CRESP Consortium for Risk Evaluation with Stakeholder Participation

Projects > Tank Waste Treatment

Tank Waste Treatment

CRESP performs research, strategic assessment and reviews with the goal of developing tools and techniques that enhance the performance and safety of engineered and institutional features of:

  • Waste treatment
  • Containment
  • Tank waste closure
  • Storage and land disposal systems for disposition of radioactive waste, used nuclear fuel and special nuclear materials
  • Land disposal systems

Projects focus on the disposition of radioactive wastes, used nuclear fuel and special nuclear materials.

Lead Researchers

David Kosson, CRESP Principal Investigator, Vanderbilt University
Kevin Brown, Vanderbilt University
Andrew C. Garrabrants, Vanderbilt University
Martha Grover, Georgia Institute of Technology
Kimberly L. Jones, Howard University
Steven L. Krahn, Vanderbilt University
Kathryn Higley, Oregon State University
Hans Meeussen, Nuclear Research and Consultancy Group (NRG)
Ronald W. Rousseau, Georgia Institute of Technology
Hans van der Sloot, Consultant
Chen Gruber, Vanderbilt University
Jiannan “Nick” Chen, University of Central Florida
Hans van der Sloot, The Netherlands
John McCloy, Washington State University

EM Sites Impacted

  • Hanford Site
  • Savannah River Site
  • Idaho Site
  • Paducah and Portsmouth Sites

Highlighted Projects

Cementitious Barrier Partnership (CBP)

LEAF – Leaching Environmental Assessment Framework

Current Project Areas

Evaluating Compositional Uncertainties Associated with Hanford Tank Waste Treatment and Disposal

Lead Investigator: Kevin G. Brown (Lead) and David S. Kosson (Vanderbilt University)

Project Objectives:

  • Develop updated CRESP 200-East and 200-West Goldsim Monte Carlo models representing important treatment, disposal, and closure-related uncertainties for the 177 Hanford Site tanks, including the 158 Single-Shell waste tanks (SST) that still require retrieval.
  • Provide important tank waste uncertainty estimates for in-tank (Double-Shell Tanks [DST] and SSTs) inventories, retrieved inventories (SST) based on the SST retrieval plan, residual inventories (that relate to potential groundwater risk), and approximate feed vectors that relate to waste treatment and waste form volumes. 
  • Evaluate potential impacts of tank waste inventory uncertainties for planning, sampling/characterization, retrievals, tank residuals, processing rates, waste form volumes, waste acceptance criteria (WAC), process capability, and risk/dose estimates.

Significance/Impact:
The potential impacts of uncertainties in tank inventories and other significant uncertainties as they propagate through the blended compositions that will be treated may necessitate changes in some Waste Treatment and Immobilization Plant (WTP) waste acceptance criteria (WAC) parameters/limits or indicate challenges to process capability (e.g., ease of vitrifying tank wastes). Potential DOE uses of the resulting uncertainty assessment tool include characterization sampling, DFLAW, DFHLW, and off-site management of grouted waste.

Public Benefits:
This research provides a general methodology to evaluate the potential impacts of uncertainties for missing Hanford tank waste inventory data (namely concentrations based on information other than samples) that can be applied to other types of data. More generally, this research provides support for treating and disposing of wastes safely, focusing on waste characteristics (i.e., risk) and not strictly waste origin.

References: (* indicates CRESP publication)

*Brown, KG & Kosson, DS (2024) “Hanford Site Tank Waste Inventory and Uncertainty Analysis – 24512,” WM’2024, WMSymposia, Phoenix, Arizona.

*Brown, KG & Kosson, DS (2019) “Hanford Tank Waste Inventory Assessment,” CRESP Technical Report (Pre-decisional – DOE staff use only).

DOE/ORP-2003-02 (2003) “Environmental Impact Statement for Retrieval, Treatment and Disposal of Tank Waste and Closure of Single-Shell Tanks at the Hanford Site, Richland, WA: Inventory and Source Term Data Package,” Office of River Protection, Richland, Washington.

RPP-40545 (2016) “Quantitative Assumptions for Single-Shell Tank Waste Retrieval Planning,” Rev. 5, Washington River Protection Solutions LLC, Richland, Washington.

RPP-40545 (2021) “Quantitative Assumptions for Single-Shell Tank Waste Retrieval Planning,” Rev. 6, Washington River Protection Solutions LLC, Richland, Washington.

RPP-7625 (2017) “Guidelines for Updating Best-Basis Inventory,” Rev. 13, Washington River Protection Solutions LLC, Richland, Washington.

RPP-PLAN-40145 (2016) “Single-Shell Tank Waste Retrieval Plan,” Rev. 6, Washington River Protection Solutions, LLC, Richland, Washington.

RPP-PLAN-40145 (2021) “Single-Shell Tank Waste Retrieval Plan,” Rev. 7, Washington River Protection Solutions, LLC, Richland, Washington.

SS-1647 (2016) “Single-Shell Tank Retrieval Assumptions for Mission Modeling,” Rev. 6, Washington River Protection Solutions LLC, Richland, Washington.

SS-1647 (2016) “Single-Shell Tank Retrieval Assumptions for Mission Modeling,” Rev. 6, Washington River Protection Solutions LLC, Richland, Washington.

SS-1647 (2021) “Single-Shell Tank Retrieval Assumptions for Mission Modeling,” Rev. 7, Washington River Protection Solutions LLC, Richland, Washington.

Reducing Uncertainty in Tank and Vault Integrity and Performance Under Closure

Lead Investigators: Kevin G. Brown, Chen Gruber (Vanderbilt University), Jiannan (Nick) Chen (University of Central Florida), David S. Kosson (Vanderbilt University)

Additional Investigators: Andy C. Garrabrants (Vanderbilt University), Hans Meeussen (Nuclear Research and Consultancy Group, Energy Research Centre of The Netherlands), and Hans van der Sloot (Hans van der Sloot Consultancy, The Netherlands)

Project Objectives
The goal of this project is to perform integrated experimental and modeling studies in support of waste tank and vault closure at the Hanford Site (DOE-ORP). These studies will support risk-informed tank waste retrieval at DOE-ORP by improving the evaluation basis for the performance of concrete barriers (tanks and vaults) after closure that contain residual wastes. Specific tasks include:

  • use LeachXS/ORCHESTRA (LXO) reactive transport models (verified and validated as indicated above) as parameterized for residual waste leaching from closed and grouted waste tanks to assess impacts of aging (carbonation and oxidation), degradation (cracking), etc.
  • evaluate the data obtained from the PNNL characterization of existing tank 241-A-106 concrete sidewall cores for alkalinity; carbonation/pH (e.g., phenolphthalein); liquid-solid partitioning (USEPA Method 1313; and mass transport (USEPA Method 1315). CRESP researchers completed a review on the PNNL test plan in July 2022.
  • complete verification and validation (V&V) and documentation for the following reactive transport (LeachXS/ORCHESTRA) models: 1) carbonation ingress and reaction in waste tank shell (i.e., dome, walls, and basemat); and 2) solid-solid interface model (e.g., cementitious waste form in contact with either barrier or surrounding backfill).
  • perform “inverse PA modeling” to evaluate the relationship between the amount of residual waste in the tanks, conditions in and around the tanks, and potential contaminant releases to the environment to assess and estimate the maximum allowable tank residuals to meet performance objectives for Hanford Site waste tanks under closure scenarios.

Significance/Impact:
This research will improve the characterization of uncertainties and allow resulting reductions in conservatisms in contaminant release and near-field transport predictions from Hanford Site waste tanks after closure (including tank integrity as an additional defense-in-depth barrier). The research will be complemented by the DOE NNLEMS Developing a Hanford Grout Modeling Framework and Property Database for Performance Assessments project to provide a transformational change in reducing unnecessary conservatism in PA modeling of grout and improve the representativeness of grout behavior in long-term predictions. The information obtained will be used to parameterize the models used. “Inverse PA modeling” will provide defensible estimates of maximum allowable tank waste residuals to satisfy risk-based closure objectives (technical basis only) and to support risk-informed decision-making under uncertainty.

Public Benefits:
Models developed for this research will be used to better understand cement and concrete performance of buried structures for a range of non-DOE applications. Collaboration with the PNNL-led NNLEMS Project: Developing a Hanford Grout Modeling Framework and Property Database for PAs will generate a centralized property database curated for general use in future Machine Learning grout model development.

References: (* indicates CRESP publication)

*Gruber, C, Kosson, D, Brown, KG, DeLapp, R, Matteo, E, Meeussen, J, Klein-BenDavid, O, Bar-Nes, G, Brown, L, Ayers, J, Taylor, A, Chven, M & Pyrak-Nolte, L 2023, ‘Characterization and Simulation of Cement–Rock Interface Long-Term Performance’, WM’2023, WMSymposia, Phoenix AZ, Feb 26-Mar 3.

*Gruber, C, Steen, M, Brown, KG, DeLapp, R, Taylor, R, Ayers, J, Kosson, DS, Matteo, E, Klein-BenDavid, O, Bar-Nes, G, Meeussen, JCL, 2022, ‘Cement-carbonate rock interaction under saturated conditions: from laboratory to modelling,’ Cement and Concrete Research, Volume 160, October 2022, 106899. https://doi.org/10.1016/j.cemconres.2022.106899

*Gruber, C, Brown, KG, Garrabrants, AC, Meeussen, JCL, van der Sloot, HA & Kosson, DS 2020 ‘Modeling Interfaces to Support Low-Level Waste Disposal System Performance Assessments – 20366’, WM Symposia 2020, Phoenix, AZ, March 8-12, 2020.

*Brown, KG, Garrabrants, AC & Kosson, DS 2020 ‘Predicting Saturated Hydraulic Conductivity over Time for Degrading Saltstone Vault Concrete – 20376’, WM Symposia 2020, Phoenix, AZ, March 8-12, 2020.

Klein-BenDavid, O, Harlavan, Y, Levkov, I, Teutsch, N, Brown, KG, Gruber, C & Ganor, J 2019, ‘Interaction between spent fuel components and carbonate rocks,’ Science of the Total Environment, 689(2019), 469-480. https://doi.org/10.1016/j.scitotenv.2019.06.396.

*Gruber, C, Steen, M, Brown, KG, DeLapp, R, Matteo, EN, Klein-BenDavid, O, Bar-Nes, G, Meeussen, JCL, Ayers, J & Kosson, DS 2019, ‘Cementitious Materials Aging in Carbonate-Rock/Cement-Paste Interfaces with Implications for Deep Geological Disposal Sites’, Mechanisms and Modelling of Waste / Cement Interactions 2019, Karlsruhe, Germany, March 25-27, 2019.

*Garrabrants, AC, Brown, L, Zhang, P, van der Sloot, HA, Brown, KG, Gruber, C & Kosson, DS 2019, ‘Experimental and modeling efforts to predict long-term geochemistry of vault concrete – salt waste interfaces at U.S. DOE disposal sites’, International Workshop on Mechanisms and Modeling of Waste/Cement Interactions 2019. Karlsruhe, Germany.

ASME NQA-1-2015. 2015. Quality Assurance Requirements for Nuclear Facility Applications. New York, NY: American Society of Mechanical Engineers.

DOE Order 414.1D, Quality Assurance. Available at: https://www.directives.doe.gov/directives-documents/400-series/0414.1-BOrder-d (17 September 2015).

Rast, RS 2011, ‘Analytical Test Plan for the Removed 241-C-107 Dome Concrete and Rebar,’ RPP-PLAN-48753, Rev. 0, Washington River Protection Solutions, Richland, Washington.

Develop On-Line Methods for Monitoring Tank Waste Processing

Lead Investigator: Martha Grover (Georgia Institute of Technology)
Additional Investigators: Ronald Rousseau (Georgia Institute of Technology)

Project Objectives:

  • Combine existing knowledge of on-line monitoring with proposed mass-balance modeling and offline sampling to produce fault detection methodologies that include uncertainty quantification (Crouse, et al. 2024).
  • Investigate the solution chemistry of the slurries inside the melter feed preparation vessel (MFPV).
  • Understand the partitioning of sodium in solid and aqueous phases when waste is mixed with the glass forming chemicals (GFCs).
  • Elucidate the nucleation and growth kinetics of sodium phosphate hydrate crystallization and related minerals at highly basic conditions, which represent a potential process fault at the Hanford site.
  • Incorporate spectral data in kinetic modeling of Savannah River Site processes in collaboration with Dan Lambert from SRNL (Woodham et al. 2021).

Significance/Impact:
It is important to assess the feasibility of using in situ ATR-FTIR and/or Raman spectroscopy for monitoring the composition of nuclear waste during processing. The methodology has the potential to reduce the number of samples that must be drawn for off-line analysis during waste processing, thereby reducing the need for time-consuming and dangerous sample analysis. The turn-around time for analysis is suitable for the Hanford Real Time In-Line Monitoring (RTIM) initiative. The integration of the use of spectral data with kinetic models will improve the understanding of redox reactions at SRS and minimize offline data collection.

The planned remediation of the waste at Hanford includes mixing the high-level waste (HLW) with glass-forming chemicals (GFCs), followed by vitrification to immobilize the waste as borosilicate glass. The GFC addition is optimized according to the conditions of the incoming waste stream so that chemical and other constraints within the melter are satisfied. Therefore, it is crucial to understand the solution chemistry of the slurries inside the melter feed preparation vessel (MFPV), where the waste is mixed with several solid GFC mixtures.

Waste remediation at the Hanford Site will follow a batch processing structure, whereby each batch of waste is handled sequentially. In each batch, a variety of unanticipated process disturbances may occur, including mixing failure, species crystallization (i.e., phosphate or gibbsite), particle settling, and waste variation, to name some possibilities. Accurate and timely detection of process faults is important so that issues may be corrected before impacting the melter and potentially causing a process delay or even process (melter) damage. Therefore, it is important to have knowledge of conditions that may cause process faults and to detect when faults occur in a timely manner.

At the Hanford Site, a Monte-Carlo approach is planned to ensure waste reaching the melter satisfies glass-forming constraints while also maximizing waste loading under uncertainty. Therefore, any real-time measurement technologies would have to integrate seamlessly into this planned control system by also estimating and reporting measurement uncertainty. For this work to be useful at the Hanford or Savannah River Sites, uncertainty estimates are vital so that risk can be understood and managed.

Public Benefits:
This project will support the development of process monitoring technology applicable to many industries (e.g., pharmaceutical and mineral processing).  Graduate students, postdocs, undergraduate students, and high school teachers will be trained to support this research; these trained persons will be able to support not only DOE-EM activities but also those scientific and engineering endeavors outside of DOE.

References (* indicates CRESP publication)

*R. Prasad, S. H. Crouse, R. W. Rousseau, Martha A. Grover, “Quantifying Dense Multicomponent Slurries with In-line ATR-FTIR and Raman Spectroscopy: A Hanford case study,” Industrial & Engineering Chemistry Research, 62, 39, 15962–15973 (2023), https://doi.org/10.1021/acs.iecr.3c01249.

*S. Kocevska, G. M. Maggioni, R.W. Rousseau, and M. A. Grover, “Spectroscopic Quantification of Target Species in a Complex Mixture Using Blind Source Separation and Partial Least-Squares Regression: A Case Study on Hanford Waste,” Industrial & Engineering Chemistry Research, 60, 27, 9885–9896 (2021), https://doi.org/10.1016/j.cherd.2022.03.002.

*D. J. Griffin, Y. Kawajiri, M. A. Grover, R. W. Rousseau, “Feedback Control of Multicomponent Salt Crystallization,” Crystal Growth & Design, 15 (1), 305-317 (2015), https://doi.org/10.1021/cg501368y.

P. Tse, J. Shafer, S. A. Bryan, A. M. Lines, “Quantification of Raman-Interfering Polyoxoanions for Process Analysis: Comparison of Different Chemometric Models and a Demonstration on Real Hanford Waste,” Environmental Science & Technology, 55, 12943–12950 (2021), https://doi.org/10.1021/acs.est.1c02512.

A. M. Lines, J. M. Bello, C. Gasbarro, S. A. Bryan, “Combined Raman and Turbidity Probe for Real-Time Analysis of Variable Turbidity Streams,” Analytical Chemistry, 94, 3652–3660 (2022), https://doi.org/10.1021/acs.analchem.1c05228

*D. Griffin, M. A. Grover; Y. Kawajiri; R. W. Rousseau, “Robust multicomponent IR-to-concentration model regression,” Chemical Engineering Science, 116 (6), 77-90 (2014), https://doi.org/10.1016/j.ces.2014.04.013.

*G. M. Maggioni, S. Kocevska, M. A. Grover, R. W. Rousseau, “Analysis of multicomponent ionic mixtures using blind source separation: A processing case study”, Industrial & Engineering Chemistry Research, 58 (50), 22640–22651 (2019), https://doi.org/10.1021/acs.iecr.9b03214.

W. H. Woodham, A. M. Howe, M. J. Siegfreid, “Sludge Batch 10 Flowsheet Testing with Non-radioactive Simulants,” SRNL Report SRNL-STI-2021-00349, Revision 0 (2021)

R. J. Lascola, M. E. Stone, “Real-Time, In-Line Monitoring for High Level Waste Applications,” SRNL Report SRNL-RP-2023-01064, Revision 0 (2023).

*S. H. Crouse, S. Kocevska, S. Noble, R. Prasad, A. M. Howe, D. P. Lambert, R. W. Rousseau, M. A. Grover, “Real-time infrared spectroscopy coupled with blind source separation for nuclear waste process monitoring,” Frontiers in Nuclear Engineering, 2 (2023), https://doi.org/10.3389/fnuen.2023.1295995.

*S. Kocevska, G. M. Maggioni, S. H. Crouse, R. Prasad, R. W. Rousseau, M. A. Grover, “Effect of ion interactions on the Raman spectrum of NO3-: Toward monitoring of low-activity nuclear waste at Hanford, Chemical Engineering Research and Design, 181, 173–194 (2022),  https://doi.org/10.1016/j.cherd.2022.03.002.

*S. H. Crouse, R. Prasad, M. A. Grover, R. W. Rousseau, “Detecting Faults in Nuclear Waste Slurry Processing with In-Line Probes: A Computational Study,” Proceedings of the Waste Management Symposium (2024), Paper 24059.

R. A. Peterson, E. C. Buck, J. Chun, R. C. Daniel, D. L. Herting, E. S. Ilton, G. J. Lumetta, S. B. Clark, “Review of the Scientific Understanding of Radioactive Waste at the U.S. DOE Hanford Site,” Environmental Science and Technology, 52, 381–396 (2018), https://doi.org/10.1021/acs.est.7b04077.

Computer codes: https://github.com/magrover?tab=repositories

Capturing Volatile Contaminants Utilizing Iron Sulfide Nanoparticles

Lead Investigator: John McCloy (Lead, Washington State University)

Project Objectives:

  • Demonstrate proof of principal removal of Tc (or proxy Re), Hg, and/or I (in various forms) from caustic waste using Fe-S magnetic particles.
  • Demonstrate one or more possible waste form paths for immobilization of the radionuclide/contaminant-laden Fe-S particles.
  • Assess overall disposal benefits of the addition of this process and propose flow sheet changes necessary to incorporate the process.

Significance/Impact:
Volatile contaminants, including radionuclides 99Tcand 129Iand hazardous elements like Hg, are problematic components for remediation in various DOE-EM cleanup sites. These can be present both in radioactive tank waste as well as in soil and groundwater. While technologies do exist to treat groundwater and soil, novel methods may enable improved separation, especially from tank waste, that would allow waste forms with lower concentrations of these compounds, which generally drive the long-term dose (e.g., Tc, I) or heavy metal leaching performance (Hg). Additionally, commercially baselined sorbents for off-gas systems (such as modified graphite for Hg capture) frequently become unavailable from manufacturers (Fountain et al., 2022), and new materialshave to be qualified. Using a magnetic sorbent could allow the removal of contaminants in a flowing stream of liquid, and the removed contaminants could then be sequestered in a purpose-designed waste form; alternatively, they could be added back into a specific existing waste form (e.g., cementitious material or recycled into the glass feed).

Public Benefits:
The technology being developed as part of this CRESP project provides a foundation for targeted contaminant removal from water and wastewater streams with wide applicability beyond DOE.​ The research also provides a potential path for lower-cost immobilization for low activity and related waste streams outside of DOE. 

References: (* indicates CRESP publication)

Asmussen, M., Levitskaia, T., Bottenus, C., and Fountain, M.S. (2020) Iodine Speciation Basis and Gap Analysis for Hanford Tank Farm Inventory and during Processing. PNNL-30105, Pacific Northwest National Laboratory.

Bannochie, C.J., Fellinger, T.L., Garcia-Strickland, P., Shah, H.B., Jain, V., and Wilmarth, W.R. (2018) Mercury in aqueous tank waste at the Savannah River Site: Facts, forms, and impacts. Separation Science and Technology, 53, 1935-1947.

Cordova, E.A., Garayburu-Caruso, V., Pearce, C.I., Cantrell, K.J., Morad, J.W., Gillispie, E.C., Riley, B.J., Colon, F.C., Levitskaia, T.G., Saslow, S.A., Qafoku, O., Resch, C.T., Rigali, M.J., Szecsody, J.E., Heald, S.M., Balasubramanian, M., Meyers, P., and Freedman, V.L. (2020) Hybrid Sorbents for 129I Capture from Contaminated Groundwater. ACS Applied Materials & Interfaces, 12, 26113-26126.

Darab, J.G., Amonette, A.B., Burke, D.S.D., Orr, R.D., Ponder, S.M., Schrick, B., Mallouk, T.E., Lukens, W.W., Caulder, D.L., and Shuh, D.K. (2007) Removal of Pertechnetate from Simulated Nuclear Waste Streams Using Supported Zero-valent Iron. Chemistry of Materials, 19, 5703-5713.

Fountain, M.S., Asmussen, M., Riley, B.J., Chong, S., Choi, S., and Matyáš, J. (2022) Roadmap to Iodine and Mercury Abatement Materials Selection in Nuclear Waste Processing Off-Gas Streams.  Pacific Northwest National Laboratory.

Gong, Y., Huang, Y., Wang, M., Liu, F., and Zhang, T. (2019) Application of Iron-Based Materials for Remediation of Mercury in Water and Soil. Bull. Environ. Contam. Toxicol., 102, 721-729.

Icenhower, J.P., Qafoku, N.P., Zachara, J.M., and Martin, W.J. (2010) The biogeochemistry of technetium: A review of the behavior of an artificial element in the natural environment. American Journal of Science, 310, 721-752.

Lere-Adams, A.J., Dixon Wilkins, M.C., Bollinger, D., Stariha, S., Farzana, R., Dayal, P., Gregg, D.J., Chong, S., Riley, B.J., Heiden, Z.M., and McCloy, J.S. (2024) Glass-bonded ceramic waste forms for immobilization of radioiodine from caustic scrubber wastes. Journal of Nuclear Materials, 591, 154938.

Moore, J., Nienhuis, E., Ahmadzadeh, M., and McCloy, J. (2019) Synthesis of greigite (Fe3S4) particles via a hydrothermal method. AIP Advances, 9, 035012.

Moore, R.C., Pearce, C.I., Morad, J.W., Chatterjee, S., Levitskaia, T.G., Asmussen, R.M., Lawter, A.R., Neeway, J.J., Qafoku, N.P., Rigali, M.J., Saslow, S.A., Szecsody, J.E., Thallapally, P.K., Wang, G., and Freedman, V.L. (2020) Iodine immobilization by materials through sorption and redox-driven processes: A literature review. Science of The Total Environment, 716, 132820.

Riley, B.J., Vienna, J.D., Strachan, D.M., McCloy, J.S., and Jerden Jr, J.L. (2016) Materials and processes for the effective capture and immobilization of radioiodine: A review. Journal of Nuclear Materials, 470, 307-326.

Wang, J., Feng, X., Anderson, C.W.N., Xing, Y., and Shang, L. (2012) Remediation of mercury contaminated sites – A review. Journal of Hazardous Materials, 221-222, 1-18.

Watson, J.H.P., and Ellwood, D.C. (2003) The removal of the pertechnetate ion and actinides from radioactive waste streams at Hanford, Washington, USA and Sellafield, Cumbria, UK: the role of iron-sulfide-containing adsorbent materials. Nuclear Engineering and Design, 226, 375-385.

Xiong, Z., He, F., Zhao, D., and Barnett, M.O. (2009) Immobilization of mercury in sediment using stabilized iron sulfide nanoparticles. Water Research, 43, 5171-5179.

Yadav, A., Chong, S., Riley, B.J., McCloy, J.S., and Goel, A. (2023) Iodine Capture by Ag-Loaded Solid Sorbents Followed by Ag Recycling and Iodine Immobilization: An End-to-End Process. Industrial & Engineering Chemistry Research, 62, 3635-3646.

Yang, Y., Chen, T., Sumona, M., Sen Gupta, B., Sun, Y., Hu, Z., and Zhan, X. (2017) Utilization of iron sulfides for wastewater treatment: a critical review. Rev. Environ. Sci. Bio/Technol., 16, 289-308.

Artificial Intelligence Model of Crossflow Filtration System for Tank Wastes

Lead Investigator: Kimberly Jones (Lead, Howard University)
Additional Investigators: Sanjib Sharma (Howard University)

Project Objectives:

  • Develop an understanding of fouling by high-activity tank waste in a crossflow filtration system based on operational parameters;
  • Develop appropriate parameters for a predictive AI membrane performance simulation model; and
  • Recommend appropriate fouling management strategies for the filtration process that would reduce fouling and increase overall process (separation) efficiency.

Significance/Impact:
Vitrification is a critical treatment process for the immobilization of radioactive wastes and eliminates corresponding environmental threats for the tank wastes at the Hanford Site. Waste volume reduction is an important step to ensure the success of vitrification, which will remove excess water, concentrate solids, and optimize waste composition for reaction with glass-forming materials. Therefore, there is a critical need to develop the most suitable solid-liquid separation method

Crossflow filtration, specifically microfiltration, is one of the principal separation technologies that has been proven to be an effective method of dewatering waste by previous work at PNNL (Daniel et al., 2010). However, due to the unique properties of tank wastes (i.e., high solid content, high pH, and high ionic strength), persistent membrane fouling hinders the treatment process. In addition, the proposed Low Activity Waste Pretreatment System (LAWPS) poses the potential to have significant depth fouling, which is little understood at this time. Therefore, fouling will remain a serious problem during crossflow membrane filtration of tank waste and will significantly impact the overall timeline and costs associated with the remediation of the Hanford site.

Prior studies have shown that typical fouling mechanisms and conventional wisdom involved in planning and operating crossflow membrane systems may not apply to the unique feed streams from waste tanks. When challenged with a synthetic feed, the membrane performance continued to decay at long timeframes and did not reach a steady state. To address this issue and attempt to explain fouling behavior, a new model was proposed to more reasonably match theory, and experimental results (Schonewillet al., 2015), but further efforts are needed to determine the mechanistic causes of this behavior in order to recommend modifications to the process to improve filtration performance.

Public Benefits:
This research improves treatment efficiency via real-time monitoring and predictive maintenance with applicability to waste streams outside of DOE. The treatment techniques developed here are scalable to different wastewater treatment facilities and flexible to fit changing waste streams and treatment requirements. The result will be increased transparency to the affected community and cost savings to the public.

References:

Asghari, M., Dashti, A., Rezakazemi, M., Jokar, E., & Halakoei, H. (2020). Application of neural networks in membrane separation. Reviews in Chemical Engineering, 36(2), 265–310. https://doi.org/10.1515/revce-2018-0011

Daniel, R., Schonewill, P., Shimskey, R., & Peterson, R. (2010). Brief review of filtration studies for waste treatment at the Hanford site. PNNL-20023, Prepared for the U.S. DOE under Contract DE-AC05-76RL01830.

Daniel, R. C., Billing, J. M., Bontha, J. R., Brown, C. F., Eslinger, P. W., Hanson, B. D., Huckaby, J. L., Karri, N. K., Kimura, M. L., Kurath, D. E., & Minette, M. J. (2010). EFRT M-12 issue resolution: Comparison of filter performance at PEP and CUF scale. PNNL-18498 Rev 1; WTP-RPT-185 Rev 1, Pacific Northwest National Laboratory, Richland, WA.

Daniel, R. C., Billing, J. M., Burns, C. A., Peterson, R. A., Russell, R. L., Schonewill, P. P., & Shimskey, R. W. (2011). Filtration understanding: FY10 testing results and filtration model update. PNNL-20299, Pacific Northwest National Laboratory, Richland, WA.

Eren, B., Ileri, R., Dogan, E., Caglar, N., & Koyuncu, I. (2012). Development of artificial neural network for prediction of salt recovery by nanofiltration from textile industry wastewaters. Desalination and Water Treatment, 50(1-3), 317–328. https://doi.org/10.1080/19443994.2012.719743

Ghandehari, S., Montazer-Rahmati, M. M., & Asghari, M. (2013). Modeling the flux decline during protein microfiltration: A comparison between feed-forward back propagation and radial basis function neural networks. Separation Science and Technology, 48(9), 1324–1330. https://doi.org/10.1080/01496395.2012.736914

Liu, Q., Kim, S. H., & Lee, S. (2009). Prediction of microfiltration membrane fouling using artificial neural network models. Separation and Purification Technology, 70(1), 96–102. https://doi.org/10.1016/j.seppur.2009.08.017

Roehl, E., et al. (2018). Modeling fouling in a large RO system with artificial neural networks. Journal of Membrane Science, 552, 95–106. https://doi.org/10.1016/j.memsci.2018.01.064

*Rollock, R., Liu, Y., Ramamoorthy, M., & Jones, K. (2014). Understanding the fouling mechanisms of inorganic particulates in a microfiltration system. Presented at the 24th annual NAMS meeting, May 31 – June 4, 2014, in Houston, TX.

Schmitt, F., & Do, K. U. (2017). Prediction of membrane fouling using artificial neural networks for wastewater treated by membrane bioreactor technologies: Bottlenecks and possibilities. Environmental Science and Pollution Research, 24(29), 22885–22913. https://doi.org/10.1007/s11356-017-0046-7

Schmitt, F., Banu, R., Yeom, I.-T., & Do, K.-U. (2018). Development of artificial neural networks to predict membrane fouling in an anoxic-aerobic membrane bioreactor treating domestic wastewater. Biochemical Engineering Journal, 133, 47–58. https://doi.org/10.1016/j.bej.2018.02.001

Schonewill, P. P., Daniel, R. C., Russell, R. L., Shimskey, R. W., Burns, C. A., Billing, J. M., Rapko, B. M., & Peterson, R. A. (2012). Development of an S-Saltcake simulant using crossflow filtration as a validation technique. Separation Science and Technology, 47(14-15), 2098–2107.

Srivastava, A., et al. (2021). Response surface methodology and artificial neural network modeling for the performance evaluation of pilot-scale hybrid nanofiltration (NF) & reverse osmosis (RO) membrane system for the treatment of brackish groundwater. Journal of Environmental Management, 278, 111497. https://doi.org/10.1016/j.jenvman.2020.111497

Develop Advanced Grout Formulations for Enhanced Wasteform Performance

Lead Investigator: Florence Sanchez (Vanderbilt University)
Additional Investigators: Lesa Brown, Kevin G. Brown, Chen Gruber, and David Kosson (Vanderbilt University)

Project Objectives:

  • Develop fiber-reinforced high-performance encapsulation grout formulations that are resistant to aging mechanisms (e.g., carbonation, cracking, autogenous shrinkage);
  • Develop grout formulations appropriate for the treatment of tank waste sludges and calcined waste to facilitate disposal as Class C or Greater-Than-Class C (GTCC) Low-Level Radioactive Waste;
  • Develop machine learning approaches for determining reaction sets and thermodynamic/kinetic constants for geochemical speciation modeling and enhanced grout formulations; and,
  • Characterize ancient and natural analogues cement samples that have been exposed to relevant climate conditions and geologic interfaces to improve confidence in long-term performance modeling.

Significance/Impact:
Grout is used in multiple applications for waste management, including for encapsulation of secondary waste (e.g., HEPA filters, equipment, resins, condensate) at the Hanford Site, and as a primary wasteform (e.g., saltstone) at the Savannah River Site (SRS). The following are specific challenges to be addressed through this project:

Encapsulation grout – High-performance encapsulation grouts have been under development based on using low water: cement ratios and admixtures to control rheology. Applications envisioned include bulk fill surrounding and within contaminated materials and equipment and containment boxes or vaults. In both applications, low porosity and permeability result in high retention of radionuclides. However, material micro- and macro-cracking has been observed in response to material aging. Identified failure mechanisms have included autogenous shrinkage, formation of expansive mineral phases, and carbonation. Objective 1 of this project will overcome these challenges by the use of microfiber reinforcement in conjunction with grout formulations resistant to the identified failure mechanisms. Grout formulations will be designed for bulk fill and additive manufacturing (cement printing).

Grout for Hanford sludge solids and Idaho calcined waste – Both Hanford tank sludge solids and Idaho calcine waste have been considered waste streams for thermal treatment (e.g., vitrification) prior to disposal as high-level waste (HLW). However, thermal treatment followed by disposal as HLW can be challenging because of high cost, material handling challenges, and the absence of a geologic repository. Alternative disposal pathways may be viable in the future as either Class C or GTCC radioactive waste when incorporated in grout wasteforms. However, these waste streams differ in composition and physical-chemical properties from other DOE wastes that are currently grouted. Thus, grout performance objectives and conforming formulations will be developed (Objective 2) to enable further consideration of potential grout disposal pathways.

Geochemical reaction sets and thermodynamic constants – Selection of the mineral assemblage and uncertainty associated with mineral reaction thermodynamic constants are central to geochemical speciation-based reactive transport modeling for long-term grout performance (Durdziński, et al. 2017). These predictions can thus influence (and at times, limit) the formulations used for grout wasteforms (e.g., saltstone, Cast Stone, tank closure grouts) critical to DOE waste management practices. Today, the selection of a mineral assemblage is influenced by the modeler’s theoretical knowledge/background, existing data, and calibration processes for uncertain reaction constants and other parameters that rely on the minimization of errors between predictions and experimental results (Wang et al., 2022; Wang et al. 2023). Automation and machine learning would expedite the mineral assemblage selection process significantly by constructing a rigorous and logical framework that incorporates differing types of information for important families of cement-based materials: physical evidence (XRD); likelihood of mineral phase existence (based on prior knowledge of families of materials – e.g., CaCO3 in carbonate rocks); and better understanding of kinetic versus thermodynamic phenomena and associated uncertainties. The ability to more accurately and consistently predict the performance of important cement-based materials would build confidence in their use for important waste streams (e.g., Hanford tank wastes). Machine learning techniques can help build such confidence (Li et al., 2022). Outcomes for Objective 3 would be to 1) minimize the arbitrary influence on the mineral assemblage selection process, and 2) provide uncertainty quantification and approaches to resolving gaps between predictions and experimental data.

Characterizing ancient cements – Grout wasteforms and concrete containment structures must be evaluated for a performance period of up to and greater than 1000 years to be fully credited in Performance Assessments (PA). However, actual performance data are available for only a few decades. Performance data for cement systems under exposure conditions relevant to DOE sites is needed to understand long-term aging mechanisms and validate models for cement materials evolution. Ancient and natural analogues cement materials, ranging in age from up to 2,500 years for man-made cements to 50,000 years (natural cements) with well-defined exposure conditions (both arid and temperate in contact with carbonate and loess soils) provides an opportunity to provide geochemical and constituent transport data that can be used to confirm current testing and modeling approaches. Outcomes for Objective 4 will use characterization data from ancient materials to build confidence in the integrated testing and modeling approach used by CRESP to evaluate and predict the long-term behavior of cement materials used for DOE waste management.

Public Benefits:
The development of effective grout formulations for a wide variety of waste streams ensures the safety of communities and mitigates the risks associated with waste storage and disposal. The formulations, data, and models developed during this research will be applicable to other industries and waste streams. The results of this work, including the characterization of ancient materials, will help build public confidence in the long-term performance and prediction of the resulting grout waste forms.

References: (* indicates CRESP publication)

*Branch, J.L., Brown, K.G., Arnold, J.R., van der Sloot, H.A. & Kosson D.S. (2015a) Reactive Transport Modeling and Characterization of Concrete Materials with Fly Ash Replacement under Carbonation Attack – 15477. WM’2015, WMSymposia, Phoenix, Arizona.

*Branch, J.L., Kosson, D.S., Brown, KG, van der Sloot, J.A. & Garrabrants, A.C. (2015b) Characterization and reactive-transport modeling of the changes in the chemical speciation and microstructure of cementitious materials as a result of carbonation. IWWG-ARB 2015 Conference, Shanghai, CHINA.

Brown, L., Allison, P. G., & Sanchez, F. (2018). Use of nanoindentation phase characterization and homogenization to estimate the elastic modulus of heterogeneously decalcified cement pastes. Materials & Design, 142, 308-318. https://doi.org/https://doi.org/10.1016/j.matdes.2018.01.030 

Brown, L., & Sanchez, F. (2016). Influence of carbon nanofiber clustering on the chemo-mechanical behavior of cement pastes. Cement and Concrete Composites, 65, 101-109. https://doi.org/https://doi.org/10.1016/j.cemconcomp.2015.10.008

Brown, L., & Sanchez, F. (2018). Influence of carbon nanofiber clustering in cement pastes exposed to sulfate attack. Construction and Building Materials, 166, 181-187. https://doi.org/https://doi.org/10.1016/j.conbuildmat.2018.01.108

Brown, L., Stephens, C. S., Allison, P. G., & Sanchez, F. (2022). Effect of Carbon Nanofiber Clustering on the Micromechanical Properties of a Cement Paste. Nanomaterials, 12(2).

*Chen, Z., Zhang, P., Brown, K. G., Branch, J. L., van der Sloot, H. A., Meeussen, J. C. L., Delapp, R. C., Um, W., & Kosson, D. S. (2021). Development of a Geochemical Speciation Model for Use in Evaluating Leaching from a Cementitious Radioactive Waste Form. Environmental Science & Technology, 55(13), 8642-8653. https://doi.org/10.1021/acs.est.0c06227

Durdziński, P. T., Ben Haha, M., Zajac, M., & Scrivener, K. L. (2017). Phase assemblage of composite cements. Cement and Concrete Research, 99, 172-182. https://doi.org/https://doi.org/10.1016/j.cemconres.2017.05.009  

*Garrabrants, A.C., Brown, L., Zhang, P., van der Sloot, H.A., Brown, K.G., Gruber, C. & Kosson, D.S. (2019) Experimental and modeling efforts to predict long-term geochemistry of vault concrete – salt waste interfaces at U.S. DOE disposal sites. International Workshop on Mechanisms and Modeling of Waste/Cement Interactions 2019. Karlsruhe, Germany.

*Gruber, C., Steen, M., Brown, K. G., Delapp, R., Matteo, E. N., Klein-BenDavid, O., Bar-Nes, G., Meeussen, J. C. L., Ayers, J. C., Kosson, D. S. (2022). Cement‑carbonate rock interaction under saturated conditions: From laboratory to modeling. Cement and Concrete Research, 160, 899-924. https://doi.org/10.1016/j.cemconres.2022.106899.

Li, Z., Yoon, J., Zhang, R., Rajabipour, F., Srubar Iii, W. V., Dabo, I., & Radlińska, A. (2022). Machine learning in concrete science: applications, challenges, and best practices. npj Computational Materials, 8(1), 127. https://doi.org/10.1038/s41524-022-00810-x

Kosson, M., Brown, L., & Sanchez, F. (2020). Early-Age Performance of 3D Printed Carbon Nanofiber and Carbon Microfiber Cement Composites. Transportation Research Record, 2674(2), 10-20. https://doi.org/10.1177/0361198120902704

Kosson, M., Brown, L., & Sanchez, F. (2023). Nanomechanical characterization of 3D printed cement pastes. Journal of Building Engineering, 66, 105874. https://doi.org/https://doi.org/10.1016/j.jobe.2023.105874

Sanchez, F., & Borwankar, A. (2010). Multi-scale performance of carbon microfiber reinforced cement-based composites exposed to a decalcifying environment. Materials Science and Engineering: A, 527(13), 3151-3158. https://doi.org/https://doi.org/10.1016/j.msea.2010.01.084

Sanchez, F., Borwankar, A & Ince, C. (2009) Effect of decalcification on the performance of carbon microfiber reinforced cement-based materials. In: L’Hostis, V., Gens, R. Gallé, C. (eds) RILEM Proceedings Book related to the NUCPERF 2009 Workshop (Long Term Performance of Cementitious Barriers and Reinforced Concrete in Nuclear Power Plants and Waste Management (EFC Event n°317)). 30 March – 2 April 2009, Cadarache, France. PRO 64 (2009), ISBN: 978-2-31158-072-1

*Sarkar, S., Kosson, D. S., Mahadevan, S., Meeussen, J. C. L., der Sloot, H. v., Arnold, J. R., & Brown, K. G. (2012). Bayesian calibration of thermodynamic parameters for geochemical speciation modeling of cementitious materials. Cement and Concrete Research, 42(7), 889-902. https://doi.org/https://doi.org/10.1016/j.cemconres.2012.02.004

Wang, X., Garrabrants, A. C., van der Sloot, H. A., Chen, Z., Brown, K. G., Hensel, B., & Kosson, D. S. (2023). Leaching and geochemical evaluation of oxyanion partitioning within an active coal ash management unit. Chemical Engineering Journal, 454, 140406. https://doi.org/https://doi.org/10.1016/j.cej.2022.140406

*Wang, X., van der Sloot, H. A., Brown, K. G., Garrabrants, A. C., Chen, Z., Hensel, B., & Kosson, D. S. (2022). Application and uncertainty of a geochemical speciation model for predicting oxyanion leaching from coal fly ash under different controlling mechanisms. Journal of Hazardous Materials, 438, 129518. https://doi.org/10.1016/j.jhazmat.2022.129518

All Publications: Waste Processing & Special Nuclear Materials, 2006-2019 (pdf)

Highlighted Publications and Reports

CRESP Waste Processing & Special Nuclear Materials

Kocevska, S, Grover, M & Rousseau, R 2019a, ‘Monitoring the Composition of Low-Activity Nuclear Waste using In-Situ Instrumentation, presentation’, WM ‘2019, WM Symposia, Phoenix, Arizona.

Kocevska, S, Grover, M & Rousseau, R 2019b, ‘Monitoring the Composition of Low-Activity Nuclear Waste using In-Situ Instrumentation, presentation’, Career, Research, and Innovation Development Conference, Atlanta Georgia.

Henry, B, Fortenberry, K, Pierce, E, Echols, R, Edwards, R & Brown, K 2019, ‘Development of the DOE Mercury Management Strategy, Panel’, WM ‘2019, WM Symposia, Phoenix, Arizona.

Greenberg, M, Apostolakis, G, Field, T, Goldstein, B, Kosson, D, Krahn, S, Matthews, R, Rispoli, J, Stewart, J & Stewart, R 2019, ‘Advancing Risk-Informed Decision Making in Managing Defense Nuclear Waste in the United States: Opportunities and Challenges for Risk Analysis’, Risk Analysis, vol. 39, no. 2, pp. 375-388. https://doi.org/10.1111/risa.13135

Zhang, P, Branch, J, Garrabrants, A, Delapp, R, Klein-Ben David, O & Kosson, D 2018, ‘The Effect of Environmental Relative Humidity on Carbonation and Oxidation in a Cementitious Waste Form–18448’, WM’2018, WM Symposia, Phoenix, Arizona. http://toc.proceedings.com/40439webtoc.pdf

Kocevska, S, Rousseau, R & Grover, M 2018, ‘Evaluation of In-Situ Infrared Spectroscopy for Direct Feed Low Activity Waste Processing’, Real-Time, In-Line Monitoring Hanford Program Review, Richland, Washington.

Kocevska, S, Grover, M & Rousseau, R 2018, ‘880 Monitoring the Composition of Low Activity Nuclear Waste using in-situ Measurement Methods, Presentation’, ACSS/SciX Conference, Atlanta, Georgia. https://www.scixconference.org/images/pdfs/program/scix-2018-final-program-wcovers-web.pdf

Brown, L, Allison, PG & Sanchez, F 2018, ‘Use of nanoindentation phase characterization and homogenization to estimate the elastic modulus of heterogeneously decalcified cement pastes’, Materials & Design, vol. 142, pp. 308-318. https://doi.org/10.1016/j.matdes.2018.01.030

Brown, K 2018, ‘Hanford Tank Waste Treatment: Foundations for Waste Treatment and Disposition Planning, Poster Session’, Vanderbilt Conference, Nashville, Tennessee. www.cresp.org

Branch, J, Epps, R & Kosson, D 2018, ‘The impact of carbonation on bulk and ITZ porosity in microconcrete materials with fly ash replacement’, Cement and Concrete Research, vol. 103, pp. 170-178. https://doi.org/10.1016/j.cemconres.2017.10.012

Branch, J 2018, ‘Impact of Aging in the Presence of Reactive Gases on Cementitious Waste Forms and Barriers’, Ph.D. dissertation in Environmental Engineering, Vanderbilt University, Nashville, Tennessee.

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