The solid sludges resulting from biodenitrification ofdiscarded aluminum nitrate arethe largest Y-12 Plantprocess solid waste.Aluminum nitrate feedstocks alsorepresent a major plantmaterials cost.The chemical constraints on aluminum nitrate recycle were investigated todetermine the feasibility ofincreasing recycle whilemaintaining acceptable aluminum nitrate purity. Reportedphasebehavior ofanalogous systems, together with benchresearch, indicated thatitwouldbe possible toraise therecycle ratefrom 35% to between70 and 90% by successive concentration and recrystallization ofthe motherliquor. A full scale pilot test successfully confirmed theability toobtain 70% recycle inexisting process equipment. Thiswork indicates thepossibility ofincreasing recycle rates above70%. Fluoride accumulation isexpected to piacean upperlimit on aluminum nitrate recycle. Better control and removaloffluorides, asbothinsoluble tankprecipitates and free fluorides, is neededtoholdcorrosion toacceptable levels. Minimizing theintroduction offluorides into therecycle systemis, ofcourse, the most effective method offluoride control. Analysis oftheconcentrations ofthe process streamsindicated thatvalence I and II cations didnotconcentrate inthealuminum nitrate crystals. However,valence IIIcations, whicharesimilar toaluminum inchemical behavior, wereless wellseparated. Methods for selectively concentrating and removingthesematerials will be neededatveryhigh aluminum nitrate recovery rates. Modification ofthecentrifuge systemto provide separate collection ofcrystal wash streamscan decrease accumulation ofvalence IIIcation contaminants. Changesintheextraction process producing acidic aluminum nitrate raffinates coulddecrease two historic problems, accumulation ofoxalate precipitates (a carbitol degradation product) and any organics contributing to surface fouling. Standard methodsforformally collecting and evaluating results on productquality couldform the basis fortheEVOPS, or evolutionary operating process standards, procedure neededto permitmaximum recycle withoutloss ofproductquality duringthe implementation of plannedprocess changes.