Process for the removal of 99Tc from liquid intermediate level waste of spent fuel reprocessing

Abstract

Provided herein is a process for removal of .sup.99Tc from liquid intermediate level waste (ILW) of spent fuel reprocessing including the steps of: adding HNO.sub.3 to ILW till the pH is 2 to destroy the carbonates, transferring the ILW derived of carbonates to a tank containing mild steel wool (msw) for 4 to 48 hrs, subjecting the ILW and MS Wool to the step of separation, discharging the supernatant solution free of .sup.99Tc and retaining the corrosion products (goethite(FeOOH/magnetite), subjecting the said corrosion products to the step of vitrification, and storing the said vitrified .sup.99Tc bearing waste.

Claims

1. A process for removal of .sup.99Tc from liquid intermediate level waste (ILW) of spent fuel reprocessing comprising: adding HNO.sub.3 to ILW until the pH is 2, to destroy carbonates; transferring the ILW deprived of carbonates to a tank containing mild steel wool for 4 to 48 hrs; subjecting the ILW and mild steel wool to a step of separation to generate a supernatant solution which is free of 99Tc and a corrosion product bearing 99Tc; discharging the supernatant solution free of 99Tc and retaining the corrosion product; subjecting the corrosion product to a step of vitrification to produce vitrified 99Tc bearing waste; and storing the vitrified 99Tc bearing waste.

2. The process as claimed in claim 1, wherein a ratio of ILW volume to mild steel wool in the tank is 1:10.

3. The process as claimed in claim 1, further comprising enhancing mixing and contact between the mild steel wool and the liquid through air bubbling.

4. The process as claimed in claim 1, wherein said 99Tc bearing corrosion product is vitrified and immobilized in glass waste form, minimizing volatilization of 99Tc during vitrification.

5. The process as claimed in claim 1, wherein composition of mild steel wool used is as follows: TABLE-US-00002 Percentage Element (%) C 0.10-0.20 S 0.02-0.03 P 0.02-0.03 Mn 0.2-1.2 Si 0.02-0.07 Cr 0.02-0.04 Ni 0.01-0.02 Mo 0.01-0.02.

Description

BRIEF DESCRIPTION OF THE ACCOMPANYING DRAWING

(1) FIG. 1: show the illustrates the basic process flowchart for removal of .sup.99Tc from liquid intermediate level waste (ILW).

DETAILED DESCRIPTION OF THE INVENTION

(2) .sup.99Tc arising from spent fuel reprocessing is a major radiation concern owing to a combination of high thermal fission yield (6%), long half life (2.1310.sup.5 y), high environmental mobility in oxidized pertechnate form combined with radioactivity as a -emitter. Further, .sup.99Tc presents a challenge to conventional high temperature vitrification in a borosilicate glass matrix owing to its volatility at glass synthesis temperatures.

(3) As a result, efforts are underway to capture and sequestrate .sup.99Tc using ion exchange resins (elutable and non-elutable), crown ethers or capture in mineral phases. Indeed, it is known that .sup.99Tc can be sequestrated into various mineral phases including perovskites, rutile, sodalite, trevorite, goethite and magnetite to name a few. However, the preparation of most of these phases requires high temperature conditions. Efforts to utilize goethite/magnetite to capture .sup.99Tc from Sanford Low Activity Waste (LAW) were carried out on bench scale by co-precipitating goethite in the LAW solutions. While Tc capture using goethite was demonstrated in these studies, the ferrihydrite precursor for goethite formation was synthesized ex-situ under anoxic conditions. Synthesis, and particularly storage, of ferrihydrite is challenging due to its instability and its conversion to Fe.sub.3O.sub.4 upon exposure to air oxygen. It has also been demonstrated that ex-situ synthesized Fe.sub.3O.sub.4 does not show Tc uptake.

(4) It is clear from literature that mineralization of Tc in Fe-oxides/oxyhydroxides is well known. Indeed, such take-up has been the subject of several papers and reports listed in the prior art (and references therein). Also well known is that mild steel can corrode in aqueous environment to produce iron oxides/oxy-hydroxide phases as corrosion product. In the process developed, we exploit corrosion of mild steel to produce the iron oxide/oxy-hydroxide phases required for Tc sequestration, while avoiding ex-situ synthesis of ferrihydrite under demanding anoxic conditions.

(5) We utilize the corrosion of mild steel (TechSorb) in acidic aqueous environment of the pH adjusted intermediate level waste (ILW) to generate goethite and/or magnetite in-situ, avoiding the necessity of anoxic conditions for ex-situ synthesis of ferrihydrite, greatly improving process applicability. In order to ensure that adequate quantity of corrosion product is formed, pH in the range 2-8 is required. If carbonate species are present in the ILW, they act as a pH buffer and prevent pH reduction below 9. In the pH range of 9 or greater, steel corrosion by galvanic process is extremely low owing to OH.sup. neutralization of anodic sites on the steel. Consequently, carbonate destruction by acid addition up to pH 2, may be required if the ILW is carbonate bearing.

(6) At pH 2, mild steel corrosion is extremely rapid, and the release of Fe.sup.2+ ions from the surface of the corroding steel also generates OH.sup. in the ILW, consequently raising its pH. In approximately 4-8 hours depending upon the ILW volume to mild steel mass ratio V/m (ranging from 100 ml.Math.g.sup.1-1000 ml.Math.g.sup.1), adequate goethite/iron oxy-hydroxide phase is formed. Phase formation is significantly accelerated by increasing temperature to 60 C. The number of Tc counts of the liquid waste reduces by over 99%, with the Tc activity being concentrated in the precipitated phase, both settled and also trapped in the mild steel wool. Goethite is able to take up Tc as it precipitates in ILW and there was no significant difference in Tc uptake behavior even with air or nitrogen bubbling through the ILW, indicating that adequate dissolved oxygen is already present in the liquid ILW.

(7) Changing the pH to 4 or 6 maintaining a V/m of 100 ml.Math.g.sup.1 slows the process down as Fe.sup.2+ release from the mild steel wool is slower at less acidic pH. However, 99%+ removal of .sup.99Tc was again obtained, but after 48 hours. It was observed that at pH 4 or pH 6, the volume of precipitated goethite is significantly less than in case of pH 2 owing to the less aggressive nature of the ILW at pH4 or pH 6 toward the mild steel wool. The quantity of corrosion product formed was lower still at pH8. However, in all cases, the quantity of goethite formed is sufficient to remove Tc from the ILW stream.

(8) The process is also effective for Tc sequestration from saline/sea water. In such a case also, one of the corrosion products formed is likely to be goethite, which may be instrumental in Tc sequestration. In case of sea water, 95% Tc removal has been demonstrated in approximately two hours.

(9) Tc free liquid can be directly discharged to environment. Additionally, the process also demonstrates substantial pick-up of Ru (80%) and Sb (>99%). .sup.99Tc bearing goethite phase is then collected for immobilization. Since .sup.99Tc has entered the crystal lattice of Goethite, it will not be released and/or volatilized during high temperature vitrification operations, allowing .sup.99Tc to be incorporated into a durable vitreous wasteform, which will ensure its isolation from the biosphere.

(10) The various steps in the process, as numbered, are described below: Carbonate destruction in ILW containing .sup.99Tc (1) by addition of HNO.sub.3 (2) is carried out till pH2 is attained. This allows complete removal of the carbonate-bicarbonate buffering action, allowing pH to be adjusted in the range 2-8 (3). ILW is then transferred to a tank containing mild steel wool (4). ILW volume to mild steel mass ratio (V/m) is between 100 ml.Math.g.sup.1 and 1000 ml.Math.g.sup.1. ILW is then allowed to stand in the tank between 4 h and 48 h, in contact with the mild steel wool. If the volume of ILW is large, then enhanced mixing and contact between the mild steel wool and the liquid can be ensured through air bubbling In this time, corrosion product of mild steel, goethite (FeOOH) and/or magnetite will precipitate in-situ and take up .sup.99Tc into their crystal lattice. The corrosion products (goethite (FeOOH)/magnetite) are separated from the waste, and the supernatant solution, now free of .sup.99Tc (6) can be safely discharged (7). .sup.99Tc bearing goethite (FeOOH)/magnetite (8) can be vitrified and immobilized in a glass wasteform (9). Since .sup.99Tc is harbored in goethite (FeOOH)/magnetite phase, volatilization of .sup.99Tc during vitrification is minimized. The vitrified .sup.99Tc bearing waste form is then stored securely (10).

(11) Composition range of mild steel wool used is as follows:

(12) TABLE-US-00001 Percentage Element (%) C 0.10-0.20 S 0.02-0.03 P 0.02-0.03 Mn 0.2-1.2 Si 0.02-0.07 Cr 0.02-0.04 Ni 0.01-0.02 Mo 0.01-0.02

EXAMPLES

Example 1: Performance of Mild Steel Wool in 99Tc Containing Intermediate Level Waste (ILW) at pH 2, V/m=100 ml.Math.g1

(13) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. After ensuring that solution pH remains stable at 2 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.5 g of mild steel wool to obtain V/m of 100 ml.Math.g.sup.1. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(14) After 4 hours, the solution pH was measured to be 6.60, while the number of counts in the solution was approximately 86 counts per ml per 100 seconds, which implies a removal of 99.7% of .sup.99Tc from the solution. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 2: Performance of Mild Steel Wool in 99Tc Containing Intermediate Level Waste (ILW) at pH 2, V/m=200 ml.Math.g1

(15) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. After ensuring that solution pH remains stable at 2 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.25 g of mild steel wool to obtain V/m of 200 ml.Math.g.sup.1. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(16) After 4 hours, the solution pH was measured to be 6.05, while the number of counts in the solution was approximately 69 counts per ml per 100 seconds, which implies a removal of 99.7% of .sup.99Tc from the solution. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 3: Performance of Mild Steel Wool in 99Tc Containing Intermediate Level Waste (ILW) at pH 2, V/m=500 ml.Math.g1

(17) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. After ensuring that solution pH remains stable at 2 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.1 g of mild steel wool to obtain V/m of 500 ml.Math.g.sup.1. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(18) After 4 hours, the solution pH was measured to be 6.05, while the number of counts in the solution was approximately 69 counts per ml per 100 seconds, which implies a removal of 99.7% of .sup.99Tc from the solution. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 4: Performance of Mild Steel Wool in 99Tc Containing Intermediate Level Waste (ILW) at pH 2, V/m=1000 ml.Math.g1

(19) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. After ensuring that solution pH remains stable at 2 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.05 g of mild steel wool to obtain V/m of 1000 ml.Math.g.sup.1. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(20) After 24 hours, the solution pH was measured to be 5.69, while the number of counts in the solution was approximately 51 counts per ml per 100 seconds, which implies a removal of 99.8% of .sup.99Tc from the solution. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 5: Performance of Mild Steel Wool in 99Tc Containing Intermediate Level Waste (ILW) at pH 2, V/m=100 ml.Math.g1; with Nitrogen Gas Bubbling

(21) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. After ensuring that solution pH remains stable at 2 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.5 g of mild steel wool to obtain V/m of 100 ml.Math.g.sup.1. Also, nitrogen gas was bubbled through the ILW solution in the conical flask for the duration of the experiment, for agitation mixing and to demonstrate Tc sequestration even under reduced oxygen availability in the ILW solution. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(22) After 8 hours, the solution pH was measured to be 7.09, while the number of counts in the solution was approximately 77 counts per ml per 100 seconds, which implies a removal of 99.7% of .sup.99Tc from the solution. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 6: Performance of Mild Steel Wool in 99Tc Containing Intermediate Level Waste (ILW) at pH 2, V/m=100 ml.Math.g1; with Air Bubbling

(23) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. After ensuring that solution pH remains stable at 2 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.5 g of mild steel wool to obtain V/m of 100 ml.Math.g.sup.1. Also, air was bubbled through the ILW solution in the conical flask for the duration of the experiment, in order to provide agitation and also increase oxygen availability in the ILW solution. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(24) After 4 hours, the solution pH was measured to be 5.97, while the number of counts in the solution was approximately 80 per ml per 100 seconds, which implies a removal of 99.7% of .sup.99Tc from the solution. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 7: Performance of Mild Steel Wool in 99Tc Containing Intermediate Level Waste (ILW) at pH 4, V/m=100 ml.Math.g1

(25) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. Solution pH was then adjusted to 4, by addition of NH.sub.4OH solution. After ensuring that solution pH remains stable at 4 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.5 g of mild steel wool to obtain V/m of 100 ml.Math.g.sup.1. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(26) After 48 hours, the solution pH was measured to be 7.93, while the number of counts in the solution was approximately 59 per ml per 100 seconds, which implies a removal of 99.8% of .sup.99Tc from the solution. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 8: Performance of Mild Steel Wool in 99Tc Containing Intermediate Level Waste (ILW) at pH 6, V/m=100 ml.Math.g1

(27) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. Solution pH was then adjusted to 6, by addition of NH.sub.4OH solution. After ensuring that solution pH remains stable at 6 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.5 g of mild steel wool to obtain V/m of 100 ml.Math.g.sup.1. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(28) After 48 hours, the solution pH was measured to be 7.87, while the number of counts in the solution was approximately 40 per ml per 100 seconds, which implies a removal of 99.8% of .sup.99Tc from the solution. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 9: Performance of Mild Steel Wool in 99Tc Containing Intermediate Level Waste (ILW) at pH 8, V/m=100 ml.Math.g1

(29) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. Solution pH was then adjusted to 8, by addition of NH.sub.4OH solution. After ensuring that solution pH remains stable at 6 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.5 g of mild steel wool to obtain V/m of 100 ml.Math.g.sup.1. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(30) After 48 hours, the solution pH was measured to be 7.96, while the number of counts in the solution was approximately 97 per ml per 100 seconds, which implies a removal of 99.7% of .sup.99Tc from the solution. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 10: Performance of Mild Steel Wool in Pure 99Tc Acidic Solution

(31) .sup.99Tc was picked up from ILW on anion exchange resin, and then eluted using M HNO.sub.3. NH.sub.4OH was then used to adjust solution pH to nearly 8. After ensuring that solution pH remains stable at 6 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.5 g of mild steel wool to obtain V/m of 100 ml.Math.g.sup.1. The eluted solution exhibited around 1200 counts per ml per 100 seconds.

(32) After 24 hours, the solution pH was 8.1, while the number of counts in the solution was approximately 126 per ml per 100 seconds, which implies a removal of 90% of .sup.99Tc from the solution. Black corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be Fe.sub.3O.sub.4 (magnetite). Pure Tc bearing solution was free of carbonates, which removed the need for carbonate destruction.

Example 11: Performance of Mild Steel Wool in 99Tc Containing Intermediate Level Waste (ILW) at pH 2, V/m=100 ml.Math.g1, Temperature 60 C. with Air Bubbling

(33) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. After ensuring that solution pH remains stable at 2 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.5 g of mild steel wool to obtain V/m of 100 ml.Math.g.sup.1. The conical flask was placed in a water bath heated to 60 C. Also, air was bubbled through the ILW solution in the conical flask for the duration of the experiment. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(34) After 30 minutes, the solution pH was measured to be 5.57, while the number of counts in the solution was approximately 79 counts per ml per 100 seconds, which implies a removal of 99.7% of .sup.99Tc from the solution. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 12: Performance of Mild Steel Wool in 99Tc Containing Intermediate Level Waste (ILW) at pH 2, V/m=200 ml.Math.g1, Temperature 60 C. with Air Bubbling

(35) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. After ensuring that solution pH remains stable at 2 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.25 g of mild steel wool to obtain V/m of 200 ml.Math.g.sup.1. The conical flask was placed in a water bath heated to 60 C. Also, air was bubbled through the ILW solution in the conical flask for the duration of the experiment. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(36) After 1 hour, the solution pH was measured to be 5.82, while the number of counts in the solution was approximately 90 counts per ml per 100 seconds, which implies a removal of 99.6% of .sup.99Tc from the solution. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 13: Performance of Mild Steel Wool in Tc Containing Intermediate Level Waste (ILW) at pH 2, V/m=500 ml.Math.g1, Temperature 60 C. with Air Bubbling

(37) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. After ensuring that solution pH remains stable at 2 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.1 g of mild steel wool to obtain V/m of 500 ml.Math.g.sup.1. The conical flask was placed in a water bath heated to 60 C. Also, air was bubbled through the ILW solution in the conical flask for the duration of the experiment. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(38) After 2 hours, the solution pH was measured to be 5.11, while the number of counts in the solution was approximately 95 counts per ml per 100 seconds, which implies a removal of 99.6% of .sup.99Tc from the solution. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 14: Performance of Mild Steel Wool in Tc Containing Intermediate Level Waste (ILW) at pH 2, V/m=1000 ml.Math.g1, Temperature 60 C. with Air Bubbling

(39) .sup.99Tc containing ILW was treated with HNO.sub.3 such that carbonate present in the waste was completely destroyed at pH 2. After ensuring that solution pH remains stable at 2 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to a conical flask containing 0.05 g of mild steel wool to obtain V/m of 1000 ml.Math.g.sup.1. The conical flask was placed in a water bath heated to 60 C. Also, air was bubbled through the ILW solution in the conical flask for the duration of the experiment. The most significant activity contributor in the ILW was .sup.99Tc with total counts of 25,000 per ml per 100 seconds of ILW.

(40) After 4 hours, the solution pH was measured to be 4.93, while the number of counts in the solution was approximately 97 counts per ml per 100 seconds, which implies a removal of 99.6% of .sup.99Tc from the solution. An increase in temperature to 60 C. allows 99.6% Tc removal in 4 hours, while for the same V/m, removal time was nearly 24 h at room temperature. A reddish brown corrosion product is formed, which settles to the bottom and most of the original activity of the ILW is concentrated in this phase, both settled and also adhering to the wool. Since the corrosion product settles to the bottom, separation is quite simple. The colour of the corrosion product indicates that the material formed is most likely to be FeOOH (goethite).

Example 15: Performance of Mild Steel Wool in 99Tc Containing Sea at pH 2, V/m Varying from 100-1000 ml.Math.g1, with Air Bubbling at Room Temperature

(41) .sup.99Tc containing sea water was adjusted to pH2 by HNO.sub.3 addition. After ensuring that solution pH remains stable at 2 for 30 minutes-1 hour, 50 ml of the pH adjusted waste was transferred to conical flasks containing required quantity of mild steel wool to obtain V/m of 100 ml.Math.g.sup.1-1000 ml.Math.g.sup.1. Air was bubbled through the solutions in the conical flasks for the duration of the experiments. The most significant activity contributor in the sea water was .sup.99Tc with total counts of 1600 per ml per 100 seconds of ILW.

(42) For all the above experiments, over 95% Tc removal was obtained between 2 h and 20 h, with solution pH after this time ranging from approximately 5 to 7. Reddish brown corrosion product is formed.

Example 16: Studies into Ru and Sb Uptake from Tc Bearing ILW

(43) Samples from experiments above, pre and post Tc removal were analyzed for potential Ru and Sb uptake by -spectroscopy. These measurements indicate substantial pick-up of Ru (80%) and Sb (>99%).

(44) General Statements:

(45) 1. Tc removal is faster at higher V/m 2. For a given V/m Tc removal is augmented by increasing temperature (60 C. in our experiments) 3. The presence of Cl.sup. and SO.sub.4.sup.2 in the liquid is likely to enhance formation of goethite/magnetite as corrosion products, which may result in accelerated Tc pick-up in such environments 4. Presence of carbonate-bicarbonate in waste inhibits formation of corrosion products, thus interfering with Tc uptake 5. The method used above also demonstrates substantial pick-up of Ru (80%) and Sb (>99%).