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PNNL-13501 - Pacific Northwest National Laboratory

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monolith is mechanically robust and tough and is much<br />

more homogeneous than samples produced using a slower<br />

cross-linking agent.<br />

Figure 3. 50% polystyrene-butadiene/50% epoxy resin<br />

waste form loaded with 20 wt% NaNO 3 synthesized using a<br />

fast acting cross-linking agent<br />

The impact of this improved homogeneity on leach<br />

resistance is shown in Figure 4, which shows the<br />

percentage of salt retained in samples loaded with 20 wt%<br />

NaNO3 as a function of time immersed in water. Salt<br />

retention was calculated from the conductivity of the<br />

immersion solution. The data indicate that using a faster<br />

cross-linking agent (20 minutes versus several hours)<br />

reduces the leaching rate by a factor of about 50. Similar<br />

improvements in salt retention were measured for waste<br />

forms loaded with 30 and 40 wt% NaNO3. It is<br />

speculated that speeding up the cross-linking rate<br />

counteracts a tendency for the emulsion to coarsen with<br />

time in the presence of the high salt concentration.<br />

Summary and Conclusions<br />

Commercially available styrene/butadiene and acrylic<br />

latex emulsions are good precursors for use in the<br />

aqueous fabrication of waste forms. When mixed with<br />

emulsified epoxy resins, they react to form monoliths<br />

with tough physical properties and good water resistance<br />

without generating significant volatile organic compound<br />

or flammability problems. The resulting waste forms can<br />

% Salt Retained<br />

100<br />

90<br />

80<br />

70<br />

60<br />

50<br />

40<br />

30<br />

20<br />

PAC-EP composite<br />

10<br />

0<br />

PSB-EP composite (slow crosslinking)<br />

PSB-EP composite (fast crosslinking)<br />

0 10 20 30<br />

Time (min)<br />

40 50 60<br />

Figure 4. Leaching behavior of aqueous-based waste forms<br />

loaded with 20 wt% NaNO 3 measured as percentage of salt<br />

retained in the sample<br />

physically incorporate large amounts of salt (up to 60%<br />

sodium nitrate) and their leach resistance is markedly<br />

improved by using fast acting cross-linking agents.<br />

These results represent an important step in developing<br />

aqueous-based polyceram flowsheets. While preliminary<br />

in nature, they indicate that optimization of the current<br />

system and extension to systems which incorporate an<br />

inorganic or ceramic component should produce materials<br />

with very attractive characteristics for encapsulating and<br />

storing a wide variety of low-level wastes. Future work<br />

will establish the optimal performance of the current<br />

formulations through adjustment of solution pH, salt<br />

content and composition, surfactant, cross-linking<br />

initiator, curing time and temperature, and micelle<br />

concentration. Also, quantum improvements in<br />

performance will be sought by developing routes to<br />

incorporate an inorganic component to form polyceram<br />

waste forms.<br />

Reference<br />

Smith G and BJJ Zelinski. 1999. Stabilize High Salt<br />

Content Waste Using Sol Gel Process. OST Reference<br />

#2036, Mixed Waste Focus Area, Prepared for U.S.<br />

Department of Energy, Office of Environmental<br />

Management, Office of Science and Technology,<br />

Washington, D.C.<br />

Materials Science and Technology 313

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