Pyrite Testing explained by Dr Bernadette Azzie

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Pyrite Testing explained by Dr Bernadette Azzie For the: Institute of Geologists of Ireland Pyrite CPD Course 4 December 2013

Start at the beginning. 2FeS 2 + 2H 2 O + 7O 2 2FeSO 4 + 2H 2 SO 4 Pyrite Water Oxygen Ferrous sulphate Sulphuric acid Water Oxidizer (Air, Fe +3 ) ARD Pyrite Bacteria H 2 SO 4 + CaCO 3 + H 2 O CaSO 4 2H 2 O + CO 2 Sulphuric acid Calcite Water Gypsum Carbon dioxide December 5, 2013 2

Our Goal Does the sample contain rock types that are, or have been, associated with pyritic heave? Need to identify the presence of reactive pyrite and secondary minerals that may be associated with heave (e.g. gypsum) December 5, 2013 3

Chemical Reaction Pyrite (FeS2) in framboidal form Reacts with moisture and air present in ground oxidizes the pyrite, releasing sulphuric acid (H2SO4) These rocks typically have 20 to 30% calcite in them (like the problematic mudstones in Ireland), though only 1-2% calcite needed to feed reaction (Québec Shales). H2SO4 dissolves the calcite releasing Ca ions in to solution. The solution eventually becomes super saturated Crystallization of gypsum (CaSO4 2H2O) Pyrite oxidising, ~20µm fov Gypsum within opened lamination ~5cm fov Pyrite framboid, ~20µm fov

I.S. 398-1 Professional Geologist s Report Laboratory Test Report Hardcore Sample Report Sampling of hardcore, with a visual inspection Laboratory tests (specific for each test suite) Overall Classification of hardcore December 5, 2013 5

I.S. 398-1 Test Suites Selection of a Suite depends on: Damage Condition Rating; Background information on the house (i.e. location, when built, etc.); Results of previous testing (if any); A Certificate is required. Test Suite 0 Test Suite Tests Geological inspection Chemical testing Geological inspection Test Suite 1 Chemical testing Mineralogical analysis (XRD) Test Suite 2 (following Suite 0 or Suite1) Thin section petrographic analysis Water absorption December 5, 2013 6

Overview of Testing Protocol Sample Handling and Preparation Visual Inspection and Geologic Description Chemical Testing Mineralogical Analysis XRD Petrographic microscopy SEM Physical Tests Water absorption Abrasion tests Particle size distribution, moisture Etc. December 5, 2013 7

BS EN 932-1: 1997 Sample Reduction How Much Sample Do you Need? What tests are going to be performed? 5kgs to 500kgs I.S. 398-1: 500g blinding sand 25kg infill (per sample) 250mL standing water (if present) Sample No. Original Bulk Mass (kg) Sample Bag Mass (kg) Representative Sample Mass (kg) Celtic-2 421 25.64 8.86 Celtic-25 209 26.62 6.56 Celtic-49 149 29.78 6.32 December 5, 2013 8

Visual Inspection (Field) Blinding Sand: Colour Estimated particle size Moisture condition (Dry, damp, wet) Infill: Colour Rock types (Mudstone, shale, limestone, carbonaceous mudstone, etc.) Particle size Particle shape (Rounded, elongate, tabular, cuboid, sub-rounded, angular) Moisture condition (Dry, damp, wet) Presence of coatings/crystal growth December 5, 2013 9

Geological Description (Lab) Does the sample contain rock types associated with pyritic heave? i.e. Weak, fine-grained sedimentary (muddy limestone, calcareous mudstone, shale) or metamorphic rocks I.S. EN 932-3 (1997) Tests for general properties of aggregates Part 3: Procedure and terminology for simplified petrographic description December 5, 2013 10

Geological Description Particle size Particle shape Rock types (including proportion thereof) Lithological detail: Colour Predominant grain size Mineralogy Laminations Surface coatings Staining Hardness / Strength Carbonates December 5, 2013 11

Chemical Testing Representative Sub-sample.. 1-2 kgs, potentially more! Identify and measure concentration and composition of selected sulphur species Sample preparation Avoid high heat and extensive milling, which may cause oxidation Tests: Total sulphur (TS) Acid-soluble sulphate (AS) Water-soluble sulphate (WS) TS and AS allow determination of estimated pyrite content WSS indicates aggressiveness of fill to concrete materials December 5, 2013 12

Total Sulphur (TS) Includes sulphates, sulphides, monosulphide sulphur, and organic sulphur. Allows an estimate of original pyrite content: Original Pyrite (FeS 2 ) = 1.87 x TS Method TRL 447 Method - Test 4 Sample Size Description A: Microwave digestion of the sample using aqua regia, with determination of the liberated sulphur in solution using ICP- AES. B: Rapid High Temperature Combustion Analysis (Leco) Sample Preparation 500g initially, then 200-300g. Test portion is 300mg. Dried at 100-105ºC; Sieved to <2mm, Mixed and quartered/riffled to 200-300g; Milled to <212µm December 5, 2013 13

Case Study Example Total Sulphur December 5, 2013 14

Acid-Soluble Sulphate (AS) Acid soluble sulphur measured, with results expressed in %S. Results then converted to acid soluble sulphate by calculation: AS (%SO 4 ) = 3 x acid soluble sulphur (as %S) Includes sulphur locked up in all sulphate minerals, such as gypsum (Ca 2 SO 4.2H 2 O), anhydrite (CaSO 4 ) and jarosite (KFe 3 (SO 4 ) 2 (OH) 6 ). Method Description TRL447 Method - Test 2 HCl digestion, followed by ICP-AES analysis Sample Size Sample Preparation 500g initially, then 200-300g. Test portion is 0.8-1.0g Dried at 100-105ºC; Sieved to <2mm, Mixed and quartered/riffled to 200-300g; Milled to <212µm December 5, 2013 15

Case Study Example Acid Soluble Sulphur December 5, 2013 16

Water Soluble Sulphate (WS) Assesses aggressiveness of fill to concrete materials in the presence of water (sulphate attack) Water soluble sulphur measured, with results expressed in %S. Results then converted to water soluble sulphate by calculation: WS (mg/l SO 4 ) = 15 x 1,000 x water soluble sulphur (as %S) Method TRL Report 447, Test 1 Sample Size Fine-grained soils 100g; Med-grained 500g; Coarse-grained 3kg Description Dissolved in distilled water, agitated for 16h then filtered; ICP- AES to determine sulphur content Sample Preparation Sample passing 2mm sieve; pulverized to pass 425μm December 5, 2013 17

Case Study Example Water Soluble Sulphate December 5, 2013 18

Estimated Pyrite Content (Current) Calculate the Oxidisable Sulphide (OS) content: OS = (3.0 x TS) - AS Where: OS = oxidisable sulphides as % SO 4 TS = Total Sulphur as % S AS = Acid-Soluble Sulphur as % SO 4 Then assume all oxidisable sulphides are pyrite: % Pyrite (FeS 2 ) = 0.623 x OS NOTE: Calculation may overestimate pyrite if barite (barium sulphate) is present December 5, 2013 19

Mineralogical analysis - XRD X-Ray Diffraction (XRD) analysis used to detect and quantify gypsum, clay minerals, and sulphur-bearing minerals 20g powdered sample Detection limits range from 0.5% - 2% depending on minerals present and degree of crystallinity December 5, 2013 20

XRD Trace Pyrite 3.52% December 5, 2013 21

Mineralogical Analysis - Petrography Determine the mineralogical characteristics of the sample Thin section analysis identifies alteration and weathering features, such as form and distribution of pyrite and presence of derived sulphate minerals (e.g. gypsum) Methods: BS 812: Part 104 (1994) Testing aggregates Part 104: Method for qualitative and quantitative petrographic examination of aggregates ASTM C295-03 Standard Guide for Petrographic Examination of Aggregates for Concrete Select samples of main lithologies for thin section preparation Use oil instead of water in sample preparation to preserve soluble minerals, e.g. gypsum Use both reflected and transmitted light December 5, 2013 22

Petrographic Thin Sections December 5, 2013 23

Mineralogical Analysis SEM Scanning Electron Microscopy (SEM) Microanalysis uses numerous points of analysis on secondary electron image to produce elemental spectral compositions Used to confirm the presence of gypsum and to provide a general chemical analysis of the host material December 5, 2013 24

Mineralogical Analysis - SEM 3000 S Spectrum 3 2500 Ca 2000 1500 1000 500 O Ca 0 0 2 4 6 8 10 12 14 16 18 20 Full Scale 3250 cts Cursor : 20.215 (0 cts) kev Spectrum 3 Gypsum 6000 Spectrum 4 5000 4000 3000 2000 1000 O Ca S Ca December 5, 2013 25 0 0 2 4 6 8 10 12 14 16 18 20 Full Scale 6267 cts Cursor : 20.086 (0 cts) kev Spectrum 4 Gypsum

Physical Tests - Water Absorption Indicator of the ease which any contained pyrite will oxidise Determined by measuring the increase in mass of an aggregate due to water being absorbed into pores I.S. EN 1097-6 (2000) Tests for mechanical and physical properties of aggregates Part 6: Determination of particle density and water absorption Representative sub-sample of bulk sample Sample size: 2kg minimum Results are expressed as a percentage of the dry mass of a sample High absorption values are indicative of high porosity and lower durability Values for the coarse fraction above 2% are of concern December 5, 2013 26

Example Water Absorption December 5, 2013 27

Physical Tests - Crushing Ten Per Cent Fines Value (TFV) Test Measure of resistance to crushing BS 812-111: 1990 Testing aggregates - Methods for determination of ten per cent fines value (TFV) 15-60kg of particles in the 10 mm to 14 mm size range Low TFV are indicative of weak aggregates, and confirm low quality NRA specification for Clause 804 (March 2000) sets a minimum TFV of 130kN December 5, 2013 28

Example Ten Percent Fines Value December 5, 2013 29

Physical Tests - Crushing Ten Per Cent Fines Value (TFV) Test Measure of resistance to crushing BS 812-111: 1990 Testing aggregates - Methods for determination of ten per cent fines value (TFV) Removed from Cl. 804 specification 15-60kg of particles in the 10 mm to 14 mm size range Low TFV are in indicative 2004 and replaced of weak with aggregates, LAA and confirm low quality NRA specification for Clause 804 (March 2000) sets a minimum TFV of 130kN December 5, 2013 30

Physical Tests Abrasion / Impact Los Angeles (LA) Abrasion Test Impact and abrasion resistance of coarse aggregate BS 1097-2: 1998 Tests for mechanical and physical properties of aggregates - Methods for the determination of resistance to fragmentation 15kg of particles in the 10 to 14 mm size range The higher the LA coefficient, the poorer the infill material NRA specification for Clause 804 (May 2000) sets a maximum LA of 30% December 5, 2013 31

Example Los Angeles Abrasion December 5, 2013 32

Physical Tests Abrasion / Impact Los Angeles (LA) Abrasion Test Impact and abrasion resistance of coarse aggregate BS 1097-2: 1998 Tests for mechanical and physical properties of aggregates - Methods for the determination of resistance to fragmentation Poor correlation with field performance 15kg of particles Test performed in the 10 on dry to 14 aggregates mm size range The higher the LA coefficient, the poorer the infill material NRA specification for Clause 804 (May 2000) sets a maximum LA of 30% December 5, 2013 33

Micro-Deval Test Physical Tests - Abrasion Wet test for abrasion resistance and durability Provides a good indication of aggregate s durability when exposed to weather and moisture BS 1097-1: 1996 Determination of Resistance to Wear 2kg of particles in the 10mm to 14mm size range Generally accepted upper limit for micro-deval coefficient is 20 (Typical standards specify maximum values of 18 to 25) December 5, 2013 34

Example - Micro-Deval December 5, 2013 35

Physical Tests Magnesium Sulphate Soundness Degree of degradation resulting from repeated crystallisation and rehydration of MgSO 4 within the materials pores depends on soundness of aggregate BS EN 1367-2: 1998 Tests for thermal and weathering properties of aggregates. Magnesium sulphate test 500g of particles in the 10mm to 14mm range Higher the MS value, the less durable the aggregate NRA specification for Clause 804 (May 2004) sets a maximum MS value of 25% Test is mainly used to determine susceptibility of an aggregate to degradation by exposure to freeze-thaw cycles December 5, 2013 36

Example Magnesium Sulphate Soundness December 5, 2013 37

Physical Tests - PSD Measures the grading of an aggregate sample with respect to different size fractions over the range of particle sizes Primary aggregate classification test Shape of grading curve and % of silt and clay fraction have large influence on aggregate performance BS EN 933-1:1997 Tests for geometrical properties of aggregates - Determination of particle size distribution. Sieving method Sample size dependent on particle size (60g to 80kg) Comparisons made with Clause 804 requirements High fines content (>8%) are of concern in high quality aggregate Fines retain moisture which feeds oxidation of pyrite Consistent with high clay content indicating a non-durable rock Fines contents of up to 12% are common December 5, 2013 38

Example Particle Size Distribution December 5, 2013 39

Physical Tests Atterberg Limits Atterberg Limits testing evaluates the nature of the fine grained fraction in relation to the water content at which the state changes from liquid to plastic to semi-solid BS 1377-2: 1990 Methods of test for soils for civil engineering purposes - Classification tests 500g of sample in natural state (not dried) Fines in crushed rock aggregates should be non-plastic High liquid limits in crushed rock indicate low quality and the presence of fines with undesirable characteristics and potentially prone to volume change with changes in moisture content The NRA specification for Clause 804 sets a maximum limit of 20% for the liquid limit for limestone aggregates, and 21% for other rock types December 5, 2013 40

Example Liquid Limit December 5, 2013 41

Physical Tests Flakiness Index Laminated fine-grained sedimentary rocks usually produce flat and elongated or highly flaky particles Test measures the percentage of particles passing a slot width specified for that particular size fraction flaky particles are those which pass through slots BS EN 933-3 1997: Tests for geometrical properties of aggregates - Determination of particle shape. Flakiness index Sample size dependent on particle dimensions and proportions NRA specification for Clause 804 (May 2004) sets a maximum Flakiness Index of 35% December 5, 2013 42

Example - Flakiness Index December 5, 2013 43

Physical Tests Methylene Blue Absorption Test used to quantify the effect of clay minerals in an aggregate and hence to indicate soundness BS EN 993 9: 1999 Tests for geometrical properties of aggregates - Assessment of fines. Methylene blue test 200g minimum in the 0mm to 2mm size range Included in NRA specification for Cl 804, but no upper limit set yet Values above 1.0g/kg would be cause for concern High MBA would be consistent with high Liquid Limit values as indicators of unsuitable construction aggregates December 5, 2013 44

Example Methylene Blue Absorption December 5, 2013 45

Professional Geologist s Report CONCLUSION PASS or FAIL or INCONCLUSIVE? December 5, 2013 46

Questions? December 5, 2013 47