SummaryEffective decontamination of alkaline solutions and Hanford Site tank waste simulants from technetium has been accomplished by reductive coprecipitation with iron(II1) hydroxide. Addition of 1 M (NH4),Fe(S04), to 0.5 to 4.0 M NaOH to a final concentration of 0.1 to 0.15 M coprecipitates more than 99% of the technetium from 0.5 to 1.0 &j NaOH and 98 to 96% from 2.0 to 4.0 M NaOH. Similar results were obtained by reduction of Tc(VII) with 0.1 to 0.15 &j hydrazine and subsequent addition of FeCI, to a final concentration of 0.15 M. Inclusion of four complex-fonning agents rO.01 &j phosphate, 0.1 M EDTA (ethylenediaminetetraacetate), 0.03 M citrate, and 0.1 M glycolate (HOCH,CO;)] to the alkaline solution decreases technetium coprecipitation with iron hydroxide to 85% under otherwise similar conditions. Inclusion of 0.04 M NqCrO, drastically decreases reductive coprecipitation of Tc(VII) in 0.5 to 4.0 M NaOH. Iron(I1) salt, added to a 0.07 M excess over that of chromate, completely reduces chromate and provides greater than 99% coprecipitation of technetium with product iron(II1) and chromium(II1) hydroxides. Technetium(VI1) reduction by hydrazine is slow in the presence of chromate in alkaline solution, and technetium coprecipitation is incomplete in these conditions. Decontamination of an alkaline Hanford Site tank waste simulant, containing 0.04 &j chromate and eleven salts and complex-forming agents, by adding 1 M iron(I1) salt solution was studied.Coprecipitation of 15 to 28% of the technetium and more than 99% of the plutonium occurred in the Fe/Cr(III) hydroxide precipitate produced by adding 0.05 to 0.10 _M iron@). Chromate reduction was incomplete. About 75% of the technetium was coprecipitated, and the chromate was completely reduced, after adding 0.2 _M iron@) salt.Technetium(VI1) capture from 0.5 to 4.0 M NaOH was insignificant or incomplete on coprecipitation carriers Pe(OH),, Cr(OH),, Mn(OH),, Co(OH),, Co(OH),J obtained by the Method of Appearing Reagents under conditions providing complete capture of Np(V) and Pu(V1). Under the same conditions, cesium-137 capture is insignificant and strontium-90 capture is incomplete with these metal hydroxide carriers. Sodium diuranate coprecipitation from 0.5 to 4 M NaOH removed about 15 to 60? -of the technetium; sodium uranate coprecipitation removed 98 to 99% of the 90Sr, and 1 to 12% of the l3'CS.Reductive sorption of Tc(VI1) on metals (Zn, Cry Sn, and two Pb alloys) from 0.5 to 4 M NaOH and from alkaline waste simulant provided poor decontamination of these solutions. In contrast, greater than 98% of the plutonium(V1) was sorbed on chromium from 0.5 M NaOH at a surface area to volume ratio of 1.6 cm-'.