

B.5.4.1 Gaseous elemental mercury and ozone during mercury

depletion events 129

B.5.4.2 Particulate-phase mercury during mercury depletion events 130

B.5.4.3 Conversion of mercury during mercury depletion events 130

B.5.4.4 The effect of mercury depletion events on mercury in snow 131

B.5.4.5 The chemistry of mercury depletion events —

halogens and mercury 133

B.5.4.6 The role of the ocean in mercury depletion event chemistry 135

B.5.4.7 Profiles and fluxes of mercury in air near the snow surface

during mercury depletion events 136

B.5.4.8 Reactive gaseous mercury during mercury depletion events 139

B.5.5 The cycle of atmospheric mercury in the Arctic 141

B.5.6 Summary 142

B.6 Mercury in sediments 143

B.6.1 Introduction 143

B.6.2 Geographic distribution of mercury in sediments from northern Canada 143

B.6.3 Changes in inputs of mercury over time 144

B.6.4 Natural and anthropogenic sources 147

B.7 Other heavy metals in the Arctic atmosphere 148

B.7.1 Introduction 148

B.7.2 Experimental methods 148

B.7.3 Seasonal variations 149

B.7.4 Long-term trends 150

B.7.5 Principal component analysis 151

B.8 Radionuclides: local and long-range sources 153

B.8.1 Introduction 153

B.8.2 Long-range transport 153

B.8.3 Local sources 156

B.9 Local sources of contaminants in the Canadian Arctic 158

B.9.1 Introduction 158

B.9.1.1 Local sources of contaminants in CACAR-I 158

B.9.1.2 Local source of contaminants in CACAR-II 159

B.9.2 Contaminated sites overview 159

B.9.3 Resolution Island, Nunavut 163

B.9.3.1 History and introduction 163

B.9.3.2 Site investigations 164

B.9.3.3 Site remediation 164

B.9.4 Saglek, Newfoundland and Labrador 164

B.9.4.1 History and introduction 164

B.9.4.2 Site investigations 165

B.9.4.3 Site remediation 169

B.9.5 Giant Gold Mine, Northwest Territories 169

B.9.5.1 Introduction 169

B.9.5.2 Environmental assessment of arsenic contamination

in the Yellowknife area 170

B.9.5.3 Subsurface stored arsenic trioxide 173

B.9.6 Port Radium Mine, Northwest Territories 174

B.9.6.1 Radioactivity sources in the Arctic 174

B.9.6.2 History of the site 174

B.9.6.3 Site assessment 175

B.9.6.4 Risk assessment 177

B.9.7 Carcross railway tie treatment plant, Yukon Territory 179

B.9.7.1 Background 179

B.9.7.2 Contaminants of concern 180

B.9.7.3 Investigation of off-site contamination 181

B.9.8 Summary 183

 

C Process Studies and Modelling     185

C.1 Air/Snow exchange of persistent organic pollutants 185

C.1.1 Introduction 185

C.1.2 Field measurements of contaminants in snow and ice 185

C.1.3 Mechanistic understanding of snow-related processes of organic contaminants 186

C.1.4 Snow scavenging of persistent organic pollutants 188

C.1.5 Fate of persistent organic pollutants in snowpack 189

C.2 Mass balance and modelling of contaminants in lakes 191

C.2.1 Introduction 191

C.2.2 Amituk Lake 191

C.2.2.1 Mercury budget for Amituk Lake 192

C.2.2.2 Persistent organic pollutants in Amituk Lake 195

C.2.2.3 Organochlorine degradation and relative age 199

C.3 Transport and fate of hexachlorocyclohexanes in the North American Arctic Ocean 202

C.3.1 Introduction 202

C.3.2 Usage and emissions of hexachlorocyclohexanes 203

C.3.3 Physical and chemical properties of the hexachlorocyclohexane isomers 203

C.3.4 Current understanding of -HCH transport to the Arctic 204

C.3.5 The enigma of -HCH 207

C.3.6 Comparative loadings of hexachlorocyclohexane isomers to the North American Arctic Ocean 209

C.3.7 Hexachlorocyclohexane removal processes in the Arctic Ocean 212

C.3.8 Conclusions 213

C.4 Modelling in support of international negotiations 213

C.4.1 Introduction 213

C.4.2 Model simulations of the global transport and fate of persistent organic pollutants 213

C.4.2.1 Simulation of the global fate of -HCH 215

C.4.2.2 Simulation of the global fate of PCBs 217

C.4.2.3 Identification of the potential for accumulation in the Arctic 219

C.4.2.4 Spatially highly resolved models of global fate and transport 220

C.4.3 Models in support of defining the persistent organic pollutants attributes of persistence and long-range transport potential 220

C.4.3.1 Models to estimate persistence 221

C.4.3.2 Models to estimate potential for long-range transport 221

C.4.3.3 Approaches to reduce input data requirements for the model based evaluation 223

C.4.3.4 Other aspects of long-range transport potential and persistence assessment 223

 

D Special Topic     225

D.1 The interaction of climate change with contaminant pathways to and within

the Canadian Arctic 225

D.1.1 Introduction 225

D.1.1.1 Contaminant transport in a changing world 226

D.1.1.2 Objectives of this chapter 228

D.1.1.3 Organization of this chapter 228

D.1.2 Long-term change in the Arctic 228

D.1.2.1 The distant past 228

D.1.2.2 The present and future 229

D.1.3 Recent change in the Arctic and the Arctic oscillation 231

D.1.3.1 The Arctic oscillation 231

D.1.3.2 Winds 235

D.1.3.3 Surface air temperature 236

D.1.3.4 Precipitation and runoff 236

D.1.3.5 The ocean 239

D.1.3.6 Adjacent polar seas and regions 248

D.1.3.7 Lake and river ice 249

D.1.3.8 Permafrost 250

D.1.3.9 Glacial ice 250

D.1.4 Biological responses to climate change 251

D.1.4.1 Terrestrial systems 251

D.1.4.2 Aquatic systems 252

D.1.5 The effects of climate change on human activities 256

D.1.6 The effects of climate change on contaminant pathways 256

D.1.6.1 Heavy metals 257

D.1.6.2 Radionuclides 264

D.1.6.3 Organochlorines 265

D.1.6.4 Hydrocarbons 275

D.1.7 Time series 277

D.1.7.1 Sediment-core records and surface sediments 278

D.1.7.2 Atmospheric time series 279

D.1.7.3 Biological tissue time series 279

 

E References      281