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Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION OF BUILDING MATERIALS: UNDERSTANDING REMOVAL MECHANISMS AND WASTE PRODUCTION DURING URBAN RADIOLOGICAL RECOVERY W ILLIAM JOLIN 1 , MATTHEW MAGNUSON 2 , AND MICHAEL KAMINSKI 1 1 ARGONNE NATIONAL LABORATORY 2 USEPA HOMELAND SECURITY RESEARCH CENTER MAY 9 TH , 2018

HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

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Page 1: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

Argonne National Laboratory is a U.S. Department of Energy

laboratory managed by UChicago Argonne, LLC.

HIGH PRESSURE

DECONTAMINATION OF BUILDING

MATERIALS: UNDERSTANDING

REMOVAL MECHANISMS AND WASTE

PRODUCTION DURING URBAN

RADIOLOGICAL RECOVERY

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WILLIAM JOLIN1, MATTHEW MAGNUSON2, AND MICHAEL KAMINSKI1

1ARGONNE NATIONAL LABORATORY

2USEPA HOMELAND SECURITY RESEARCH CENTER

MAY 9TH, 2018

Page 2: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

ACKNOWLEDGEMENTS

Argonne

– Mike Kaminski

– Nico Santiago

– Katherine Helper

– Chris Oster

EPA Homeland Security

– Matthew Magnuson

2

Disclaimer: The U.S. Environmental Protection Agency, through its Office of Research and Development, funded

and collaborated in the research described here under Interagency Agreement 92380201 with Argonne National

Laboratory. This document was reviewed in accordance with EPA policy prior to publication. Note that approval for

publication does not signify that the contents necessarily reflect the views of the Agency. Mention of trade names

or commercial products does not constitute endorsement or recommendation for use of a specific product.

Page 3: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

INTRODUCTION

Reduce dose to first responders

Reopen critical infrastructure:

– Response vehicles

– Roadways

– Hospitals

– Airports

Need readily available methods

Guidance documents

Rapid wide area decontamination

Kyodo/Reuters3

Page 4: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

HIGH PRESSURE DECONTAMINATION (HPD) EXPERIMENTAL CHAMBER

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Page 5: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

HPD CHAMBER OPERATION

5

Removals from:

– Chemical: ion

exchange, dissolution

– Physical: surface

ablation

We can control:

– Movement speed

– Coupon type

– Nozzle angle

– Wand length

– Different solutions

– System angle

– Number of passes

– Offset angles

CHEM/BIO also possible

Page 6: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

RADIONUCLIDE APPLICATION Coupons spiked with solution containing:

– Cs-137: strong interaction with minerals

– Sr-85 (Sr-90): somewhat insoluble

– Eu-152 (other lanthanides, Am-241):

insoluble, strong interactions

Aged for 24 hours or 8 days open to the

atmosphere (humidity low and monitored)

Depth profile determined by grinding on

sand paper

Mass removed used to create depth

profiles:

6

𝑓𝑎𝑐𝑡,𝑖 =𝐶𝑃𝑀𝑖

൘σ𝐶𝑃𝑀

𝑓𝑟𝑒𝑚𝑜𝑣𝑒𝑑

Page 7: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

RADIONUCLIDE PENETRATION

Penetration of all radionuclides followed:

– Brick > Concrete > Asphalt

– From this we can already establish which

surfaces to HPD

Brick: Sr > Eu ≥ Cs

– Sorption dependent

Concrete: Sr > Cs > Eu

– Sorption/precipitation dependent

Asphalt: Sr ≈ Cs ≈ Eu

24 hours after deposition

7

Asphalt

Brick

Concrete

Page 8: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

RADIONUCLIDE PENETRATION

8

Brick

Concrete24 hours 1 week later

Page 9: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

RADIONUCLIDE PENETRATION

Penetration again followed:

– Brick > Concrete > Asphalt

Brick: Eu penetrates deeper

Concrete: No obvious change

Asphalt: Cs and Sr penetrate deeper

1 week later: conclusions

9

Asphalt

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HIGH PRESSURE REMOVALS

HPD was performed after 24 hours of aging

First we looked at concrete coupons with various speeds through the spray path

Removals from concrete decreased and become less precise with increased

speed through the spray path

Speed through spray path

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Page 11: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

HIGH PRESSURE REMOVALS

HPD was performed after 24 hours of aging

Removals was generally dependent on penetration distance and coupon “strength”

Exception: High removals of Sr-85 from asphalt

Different surfaces types

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Page 12: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

REMOVAL MECHANISMS

Coupons were dried and

weighed after HPD

Depth removed was

determined and compared the

to depths corresponding to

removals of each radionuclide

Concrete removals beyond

ablation were attributed to the

loss of light, small grains of

sand or cement binder

Comparing mass removed and radionuclide removal

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Depth removed from

ablation

Depths corresponding

to nuclide removal

Page 13: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

REMOVAL MECHANISMS Various speeds

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25 mm/s

5 mm/s 125 mm/s

Page 14: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

REMOVAL MECHANISMS

For brick and asphalt additional chemical removal of strontium is evident

Cesium and europium could either be small grain ablation or chemical removal

Brick & Asphalt

14

BrickAsphalt

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WHAT’S LEFT?

Grind profile in decontaminated concrete coupons

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Coupons were allowed to sit on a

benchtop for 1 week after

decontamination

Profiles were created incorporating

removals of radionuclides and depth

ablated

If the profiles are similar to non

decontaminated coupons: surface

ablation dominant removal mechanism

Differences indicate chemical

removals or other processes are

involved

Important for “Final Decontamination”

Original

Surface Surface after

decontamination

Page 16: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

GRIND PROFILE IN DECONTAMINATED COUPONSConcrete coupons with varied contact time

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No decon – 8

day aging

125 mm/s25 mm/s

5 mm/s

Page 17: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

DEPTH PROFILE IN DECONTAMINATED COUPONSBrick & Asphalt

17

Brick

Asphalt

No decon

No decon HPD

HPD

Page 18: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

COMPARING RADIONUCLIDE FRACTIONATION IN WASTEWATER Treatment possibilities are determined by fractionation

Fractionation can be caused by either removal mechanism or speciation after

removal

Strontium is dissolved in the waste: chemical removal and dissolution

Cesium and europium are attached to particulate: ablation and sorption

Cesium percentages change with speed: more chemical removal or less particle

production

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Fraction of each radionuclide attached to particles larger than 0.2 µm

Page 19: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

CONCLUSIONS AND FUTURE DIRECTIONS

Removal mechanisms help establish a plan of attack: “bang for your dose”

Cesium and europium generally require ablation; strontium may only need to

be “washed”

Too fast of washing may lead to residuals left in surfaces

Conclusions and Impact

Future Directions

Radioactive particulates

Sequestering dissolved strontium: soils and minerals

Temperatures and salt content

Continue to study the effects of lower and higher pressures

Correlate those pressures for those capable with specialty

ultra high pressure systems, off the shelf pressure washers,

and in street sweepers.

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WHAT ABOUT ALL THAT WATER?

(Jolin and Kaminski 2016)20

Page 21: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

DEVELOPMENT OF FAR-FIELD FALLOUT SURROGATES

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Minimal leaching into solutions

Silicate radiolabeling method

Page 22: HIGH PRESSURE DECONTAMINATION OF BUILDING : U€¦ · Argonne National Laboratory is a U.S. Department of Energy laboratory managed by UChicago Argonne, LLC. HIGH PRESSURE DECONTAMINATION

REFERENCES Jolin, W. C. and M. Kaminski (2016). "Sorbent materials for rapid remediation of

wash water during radiological event relief." Chemosphere 162: 165-171.

Kaminski, Michael,,Kivenas, Nadia, Oster, Chris, Jolin, Will, Hepler, Katherine,

and Magnuson, Matthew (2017) “Integrated Wash-Aid, Treatment, and

Emergency Reuse System (IWATERS) for Strontium Contaminations,” Paper

17390, Waste Management Symposia 2017, Phoenix, AZ,

.

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