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Shale Gas Wastes: Radioactive
Decay, NORM & TENORM for
Marcellus and Utica Shales
Julie Weatherington-Rice, PhD, CPG,
CPSS
Bennett & Williams Environmental
Consultants Inc.
An Ohio Fracture Flow
Working Group Presentation
April 24, 2013
Adj. Asst. Prof,
Ohio State U.
Food, Ag & Bio
Eng.
2013 Focusing on Shale Gas Wastes2013 Focusing on Shale Gas Wastes
• Ground Shale Rock:Ground Shale Rock: hydrocarbons, heavy &hydrocarbons, heavy &
radioactive metals, Ohio–NORM,radioactive metals, Ohio–NORM, US EPA-TENORMUS EPA-TENORM
• Drilling Muds:Drilling Muds: who knows what,who knows what, TENORMTENORM
• Fracking FluidsFracking Fluids :: water, sand, who knows what, iwater, sand, who knows what, if
recycled, are theyrecycled, are they TENORM?TENORM?
• Brine:Brine: salts, hydrocarbons, heavy & radioactivesalts, hydrocarbons, heavy & radioactive
metals, Ohio-NORM,metals, Ohio-NORM, US EPA-TENORMUS EPA-TENORM
• Drilling Site Wastes & Accidental Releases:Drilling Site Wastes & Accidental Releases:
who knows what is being releasedwho knows what is being released
• Where are they coming from?Where are they coming from?
• Where are they going?Where are they going?
Why the Current Concern?Why the Current Concern?
• Blacks shales are early sources of UraniumBlacks shales are early sources of Uranium
ore for the “Atomic Age”ore for the “Atomic Age” (Chattanooga Shale, TN;(Chattanooga Shale, TN;
USGS, 1960 & 1961)USGS, 1960 & 1961)
• Black shales like coal are full of heavy andBlack shales like coal are full of heavy and
radioactive metals:radioactive metals: 232232
Th toTh to 228228
Ra &Ra & 238238
U toU to 226226
Ra areRa are
most common seriesmost common series
• 228228
Ra,Ra, 238238
U &U & 226226
Ra water soluble, also in brinesRa water soluble, also in brines
• US EPA limit on Uranium mill tailings, 5 pCi/gUS EPA limit on Uranium mill tailings, 5 pCi/g
because of the Radium:because of the Radium: > LLRW Landfill, Utah or> LLRW Landfill, Utah or
Washington State accept NORMWashington State accept NORM
• US EPA Drinking Water MCLs 5 pCi/l forUS EPA Drinking Water MCLs 5 pCi/l for
Figure 1. Graph from Radioactive Elements in Coal and Fly Ash:
Abundance, Forms, and Environmental Significance. U.S.
Geological Survey Fact Sheet FS-163-97. October, 1997
Why the Current ConcernWhy the Current Concern
Cont?Cont?
• Very limited chem dataVery limited chem data (gamma)(gamma) for Uticafor Utica
shale,shale, TENORMTENORM & brines:& brines: 100’s to 1,000’s X 5100’s to 1,000’s X 5
pCi/g or LpCi/g or L
• PA DEP NOTPA DEP NOT ConfidentConfident with their monitoringwith their monitoring
programs at landfillsprograms at landfills
• PA DEP Marcellus Shale U content:PA DEP Marcellus Shale U content: 10-10010-100
ppmppm
• Uranium-238 content:Uranium-238 content: ~3.4 to 34 pCi/g~3.4 to 34 pCi/g
• Radium-226 content:Radium-226 content: ~ 3.4 to 34 pCi/g~ 3.4 to 34 pCi/g
• Frac Water Ra-226:Frac Water Ra-226: 300 to 9,000 pCi/l300 to 9,000 pCi/l
• PA Marcellus brine chemistry up to 3,609 xPA Marcellus brine chemistry up to 3,609 x
MCLs for radioactivity:MCLs for radioactivity: 5 pCi/l US EPA5 pCi/l US EPA
Gamma
Spec Data
Water Soluble
Sample
Description
Date
Analyze
d (initial
sample
analysis
)
Nuclides
Observed
Above
Minimum
Detection
Activity
(21 day
hold)
Thori
um-
232 /
Radi
um-
228
serie
s
(From
Ra-228
decay
5.8
yrs.)
Actiniu
m-228
(6.1
hrs)
(From
Ra-224
decay
3.6 day)
Pb-212
(10.6
hr)
(From
Ra-224
decay
3.6
day) Bi-
212 (61
min)
Uraniu
m-238 /
Radium
-226
series
(From
Ra-226
decay,
1602
yrs) Pb-
214 (27
min)
Bi-214
(19.7
min) Units Notes
Unused Sand
10/4/201
2    
0.0536
+/-
0.00291
0.0561
+/-
0.00344
0.0393
+/-
0.00509  
0.118
+/-
0.00478
0.116
+/-
0.00435 pCi/g
This sample
should be free of
Utica Shale
contamination
Flow Back
10/4/201
2    
88.4 +/-
3.41
9.08 +/-
0.949 N/A  
116 +/-
4.31
95.6 +/-
3.75 pCi/L
Some level of
mixing of frack
water and radiums
from the brine
Mud
10/4/201
2    
224 +/-
6085
173 +/-
10.9
132 +/-
20.2  
611 +/-
19.8
663 +/-
13.5 pCi/L
some level of
mixing of drilling
mud with radiums
from the brine
"Production
Water"
11/20/20
12    
1070 +/-
27.5 N/A N/A  
947 +/-
29.6
838 +/-
31.3 pCi/L
Is this actually
"brine" or some
combination pf
frack water and
brines?
Vertical (Mud)
12/3/201
2     N/A
159 +/-
16.2 N/A  
566 +/-
27.3 N/A pCi/L
Some mixing of
drilling mud with
brine, don't know
where in hole
Horizontal
Mud
12/3/201
2    
264 +/-
026.7
171 +/-
016.3
229 +/-
59.5  
601 +/-
28.6
578 +/-
34.3 pCi/L
Some mixing of
drilling mud with
brine but from the
horizontal section
of the boring
Mud
12/6/201
2    
206 +/-
24.7
205 +/-
15.1 N/A  
630 +/-
28.0
662 +/-
27.4 pCi/L
Some mixing of
drilling mud with
brine, don't know
where in hole
Data Summary from ODH Samples
Why the Current Concern Cont?Why the Current Concern Cont?
• NY brine up toNY brine up to 15,000 pCi/L15,000 pCi/L
226226
RaRa
• Hard scale in usedHard scale in used
drilling pipes up todrilling pipes up to 6,0006,000
pCi/gpCi/g 226226
Ra and up to 2,000 pCi/gRa and up to 2,000 pCi/g
228228
RaRa
• Ohio still contaminatedOhio still contaminated
from the Manhattanfrom the Manhattan
ProjectProject
– we know better nowwe know better now
Radioactivity = TOC = GasRadioactivity = TOC = Gas
• Gamma RayGamma Ray
signature showssignature shows
highest levels ofhighest levels of
radioactivity in theradioactivity in the
shaleshale
• Horizontal lateralsHorizontal laterals
installed in hottestinstalled in hottest
zoneszones
• Shale cuttings areShale cuttings are
from hottest areasfrom hottest areas
5 pCi/l MCL: Why the Health5 pCi/l MCL: Why the Health
Risk?Risk?
Because water-soluble Radium replaces
Calcium in your bones if you drink it
Legal disposal for
shale rock cuttings,
drilling muds and
associated wastes
HB 59 required
downblending if Ra
levels above MCLs for
TENORM only,
removed from bill,
expected back this fall
Press releases do not
indicate that chemical
binding of radioactive
Landfilling the WastesLandfilling the Wastes
Radium can be
Bound in Barite
• But Ra will still
decay in landfill &
release radon gas
• Radon gas is noble
gas, collected in
gas collection
system but NOT
destroyed at flair,
simply released
• Radon gas
generation
continues until all
Th, U & Ra is spent
in landfill
• New soluble Ra, not
bound, is formed
from Th & U in
landfill from rock
Chemical precipitate of flow-
back water: Dr. Radisav
Vidic, PE presentation U
But are they LLRWBut are they LLRW
Landfills?Landfills?• No solid wasteNo solid waste
and C&DD wasteand C&DD waste
landfills in Ohiolandfills in Ohio
meet our siting &meet our siting &
design criteria fordesign criteria for
LLRW disposalLLRW disposal
• OSU ExtensionOSU Extension
Research “Low-Research “Low-
Level RadioactiveLevel Radioactive
Waste Fact SheetWaste Fact Sheet
Series” (RER-00)Series” (RER-00)
explains whyexplains why
Cement vaults above ground,
wastes drummed,
overpacked and sealed
Ohioline.osu.edu/rer-fact/
How Long to Protect from Human
Interaction if We use Michigan’s
50 pCi/g Landfill Limit
• 50 pCi/g to 25 pCi/g to 12.5 pCi/g to 6.25
pCi/g to 5 pCi/g
• 50 pCi/g Radium-226 (1,609 yrs/1/2 life) to 5
pCi/g is 3+ half lives, ~5,000 yrs, back to the
beginning of Egypt's pyramids
• 50 pCi/g Uranium-238 (4.468 Billion yrs/1/2
life, from almost the birth of the earth until
now is one ½ life) to 5 pCi/g, so 3+ half-lives,
back to the beginning of the Universe
• 50 pCi/g Thorium-232 (14.05 Billion yrs/1/2
life, longer than the age of the Universe until
now one ½ life) to 5 pCi/g, ~45 Billion years,
Contacts for this presentation &Contacts for this presentation &
Ohio Journal of Science PapersOhio Journal of Science Papers
OFFWG,OFFWG, Dr. Julie Weatherington-Rice, B&W,Dr. Julie Weatherington-Rice, B&W,
OSU FABE,OSU FABE, weatherington-ri.1@osu.eduweatherington-ri.1@osu.edu
OFFWG,OFFWG, Dr. Ann Christy, OSU FABE,Dr. Ann Christy, OSU FABE,
christy.14@osu.educhristy.14@osu.edu
Bennett & WilliamsBennett & Williams , Linda Aller RS,, Linda Aller RS,
Laller@bennettandwilliams.comLaller@bennettandwilliams.com
Ohio Journal of Science Web Link atOhio Journal of Science Web Link at
OSU,OSU,
https://kb.osu.edu/dspace/handle/1811/686https://kb.osu.edu/dspace/handle/1811/686
Ohio EPAOhio EPA Division of Drinking and GroundDivision of Drinking and Ground
Waters Source Water Assessment andWaters Source Water Assessment and
Protection Program,Protection Program,
www.epa.ohio.gov/ddagw/swap_ssa.aspxwww.epa.ohio.gov/ddagw/swap_ssa.aspx
Keeping Ohio’s Water Clean
Ohio Fracture Flow Working
Group

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Tip & Glow Radioactive Waste Amendment in the State Budget Bill Webinar

  • 1. Shale Gas Wastes: Radioactive Decay, NORM & TENORM for Marcellus and Utica Shales Julie Weatherington-Rice, PhD, CPG, CPSS Bennett & Williams Environmental Consultants Inc. An Ohio Fracture Flow Working Group Presentation April 24, 2013 Adj. Asst. Prof, Ohio State U. Food, Ag & Bio Eng.
  • 2. 2013 Focusing on Shale Gas Wastes2013 Focusing on Shale Gas Wastes • Ground Shale Rock:Ground Shale Rock: hydrocarbons, heavy &hydrocarbons, heavy & radioactive metals, Ohio–NORM,radioactive metals, Ohio–NORM, US EPA-TENORMUS EPA-TENORM • Drilling Muds:Drilling Muds: who knows what,who knows what, TENORMTENORM • Fracking FluidsFracking Fluids :: water, sand, who knows what, iwater, sand, who knows what, if recycled, are theyrecycled, are they TENORM?TENORM? • Brine:Brine: salts, hydrocarbons, heavy & radioactivesalts, hydrocarbons, heavy & radioactive metals, Ohio-NORM,metals, Ohio-NORM, US EPA-TENORMUS EPA-TENORM • Drilling Site Wastes & Accidental Releases:Drilling Site Wastes & Accidental Releases: who knows what is being releasedwho knows what is being released • Where are they coming from?Where are they coming from? • Where are they going?Where are they going?
  • 3. Why the Current Concern?Why the Current Concern? • Blacks shales are early sources of UraniumBlacks shales are early sources of Uranium ore for the “Atomic Age”ore for the “Atomic Age” (Chattanooga Shale, TN;(Chattanooga Shale, TN; USGS, 1960 & 1961)USGS, 1960 & 1961) • Black shales like coal are full of heavy andBlack shales like coal are full of heavy and radioactive metals:radioactive metals: 232232 Th toTh to 228228 Ra &Ra & 238238 U toU to 226226 Ra areRa are most common seriesmost common series • 228228 Ra,Ra, 238238 U &U & 226226 Ra water soluble, also in brinesRa water soluble, also in brines • US EPA limit on Uranium mill tailings, 5 pCi/gUS EPA limit on Uranium mill tailings, 5 pCi/g because of the Radium:because of the Radium: > LLRW Landfill, Utah or> LLRW Landfill, Utah or Washington State accept NORMWashington State accept NORM • US EPA Drinking Water MCLs 5 pCi/l forUS EPA Drinking Water MCLs 5 pCi/l for
  • 4. Figure 1. Graph from Radioactive Elements in Coal and Fly Ash: Abundance, Forms, and Environmental Significance. U.S. Geological Survey Fact Sheet FS-163-97. October, 1997
  • 5. Why the Current ConcernWhy the Current Concern Cont?Cont? • Very limited chem dataVery limited chem data (gamma)(gamma) for Uticafor Utica shale,shale, TENORMTENORM & brines:& brines: 100’s to 1,000’s X 5100’s to 1,000’s X 5 pCi/g or LpCi/g or L • PA DEP NOTPA DEP NOT ConfidentConfident with their monitoringwith their monitoring programs at landfillsprograms at landfills • PA DEP Marcellus Shale U content:PA DEP Marcellus Shale U content: 10-10010-100 ppmppm • Uranium-238 content:Uranium-238 content: ~3.4 to 34 pCi/g~3.4 to 34 pCi/g • Radium-226 content:Radium-226 content: ~ 3.4 to 34 pCi/g~ 3.4 to 34 pCi/g • Frac Water Ra-226:Frac Water Ra-226: 300 to 9,000 pCi/l300 to 9,000 pCi/l • PA Marcellus brine chemistry up to 3,609 xPA Marcellus brine chemistry up to 3,609 x MCLs for radioactivity:MCLs for radioactivity: 5 pCi/l US EPA5 pCi/l US EPA
  • 7. Sample Description Date Analyze d (initial sample analysis ) Nuclides Observed Above Minimum Detection Activity (21 day hold) Thori um- 232 / Radi um- 228 serie s (From Ra-228 decay 5.8 yrs.) Actiniu m-228 (6.1 hrs) (From Ra-224 decay 3.6 day) Pb-212 (10.6 hr) (From Ra-224 decay 3.6 day) Bi- 212 (61 min) Uraniu m-238 / Radium -226 series (From Ra-226 decay, 1602 yrs) Pb- 214 (27 min) Bi-214 (19.7 min) Units Notes Unused Sand 10/4/201 2     0.0536 +/- 0.00291 0.0561 +/- 0.00344 0.0393 +/- 0.00509   0.118 +/- 0.00478 0.116 +/- 0.00435 pCi/g This sample should be free of Utica Shale contamination Flow Back 10/4/201 2     88.4 +/- 3.41 9.08 +/- 0.949 N/A   116 +/- 4.31 95.6 +/- 3.75 pCi/L Some level of mixing of frack water and radiums from the brine Mud 10/4/201 2     224 +/- 6085 173 +/- 10.9 132 +/- 20.2   611 +/- 19.8 663 +/- 13.5 pCi/L some level of mixing of drilling mud with radiums from the brine "Production Water" 11/20/20 12     1070 +/- 27.5 N/A N/A   947 +/- 29.6 838 +/- 31.3 pCi/L Is this actually "brine" or some combination pf frack water and brines? Vertical (Mud) 12/3/201 2     N/A 159 +/- 16.2 N/A   566 +/- 27.3 N/A pCi/L Some mixing of drilling mud with brine, don't know where in hole Horizontal Mud 12/3/201 2     264 +/- 026.7 171 +/- 016.3 229 +/- 59.5   601 +/- 28.6 578 +/- 34.3 pCi/L Some mixing of drilling mud with brine but from the horizontal section of the boring Mud 12/6/201 2     206 +/- 24.7 205 +/- 15.1 N/A   630 +/- 28.0 662 +/- 27.4 pCi/L Some mixing of drilling mud with brine, don't know where in hole Data Summary from ODH Samples
  • 8. Why the Current Concern Cont?Why the Current Concern Cont? • NY brine up toNY brine up to 15,000 pCi/L15,000 pCi/L 226226 RaRa • Hard scale in usedHard scale in used drilling pipes up todrilling pipes up to 6,0006,000 pCi/gpCi/g 226226 Ra and up to 2,000 pCi/gRa and up to 2,000 pCi/g 228228 RaRa • Ohio still contaminatedOhio still contaminated from the Manhattanfrom the Manhattan ProjectProject – we know better nowwe know better now
  • 9. Radioactivity = TOC = GasRadioactivity = TOC = Gas • Gamma RayGamma Ray signature showssignature shows highest levels ofhighest levels of radioactivity in theradioactivity in the shaleshale • Horizontal lateralsHorizontal laterals installed in hottestinstalled in hottest zoneszones • Shale cuttings areShale cuttings are from hottest areasfrom hottest areas
  • 10. 5 pCi/l MCL: Why the Health5 pCi/l MCL: Why the Health Risk?Risk? Because water-soluble Radium replaces Calcium in your bones if you drink it
  • 11. Legal disposal for shale rock cuttings, drilling muds and associated wastes HB 59 required downblending if Ra levels above MCLs for TENORM only, removed from bill, expected back this fall Press releases do not indicate that chemical binding of radioactive Landfilling the WastesLandfilling the Wastes
  • 12. Radium can be Bound in Barite • But Ra will still decay in landfill & release radon gas • Radon gas is noble gas, collected in gas collection system but NOT destroyed at flair, simply released • Radon gas generation continues until all Th, U & Ra is spent in landfill • New soluble Ra, not bound, is formed from Th & U in landfill from rock Chemical precipitate of flow- back water: Dr. Radisav Vidic, PE presentation U
  • 13. But are they LLRWBut are they LLRW Landfills?Landfills?• No solid wasteNo solid waste and C&DD wasteand C&DD waste landfills in Ohiolandfills in Ohio meet our siting &meet our siting & design criteria fordesign criteria for LLRW disposalLLRW disposal • OSU ExtensionOSU Extension Research “Low-Research “Low- Level RadioactiveLevel Radioactive Waste Fact SheetWaste Fact Sheet Series” (RER-00)Series” (RER-00) explains whyexplains why Cement vaults above ground, wastes drummed, overpacked and sealed Ohioline.osu.edu/rer-fact/
  • 14. How Long to Protect from Human Interaction if We use Michigan’s 50 pCi/g Landfill Limit • 50 pCi/g to 25 pCi/g to 12.5 pCi/g to 6.25 pCi/g to 5 pCi/g • 50 pCi/g Radium-226 (1,609 yrs/1/2 life) to 5 pCi/g is 3+ half lives, ~5,000 yrs, back to the beginning of Egypt's pyramids • 50 pCi/g Uranium-238 (4.468 Billion yrs/1/2 life, from almost the birth of the earth until now is one ½ life) to 5 pCi/g, so 3+ half-lives, back to the beginning of the Universe • 50 pCi/g Thorium-232 (14.05 Billion yrs/1/2 life, longer than the age of the Universe until now one ½ life) to 5 pCi/g, ~45 Billion years,
  • 15. Contacts for this presentation &Contacts for this presentation & Ohio Journal of Science PapersOhio Journal of Science Papers OFFWG,OFFWG, Dr. Julie Weatherington-Rice, B&W,Dr. Julie Weatherington-Rice, B&W, OSU FABE,OSU FABE, weatherington-ri.1@osu.eduweatherington-ri.1@osu.edu OFFWG,OFFWG, Dr. Ann Christy, OSU FABE,Dr. Ann Christy, OSU FABE, christy.14@osu.educhristy.14@osu.edu Bennett & WilliamsBennett & Williams , Linda Aller RS,, Linda Aller RS, Laller@bennettandwilliams.comLaller@bennettandwilliams.com Ohio Journal of Science Web Link atOhio Journal of Science Web Link at OSU,OSU, https://kb.osu.edu/dspace/handle/1811/686https://kb.osu.edu/dspace/handle/1811/686 Ohio EPAOhio EPA Division of Drinking and GroundDivision of Drinking and Ground Waters Source Water Assessment andWaters Source Water Assessment and Protection Program,Protection Program, www.epa.ohio.gov/ddagw/swap_ssa.aspxwww.epa.ohio.gov/ddagw/swap_ssa.aspx Keeping Ohio’s Water Clean Ohio Fracture Flow Working Group