DOCSLIB.ORG

Fly-Ash Particles in Lake Sediments

Total Page：16

File Type：pdf, Size：1020Kb

Download full-text PDF Read full-text
Fly-Ash Particles in Lake Sediments FLY-ASH PARTICLES IN LAKE SEDIMENTS: EXTRACTION, CHARACTERISATION & DISTRIBUTION. Thesis submitted for the degree of Doctor of Philosophy in the University of London by Neil Leslie Rose University College London May 1991 1 ProQuest Number: 10609404 All rights reserved INFORMATION TO ALL USERS The quality of this reproduction is dependent upon the quality of the copy submitted. In the unlikely event that the author did not send a com plete manuscript and there are missing pages, these will be noted. Also, if material had to be removed, a note will indicate the deletion. uest ProQuest 10609404 Published by ProQuest LLC(2017). Copyright of the Dissertation is held by the Author. All rights reserved. This work is protected against unauthorized copying under Title 17, United States C ode Microform Edition © ProQuest LLC. ProQuest LLC. 789 East Eisenhower Parkway P.O. Box 1346 Ann Arbor, Ml 48106- 1346 ABSTRACT Fly-ash particles produced from the high temperature combustion of fossil-fuels are found in high concentrations in the lake sediments of regions of high acid deposition. The sediment record of these particles showing the onset of industrialisation correlates well with the record of acidification as indicated by diatom analysis. There are two types of fly-ash particle; spheroidal carbonaceous particles produced from the incomplete combustion of the fossil-fuel and inorganic ash spheres formed by the fusing of mineral inclusions present within the fuel. Procedures were developed to extract both types of particle from lake sediments. These involved selective chemical attack to remove unwanted sediment fractions thus enabling quick and accurate particle enumeration. A reference data-set of carbonaceous particle surface chemistries was produced using EDS measurements and a fuel-type characterisation developed using multivariate statistics. This characterisation allocated over 97% of the particles to the correct fuel-type. These methods were then applied to a series of sediment cores to study temporal changes in particle deposition and spatial trends over Scotland. The concentrations of both particle types in sediment cores correlate well to fossil- fuel combustion histories, and the characterisation of the carbonaceous particles from a 210Pb-dated core from a north London lake showed good agreement with the change in coal and oil use through time in the area. Spatial trends were studied using surface sediments from 94 lakes in Scotland and the north of England. These showed higher concentrations near industrial areas and generally good agreement with sulphur deposition data. Characterisation revealed two areas where above average concentrations of oil particles occurred, indicating source areas outside the country to the east and the south-west There is potential to extend this characterisation to other fossil-fuel types such as peat, lignite and brown coal and to apply the techniques to a range of environmental questions in Britain, Europe and on a global scale. 2 ACKNOWLEDGEMENTS. Many people have aided and abetted this project and I would especially like to thank all the members of the Palaeoecology Research Unit for their friendship and buying me drinks when necessary. In particular I would like to thank my supervisor Rick Battarbee for his encouragement and guidance throughout. I am also grateful to the following people: Don Monteith, Simon Patrick, Julie Simpson, Helen Bennion, Tim Allott, Viv Jones and Roger Flower for their help with the fieldwork; Steve Juggins for all his help and advice with the computing and statistics and for reading various versions of Chapter 3 and to Martin Munro and Tony Stevenson for their comments on computing matters; Peter Street (formerly of CERL at Leatherhead) for his useful advice in the very early stages; John Watt of Imperial College, London for all his time with the EDS analyses and for reading a few sections of this work; Annette Kreiser, Nigel Cameron, Paul Schooling and Bill Campbell for ’top tips’ in the use of MAPICS; Ingemar Renberg, Maria Wik and Judi Natkanski for discussing ideas; Cath Fletcher for, amongst other things, proof-reading the chapters; Tim Aspden, Robert Bradbrook and Louise Saunders of the Geography Department Cartographic Unit for drawing most of the diagrams; Messrs’ Page, Plant, Bonham and Jones for many hours company during particle counting. This project was partially funded by the Central Electricity Generating Board, and the Department of the Environment. Last but certainly not least, I would like to thank my parents for their continuing support and encouragement. 3 Title Page 1 Abstract 2 Acknowledgements 3 Contents 4 List of Figures 8 List of Plates 14 List of Tables 15 Chapter One Introduction. 18 1.1. Particle formation 18 1.2. Fly-ash particles in the environment 21 1.3. Fly-ash particles in lake sediments 24 1.4. Outline of the thesis. 25 Chapter Two Sites and Methods. 30 2.1. Site selection 30 2.1.1. Sites for spatial distribution studies 30 2.1.2. Sites for temporal distribution studies 32 2.2. Coring techniques 38 2.3. Laboratory methods 38 2.3.1. Sediment analysis 38 2.3.2. Dating techniques 38 2.4. A method for the extraction of carbonaceous 39 particles from lake sediment 2.4.1. Laboratory procedure 40 2.4.2. Density separations 41 2.4.3. Filtration 42 2.4.4. Counting 42 2.4.5. Repeatability 43 2.4.6. Recovery rate 44 2.4.7. Detection limit 45 2.4.8. Application to a sediment core 45 2.4.9. Discussion 47 2.5. An extraction technique for inorganic ash 47 spheres from lake sediments 2.5.1. Organic material 49 2.5.2. Biogenic silica 49 2.5.3. Carbonates 50 2.5.4. Mineral silica 50 2.5.5. Magnetic separation 50 2.5.6. Density separations 52 2.5.7. Laboratory procedure 52 2.5.8. Counting 53 4 2.5.9. Repeatability 54 2.5.10. Recovery rate 54 2.5.11. Detection limit 55 2.5.12. Application to a sediment core 55 2.6. Reference material 57 9 7 U » 1 • Energy Dispersive Spectroscopy (EDS) 57 2.7.1. Sample preparation 57 2.7.2. EDS of carbonaceous particles 58 2.8. Computer software 58 2.8.1. Manipulation of EDS generated data 58 2.8.2. Statistical techniques 59 Chapter Three Carbonaceous particle characterisation. 60 3.1. Introduction 60 3.2. Previous attempts at fuel type separations 61 3.2.1. External morphology 61 3.2.2. Internal structure using thin sectioning 61 3.2.3. Chemical parameters 62 3.3. Principles of Energy Dispersive Spectroscopy 63 (EDS) 3.4. Power station reference material 65 3.5. EDS of reference material 69 3.5.1. Element selection 69 3.5.2. Automated data acquisition 69 3.5.3. X-ray corrections 70 3.5.4. Setting the wave-form thresholds 72 3.5.5. Data output 74 3.5.6. Negative values in chemical data 78 3.6. The reference data-set 78 3.6.1. Removal of outliers using MIDAS 78 3.6.2. Basic statistics of the reference data-set 81 3.7. Preliminary data analysis of EDS data 93 3.7.1. MIDAS analysis using data from Lxmbridge, 93 Pembroke and Gweedore power stations 3.7.2. Multivariate analysis using data from Ironbridge 100 and Pembroke power stations 3.8. Multivariate analysis of the full reference 105 data-set 3.8.1. Principal components analysis 106 3.8.2. Discriminant analysis on die reference data-set 113 3.8.3. Probabilities of allocation 118 3.8.4. Derivation of a coal/oil discriminant function 121 3.9. Extensions to the characterisation technique 125 3.9.1. Power station allocation 125 3.9.2. Extension to other fuel types 127 Chapter Four Temporal distribution of fly-ash particles in 128 lake sediments. 4.1. Introduction 128 5 4.2. Temporal trends in carbonaceous particle 131 profiles in lake sediments 4.2.1. Scotland 131 4.2.2. Wales 148 4.2.3. Ireland 154 4.2.4. England 161 4.2.5. Sites in Norway and France 164 4.3. Characterisation of carbonaceous particles 170 extracted from lake sediments 4.3.1. Extending particle characterisation to 170 ’fossil’ material 4.3.2. Application of particle characterisation to 174 a sediment core 4.4. Trends in inorganic ash sphere profiles 179 4.5. Discussion 183 4.5.1. Trends in particle deposition 1800 - 1980 183 4.5.2. Causes of a decrease in particle deposition 185 4.5.3. Reasons for the delay in sediment response 187 to the decrease in atmospheric particle deposition 4.5.4. Dating 189 4.5.5. Particle allocations through time 197 Chapter Five Spatial distribution of fly-ash particles in 198 lake sediments 5.1. Introduction 198 5.2. The spatial distribution of fly-ash particles 199 in Scottish surface sediments 5.2.1. Carbonaceous particles 199 5.2.2. Inorganic ash spheres 210 5.3. The spatial distribution of carbonaceous 214 particles in Scottish surface sediments according to fuel-type. 5.3.1. Characterised carbonaceous particles and the 221 IA:CP ratio 5.4. The relationship between fly-ash particle 223 concentrations and sulphur deposition 5.4.1. The sulphur deposition data 224 5.4.2. Particle concentrations and modelled sulphur 225 deposition 5.4.3. Particle concentrations and measured sulphur 236 deposition 5.4.4. Logarithmic transformations of the data 239 5.4.5. Particle fluxes and sulphur deposition 241 5.5. The spatial distribution of carbonaceous 245 particles on a European scale 5.6. Discussion 246 5.6.1. Concentrations and fluxes 246 5.6.2. Characterisation 247 5.6.3. Fly-ash particles and sulphur deposition 248 6 Chapter Six Conclusions 250 6.1.
Load more

Recommended publications
  • HEAVY T-1ETAL ANALYSIS of LAKE SEDJ:I
    HEAVYT-1ETAL ANALYSIS OF LAKE SEDJ:i:.IENTSAS AN INDICATOR OF ElfVIRONME:i:rTALCONTAl'•LmATION: A1'f SXAHPLE FROMROUND LOCH OF GLENEEAD, SOUTH r:lEST SCOTLAND. 7 ·- --l l - l Aclmowledgements I would like to thank Dro Rick Battarbee, Dr. Brian Rippey, John Anderson and Vivienne Jones for their help and encouragement through­ - out the preparation and writing of this project. 7 -, - - - J Contents. Page Abstract Introduction 3 Literature Review (a) Source 4 (b) Transport 6 (c) Deposition 7 (d) Sinks 1. Lake sediments 8 2. Temporary catchment sinks 13 Diagenesis and remobilization of heavy metals 15 Site Description 17 Methods (i) Core extraction 20 (ii) Sediment digestion 21 (iii) Analysis of the digested sediment 21 (iv) Analytical Quality Control 25 Core correlation 25 Results (i) Heavy metal analysis 27 (ii) Analytical Quality Control 35 Discussion Introduction 41 Section 1 (1) Comments on the methodology 41 (2) Heavy metal analysis as an indicator of contamination 43 (3) Discussion of individual profiles 45 Zinc 45 Lead 49 Copper 51 Contents cont. Section? -, (i) Transport and deposition of Zn, Pb and - Cu in Round Loch of Glenhead 51 (ii) Diagenesis and remobilization in Round Loch of Glenhead 53 -·- (iii) Catchment factors 54 (iv) A comparison of Round Loch with other - Northern Hemisphere studies 57 Conclusion 62 Bibliography 64 Appendix 70 - J _..., .u~a v .y 1•1i= l,a.L .ana.1ys is or .La.ke ::::.ectiments as an Indicator of Environmental Contamination: An Example from Round Loch of Glenhead 1 South West Scotland. ,... Abstract. The technique of heavy metal analysis was used to determine the zinc, lead and copper concentrations in a single core (RLGH3) from Round Loch of Glenhead, Galloway.
    [Show full text]
  • Critical Loads for Vegetation
    , '‘`a , 1 e-'-: , % ' , - 7 * liV V$ V 0 , ,„, ' . , 1 4, k. 0. • 4 ' t .r.,.. l'i ,r4' Rat . ' $ i • 11:',11 "P• 1 1, • e á h3A IFISTMAE OF11TRIESTIOL ECOIAGV BUS,- ESTATE. PENICUIK MIDLOTHIAN \ Institute of EH26 OQB Terrestrial 7 Ecology Critical loads: concept and applications ITE symposium no. 28 Proceedings of a Conference held on 12-14 February 1992 in Grange-over-Sands, under the auspices of the British Ecological Society Industrial Ecology Group and the Natural Environment Research Council, and partly sponsored by the National Power/PowerGen Joint Environmental Programme. Edited by M Hornung and R A Skeffington London : HMSO Crown.Copyright 1993 Applications for reproduction should be made to HMSO First published 1993 ISBN 0 11 701666 7 The Institute of Terrestrial Ecology (ITE) is a component research organisation within the Natural Environment Research 'Council. The Institute is part of the Terrestrial and Freshwater Sciences Directorate, and was established in 1973 by the merger of the research stations of the Nature Conservancy with the Institute of Tree Biology. It has been at the forefront of ecological research ever since. The six research stations of the Institute provide a ready access to sites and to environmental and ecological problems in any part of Britain. In addition to the broad environmental knowledge and experience expected of the modern ecologist, each station has a range of special expertise and facilities. Thus, the Institute is able to provide unparallelled opportunities for long-term, multidisciplinary studies of complex environmental and ecological problems. ITE undertakes specialist ecological research on subjects ranging from micro- organisms to trees and mammals, from coastal habitats to uplands, from derelict land to air pollution.
    [Show full text]
  • Water Environment State of the Environment Report Page 1
    East Ayrshire Council Chapter 5 – Water Environment State of the Environment Report Page 1 EAST AYRSHIRE COUNCIL STATE OF THE ENVIRONMENT REPORT CHAPTER 5 – WATER ENVIRONMENT SUMMARY Key Messages Water is a valuable resource, which has multiple uses, e.g. potable water supply, waste water disposal, and water for agriculture and industry, ecology and conservation, recreation, sport and transport. There is robust regulation in Scotland which regulates activities to protect the water environment and has led to an improvement in water quality across Scotland and East Ayrshire. In respect of East Ayrshire’s water resources: There are no estuaries or coastal waters. All surface water bodies are within either the Clyde or Solway sub basins. Nine catchments have been identified within or partially within East Ayrshire, i.e. River Ayr, River Clyde, River Dee (Solway), River Doon, River Garnock, River Irvine, River Nith, Water of Girvan and White Cart Water. There are 64 identified surface water bodies including some water bodies with only part of their catchments within East Ayrshire, such as rivers and lochs at the region’s boundary. These comprise a total of 58 river water bodies and 6 lochs. Most of the rivers are mid-altitude or lowland, calcareous or siliceous and medium or small in scale. The lakes, 4 of which are reservoirs (Lochgoin Reservoir, Loch Riecawr, Loch Finlas and Loch Doon) are mid-altitude low or medium alkalinity, deep and large. Compared with the whole of Scotland, East Ayrshire has proportionately less rivers and lochs of good status. Although groundwater in East Ayrshire tended to be of lower quality than Scotland-wide, the new system has noted that since 2012 there are proportionately more groundwater bodies of good status in East Ayrshire than Scotland-wide.
    [Show full text]
  • Integration of (Federal) Responses to Comments Recieved Through Review of February Draft 2010 and Acceptance of Addendum Road Map
    Integration of (Federal) responses to comments recieved through review of February Draft 2010 and acceptance of addendum Road Map Regulator Comments Adequacy of Response Type Future Follow-up Issue Response following EIS Integration Addressed In September Provided in Draft EIS Requirments September 2010 2010 Addendum (received via submission of Addendum review of February 2010 Draft EIS) CNSC-4 (1) Adequate Yes clean waste rock Acceptable no further integration required CNSC-4 (4) incomplete Type II lake dewatering offset Adequate contingency Figure 3.5-2 updated CNSC-7 unacceptable Type II chemicals/reagents and hazards Adequate no further integration required CNSC-14 incomplete Type II Atmospheric modelling - Acceptable Figure 4.2-1 provided in Appendix temperature as a variable XIV CNSC-15 incomplete Type II Atmospheric modelling - power Acceptable remove reference to diesel power gen sets generation being main source of power CNSC-17 incomplete Type II Stack Emissions Adequate Appendix XII CNSC-19 Acceptable Yes Selenium NR CNSC-21 Acceptable Yes Selenium NR CNSC-22 (1) unacceptable Type I Mink Arm Sediment Adequate Section 3.2.2.2.3 unacceptable Type I Midwest water treatment Adequate Main Document, Section CNSC-22 (2) 3.5.1.2.2, Figure 3.5-2. unacceptable Type I Midwest special waste and Adequate CNSC 22 (4) dewatering system NR CNSC-25 (2) incomplete Type II Traffic on proposed road Adequate Section 7 CNSC-26 requires clarification Type II Traffic wildlife interactions Adequate NR CNSC-27 incomplete Type II Mink Arm dewatering Adequate Section 3.2.1.1.2 CNSC-29 Acceptable Yes Phyto/Zooplankton monitoring NR EEM TAP CNSC-A incomplete Type II Appendix XII Adequate chemicals/reagents, hazards and transport Appendix XII, Section 3.5.
    [Show full text]
  • Acidification, Eutrophication and Ground-Level Ozone in the UK NEGTAP 2001
    ! ! ! Prepared by M Coyle (CEH Edinburgh). ! ! Transboundary Air Pollution: Acidification, Eutrophication and Ground-Level Ozone in the UK ISBN 1 870393 61 9 For further copies, please contact: Mhairi Coyle Dr. Alison Vipond CEH Edinburgh Air and Environment Quality Division Bush Estate Department for Environment, Food and Rural Affairs Penicuik Ashdown House, Zone 4/D11 Midlothian 123 Victoria Street EH26 0QB London, SW1E 6DE UK UK [email protected] [email protected] tel. ++44(0) 131 445 8528 fax. ++44(0) 131 445 3943 The report is also available in electronic format at http://www.nbu.ac.uk/negtap/. For technical enquires, please contact: Prof. David Fowler CEH Edinburgh Bush Estate Penicuik Midlothian, EH26 0QB UK [email protected] tel. ++44(0) 131 445 4343 fax. ++44(0) 131 445 3943 NEGTAP 2001 Prepared by the National Expert Group on Transboundary Air Pollution (NEGTAP) at CEH Edinburgh on behalf of the UK Department for Environment, Food and Rural Affairs, Scottish Executive, The National Assembly for Wales/Cynulliad Cenedlaethol Cymru, Department of the Environment for Northern Ireland. DEFRA Contract EPG 1/3/153 © NEGTAP 2001 ! ! National Expert Group on Transboundary Air Pollution http://www.nbu.ac.uk/negtap/ D Fowler (Chairman) M Coyle (Secretary) Centre for Ecology and Hydrology Edinburgh H M ApSimon Department of Environmental Science and Technology, Imperial College of Science, Technology and Medicine M R Ashmore University of Bradford S A Bareham Cyngor Cefn Gwlad Cymru/Countryside Council for Wales, Joint Nature Conservancy
    [Show full text]
  • Chapter 5 – Water Environment State of the Environment Report Page 1
    East Ayrshire Council Chapter 5 – Water Environment State of the Environment Report Page 1 EAST AYRSHIRE COUNCIL STATE OF THE ENVIRONMENT REPORT CHAPTER 5 – WATER ENVIRONMENT SUMMARY Key Messages Water is a valuable resource, which has multiple uses, e.g. potable water supply, waste water disposal, and water for agriculture and industry, ecology and conservation, recreation, sport and transport. There is robust regulation in Scotland which regulates activities to protect the water environment and has led to an improvement in water quality across Scotland and East Ayrshire. In respect of East Ayrshire’s water resources: • There are no estuaries or coastal waters. • All surface water bodies are within either the Clyde or Solway sub basins. Nine catchments have been identified within or partially within East Ayrshire, i.e. River Ayr, River Clyde, River Dee (Solway), River Doon, River Garnock, River Irvine, River Nith, Water of Girvan and White Cart Water. • There are 64 identified surface water bodies including some water bodies with only part of their catchments within East Ayrshire, such as rivers and lochs at the region’s boundary. These comprise a total of 58 river water bodies and 6 lochs. • Most of the rivers are mid-altitude or lowland, calcareous or siliceous and medium or small in scale. The lakes, 4 of which are reservoirs (Lochgoin Reservoir, Loch Riecawr, Loch Finlas and Loch Doon) are mid-altitude low or medium alkalinity, deep and large. • Compared with the whole of Scotland, East Ayrshire has proportionately less rivers and lochs of good status. • Although groundwater in East Ayrshire tended to be of lower quality than Scotland-wide, the new system has noted that since 2012 there are proportionately more groundwater bodies of good status in East Ayrshire than Scotland-wide.
    [Show full text]