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DOE OSTI2021

Characterizing Impacts of Dry Coal Feeding in High Pressure Oxy-Coal Combustion Systems

Reaction Engineering International (REI) has managed a team of experts from the University of Utah, Southeast University (SEU) in Nanjing, China, Electric Power Research Institute (EPRI), Corrosion Management Ltd. (C-M), Praxair, and Brigham Young University (BYU) to investigate dry pulverized coal feeding for pressurized oxy-coal combustion. Dry feed firing systems for entrained flow, pressurized, oxy-coal combustors have not been well developed, although related technologies have been used in the Shell Gasification Process and for pressurized fluid bed combustion. DOE-funded research recently completed at REI and the University of Utah focused on characterizing impacts of high temperatures and pressures in oxy-coal combustion systems. For high pressure combustion, that research used a coal slurry feed into a 17 bar pressurized combustor. As a consequence of that research, it was identified that fuel feeding and firing system flexibility are challenges that require attention. Based on that experience, the approach of using a coal slurry feed system leads to challenges in producing consistent atomization of the slurry, which causes burnout problems, especially at high pressures. In addition, slurry atomization processes may be difficult to scale to sizes appropriate for practical commercial use. Dry pressurized coal burner systems, on the other hand, have the potential to yield efficiency gains, improve flexibility and facilitate applications at larger scales. Experimental work was conducted at the University of Utah Industrial Combustion and Gasification Research Facility as well as the 100 kW pressurized oxy-coal combustor (POC) facility at Brigham Young University. Mechanism development and CFD-based combustion and dense-phase flow modeling were performed at REI. Successful completion of the project objectives has resulted in the following key deliverables: 1) Design and prototype of a pressurized pulverized coal feeding and oxy-firing system 2) Data from a 100kW, pressurized (15 bar) entrained flow reactor with a dry feeding delivery and burner system that describes flame characteristics, radiative heat flux profiles, carbon burnout, along with characteristics of ash aerosols, fouling, and slagging. 3) Validated and transportable models that describe the relevant conditions in pressurized oxy-combustion systems and that can be used for scale-up and optimization. 4) Principles to guide design of high pressure, pilot-scale and full-scale coal oxy-firing systems. 5) Assessment of pressurized oxy-combustion impacts on key parameters relevant to oxy-coal fired utility boilers such as coal devolatilization, char oxidation, mineral matter transformation, deposition, and corrosion. The experimental data, pressurized oxy-firing system principles, and process mechanisms provided by this work can be used by electric utilities, boiler OEMs, equipment suppliers, design firms, software vendors, consultants and government agencies to assess the use of high temperature and high pressure oxy-combustion in current research and to guide development of new oxy-coal boiler designs.

pressurized oxy-coal combustion, sub-micron ash ae↗

DOE OSTI2022

Characterizing Impacts of Dry Coal Feeding in High Pressure Oxy-Coal Combustion Systems

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2023

Catalytic Upgrading of Carbohydrates in Waste Streams to Hydrocarbons: Paper Sludge to Fuel Project (PStF)

This research, funded by the Department of Energy Bioenergy Technologies Office (DOE BETO), aims to understand the barriers and assess opportunities for transforming carbohydrates in paper sludge, a solid lignocellulosic residue from the pulp and paper industry. The goal is to turn the paper sludge into a liquid hydrocarbon product that can be blended into jet fuel, both economically and sustainably. Research groups at North Carolina State University, National Renewable Energy Laboratory, and Yale University collaborated synergistically, leveraging their expertise in pulp and paper operations, biomass deconstruction, and catalytic upgrading to propose a pathway that efficiently captures the energy in paper sludge. Findings from this study could potentially contribute to advancing biomass conversion technologies, aligning with the efforts of the U.S. DOE BETO. This report documents the experimental and simulation results of a biochemical and catalytic pathway designed to transform paper sludge into a liquid hydrocarbon product. The process involves a sequence of seven steps, including ash removal, carbohydrate enzymatic hydrolysis, sugar dehydration, solvent recovery, aldol-condensation between furans and ketone, hydrogenation, and hydrodeoxygenation to obtain a hydrocarbon blend in the ~C10 range. The experimental efforts from the initiation of the project were guided by techno-economic analysis (TEA) and sensitivity analysis results including around seventy-eight operational parameters. This methodology facilitated the efficient use of resources over time. This study relies on detailed process simulations and TEA to determine the minimum fuel selling price (MFSP) for the hydrocarbon fuel product. Preliminary TEA results led to the evaluation of eight case studies considering alternative dehydration co-solvents, operational settings, and biorefinery layouts. Finally, the life cycle assessment of twenty-eight scenarios, comparing various dehydration co-solvents, fuel sources, chemical feedstock sources, side product utilization, and other process settings, was conducted. Landfilling scenarios with and without landfill gas recovery were also estimated, analyzed, and compared.

09 BIOMASS FUELS↗

DOE OSTI2025

Gulf Coast Basin CORE-CM Initiative (Final Report)

This report describes critical mineral/rare earth element resources, including Gulf Coast coal resources, and waste streams including coal ash from power plants, red mud from alumina processing, heavy mineral concentrates from sand mining industry, zeolite, graphite, and produced water with oil and gas.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2010

Self-degradable Cementitious Sealing Materials

A self-degradable alkali-activated cementitious material consisting of a sodium silicate activator, slag, Class C fly ash, and sodium carboxymethyl cellulose (CMC) additive was formulated as one dry mix component, and we evaluated its potential in laboratory for use as a temporary sealing material for Enhanced Geothermal System (EGS) wells. The self-degradation of alkali-activated cementitious material (AACM) occurred, when AACM heated at temperatures of {ge}200 C came in contact with water. We interpreted the mechanism of this water-initiated self-degradation as resulting from the in-situ exothermic reactions between the reactants yielded from the dissolution of the non-reacted or partially reacted sodium silicate activator and the thermal degradation of the CMC. The magnitude of self-degradation depended on the CMC content; its effective content in promoting degradation was {ge}0.7%. In contrast, no self-degradation was observed from CMC-modified Class G well cement. For 200 C-autoclaved AACMs without CMC, followed by heating at temperatures up to 300 C, they had a compressive strength ranging from 5982 to 4945 psi, which is {approx}3.5-fold higher than that of the commercial Class G well cement; the initial- and final-setting times of this AACM slurry at 85 C were {approx}60 and {approx}90 min. Two well-formed crystalline hydration phases, 1.1 nm tobermorite and calcium silicate hydrate (I), were responsible for developing this excellent high compressive strength. Although CMC is an attractive, as a degradation-promoting additive, its addition to both the AACM and the Class G well cement altered some properties of original cementitious materials; among those were an extending their setting times, an increasing their porosity, and lowering their compressive strength. Nevertheless, a 0.7% CMC-modified AACM as self-degradable cementitious material displayed the following properties before its breakdown by water; {approx}120 min initial- and {approx}180 min final-setting times at 85 C, and 1825 to 1375 psi compressive strength with 51.2 to 55.0% porosity up to 300 C.

15 GEOTHERMAL ENERGY↗

DOE OSTI2019

Overhead Protection Increases Fuel Quality and Natural Drying of Leaf-On Woody Biomass Storage Piles

Short-rotation woody crops (SRWC) have the potential to make substantial contributions to the supply of biomass feedstock for the production of biofuels and bioproducts. This study evaluated changes in the fuel quality (moisture, ash, and heating value) of stored spring harvested shrub willow (Salix spp.) and hybrid poplar (Populus spp.) chips with respect to pile protection treatments, location within the storage piles, and length of storage. Leaf-on willow and poplar were harvested in the spring, and wood chips and foliage with moisture content in the range of 42.1% to 49.9% (w.b.) were stored in piles for five months, from May to October 2016. Three protection treatments were randomly assigned to the piles. The control treatment had no cover (NC), so piles were exposed to direct solar radiation and rainfall. The second treatment had a canopy (C) installed above the piles to limit direct rainfall. The final treatment had a canopy plus a dome aeration system (CD) installed over the piles. Covering piles reduced and maintained the low moisture content in wood chip piles. Within 30 days of establishment, the moisture content in the core of the C pile decreased to less than 30%, and was maintained between 24%–26% until the end of the storage period. Conversely, the moisture content in the NC piles decreased in the first two months, but then increased to the original moisture content in the core (>45 cm deep) and up to 70% of the original moisture content in the shell (<45 cm deep). For all the treatments in the tested conditions, the core material dried faster than the shell material. The higher heating value (HHV) across all the treatments increased slightly from 18.31 ± 0.06 MJ/kg at harvest to 18.76 ± 0.21 MJ/kg at the end of the storage period. The lower heating value (LHV) increased by about 50% in the C and CD piles by the end of the storage period. However, in the NC piles, the LHV decreased by 3% in the core and 52% in the shell. Leaf-on SRWC biomass stored in piles created in late spring under climatic conditions in central and northern New York showed differing moisture contents when stored for over 60–90 days. Overhead protection could be used to preserve or improve the fuel quality in terms of the moisture content and heating value if more than two months of storage are required. However, the implementation of such management practice will depend on whether the end users are willing to pay a higher price for dryer biomass and biomass with a higher LHV.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

A Millennium-long Evolution of the 1 yr Recurrence Period Nova—Search for Any Indication of the Forthcoming He Flash

We present 1500 cycles of hydrogen shell flashes on a 1.38 M{sub ⊙} white dwarf (WD) for a mass accretion rate of 1.6×10{sup −7} M{sub ⊙} yr{sup −1}, the mass ejection of which is calculated consistently with the optically thick winds. This model mimics the 1 yr recurrence period nova M31N 2008-12a. Through these hydrogen flashes a helium ash layer grows in mass and eventually triggers a helium nova outburst. Each hydrogen flash is almost identical, and there is no precursor for the forthcoming He flash either in the outburst or in the quiescent until the next He flash suddenly occurs. Thus, M31N 2008-12a is a promising candidate of He novae, outbursting in any time within a millennium. The prompt X-ray flash of He nova lasts as short as 15 minutes, with the X-ray luminosity being about half of the Eddington luminosity, making the observation difficult. In the very early phase of a He flash, the uppermost H-rich layer is convectively mixed into the deep interior and most of the hydrogen is consumed by nuclear burning. In comparison with hydrogen shell flashes of M31N 2008-12a, we expect the forthcoming He nova to have a very short prompt X-ray flash (15 minutes), a very bright optical/near-IR peak (∼3.5 mag brighter than M31N 2008-12a), a much longer nova duration (>2 yr), and a longer supersoft X-ray source phase (40–50 days or more).

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2017

Bond Durability of Carbon-Microfiber-Reinforced Alkali-Activated High-Temperature Cement Adhering to Carbon Steel

The study aims at evaluating the bond durability of a carbon microfiber (CMF)-reinforced alkali-activating calcium aluminate cement (CAC)/fly ash F (FAF) blend cementitious material adhering to carbon steel (CS) under stresses induced by a 350°C heat-25°C water cooling cycle. This cementitious material/CS joint sample was originally prepared in an autoclave at 300°C under a pressure of 8.3 MPa. For comparison, two reference geothermal well cements, Class G modified with silica (G) and calciumaluminum phosphate (CaP), were employed as well reinforced with CMF. In the CAC/FAF blending cement systems, the CAC-derived cementitious reaction products preferentially adhered to CS surfaces, rather than that of FAF-related reaction products. CMF played a pivotal role in creating tough interfacial bond structure of cement layer adhering to CS. The bond toughness also was supported by the crystalline cementitious reaction products including sodalite, brownmillerite, and hedenbergite as major phases, and aragonite, boehmite, and garronite as minor ones. The brownmillerite as an interfacial reaction product between cement and CS promoted the chemical bonding of the cement to CS, while the other phases served in providing the attractive bonding of the cement to CS. The post-stress-test joint samples revealed the formation of additional brown-millerite, aragonite, and garronite, in particular brownmillerite as the major one. The combination of chemical bonding and self-advancing adherence behavior of the cement was essential for creating a better interfacial bond structure. A similar interfacial bond structure was observed with CaP. The crystalline phase composition of the autoclaved cement revealed apatite, zeolite, and ferrowyllieite as major reaction products, and aragonite and al-katoite as the minor ones. Ferrowyllieite was identified as cement/CS interfacial reaction product contributing to the chemical bond of cement, while the other phases aided in providing the attractive bond of cement. After a stress test, two phases, ferrowyllieite and aragonite, promoted the self-advancing adherence of cement to CS. However, the effectiveness of these phases in improving adherence performance of cement was less than that of CAC/FAF blend cement, reflecting the fact that the bond durability of CAC/FAF blend cement was far better than that of the CaP. In contrast, the autoclaved silica-modified G cement consisting of xonotlite, and 0.9 nm-to-bermorite and riversideite, with calcite as the crystalline reaction products, had no significant effect on improving the shear bond strength and the bond’s toughness. No interaction product with CS was found in the cement adhering to CS. After a stress test, the calcite phase acted only to promote the self-advancing adherence of cement, but its extent was minimal compared with that of the other cements, thereby resulting in poor bond durability.

15 GEOTHERMAL ENERGY↗

DOE OSTI2014

An Alternative Interpretation of Plasma Selenium Data from Endangered Patagonian Huemul Deer ( Hippocamelus bisulcus )

The prevalence of osteopathology in 57% in the endangered adult Patagonian huemul deer (Hippocamelus bisulcus), malformed antler development, and general lack of recovery were previously suggested to possibly be related to mineral imbalances like selenium (Se) deficiency, and not to stem from fluorosis. From recent bone analyses of these diseased huemul, fluoride levels averaged 58 ppm (SE=10.7), thus eliminating fluorosis as a causal factor for the osteopathology reported in huemul. In contrast, when analyzing high-elevation sites commonly used by extant populations, we found soils deficient in Se. Ashes from recent volcanism also were very low in Se. As Se-responsive diseases in livestock have been documented in Chile, we reclassified recently published Se levels in huemul and determined that 73% were deficient and 18% marginal. Together with these several lines of indirect evidence, we conclude that Se deficiency plays a role in the lack of recovery of huemul populations.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS2010

Contamination Impact of Station Brush Fire on Cleanroom Facilities

Brush and forest fires, both naturally occurring and anthropogenic in origin, in proximity to space flight hardware processing facilities raise concerns about the threat of contamination resulting from airborne particulate and molecular components of smoke. Perceptions of the severity of the threat are possibly heightened by the high sensitivity of the human sense of smell to some components present in the smoke of burning vegetation.On August 26th, 2009, a brushfire broke out north of Pasadena, California, two miles from the Jet Propulsion Laboratory. The Station Fire destroyed over 160,000 acres, coming within a few hundred yards of JPL. Smoke concentrations on Lab were very heavy over several days. All Lab operations were halted, and measures were taken to protect personnel, critical hardware, and facilities. Evaluation of real-time cleanroom monitoring data, visualinspection of facilities, filter systems, and analysis of surface cleanliness samples revealed facility environments andhardware were minimally effected.Outside air quality easily exceeded Class Ten Million. Prefilters captured most large ash and soot; multi-stage filtration greatly minimized the impact on the HEPA/ULPA filters. Air quality in HEPA filtered spacecraft assembly cleanrooms remained within Class 10,000 specification throughout. Surface cleanliness was inimally affected, as large particles were effectively removed from the airstream, and sub-micron particles have extremely long settling rates. Approximate particulate fallout within facilities was 0.00011% area coverage/day compared to 0.00038% area coverage/day during normal operations. Deposition of condensable airborne components, as measured in real time, peaked at approximately1.0 ng/cm2/day compared to 0.05 ng/cm2/day nominal.

airborne particulate contamination↗

NASA NTRS2023

Analysis of the Solid Products from the OSCAR and the AOWG Trash Processing Systems

Two trash conversion systems that process space logistical trash for conversion into gases and liquids have minor solid product formation consisting of primarily high carbon ash, inorganic salts, and aluminum metal flakes. These solid products necessarily comprise part of the system output because the thermal degradation processes intentionally operate at temperatures below aluminum vaporization and do not convert all solid inorganics or carbon-based compounds into gaseous compounds (i.e., CO 2 or CH 4 ). The two systems included the Orbital Syngas/Commodity Augmentation Reactor (OSCAR) combustion system funded by the NASA Space Technology Mission Directorate (STMD) located at NASA’s Kennedy Space Center, and the Advanced Organic Waste Gasifier (AOWG) steam reforming system developed by Pioneer Astronautics in Lakewood, Colorado, and funded by the NASA Small Business Innovation Research (SBIR) Exploration Systems Development Mission Directorate (ESDMD). OSCAR residual solids were collected from suborbital flight and ground-based laboratory testing, while all AOWG samples were collected from ground testing. This report discusses the solid product characterization, including elemental analyses performed with scanning electron microscopy (SEM) with energy dispersive X-ray spectroscopy (EDS), and a surface chemistry performed with x-ray photoelectron spectroscopy (XPS). A particle size analysis was performed with sieves, followed by SEM analyses. These analyses were performed to elucidate what high value products can be extracted or utilized from the solid products for follow on infusion into chemical feedstocks, manufacturing additives, or in-situ construction-based material needs.

OSCAR↗

DOE OSTI2011

Zero Liquid Discharge (ZLD) System for Flue-Gas Derived Water From Oxy-Combustion Process

Researchers at the National Energy Technology Laboratory (NETL) located in Albany, Oregon, have patented a process - Integrated Pollutant Removal (IPR) that uses off-the-shelf technology to produce a sequestration ready CO{sub 2} stream from an oxy-combustion power plant. Capturing CO{sub 2} from fossil-fuel combustion generates a significant water product which can be tapped for use in the power plant and its peripherals. Water condensed in the IPR{reg_sign} process may contain fly ash particles, sodium (from pH control), and sulfur species, as well as heavy metals, cations and anions. NETL is developing a treatment approach for zero liquid discharge while maximizing available heat from IPR. Current treatment-process steps being studied are flocculation/coagulation, for removal of cations and fine particles, and reverse osmosis, for anion removal as well as for scavenging the remaining cations. After reverse osmosis process steps, thermal evaporation and crystallization steps will be carried out in order to build the whole zero liquid discharge (ZLD) system for flue-gas condensed wastewater. Gypsum is the major product from crystallization process. Fast, in-line treatment of water for re-use in IPR seems to be one practical step for minimizing water treatment requirements for CO{sub 2} capture. The results obtained from above experiments are being used to build water treatment models.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2011

Simultaneous leaching and carbon sequestration in constrained aqueous solutions

The behavior of metal ions leaching and precipitated mineral phases of metal-rich fly ash (FA) was examined in order to evaluate microbial impacts on carbon sequestration and metal immobilization. The leaching solutions consisted of aerobic deionized water (DW) and artificial eutrophic water (AEW) that was anaerobic, organic- and mineral-rich, and higher salinity as is typical of bottom water in eutrophic algae ponds. The Fe- and Ca-rich FAs were predominantly composed of quartz, mullite, portlandite, calcite, hannebachite, maghemite, and hematite. After 86 days, only Fe and Ca contents exhibited a decrease in leaching solutions while other major and trace elements showed increasing or steady trends in preference to the type of FA and leaching solution. Ca-rich FA showed strong carbon sequestration efficiency ranging up to 32.3 g CO(2)/kg FA after 86 days, corresponding to almost 65% of biotic carbon sequestration potential under some conditions. Variations in the properties of FAs such as chemical compositions, mineral constituents as well as the type of leaching solution impacted CO(2) capture. Even though the relative amount of calcite increased sixfold in the AEW and the relative amount of mineral phase reached 37.3 wt% using Ca-rich FA for 86 days, chemical sequestration did not accomplish simultaneous precipitation and sequestration of several heavy metals.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2011

A review on biomass classification and composition, cofiring issues and pretreatment methods

Presently around the globe there is a significant interest in using biomass for power generation as power generation from coal continues to raise environmental concerns. Biomass alone can be used for generation of power which can bring lot of environmental benefits. However the constraints of using biomass alone can include high investments costs for biomass feed systems and also uncertainty in the security of the feedstock supply due to seasonal variations and in most of the countries biomass is dispersed and the infrastructure for biomass supply is not well established. Alternatively cofiring biomass along with coal offer advantages like (a) reducing the issues related to biomass quality and buffers the system when there is insufficient feedstock quantity and (b) costs of adapting the existing coal power plants will be lower than building new systems dedicated only to biomass. However with the above said advantages there exists some technical constrains including low heating and energy density values, low bulk density, lower grindability index, higher moisture and ash content to successfully cofire biomass with coal. In order to successfully cofire biomass with coal, biomass feedstock specifications need to be established to direct pretreatment options that may include increasing the energy density, bulk density, stability during storage and grindability. Impacts on particle transport systems, flame stability, pollutant formation and boiler tube fouling/corrosion must also be minimized by setting feedstock specifications including composition and blend ratios if necessary. Some of these limitations can be overcome by using pretreatment methods. This paper discusses the impact of feedstock pretreatment methods like sizing, baling, pelletizing, briquetting, washing/leaching, torrefaction, torrefaction and pelletization and steam explosion in attainment of optimum feedstock characteristics to successfully cofire biomass with coal.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2012

Combustion and inorganic bromine emission of waste printed circuit boards in a high temperature furnace

Highlights: Black-Right-Pointing-Pointer The combustion efficiency of waste printed circuit boards (PCBs) depends on temperature, excess air factor, and high temperature zone residence time. Temperature has the most significant impact. Under the proposed condition, combustion of waste PCBs alone is quite complete within the furnace. Black-Right-Pointing-Pointer High temperature prompts a more complete bromine release and conversion. When temperature is high enough, 99.9% organobrominated compounds, the potential precursors for brominated dixoins formation, are destroyed efficiently and convert to inorganic bromine in flue gas, as HBr and Br{sub 2}. Black-Right-Pointing-Pointer Temperature has crucial influence over the inhibition of HBr conversion to Br{sub 2}, while the oxygen partial pressure plays a reverse role in the conversion to a very small extent. Increasing temperature will decrease the volume percentage ratio of Br{sub 2}/HBr in flue gas greatly. Black-Right-Pointing-Pointer The thermodynamic equilibrium approach of bromine conversion was investigated. The two forms of inorganic bromine in flue gas substantially reach thermodynamic equilibrium within 0.25 s. Under the proposed operating condition, the reaction of Br transfer and conversion finish. - Abstract: High temperature combustion experiments of waste printed circuit boards (PCBs) were conducted using a lab-scale system featuring a continuously-fed drop tube furnace. Combustion efficiency and the occurrence of inorganic bromine (HBr and Br{sub 2}) were systematically studied by monitoring the main combustion products continuously. The influence of furnace temperature (T) was studied from 800 to 1400 Degree-Sign C, the excess air factor (EAF) was varied from 1.2 to 1.9 and the residence time in the high temperature zone (RT{sub HT}) was set at 0.25, 0.5, or 0.75 s. Combustion efficiency depends on temperature, EAF and RT{sub HT}; temperature has the most significant effect. Conversion of organic bromine from flame retardants into HBr and Br{sub 2} depends on temperature and EAF. Temperature has crucial influence over the ratio of HBr to Br{sub 2}, whereas oxygen partial pressure plays a minor role. The two forms of inorganic bromine seem substantially to reach thermodynamic equilibrium within 0.25 s. High temperature is required to improve the combustion performance: at 1200 Degree-Sign C or higher, an EAF of 1.3 or more, and a RT{sub HT} exceeding 0.75 s, combustion is quite complete, the CO concentration in flue gas and remained carbon in ash are sufficiently low, and organobrominated compounds are successfully decomposed (more than 99.9%). According to these results, incineration of waste PCBs without preliminary separation and without additives would perform very well under certain conditions; the potential precursors for brominated dioxins formation could be destroyed efficiently. Increasing temperature could decrease the volume percentage ratio of Br{sub 2}/HBr in flue gas greatly.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2013

The Use of Subsurface Barriers to Support Treatment of Metals and Reduce the Flux of Tritium to Fourmile Branch at the Savannah River Site in South Carolina - 13358

The Savannah River Site (SRS) produced tritium, plutonium, and special nuclear materials for national defense, medicine, and the space programs. Acidic groundwater plumes containing metals, metallic radionuclides, non-metallic radionuclides and tritium sourced from the F and H Area Seepage Basins have impacted the surface water of Fourmile Branch on SRS. Tritium releases from Fourmile Branch have impacted the water quality within areas of the Savannah River adjacent to the SRS, and this circumstance has been an ongoing regulatory concern. The F and H Area Seepage Basins operated until 1988 for the disposition of deionized acidic waste water from the F and H Separations Facilities. The waste water contained dilute nitric acid and low concentrations of non-radioactive metals, and radionuclides, with the major isotopes being Cs-137, Sr-90, U-235, U-238, Pu-239, Tc-99, I-129, and tritium. The tritium concentration in the waste water was relatively elevated because there is not a practicable removal method in water. The acid content of the waste water during the operational period of the basins was equal to 12 billion liters of nitric acid. The seepage basins were closed in 1988 and backfilled and capped by 1991. The plumes associated with the F and H basins cover an area of nearly 2.4 square kilometers (600 acres) and discharge along ∼2,600 meters of Fourmile Branch. The acidic nature of the plumes and their overall discharge extent along the branch represent a large challenge with respect to reducing contaminant flux to Fourmile Branch. The introduction of nitric acid into the groundwater over a long time effectively reduced the retardation of metal migration from the basins to the groundwater and in the groundwater to Fourmile Branch, because most negatively charged surfaces on the aquifer materials were filled with hydrogen ion. Two large pump and treat systems were constructed in 1997 and operated until 2003 in an attempt to capture and control the releases to Fourmile Branch. The operating cost, including waste disposal, for the two systems was ∼$1.3 M/month. Both systems employed reinjection of tritiated water up gradient of the extraction, and produced large quantities of waste from non-tritium isotopes and metals removal prior to reinjection. Both systems were determined to be ineffective and potentially detrimental with respect to limiting the flux of contaminants to Fourmile Branch. After it became apparent that there was very little benefit to continued operation of the systems, and the staggering cost of operations was recognized by the SRS and regulators, a new remedy was developed. The new system uses vertical subsurface barriers to redirect groundwater flow to limit the transport of contaminants to the stream. The barriers were constructed of acid resistant grout using deep soil mixing techniques. The grout mixture used low swelling clay, fly ash, and sodium hydroxide to form a pozzolana material with low permeability and low strength. The SRS and regulators agreed to a series of remedial goals, with the first goal to reduce tritium flux to the stream by 70% and bring constituents other than tritium to groundwater protection standards. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2012

Grout Isolation and Stabilization of Structures and Materials within Nuclear Facilities at the U.S. Department of Energy, Hanford Site, Summary - 12309

Per regulatory agreement and facility closure design, U.S. Department of Energy Hanford Site nuclear fuel cycle structures and materials require in situ isolation in perpetuity and/or interim physicochemical stabilization as a part of final disposal or interim waste removal, respectively. To this end, grout materials are being used to encase facilities structures or are being incorporated within structures containing hazardous and radioactive contaminants. Facilities where grout materials have been recently used for isolation and stabilization include: (1) spent fuel separations, (2) uranium trioxide calcining, (3) reactor fuel storage basin, (4) reactor fuel cooling basin transport rail tanker cars and casks, (5) cold vacuum drying and reactor fuel load-out, and (6) plutonium fuel metal finishing. Grout components primarily include: (1) portland cement, (2) fly ash, (3) aggregate, and (4) chemical admixtures. Mix designs for these typically include aggregate and non aggregate slurries and bulk powders. Placement equipment includes: (1) concrete piston line pump or boom pump truck for grout slurry, (2) progressive cavity and shearing vortex pump systems, and (3) extendable boom fork lift for bulk powder dry grout mix. Grout slurries placed within the interior of facilities were typically conveyed utilizing large diameter slick line and the equivalent diameter flexible high pressure concrete conveyance hose. Other facilities requirements dictated use of much smaller diameter flexible grout conveyance hose. Placement required direct operator location within facilities structures in most cases, whereas due to radiological dose concerns, placement has also been completed remotely with significant standoff distances. Grout performance during placement and subsequent to placement often required unique design. For example, grout placed in fuel basin structures to serve as interim stabilization materials required sufficient bearing i.e., unconfined compressive strength, to sustain heavy equipment yet, low breakout force to permit efficient removal by track hoe bucket or equivalent construction equipment. Further, flow of slurries through small orifice geometries of moderate head pressures was another typical design requirement. Phase separation of less than 1 percent was a typical design requirement for slurries. On the order of 30,000 cubic meters of cementitious grout have recently been placed in the above noted U.S. Department of Energy Hanford Site facilities or structures. Each has presented a unique challenge in mix design, equipment, grout injection or placement, and ultimate facility or structure performance. Unconfined compressive and shear strength, flow, density, mass attenuation coefficient, phase separation, air content, wash-out, parameters and others, unique to each facility or structure, dictate the grout mix design for each. Each mix design was tested under laboratory and scaled field conditions as a precursor to field deployment. Further, after injection or placement of each grout formulation, the material was field inspected either by standard laboratory testing protocols, direct physical evaluation, or both. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2017

Preparation, Performance and Mechanism of Tc and I Getters in Cementitious Waste Forms - 17124

Cementitious waste forms offer a low temperature, cost effective technology for the solidification of liquid wastes. At the Department of Energy Hanford Site, 99-Tc and 129-I are radionuclides contained within low activity waste (LAW) which contribute significantly to environmental impacts associated with clean-up of the site. Cast Stone, a cementitious waste form comprised of 47 wt% blast furnace slag, 45 wt% fly ash and 8 wt% ordinary Portland cement, has undergone investigation as a possible candidate technology for the solidification of LAW. In screening tests using EPA Method 1315 leach testing of various mixes of Cast Stone with simulated LAW, Tc observed effective diffusivities (Dobs) had an average of 5.3 x 10-11 cm{sup 2}/s and I Dobs had an average of 5.7 x 10-9 cm{sup 2}/s. From these measurements, an opportunity exists to improve retention of Tc and I by Cast Stone. One approach to accomplish this is through the incorporation of Tc and I getters to selectively sequester Tc and I in the waste stream and eventual waste form. Initial testing conducted at PNNL identified potassium metal sulfide (KMS-2) and Sn(II)-apatite (Sn-A) as the strongest performing Tc getters and silver exchanged zeolite (Ag-Z) as the top performing I getter. This research also demonstrated that the Tc and I getters, when added to solution simultaneously, can have deleterious interactions with one another and lower the Tc and I removal levels. However, these interactions can be overcome through sequential treatment of solution with the getters. Cast Stone samples were fabricated using a 6.5 M Na average LAW simulant spiked with Tc and I with the addition of various combinations of Tc and I getters. Through EPA Method 1315 and Method 1313 testing it was found that the KMS-2 Tc getter was most successful at lowering Tc Dobs. The I getters were not effective, as apparent interference from sulfide components of the waste form may have led to dissociation of the AgI formed by the Ag-Z getter in sequestering the I from solution. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗