Radiological Investigation Results for
Pennsylvania Landfill Leachate
Pennsylvania Department of Environmental Protection
Bureau of Radiation Protection
Bureau of Waste Management
Project No. 040-195
October 3, 2005
333 Baldwin Road
Pittsburgh, PA 15205-9702
Table of Contents
1.3 Data Needs
1.4 Project Organization and Responsibility
1.4.1 PADEP Regional Office Solid Waste Managers
1.4.2 SAP Operations and Data Management
1.4.3 Laboratory Operations
2.0 Field Sampling Plan and Laboratory Analyses
2.1 Sampling Locations, Frequency, and Media
2.1.1 Sample Collections and Analyses
2.1.2 Sample Identification
2.2 Quality Control Samples
2.3 Chain ofCustody Record
2.4 Handling and Disposition oflnvestigation-Derived Waste
2.5 Sample Handling, Packaging, and Shipping
2.5.1 Field Screening for Radioactivity
3. 0 Leachate Analysis Results
3.l Initial Measurements Phase
3 .1.1 Gross Alpha Radioactivity Concentration
3 .1.2 Gross Beta Radioactivity Concentration
3 .1.3 Fission/ Activation Product Radionuclide Concentrations
3.1.4 Naturally-Occurring Radionuclide Concentrations
3.2 Follow-On Measurements Phase
3.2.1 Total Uranium
3.2.2 Radium-226 e26Ra)
3.2.3 Radium-228 e28Ra)
4.1.1 Uranium and Thorium
4.1.3 Applicable or Relevant and Appropriate Requirements Standard of Consideration
Attachment A-Radioactivity Concentration Data Displays
Attachment B-Analytical Data Summary
Attachment C-Laboratory Analysis Reports
3 3 3 3
4 4 4 4
5 5 7 9 9 10 10 10
l3 l3 l3
15 19 19 20 20
21 21 22
During the fourth quarter of 2004, the Pennsylvania Department of Environmental Protection (PADEP) implemented a sampling and analysis plan (SAP) to investigate radioactive material potentially present in landfill untreated leachate. The investigation included all active and permitted landfills in the Commonwealth of Pennsylvania having a leachate collection system (half of the 108 solid waste landfills in the Commonwealth met this selection criterion). Samples of raw, untreated leachate were collected at each of the 54 landfills (an additional 5 quality control sample sets were collected for a total of 59 sets) and sent to a commercial radioanalyticallaboratory for analysis. During the initial analysis phase of the 59 sample sets, the following radioactivity concentration parameters were measured: gross alpha, gross beta, gamma emitters by spectroscopy, and tritium eH as HTO). A subsequent “follow-on” analysis phase was performed for landfills whose leachate gross alpha radioactivity concentration exceeded approximately a 5 picocuries per liter (pCi/L; 1 pCi = 0.000000000001 Ci) threshold. The follow-on analyses measured the radioactivity concentration of radium-226 e26Ra, a member of the natural uranium decay series) and radium-228 e28Ra, a member of the natural thorium decay series), as well as the mass concentration (micrograms per liter; j.Jg/L) of total uranium.
The initial analysis phase results showed that tritium was the most prevalent (identified in 57 or 97% of the 59 samples analyzed) radionuclide present in leachate, ranging from 6.86 to 94,400 pCi/L, with a mean activity concentration of 25,200 pCi/L. Tritium is both a naturally-occurring and man-made radionuclide. The next most prevalent radionuclide measured was potassium-40 (4°K; identified in 53 samples), a completely naturally-occurring radioactive material whose identification was inconsequential. Other than tritium and some of the gross alpha radioactivity concentration results (those that exceeded the follow-on analysis threshold of 5 pCi/L), none of the initial phase measurements results warranted additional investigation or interpretation.
Because uranium and thorium are native constituent elements of landfill soil and daily cover material (and thus in leachate produced in contact with that soil) in concentrations that are readily detectable in the laboratory, the follow-on analysis of 18 archived samples whose gross alpha radioactivity concentration exceeded 5 pCi/L was inconsequential with a single exception. The 226Ra activity concentration ranged from 0.18 to 24.2 pCi!L, with a mean activity concentration of 3.46 pCi/L (the median was 2.22 pCi/L). For 228Ra, its activity concentration ranged from 0.71 to 42.0 pCi/L, with a mean activity concentration of
5.40 pCi/L (the median was 2.96 pCi/L). The total uranium mass concentration ranged from 0.00 to 2.50 j.Jg/L, with a mean mass concentration of 0.53 j.Jg/L (the median was 0.27 j.Jg/L). The single exception
was a landfill in Lancaster County whose follow-on results were those reported above as the upper range. Those results exceed expected concentrations by a wide margin and are indicative of possible burials of technologically-enhanced naturally-occurring radioactive material (TENORM) e.g., foundry sand or bricks, coal-powered power plant ash, stack flyash and/or stack scrubber residue at that landfill.
Ignoring reasonable human exposure scenanos, some of the tritium activity concentrations measured exceed applicable or relevant and appropriate requirement (ARAR) standards postulated by the Commonwealth. However, when one considers the treatment and discharge processes leachate actually undergo, and dilution is factored into a human exposure scenario, none of the tritium results exceed ARAR levels. While it is not feasible or practical to confirm the exact sources of the observed tritium in leachate, the Commonwealth believes that gaseous tritium light source (GTLS) ‘EXIT’ signs have been, and continue to be, disposed in landfills. These GTLS devices contain significant quantities of tritium gas that, once ruptured in a landfill, are readily oxidized into tritiated water that is eventually captured as leachate.
The Commonwealth is planning to conduct a subsequent seasonal round of tritium sampling at the landfills included in this report during the fall of 2005.
A radiological sampling and analysis plan (SAP) was implemented at active (permitted) solid waste
landfills (LFs) in the state of Pennsylvania. The LF SAP was designed to investigate soluble and
insoluble radiological constituents of concern (COCs) potentially present in LF untreated leachate. The
sampling and analysis activities were conducted during the fourth quarter of 2004 at the direction of the
Pennsylvania Department of Environmental Protection (PADEP) Bureau ofRadiation Protection to obtain
baseline radiological data for LF untreated leachate. This report documents this baseline data and how it
There are a total of 108 solid waste LFs in Pennsylvania designated for receipt of municipal waste (MW),
residual waste (RW), sanitary waste, and construction/demolition (C/D) debris. Of this total, 54 LFs are
permitted and active with the remaining 54 inactive or designated by the PADEP not to be included in
this sampling event. Most of the active LFs (Table l) feature a leachate collection system to capture
liquids percolating through the LF for wastewater treatment facility processing. Active LF operators are
required by PADEP regulations to periodically sample and characterize their leachate for a suite of non.
radioactive COCs (radioactive COCs are not required).
1.3 Data Needs
The primary data needs fulfilled by the SAP were:
Identification and quantification (radioactivity concentration) of gamma-emitting radionuclides
that may be present above laboratory limits of detection (minimum detectable concentration or
Tritium radioactivity concentration.
Gross alpha/beta radioactivity concentration.
If prompted by a technical review of the primary data obtained, secondary data needs include some or all of the following COCs:
226Ra radioactivity concentration.
228Ra radioactivity concentration.
Total uranium radioactivity concentration.
The technical review of the primary data performed by the LF leachate SAP team (see section 1.4) focused on resolving gross alpha/beta radioactivity concentration anomalies as well as unusual gamma.emitting radionuclide activity concentrations.
1.4 Project Organization and Responsibility Specific individuals of the radiological SAP LF leachate team were assigned the following project positions during performance of the monitoring activities:
PADEP Bureau of Radiation Protection (BRP) Sponsor-David J. Allard PADEP Bureau of Waste Management Point of Contact (POC)-Steve Socash Sampling Surveillance/Laboratory Shipments-PADEP Regional Offices
1.4.1 PADEP Regional Office Solid Waste Managers Region I (Southeast) POC-Ronald Furlan Region II (Northeast) POC-William Tomayko Region III (South Central) POC-John Krueger Region IV (North Central) POC-James Miller Region V (Southwest) POC-David Eberle Region VI (Northwest) POC-Todd Carlson
1.4.2 SAP Operations and Data Management Civil and Environmental Consultants, Inc. POC -Rick Orthen
1.4.3 Laboratory Operations Pace Analytical Services POC -Ed F orrai
2.0 Field Sampling Plan and Laboratory Analyses
2.1 SamQling Locations, Freguency, and Media
Sampling and sample packaging for shipment were performed by properly trained and qualified LF site representatives and/or authorized PADEP representatives. Representative samples of untreated leachate from each leachate management system were collected using sampling kit instructions provided to each LF. The LF facility and media to be sampled was determined by PADEP and specified on the Chain of Custody (COC) record (see below and Attachment C) accompanying each sampling kit. Additional details of each of these sampling methods are presented in the following subsections.
Table l Leachate Sample Collections at Active Pennsylvania Solid Waste Landfills
SAPID Permit Facilit~ Name Cit~ Count~
-~ l 3 80 70 Bethlehem Steel Corp R WLF GROWSMWLF Coatesville Morrisville Chester Bucks
….. “‘ 4 72 Pottstown MWLF Pottstown Montgomery
Q,l.c:….. = 5 107 SECCRAMWLF West Grove Kennett Square Chester
0 00. Tullytown Resource Recovery
6 71 MWLF Tullytown Bucks
ll l Alliance Sanitary LF /MWLF Taylor Lackawanna
12 3 Chrin Brothers Inc. MWLF Easton Northampton
~ ….. “‘~ l3 12 Commonwealth Environmental Systems MWLF Foster Township Hegins Schuylkill
Q,l.c:….. :.. 0 15 75 Grand Central Sanitary LF/MWLF Pen Argyl Northampton
z 16 52 IESI Bethlehem LF /MWLF Bethlehem Northampton
17 14 Keystone Sanitary LF /MWLF Dunmore Lackawanna
18 53 Pine Grove LF /MWLF Pine Grove Schuylkill
38 66 Cumberland County MWLF Newburg Cumberland
— 39 58 Conestoga MWLF Greater Lebanon Refuse Morgantown Berks
~ -; :.. ….. = 40 41 16 62 Authority MWLF IESI Blue Ridge MWLF Lebanon Scotland Lebanon Franklin
<:.J.c: ..... = Lancaster County Solid Waste 0 00. 42 18 (Frey Farm) Resource Recovery LF /Transfer Station Bainbridge I Conestoga Lancaster 43 86 Lanchester MWLF Narvon Lancaster 44 64 Mifflin County SW A MWLF Lewistown Mifflin Leachate Sample Collections at Active Pennsylvania Solid Waste Landfills SAPID Permit Facility Name City County - 45 81 Milton Grove CIDLF Mt. Joy Township Lancaster- -~ 46 56 ModernMWLF York York -; :.. 47 60 Mountain View MWLF Greencastle Franklin ...... = Q) <:.J 48 55 Pioneer Crossing MWLF Birdsboro I Harleysville Berks ...... -= 49 63 Rolling Hills MWLF Boyertown Berks = 0 00. 50 65 Sandy Run MWLF Hopewell Bedford 51 59 Western Berks RA MWLF Birdsboro Berks -; 54 48 Allenwood MWLF Brady Township Lycoming :.. ...... West Burlington §>
<:.J- 56 51 Northern Tier MWLF #2 Township Bradford -5~ :.. 59 47 Wayne Township MWLF Wayne Township Clinton 0 z 60 2 White Pines MWLF Pine Township Columbia 64 33 Arden Inc. MWLF Washington Washington 65 102 BFI Imperial MWLF Imperial Allegheny 66 84 Brunner MWLF Zelienople Beaver 67 68 Deep Valley CIDLF North Fayette Township Allegheny 68 39 Evergreen MWLF Coral Indiana 69 67 Greenridge Reclamation MWLF Scottdale Westmoreland J & J MWLF -CBF Inc.(Onyx 70 74 Chestnut) McClellandtown Fayette 71 61 Kelly Run Sanitation MWLF Elizabeth Allegheny 72 69 Laurel Highland MWLF Johnstown Cambria ~ MAX Environmental Tech ...... Q) "' (Noncaptive RW Disposal ~ 73 35 Impoundment) South Huntington Westmoreland ...... -= 0 = Monroeville (Chambers 00. 74 57 Development) MWLF Monroeville Allegheny 75 42 Mostoller MWLF Somerset Somerset 76 77 Paris Flyash Noncaptive RWLF Hanover Township Beaver Westmoreland (Rostraver) 77 73 MWLF Belle Vern on Westmoreland 78 40 ShadeMWLF Cairnbrook Somerset 79 41 South Hills MWLF South Park I Library Allegheny 80 38 Southern Alleghenies MWLF Davidsville Somerset 81 37 ValleyMWLF Irwin Westmoreland Leachate Sample Collections at Active Pennsylvania Solid Waste Landfills SAPID Permit Facility Name City County 90 32 Clarion County MWLF Leeper Clarion 91 105 McKean Kness MWLF Kane McKean - >
92 44 Lake View MWLF Erie Erie
Q) 94 45 Northwest Sanitary MWLF West Sunbury Butler
:.. 95 43 SenecaMWLF Evans City I Mars Butler
96 46 Superior Greentree MWLF Kersey Elk
2.1.1 Sample Collections and Analyses Each LF facility received up to five sample containers: 1 grab composite Cubitainer® (a low-density flexible polyethylene cube-shaped insert) for the unfiltered liquid, 1 pre-preserved Cubitainer® for the filtered sample, 1 glass bottle for the filtered sample, and as necessary, 1 QC duplicate Cubitainer® and 1 QC duplicate glass bottle. Each Cubitainer® and glass bottle was appropriately marked or labeled with the sample identification code and the analysis required. A shipping box specifically designed for the Cubitainer® was also included. All containers except tritium (250 ml glass container) were pre-preserved with a small volume of nitric acid. Also included were two high-capacity canister QuickFilters (609 cm2 area 0.45 micron polyethersulfone media) and a filtration pressure bottle for use with a hand pump. Two QuickFilters were supplied to each LF should the sample matrix be difficult to filter. However, sample filtration was discontinued early in the sampling phase of the project because the leachate matrix was found to be exceedingly difficult to filter in the field setting. Filtration by laboratory personnel also proved impossible; consequently, radiological data for only eight leachate residue samples was obtained.
Because sample filtration was not possible for all but eight samples, unfiltered samples were collected into unpreserved containers as a continuous grab composite. To comply with the 5-day holding time specified by the laboratory, the samples were expeditiously packaged for shipment to the laboratory after collection.
Each sample collected was analyzed per the following schedule:
Liquid Sample Collection and Analysis Schedule
Bottle Analysis Sample Volume Laboratory Analysis
A Gross 1,000 Gross alpha/beta radioactivity (EPA Method 900.0)
B y Spec 1,000 Gamma spectrometry (EPA Method 901.1)
c 3H 250 Tritium (EPA Method 906.0) ~lass container only
D Total U 1,000 Total uranium-KPA screen (ASTM-D5174)
E 226Ra 1,000 Radium-226 (EPA Method 903.1)
F nsRa 1,000 Radium-228 (EPA Method 904.0)
X -. -. Non-routine analyte to be specified on a case-by-case basis
1. Letter in position 9 of the sample identification (ID) code string marked or labeled on the sample bottle and the COC (see section 2.1.2 for ID code scheme).
Note: Analyses for radium and total uranium were not performed (“Z” coded; see section
2.1.2 below) per direction from PADEP.
The gross alpha/beta analyses were conducted using a Protean MDS gas flow proportional counting (GFPC) System. The Protean MDS is a complete system consisting of three, quad-detector low.background MPC-9604 detector subsystems operated with ultra-high purity P-10 gas, plus a PC and Protean control software.
Gamma spectroscopy was conducted with a Canberra GC6020 high purity germanium (HPGe) gamma detector with a Canberra Genie 2000 V AXNMS operating system. The HPGe detector is a high resolution, high efficiency (40%) gamma detector. The Genie 2000 spectroscopy software 1s a comprehensive environment for data acquisition, display, and analysis in personal computers. It provides independent support for multiple detectors, extensive networking capabilities, windowing interactive human interface and comprehensive batch procedure capabilities.
Tritium measurements were made with a Packard TriCarb 2900TR liquid scintillation counter. The TriCarb counter is an ultra low-background analyzer offering automatic window optimization to provide a high efficiency-to-background ratio. Internal quench correction is also provided to determine sample.specific detection efficiencies.
2.1.2 Sample Identification Systematic ll-character sample identification (ID) codes were used to uniquely identify all samples. The ID code format was “AAbbCCCCdEf’ meaning:
AA-a two-digit LF identification number: 01 to 97 (see Table l, column “SAPID”).
bb -a two-letter sample matrix designator: LE (Untreated Leachate), GW (Groundwater), SW
(Surface Water), PT (Precipitation), OT (Other).
ecce-a four-digit project sequential sample number beginning 0001
d-a single letter sample analysis designator: A (Gross aj3), B (y Spec), C eH), D (Total U), E
26Ra), F e28Ra), X (Other).
E-a single-digit sample type designator: l (original), 2 (field QC duplicate).
f-a single letter designating analysis turn around time: N (normal 15 day TAT), Z (archive
All samples with an analysis designation “D”, “E”, or “F” had a “Z” in the last position of the ID code string pending direction from P ADEP to retrieve the archived sample for initial analysis. For example, if the 25th project sample were an original sample collected to determine the tritium concentration in untreated leachate collected at the Monroeville MWLF, it would be designated “74LE0025ClN.” An LF SAP Excel® Workbook was used to record and maintain all pertinent information associated with each sample ID code marked/labeled on sample bottles and COC records issued to field personnel.
2.2 Quality Control Samples Quality assurance objectives were specified so that the data produced are of a known and sufficient quality for determining whether a risk to human health or the environment exists. Because this investigation was preliminary, all data was considered noncritical; accordingly, an extensive effort to validate the precision and accuracy of field sampling adversely affecting results produced in the laboratory setting was not warranted or justifiable. By design, the SAP assured representative sampling because all sample aliquots were taken from a single composite sample. In the field, precision was affected by sample collection procedures and by the natural heterogeneity encountered in the environment. Overall, both field and laboratory precision was evaluated by examining the results of field duplicate samples and laboratory quality control (QC) samples. Laboratory precision was based on the use of laboratory-generated duplicate samples or matrix spike/matrix spike duplicate samples. The field QC duplicate sample load used for this investigation was 10% of the total samples collected (i.e., five duplicate sample sets). Each duplicate sample was analyzed for the same radiological parameters as the original paired sample.
Trip blanks were unnecessary since no volatile organic compound analyses were included in the SAP. Since sampling equipment was not reused, equipment rinsate samples were not obtained and analyzed to identify instances of sample cross-contamination.
The analytical laboratory chosen for this investigation has extensive experience analyzing the COCs and sample matrices required by this investigation. Further, the laboratory maintains and implements an approved quality assurance program (QAP) to provide objective evidence that all measurements satisfy specific quality assurance objectives. Accordingly, performance evaluation samples (e.g., samples spiked with known concentrations of radionuclides in levels similar to those expected in the actual samples or blanks) were not to be prepared beyond those included in the laboratory’s QAP to further document the accuracy and precision of their measurements process.
2.3 Chain ofCustody Record The chain-of-custody record serves as a written record of sample handling from the field through laboratory receipt. When a completed sample changes custody, those relinquishing and receiving the sample signed the chain-of-custody record. Each change of possession was documented, from the sampler to sample courier, and finally from the courier to the laboratory. The completed chain-of-custody records are included with the laboratory analytical reports (Attachment C).
2.4 Handling and Disposition oflnvestigation-Derived Waste All waste dispositions were coordinated with the appropriate LF site representative to ensure compliance with applicable waste storage, characterization, treatment, and disposal requirements. The investigation.derived waste produced during sampling included spent and unused sample material, personal protective equipment, miscellaneous sampling supplies, decontamination water, purge water, and samples. The LF site representative provided a determination for the disposition of all waste (including purge water) that is based on a waste determination.
2.5 Sample Handling, Packaging, and Shipping All personnel handling samples wore personal protective equipment commensurate with the level of hazard and facility procedures. The exterior of the filled sample container(s) was decontaminated as appropriate. Sample containers were properly secured pending shipment. The sample custodian/shipper was responsible for ensuring that bottle caps were checked for tightness, a tamper-evident seal placed across bottle caps, and samples were properly packaged for custody transfer and shipment to the laboratory. Samples for radioactivity analysis did not require refrigeration, but were shipped to the laboratory to comply with the five-day holding time requirement.
2.5.1 Field Screening for Radioactivity
Screening filled sample containers for radioactivity was not performed prior to sample shipment.
3.0 Leachate Analysis Results
Laboratory analyses were conducted in two phases: initial and follow-on. The initial phase results, discussed in Section 3.1, were obtained by measurements of gross alpha/beta radioactivity, tritium, and gamma emitters by gamma spectrometry. After interpretation of the initial phase results, additional measurements were made in an attempt to further reconcile some of the initial phase results. These ‘follow-on’ phase results are discussed in Section 3.2.
3.1 Initial Measurements Phase
The aqueous portion of the leachate samples collected at 54 landfills was initially analyzed for gross alpha/beta radioactivity, tritium, and gamma emitters by gamma spectrometry. There were five QC duplicate samples collected, for a total of 59 samples. The laboratory processed 6 method blanks to accompany the initial batch processing of the 59 samples. Additionally, the residue collected by filtration of eight samples (SAPID’s 1, 4, 18, 38, 74, 78, 92, and 94) was analyzed by gamma spectrometry. The gamma spectrometry measurements featured search libraries for two nuclide families: fission/activation products and naturally occurring. For the fission/activation products family, the following radionuclides were sought: 6°Co, 137Cs, 154Eu, and 241Am. In the naturally occurring family, 4°K and the 235U/238U/232Th-decay series’ radionuclides were sought. The 235U series was represented by 235U in the gamma spectra. For the 238U series, 234Th, 214Pb, and 214Bi were the radionuclides identified. The 232Th series was identified by 228 Ac, 208Tl, 212Pb, and 212Bi.
A total of 1,048 initial radioactivity concentration measurements were performed on the 59 aqueous and 8 residue leachate samples: 944 measurements of aqueous fractions and 104 measurements of residue fractions. In the aqueous fraction measurement category, 275 (29%) of the 944 results obtained were positive determinations. For the remaining residue measurement category, 9 (9%) of the 104 results were positive determinations. A positive determination was concluded if the upper bound of the result (result and its 2cr counting uncertainty) equaled or exceeded the corresponding minimum detectable concentration reported by the laboratory for that measurement. The most prevalent radionuclides identified were 3H (57 positive determinations) and 4°K (53 positive determinations). The prevalence of the remaining radionuclides sought declined dramatically-214Pb (26), 212Pb (13), 137CsP41Am (4 each), 154Eu/235U (2 each), and 6°Co (1 ). The summary of these initial analytical results is presented in sections 3.1.1 (gross alpha), 3.1.2 (gross beta), 3.1.3 (fission/activation product family), and 3.1.4 (naturally occurring family).
3 .1.1 Gross Alpha Radioactivity Concentration The gross alpha results ranged from -7.72 to 21.1 pCi/L, with a mean activity concentration of 3.3 7 pCi/L. The corresponding gross alpha MDC’s ranged from 1.19 to 37.5 pCi/L with a mean of6.29 pCi/L (37 or 63% of the 59 results were positive determinations). The gross alpha radioactivity concentration results are displayed in Attachment A.
The precision of the duplicate sample gross alpha analyses was evaluated by determining the relative percent difference (RPD) of duplicate measurements that resulted in paired positive determination results. The RPD is equal to the positive difference of the paired positive determination results multiplied by 100 and divided by the average of the two measured values. For the 5 duplicate samples submitted for gross alpha analysis, there were 3 positive determination result pairs. The RPD calculated for these result pairs ranged from 2.5% to 17.3%, with an average RPD of 10.1%.
Residue samples were not analyzed for gross alpha radioactivity.
3 .1.2 Gross Beta Radioactivity Concentration
The gross beta results ranged from 7.25 to 564 pCi/L, with a mean activity concentration of 152 pCi/L. The corresponding gross beta MDC’s ranged from 0.751 to 26.0 pCi/L with a mean of3.48 pCi/L (all of the 59 results were positive determinations). The gross beta radioactivity concentration results are displayed in Attachment A. For the 5 duplicate samples submitted for gross beta analysis, there were 5 positive determination result pairs. The RPD calculated for these result pairs ranged from 19.6% to 59.1%, with an average RPD of37.7%.
Residue samples were not analyzed for gross beta radioactivity.
3 .1.3 Fission/ Activation Product Radionuclide Concentrations
220.127.116.11 Tritium (1H as Tritium Oxide or HTO)
The tritium results ranged from 6.86 to 94,400 pCi/L, with a mean activity concentration of 25,200 pCi/L. The corresponding tritium MDC’s ranged from 275 to 512 pCi/L with a mean of337 pCi/L (57 or 97% of the 59 results were positive determinations). The tritium concentration results are displayed in Attachment A. For the 5 duplicate samples submitted for tritium analysis, there were 5 positive determination result pairs. The RPD calculated for these result pairs ranged from 0.6% to 12.8%, with an average RPD of7.1%.
Residue samples were not analyzed for tritium.
18.104.22.168 Cobalt-60 (22co) For the aqueous samples, the 6°Co results ranged from -4.24 to 3.81 pCi/L, with a mean actlvtty concentration of -0.366 pCi/L. The corresponding 6°Co MDC’s ranged from 2.78 to 9.16 pCi/L with a mean of 6. 75 pCi/L (1 or 2% of the 59 results was a positive determination). For the 5 duplicate samples submitted for 6°Co analysis, there were no positive determination result pairs. Consequently, RPD calculations were not performed for 6°Co.
For the residue samples, the 6°Co results ranged from -2.73 to 2.87 pCi/g, with a mean actlvtty concentration of 0.303 pCi/g. The corresponding 6°Co MDC’s ranged from 4.00 to 9.83 pCi/g with a mean of 6.3 pCi/g (1 or 13% of the 8 results was a positive determination). There were no duplicate residue samples submitted for 6°Co analysis.
22.214.171.124 Cesium-137 (~ For the aqueous samples, the 137Cs results ranged from -7.91 to 4.23 pCi/L, with a mean actlvtty concentration of 0.012 pCi/L. The corresponding 137Cs MDC’s ranged from 2.93 to 7.90 pCi/L with a mean of6.29 pCi/L (4 or 7% of the 59 results were positive determinations). For the 5 duplicate samples submitted for 137Cs analysis, there were no positive determination result pairs. Consequently, RPD calculations were not performed for 137Cs.
For the residue samples, the results ranged from -3.40 to 4.54 pCi/g, with a mean activity concentration of -0.385 pCi/g. The corresponding 137Cs MDC’s ranged from 3.62 to 10.5 pCi/g with a mean of 6.23 pCi/g (1 or 13% of the 8 results was a positive determination). There were no duplicate residue samples submitted for 137Cs analysis.
126.96.36.199 Europium-154 (54Eu) For the aqueous samples, the 154Eu results ranged from -14.2 to 15.2 pCi/L, with a mean actlvtty concentration of -0.268 pCi/L. The corresponding 154Eu MDC’s ranged from 8.40 to 23.8 pCi/L with a mean of 18.0 pCi/L (2 or 3% of the 59 results were positive determinations). For the 5 duplicate samples submitted for 154Eu analysis, there were no positive determination result pairs. Consequently, RPD calculations were not performed for 154Eu.
For the residue samples, the 154Eu results ranged from -12.1 to 8.94 pCi/g, with a mean activity concentration of -1.66 pCi/g. The corresponding 154Eu MDC’s ranged from 10.9 to 29.1 pCi/g with a mean of 17.9 pCi/g (none of the 8 results was a positive determination). There were no duplicate residue samples submitted for 154Eu analysis.
188.8.131.52 Americium-241 (241Am) For the aqueous samples, the 241 Am results ranged from -44.4 to 86.9 pCi/L, with a mean actlvtty concentration of -1.60 pCi/L. The corresponding 241 Am MDC’s ranged from 9.83 to 233 pCi/L with a mean of 31.6 pCi/L ( 4 or 7% of the 59 results were positive determinations). For the 5 duplicate samples submitted for 241 Am analysis, there were no positive determination result pairs. Consequently, RPD calculations were not performed for 241 Am.
For the residue samples, the 241Am results ranged from -28.5 to 2.47 pCi/g, with a mean activity concentration of -7.02 pCi/g. The corresponding 241Am MDC’s ranged from 9.54 to 49.1 pCi/g with a mean of 25.0 pCi/g (none of the 8 results was a positive determination). There were no duplicate residue samples submitted for 241 Am analysis.
3.1.4 Naturally-Occurring Radionuclide Concentrations
184.108.40.206 Potassium-40 (‘ill.Kl
For the aqueous samples, the 4°K results ranged from 16.3 to 1,080 pCi/L, with a mean actlvtty concentration of270 pCi/L. The corresponding 4°K MDC’s ranged from 26.4 to 124 pCi/L with a mean of
66.9 pCi/L (53 or 90% of the 59 results were positive determinations). For the 5 duplicate samples submitted for 4°K analysis, there were 4 positive determination result pairs. The RPD calculated for these result pairs ranged from 2.4% to 22. 7%, with an average RPD of 14.0%.
For the residue samples, the 4°K results ranged from -55.7 to 105 pCi/g, with a mean activity concentration of 18.4 pCi/g. The corresponding 4°K MDC’s ranged from 37.5 to 201 pCi/g with a mean of 104 pCi/g (1 or 13% of the 8 results was a positive determination). There were no duplicate residue samples submitted for 4°K analysis.
220.127.116.11 Uranium-235 (235U) Decay Series For the aqueous samples, the 235U results ranged from -245 to 27.9 pCi/L, with a mean actlvtty concentration of -25.7 pCi/L. The corresponding 235U MDC’s ranged from 19.5 to 430 pCi/L with a mean of 47.7 pCi/L (2 or 3% of the 59 results were positive determinations). For the 5 duplicate samples submitted for 235U analysis, there were no positive determination result pairs. Consequently, RPD calculations were not performed for 235U.
For the residue samples, the 235U results ranged from -73.8 to 2.77 pCi/g, with a mean activity concentration of -24.3 pCi/g. The corresponding 235U MDC’s ranged from 13.3 to 72.7 pCi/g with a mean of 35.2 pCi/g (none of the 8 results was a positive determination). There were no duplicate residue samples submitted for 235U analysis.
18.104.22.168 Uranium-238 (238U) Decay Series
22.214.171.124.1 Bismuth-214 e14!ill For the aqueous samples, the 214Bi results ranged from -27.3 to 35.1 pCi/L, with a mean actlvtty concentration of2.08 pCi/L. The corresponding 214Bi MDC’s ranged from 23.0 to 62.1 pCi/L with a mean of 47.4 pCi/L ( 4 or 7% of the 59 results were positive determinations). For the 5 duplicate samples submitted for 214Bi analysis, there were no positive determination result pairs. Consequently, RPD calculations were not performed for 214Bi.
For the residue samples, the 214Bi results ranged from -18.3 to 16.8 pCi/g, with a mean activity concentration of 0.43 pCi/g. The corresponding 214Bi MDC’s ranged from 28.0 to 75.3 pCi/g with a mean of 46.4 pCi/g (none of the 8 results was a positive determination). There were no duplicate residue samples submitted for 214Bi analysis.
126.96.36.199.2 Lead-214 e14Pb)
For the aqueous samples, the 214Pb results ranged from -4.75 to 17.9 pCi/L, with a mean actlvtty
concentration of 4.53 pCi/L. The corresponding 214Pb MDC’s ranged from 6.70 to 18.1 pCi/L with a
mean of 13.5 pCi/L (27 or 46% of the 59 results were positive determinations). For the 5 duplicate
samples submitted for 214Pb analysis, there were no positive determination result pairs. Consequently,
RPD calculations were not performed for 214Pb.
For the residue samples, the 214Pb results ranged from -3.74 to 7.98 pCi/g, with a mean activity concentration of 1.25 pCi/g. The corresponding 214Pb MDC’s ranged from 5.90 to 22.5 pCi/g with a mean of 12.2 pCi/g (3 or 38% of the 8 results were positive determinations). There were no duplicate residue samples submitted for 214Pb analysis.
188.8.131.52.3 Thorium-234 e34Th) For the aqueous samples, the 234Th results ranged from -1,420 to 141 pCi!L, with a mean activity concentration of -92.1 pCi/L. The corresponding 234Th MDC’ s ranged from 92.3 to 2,500 pCi/L with a mean of 297 pCi/L (1 or 2% of the 59 results were positive determinations). For the 5 duplicate samples submitted for 234Th analysis, there were no positive determination result pairs. Consequently, RPD calculations were not performed for 234Th.
For the residue samples, the 234Th results ranged from -219 to 45.4 pCi/g, with a mean activity concentration of -94.6 pCi/g. The corresponding 234Th MDC’s ranged from 41.9 to 496 pCi/g with a mean of 202 pCi/g (none of the 8 results was a positive determination). There were no duplicate residue samples submitted for 234Th analysis.
184.108.40.206 Thorium-232 e33Th) Decay Series
220.127.116.11.1 Actinium-228 (228 Ac) 228Ac
For the aqueous samples, the results ranged from -5.68 to 47.6 pCi!L, with a mean actlvtty concentration of 4.84 pCi/L. The corresponding 228Ac MDC’s ranged from 9.41 to 29.7 pCi/L with a mean of23.5 pCi/L (8 or 14% of the 59 results were positive determinations). For the 5 duplicate samples submitted for 228 Ac analysis, there were no positive determination result pairs. Consequently, RPD calculations were not performed for 228 Ac.
For the residue samples, the results ranged from -7.46 to 12.8 pCi/g, with a mean activity concentration of 4.36 pCi/g. The corresponding 228Ac MDC’s ranged from 13.4 to 40.7 pCi/g with a mean of 23.7 pCi/g (2 or 25% of the 8 results were positive determinations). There were no duplicate residue samples submitted for 228 Ac analysis.
18.104.22.168.2 Thallium-208 eosm For the aqueous samples, the 208Tl results ranged from -4.18 to 5.04 pCi/L, with a mean actlvtty concentration of0.19 pCi/L. The corresponding 208Tl MDC’s ranged from 3.47 to 8.83 pCi/L with a mean of 6.99 pCi/L (7 or 12% of the 59 results were positive determinations). For the 5 duplicate samples submitted for 208Tl analysis, there were no positive determination result pairs. Consequently, RPD calculations were not performed for 208Tl.
For the residue samples, the 208Tl results ranged from -1.41 to 6.30 pCi/g, with a mean activity concentration of 1.96 pCi/g. The corresponding 208Tl MDC’s ranged from 3.35 to 12.4 pCi/g with a mean of 6.42 pCi/g (3 or 38% of the 8 results were positive determinations). There were no duplicate residue samples submitted for 208Tl analysis.
22.214.171.124.3 Bismuth-212 (212.lli} For the aqueous samples, the 212Bi results ranged from -46.5 to 76.0 pCi/L, with a mean actlvtty concentration of 10.1 pCi/L. The corresponding 212Bi MDC’s ranged from 38.2 to 127 pCi/L with a mean of 87.6 pCi/L (7 or 12% of the 59 results were positive determinations). For the 5 duplicate samples submitted for 241 Am analysis, there were no positive determination result pairs. Consequently, RPD calculations were not performed for 212Bi.
For the residue samples, the 212Bi results ranged from -17.0 to 42.0 pCi/g, with a mean activity concentration of 12.7 pCi/g. The corresponding 212Bi MDC’s ranged from 50.2 to 146 pCi/g with a mean of 86.0 pCi/g (none of the 8 results was a positive determination). There were no duplicate residue samples submitted for 212Bi analysis.
126.96.36.199.4 Lead-212 e12Pb)
For the aqueous samples, the 212Pb results ranged from -9.34 to 13.3 pCi/L, with a mean actlvtty
concentration of 2.33 pCi/L. The corresponding 212Pb MDC’s ranged from 5.97 to 43.4 pCi/L with a
mean of 12.3 pCi/L (13 or 22% of the 59 results were positive determinations). For the 5 duplicate
samples submitted for 212Pb analysis, there were no positive determination result pairs. Consequently,
RPD calculations were not performed for 212Pb.
For the residue samples, the 212Pb results ranged from -12.6 to 1.88 pCi/g, with a mean actlvtty concentration of -2.25 pCi/g. The corresponding 212Pb MDC’s ranged from 5.02 to 19.8 pCi/g with a mean of 10.2 pCi/g (none of the 8 results was a positive determination). There were no duplicate residue samples submitted for 212Pb analysis.
3.2 Follow-On Measurements Phase
Because 21 1 of the initial 3 7 positive determinations for gross alpha radioactivity concentration exceeded 5 pCi/L (a US EPA drinking water ARAR; refer to section 188.8.131.52), those samples were selected for additional analyses to identify total uranium content, 226Ra, and 228Ra activity concentrations. By doing so, the initial gross alpha measurement results could possibly be reconciled with the contribution of the alpha-emitting progeny of the natural uranium (238U) and thorium e32Th) decay series in the samples. The selected landfill samples, by SAPID, were: l, 4, 6, 12, 15, 16, 42, 44, 45, 46, 64, 68, 71, 72, 73, 75, 81, 95, and 96. The follow-on measurement results are summarized below.
[The Commonwealth is planning to conduct a subsequent seasonal round of tritium sampling at the landfills included in this report during the fall of 2005.]
3.2.1 Total Uranium The total uranium results ranged from 0.00 to 2.50 microgram/liter (1-Jg/L), with a mean mass concentration of 0.53 1-Jg/L. The total uranium MDC was 0.200 !Jg/L for all analyses, making ll or 58% of the 19 results positive determinations. With a single exception, the positive determinations were for landfills located in the southeast, northeast, south central geographic regions of the Commonwealth. Using an assumed mass-to-activity conversion factor of 0.67 pCi/!Jg total uranium2, the activity.equivalent total uranium results ranged from 0.00 to 1.68 pCi/L, with a mean activity concentration of
1 Only 19 of the 21 samples identified for follow-on analysis were measured because one of the samples was a duplicate and the other (SAP ID 18) was inadvertently disposed by the laboratory after the initial measurements phase.
2 For reporting purposes, mass concentration results may be converted to activity concentration assuming a specific activity of 0.67 pCi total U alpha/j..lg total U. This conversion factor presupposes however that the natural relative abundance of 234U to 238U in these samples reflects secular equilibrium and equal solubility conditions, i.e., 1:1
(0.336 pCi/j..lg 238U). The State of California and the USEPA have suggested other mass-to-activity conversion
factors (0.79 pCi/j..lg and 1.3 pCi/j..lg, respectively) reflecting higher relative abundances of 234U to 238U. The mass
of uranium in water is largely determined by 238U, due to its longer half-life, while the total activity in the water is
determined by the activity of all uranium isotopes. In natural water, the 234U is slightly more soluble and the
activity ratio of 234U to 238U varies from 1:1 to more than 20: l. Consequently, accurate conversion from mass to
activity or vice versa requires knowledge of the concentration of each of the three uranium isotopes.
3.2.2 Radium-226 e26Ra)
The 226Ra results ranged from 0.18 to 24.20 pCi/L, with a mean activity concentration of3.46 pCi/L. The
corresponding 226Ra MDC’s ranged from 0.15 to 0.90 pCi/L with a mean of0.62 pCi/L (18 or 95% of the
19 results were positive determinations).
3.2.3 Radium-228 e28Ra)
The 228Ra results ranged from 0.71 to 41.95 pCi/L, with a mean activity concentration of 5.40 pCi/L. The
corresponding 228Ra MDC’s ranged from 0.79 to 3.03 pCi/L with a mean of 1.23 pCi/L (all of the 19
results were positive determinations).
Any conclusions about the leachate results are subject to the following principal limitations:
The sampling campaign was performed as a single grab sample composite of raw leachate at each LF. Temporal compositing would provide a sample which would be representative of changes in leachate quality due to seasonal and operational influences.
…. No LF-specific environmental control (precipitation, groundwater, surface water) samples were planned to be obtained as part of the sampling campaign. Consequently, it was not possible to establish a concurrent baseline against which these leachate results may be compared Nearly across the board, the LF leachate sample matrix obtained was a complex one with high amounts of dissolved and suspended solids. While this matrix did not adversely affect the quality of results obtained by liquid scintillation counting (tritium) and alpha/gamma spectrometry, it did pose difficulties for the gross alpha and beta determinations. Consequently, interpretation of the gross alpha and beta activity concentration results is considered useful only for relative (inter.sample) comparisons.
Despite these fundamental limitations, it is possible to interpret some of the results in a meaningful manner. With the exception of tritium and a single set of radium/total uranium analyses, all the leachate results support a finding that radioactive material is not present in concentrations sufficient to warrant further investigation. This does not rule-out that radionuclides other than tritium are not present in LF solid wastes; rather, their absence in this sampling campaign could also be attributed to insufficient partitioning of other waste radionuclides to the leachate phase. Specific areas of analytical interest are discussed below.
4.1.1 Uranium and Thorium The follow-on analyses of samples exceeding about 5 pCi/L gross alpha radioactivity concentration revealed the presence of uranium and thorium decay series nuclides. This is not unexpected because of the way landfills are operated with native soil being used as cover. With the exception of a single landfill (SAP ID 42), all the uranium and thorium results are considered to be typical of water that has been in contact with soil. The results for SAP ID 42 e28Ra, 226Ra, and Total Uranium at 42, 24, and 2 pCi/L respectively) are far above any concentrations considered typical and may be evidence that burials of solid waste enriched in these nuclides has and/or continues to occur. Such burials may include technologically-enhanced naturally-occurring radioactive material (TENORM) e.g., foundry sand or bricks, coal-powered power plant ash, stack flyash and/or stack scrubber residue. The PA DEP is investigating possible scenarios for discharge and dilution of leachate from the SAP ID 42 facility (the dilution is 110:1 at the point of discharge). This investigation did not evaluate the possible buildup in
POTW solids, or fractional release ofU/Th to the Susquehanna River after POTW filtration.
When companng the data produced by the follow-on analyses with the corresponding gross alpha radioactivity concentrations reported during the initial analysis phase, a reliable relationship between the two is not apparent. The ratios of the summed 228RaF6Ra/Total Uranium results to the corresponding
gross alpha results are inconsistent, ranging from 0.1 to 4 (8 of the 19 ratios exceeded 1). This is an unexpected observation that could be rooted in (1) the complex leachate matrix and the radioanalytical challenges it presents, as well as (2) radioactive disequilibrium or solubility phenomena invalidating the total uranium conversion factor. Nonetheless, this observation hints that gross alpha measurements of leachate may not be the most suitable indicator of ARAR compliance.
As presented earlier, positive determinations for tritium were observed in 57 (97%) of the 59 samples analyzed. The corresponding tritium MDC range was 275 to 512 pCi/L, with a mean of 337 pCi/L. The 59-sample range was 7 to 94,400 pCi/L, with a mean activity concentration of 25,200 pCi/e [31 (53%) of the 59 sample results exceeded 20,000 pCi/L, a limit discussed in section 184.108.40.206]. Despite the fact that tritium has ubiquitous environmental presence4, most of the observed leachate tritium concentrations exceed typical environmental concentrations that are generally below an MDC of 200 pCi/L in surface water and precipitation samples. Possible sources of this leachate tritium include NRC “generally licensed” gaseous tritium light source (GTLS) devices that are unused and no longer needed or wanted (“disused sources”) that are unknowingly disposed as a solid waste. It is a common occurrence for disused GTSL to be accidentally disposed in landfills. Most notable among these devices are GTLS
3 Tritium assay at the very low levels in the enviromnent is often given in tritium units (TU), an absolute concentration requiring no reference standard. One TU represents a tritium/hydrogen atom ratio of 10·18 ; in water of 1 TU, the specific activity is equal to 3.2 pCi/L. For comparison, groundwater seldom has more than 50 TU (160 pCi/L) and is typically in the <1 to 10 TU (<3 to 32 pCi!L) range. 4 Tritium is produced naturally in the upper atmosphere by cosmic ray interaction with 14N in air. Tritium is also produced artificially during nuclear weapons explosions, as a byproduct in nuclear power production, and in defense production reactors via neutron activation of 6Li. In the atmosphere, tritium exists in low concentrations in three different chemical forms: hydrogen (HT), water vapor (HTO) and hydrocarbons (CH3T). The steady-state global inventory is approximately 2.65 kilograms. By comparison, total U.S. tritimn production since 1955 has been approximately 225 kilograms, an estimated 150 kilograms of which have decayed into helium-3, leaving a current (1996) artificial inventory ofapproximately 75 kilograms. 22 WLLFOIA4312-001 -0023377 emergency 'EXIT' signs that are used to satisfy the National Fire Protection Association (NFPA) Life Safety Code 101 mandate for illuminated exit markers. For more information on the disused source problem, see the Product Stewardship Institutes' (PSI) background GTLS 'EXIT' sign dimensions are nominally 13 x 8 x 1 inches and employ several sealed borosilicate glass tubes arranged to form the word 'EXIT.' The tubes are positioned in parabolic channels of a backing material that also serves as a reflector. Each tube is coated on the inside with a thin layer of a phosphor (e.g. zinc sulfide) and filled with up to 25 curies (Ci) of tritium gas. The typical amount is 10 Ci or 10,000,000,000,000 pCi. From a regulatory perspective, each GTLS sign manufacturer holds a 10 CFR 31.5 general license to load tritium per 10 CFR 32.51 in order to market GTLS signs for commercial use. Each purchaser is assigned to the manufacturer's general license at the time of sale and cannot transfer, resell, dispose or dismantle the sign. GTLS labeling is typically small and inconspicuous, thus not readily alerting the sign's owner to it's radioactive contents. Further, there is often insufficient financial incentive offered to end users to prompt return of a disused GTLS. However, the recent initiative prompts many manufacturers of GTLS exit signs and nuclear fixed gauges to take back their products at the end of the products' useful life. It should be noted that the quantity of tritium in a GTLS 'EXIT' sign is significant and can be readily detected when GTLS tubes are broken, releasing tritium gas that eventually oxidizes as a vapor and condenses as tritiated water. In fact, the tritium gas released from building signs and aircraft instruments destroyed at the former was readily detected in air samples. Laboratory experiments have that the conversion of tritium gas eH2) to tritiated water eH20 or HTO) is a first-order reaction (a linear function of the concentration) at low (<10 Ci/m3) and high (>104 Ci/m3) 3H2 concentrations and follows the equation:
where N is the fraction as 3H2 and A is the total conversion rate constant. At intermediate 3H2 concentrations, the conversion proceeds through a second-order reaction. The oxidation of 3H2 is controlled by the ions generated by radioactive decay that combine with atmospheric oxygen to form tritiated water. Some of the oxidation reaction rates reported are: 0.03%/day (dry air, no metal surfaces), 0.06% (photochemical reaction), 0.1 %/day (isotopic exchange with moisture in air, no metal surfaces), 20%/min (soil with 32% water content), and 5%/min (soil with 28% water content). More information about the environmental fate of tritium is available elsewhere9 . It is apparent, then, that the conversion of tritium gas released from broken GTLS tubes into tritiated water under compacted landfill cover would proceed relatively rapidly in the presence of moisture.
4.1.3 Applicable or Relevant and Appropriate Requirements Standard of Consideration
The introduction of above-normal concentrations of tritium to the environment from leachate effluent may have regulatory implications that are best understood in the context of applicable or relevant and appropriate requirement (ARAR) standards for radioactive effluents. Both the NRC and the EPA have promulgated ARARs for tritium in liquid effluents. The NRC’s effluent apply to licensed operations and are contained in Appendix B to 10 CFR Part 20, Annual Limits on Intake (AL!s) and Derived Air Concentrations (DACs) of Radionuclides for Occupational Exposure; Ejjluent
Concentrations; Concentrations for Release to Sewerage. Additionally,
Numerical Guides for Design Objectives and Limiting Conditions for Operation to Meet the Criterion ”As Low as is Reasonably Achievable” for Radioactive Material in Light-Water-Cooled Nuclear Power Reactor Ejjluents, establishes nuclear power plant design objectives and operational constraints to ensure radioactive effluent releases result in human exposures that are As Low As Reasonably Achievable (ALARA). Because Appendix I does not establish a limit per se, but rather effluent levels above which power reactor licensee ALARA evaluations are triggered, it is not considered an ARAR limit for landfill leachate.
The EPA the annual average concentration of tritium in drinking water under authority of the National Primary Drinking Water Regulations (NPDWR; 40 CFR 141). The EPA has also limited the
fuel cycle, this regulation is not considered an ARAR for landfill leachate). The NRC and EPA limitations and possible inferences prompted by the leachate results are discussed below.
220.127.116.11 NRC Limitations
9 “Overview of Tritium: Characteristics, Sources, and Problems” by S. Okada and N. Momoshima in Health Physics 65(6):595-609; 1993.
In Subpart K of 10 CFR 20, the NRC authorizes licensees to dispose of licensed material in effluents ,==~~=::::LI and to sanitary sewers within nuclide-specific effluent concentration limitations. The effluent concentration limits were established to ensure that the total effective dose equivalent (TEDE) to individual members of the public from all licensed operation radiation sources does not exceed 100 mrem (l mSv) in a year To accomplish this objective, the NRC derived annual average liquid effluent concentration (e.g., l x 106 pCi/L as 3H) corresponding to a ‘Reference Man’ of 50 mrem/year. In contrast, the monthly average concentration sanitary sewer
(e.g., l x 107 pCi/L as 3H) were derived to correspond to a ‘Reference Man’ committed effective dose equivalent of 500 mrem. It is notable that §20.l30l(a)(l) specifically excludes dose contributions attributed to radionuclides in sanitary sewer discharges from licensee compliance demonstrations with the 100 mrem/year public TEDE limit. The practice of radionuclide disposal by
Released materials are readily soluble (or dispersible biological material).
Quantity of material released in month, divided by the average monthly volume of water released
into the sewer by the licensee, does not exceed the Appendix B, Table 3 monthly average sewer
concentration (e.g., l x 107 pCi/L as 3H).
Total annual quantity of radioactive material released into sanitary sewerage does not exceed 5 Ci
of 3H, l Ci of 14C, and l Ci of all other radioactive material combined.
All of the leachate tritium activity concentrations measured by this sampling campaign are below the NRC effluent and sewer concentrations limits discussed above, assuming those grab sample results are indicative of actual average monthly concentrations. As a conservative evaluation, if the observed highest leachate tritium activity concentration (94,400 pCi/L) persisted as a sanitary sewerage discharge over the course of a year, the total leachate volume released would have to approach 14 million gallons before the §20.2003 5 Ci limitation would be of concern.
18.104.22.168 US EPA Limitations
In a final rulemaking for Subpart G of the NPDWR (40 CFR 141) in 2000, the EPA established maximum CWS MCL indirectly limits the beta particle and photon radioactivity in drinking water to annual average concentration not to exceed an annual dose equivalent to the total body or any internal organ of 4 mrem/year. For all radionuclides except 3H and 90Sr, conversion of activity concentration to dose equivalent must be performed assuming a drinking water ingestion rate of 2 L/day and the National Bureau of Standards (NBS) Handbook 69 (published 1959 and amended 1963; also referred to as NCRP Report 22) compilation of maximum permissible concentrations (MPCs) in water.
tritium in drinking water that was assumed to produce a total body or organ dose of 4 mrem/year, the MCL. The concentrations for these contaminants were derived from a historical dosimetry model (ICRP Publication 2) used at the time the Subpart G rule was promulgated in 1976. When these risks are calculated in accordance with the latest dosimetry models described in Federal Guidance Report 13
, the risks associated with these concentrations, while varying considerably, generally fall within the EPA’s current risk target range for drinking water contaminants of 10-4 to 10·6 . Accordingly, the EPA did not change the MCL for beta particle and photon radioactivity during its final rulemaking in 2000. Using contemporary ICRP Publication 30 dosimetry, the concentration of tritium needed to deliver the MCL 4 mrem m one year is approximately 86,000 pCi/L, over four times the concentration in the current NPDWS.
Thirty-one (53%) of the 59 leachate tritium activity concentrations measured by this sampling campaign are above 20,000 pCi/L, the EPA NPDWS assumed to equal the 4 mrem/year MCL. The highest measured tritium activity concentration exceeds the MCL by a factor of 4.7. It is apparent, then, that a potential exists for CWS to be adversely affected if the CWS influent is developed within the treated leachate ‘watershed.’ However, the scope of the leachate sampling campaign does not permit a determination of which, if any, CWS are vulnerable under the NPDWS and the implications for CWS
distribution point radionuclide monitoring frequency pursuant to ~~=~and ;:L!_~=~· These considerations should be pursued as a separate initiative.
1°Community water systems are privately-or publicly-owned and provide water for human consumption through pipes or other constructed conveyances to at least 15 service connections or serve an average of at least 25 people year-round.
11 =~=’-‘-‘-‘==~~====~=~=~=~=w…..o;;:>:>t;u April 7, 2005.
22.214.171.124 Dilution Factors
DEP BRP conducted interviews with landfill operators and DEP personnel to determine the approximate dilution that occurs at the initial point of leachate discharge from the landfill site. The discharge locations vary according to the EPA permit issued. The information gathered represents the average leachate effluent flow, compared to the average Publicly Owned Treatment Works influent or the low-flow Q7,1 0 (“7-day, 10-year low flow”; the average minimum stream flow expected for seven consecutive days once every ten years.) data12 for leachate released to a stream or river. These ratios are considered the dilution factor for leachate. Of the 29 landfills with leachate samples indicating >20,000 pCi/L tritium, 18 were queried with regard to dilution factors. The dilution factors ranged from 1.4 to 546, with resulting concentrations of tritium being less than 20,000 pCi/L. The results of the interviews conducted indicate that at the point of discharge, landfill leachate is adequately diluted to reduce tritium concentrations to below the Maximum Contaminant Levels required by the National Primary Drinking Water Regulations (see section4.l.3.2 above).
12 Low-flow statistics for Pennsylvania streams developed by the U.S. Geological Survey, Water Resources Division, New Cumberland, Pa. . ~~~=~~”-=~=~~=”‘.
Radioactivity Concentration Data Displays
Leachate Tritium Concentration
1 3 4 56 11 12131515161718383940 41424344444546 47484950515456595960646566676869707172727374757677787980 8190 9191929495 96
Leachate Gross Alpha Radioactivity Concentration
Leachate Gross Beta Radioactivity Concentration
Analytical Data Summary
Leachate Aqueous Analytical Results (pCi/L) Bold results exceed the corresponding MDC.
Gross a Gross 13 Tritium
SAPID Sample Date Result 2cr Unc. MDC Result 2cr Unc. MDC Result 2cr Unc. MDC
1 27-0ct-04 4.22E+OO 2.59E+OO 3.79E+OO 7.46E+01 1.40E+01 2.09E+OO 2.82E+02 1.98E+02 3.09E+02
3 2-Nov-04 1.45E+01 2.22E+01 3.75E+01 5.57E+02 1.05E+02 2.60E+01 9.35E+04 1.23E+04 5.12E+02
4 28-0ct-04 1.25E+OO 2.90E+OO 5.02E+OO 1.05E+02 1.95E+01 2.68E+OO 1.12E+04 1.56E+03 3.08E+02
5 16-Nov-04 -6.40E-01 1.35E+OO 2.50E+OO 9.37E+01 1.73E+01 1.27E+OO 3.92E+04 5.17E+03 3.29E+02
6 2-Nov-04 7.77E+OO 2.34E+OO 2.22E+OO 1.37E+02 2.53E+01 1.15E+OO 3.17E+04 4.21E+03 3.80E+02
11 2-Nov-04 -1.24E+OO 9.85E+OO 1.78E+01 3.09E+02 5.77E+01 1.03E+01 2.78E+04 3.71E+03 4.17E+02
12 28-0ct-04 8.28E+OO 6.78E+OO 1.06E+01 2.71E+02 5.04E+01 6.32E+OO 4.44E+04 5.84E+03 4.23E+02
13 8-Nov-04 3.27E+OO 1.59E+OO 2.33E+OO 9.73E+01 1.80E+01 9.10E-01 1.91E+04 2.58E+03 3.30E+02
15 8-Nov-04 4.94E+OO 3.99E+OO 6.29E+OO 1.53E+02 2.84E+01 3.27E+OO 9.44E+04 1.23E+04 4.96E+02
15 8-Nov-04 7.28E-01 3.82E+OO 6.71E+OO 2.77E+02 5.10E+01 2.78E+OO 8.39E+04 1.09E+04 4.50E+02
16 28-0ct-04 1.22E+01 5.57E+OO 7.73E+OO 1.45E+02 2.71E+01 3.27E+OO 5.67E+04 7.43E+03 4.23E+02
17 2-Nov-04 1.21E+OO 1.18E+OO 2.03E+OO 1.03E+02 1.90E+01 1.25E+OO 2.38E+04 3.18E+03 2.77E+02
18 20-0ct-04 5.85E+OO 4.55E+OO 7.06E+OO 1.80E+02 3.34E+01 3.74E+OO 5.43E+04 7.11E+03 2.96E+02
38 18-0ct-04 O.OOE+OO 3.12E+OO 6.05E+OO 7.53E+01 1.43E+01 3.23E+OO 3.18E+04 4.22E+03 3.06E+02
39 2-Nov-04 3.26E+OO 8.11E+OO 1.40E+01 2.42E+02 4.52E+01 7.76E+OO 5.60E+04 7.33E+03 3.06E+02
40 19-0ct-04 3.26E+OO 1.44E+OO 1.88E+OO 6.11E+01 1.13E+01 1.16E+OO 9.77E+03 1.38E+03 2.78E+02
41 4-Nov-04 2.59E+OO 1.41E+OO 2.05E+OO 1.38E+02 2.54E+01 1.14E+OO 2.30E+03 4.75E+02 3.85E+02
42 1-Nov-04 1.85E+01 8.97E+OO 1.25E+01 5.64E+02 1.04E+02 6.53E+OO 6.41E+03 9.46E+02 2.80E+02
43 20-0ct-04 1.56E+OO 1.26E+OO 2.05E+OO 1.43E+02 2.63E+01 1.05E+OO 3.09E+04 4.09E+03 2.82E+02
44 3-Nov-04 9.23E+OO 3.63E+OO 4.52E+OO 4.34E+01 8.50E+OO 3.26E+OO 1.98E+02 1.89E+02 3.07E+02
44 3-Nov-04 7.76E+OO 3.53E+OO 4.79E+OO 5.30E+01 1.01E+01 2.76E+OO 2.25E+02 1.90E+02 3.04E+02
45 1-Nov-04 2.11E+01 6.05E+OO 5.51E+OO 1.74E+02 3.23E+01 3.85E+OO 2.93E+04 3.89E+03 3.08E+02
46 1-Nov-04 1.55E+01 7.58E+OO 1.02E+01 2.08E+02 3.88E+01 6.57E+OO 2.59E+04 3.46E+03 4.01E+02
47 1-Nov-04 1.46E+OO 7.11E+OO 1.25E+01 2.84E+02 5.26E+01 6.36E+OO 2.98E+04 3.96E+03 3.80E+02
48 2-Nov-04 -7.72E+OO 5.29E+OO 1.02E+01 1.26E+02 2.36E+01 4.54E+OO 1.65E+04 2.24E+03 3.02E+02
49 2-Nov-04 1.16E+OO 7.60E+OO 1.34E+01 3.92E+02 7.24E+01 5.56E+OO 2.36E+04 3.16E+03 2.77E+02
50 3-Nov-04 2.43E+OO 1.66E+OO 2.68E+OO 1.77E+02 3.27E+01 1.05E+OO 8.75E+04 1.14E+04 3.80E+02
51 2-Nov-04 2.50E+OO 1.75E+OO 2.82E+OO 4.63E+01 8.72E+OO 1.50E+OO 6.07E+03 9.01E+02 2.80E+02
54 15-Nov-04 1.40E+OO 1.66E+OO 3.01E+OO 5.71E+01 1.07E+01 1.64E+OO 3.68E+04 4.86E+03 3.28E+02
56 16-Nov-04 -4.22E+OO 3.52E+OO 6.71E+OO 1.83E+02 3.39E+01 2.78E+OO 6.70E+03 9.87E+02 3.27E+02
59 15-Nov-04 -4.85E+OO 2.25E+OO 4.40E+OO 1.24E+02 2.29E+01 2.01E+OO 2.30E+04 3.09E+03 3.35E+02
59 15-Nov-04 4.85E-01 2.37E+OO 4.17E+OO 2.28E+02 4.20E+01 1.85E+OO 2.46E+04 3.28E+03 3.29E+02
60 16-Nov-04 -3.49E+OO 3.20E+OO 5.86E+OO 1.01E+02 1.87E+01 2.08E+OO 2.62E+04 3.49E+03 3.30E+02
64 8-Nov-04 5.61E+OO 2.10E+OO 2.44E+OO 3.77E+01 7.08E+OO 1.36E+OO 2.12E+04 2.85E+03 3.28E+02
65 9-Nov-04 2.97E+OO 1.55E+OO 2.25E+OO 1.24E+02 2.29E+01 1.22E+OO 6.37E+04 8.32E+03 3.84E+02
66 10-Nov-04 -2.62E+OO 2.40E+OO 4.39E+OO 9.00E+01 1.66E+01 1.56E+OO 1.09E+04 1.53E+03 3.31E+02
67 10-Nov-04 3.43E+OO 1.28E+OO 1.48E+OO 7.25E+OO 1.50E+OO 8.22E-01 3.58E+03 5.92E+02 3.30E+02
68 16-Nov-04 2.91E+OO 2.04E+OO 3.14E+OO 1.05E+02 1.93E+01 1.64E+OO 5.85E+02 2.39E+02 3.32E+02
69 22-Nov-04 -9.68E-01 2.25E+OO 4.16E+OO 1.00E+02 1.19E+02 1.84E+OO 1.97E+04 2.65E+03 3.27E+02
70 1-Nov-04 1.92E+OO 1.36E+OO 2.20E+OO 8.85E+01 1.64E+01 1.13E+OO 2.99E+03 5.09E+02 2.78E+02
71 2-Nov-04 2.88E+OO 2.17E+OO 3.47E+OO 2.39E+01 4.83E+OO 2.36E+OO 3.41E+03 5.66E+02 3.04E+02
72 2-Nov-04 3.98E+OO 1.73E+OO 2.30E+OO 1.66E+02 3.03E+01 1.19E+OO 4.96E+04 6.51E+03 3.82E+02
72 2-Nov-04 3.88E+OO 1.63E+OO 2.06E+OO 1.20E+02 2.22E+01 1.16E+OO 4.93E+04 6.47E+03 3.75E+02
73 8-Nov-04 1.24E+01 6.26E+OO 8.63E+OO 4.88E+02 8.99E+01 5.29E+OO 4.54E+01 1.58E+02 2.79E+02
74 18-0ct-04 1.96E+OO 2.58E+OO 4.30E+OO 4.40E+01 8.51E+OO 2.75E+OO 1.29E+04 1.78E+03 3.07E+02
75 10-Nov-04 5.16E+OO 1.90E+OO 2.23E+OO 8.85E+01 1.64E+01 1.15E+OO 3.75E+04 4.95E+03 2.75E+02
76 19-Nov-04 2.04E+OO 2.51E+OO 4.17E+OO 4.43E+01 8.38E+OO 2.12E+OO 6.86E+OO 1.86E+02 3.32E+02
77 15-Nov-04 2.16E+OO 1.08E+OO 1.52E+OO 1.45E+01 2.80E+OO 7.51E-01 3.74E+03 6.11E+02 3.26E+02
78 18-0ct-04 -2.86E+OO 5.96E+OO 1.13E+01 2.71E+02 5.05E+01 6.43E+OO 2.13E+04 2.87E+03 4.08E+02
79 15-Nov-04 -5.24E