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[en] A process for removing aluminum from tank waste simulants by adding lithium and precipitating Li-Al-dihydroxide (Lithiumhydrotalcite, (LiAl2(OH)6)+X-) has been verified. The tests involved a double-shell tank (DST) simulant and a single-shell tank (SST) simulant. In the case of the DST simulant, the product was the anticipated Li-hydrotalcite. For the SST simulant, the product formed was primarily Li-phosphate. However, adding excess Li to the solution did result in the formation of traces of Li-hydrotalcite. The Li-hydrotalcite from the DST supernate was an easily filterable solid. After four water washes the filter cake was a fluffy white material made of < 100 (micro)m particles made of smaller spheres. These spheres are agglomerates of ∼ 5 (micro)m diameter platelets with < 1 (micro)m thickness. Chemical and mineralogical analyses of the filtrate, filter cake, and wash waters indicate a removal of 90+ wt% of the dissolved Al for the DST simulant. For the SST simulant, the main competing reaction to the formation of lithium hydrotalcite appears to be the formation of lithium phosphate. In case of the DST simulant, phosphorus co-precipitated with the hydrotalcite. This would imply the added benefit of the removal of phosphorus along with aluminum in the pre-treatment part of the waste treatment and immobilization plant (WTP). For this endeavor to be successful, a serious effort toward process parameter optimization is necessary. Among the major issues to be addressed are the dependency of the reaction yield on the solution chemistry, as well as residence times, temperatures, and an understanding of particle growth.