초록 ▼

The present invention is directed to an improved reaction process that allows for the achievement of excellent NF3 production yields, while minimizing the amount of unreacted fluorine exiting with the process gases and minimizing the amount of liquid melt waste (HF/NH3) produced by the process. The

The present invention is directed to an improved reaction process that allows for the achievement of excellent NF3 production yields, while minimizing the amount of unreacted fluorine exiting with the process gases and minimizing the amount of liquid melt waste (HF/NH3) produced by the process. The basic NF3 process resides in reacting F2 with an ammonium ion source, e.g., ammonium acid fluoride, under conditions for forming NF3. The improvement in the process comprises: introducing F2 and said ammonium ion source cocurrently and downflow through a packed column or monolith column at a first temperature; reacting said F2 and ammonium ion source in said column; and, removing a mixture of NF3 and byproducts from said column at a second temperature higher than said first temperature.

대표청구항 ▼

The invention claimed is: 1. A process for producing NF3 by the fluorination of an ammonium ion source which comprises: introducing a liquid mixture comprised of F2 and an ammonium ion source to an inlet of a column selected from the group consisting of random packing column and structured packing

The invention claimed is: 1. A process for producing NF3 by the fluorination of an ammonium ion source which comprises: introducing a liquid mixture comprised of F2 and an ammonium ion source to an inlet of a column selected from the group consisting of random packing column and structured packing column; passing said liquid mixture cocurrently through the column whereby reaction of said F2 and ammonium ion source occurs in said column generating a reaction product comprised of NF3 and byproduct HF; removing a reaction product containing NF3 from an exit of said column; maintaining conditions such that the temperature of the liquid mixture comprised of reactant F2 and said ammonium ion source introduced to the inlet of said column is lower than the temperature of the reaction product at the exit of said column, and thereby establishing a temperature rise in said column; and, recovering NF3 from the reaction product. 2. The process of claim 1 wherein the ammonium ion source is selected from the group consisting of NH4NO3, (NH 4)3PO4, (NH4)2SO4, (NH4)2CO3, NH4HCO3, NH 4HSO4, NH4IO4, NH4ClO4, and NH4BrO4; NH3, NH4F, NH4 HF2, NH4Cl, NH4Br, NH4I, NH4 NO3, (NH4)3PO4, (NH4) 2SO4, (NH4)2CO3, NH4 HCO3, NH4HSO4, NH4OSO2F, NH4OSO2Cl, NH4OSO2CF3, NH 4OSO2CH3, NH4OC(O)CF3, NH 4OC(O)CH3, NH4N(SO2CF3)2 , NH4OIOF4, NH4OTeF5, (NH4) 2 (B12F12), NH4BrF6, NH 4BrF6, NH4ClF6, NH4VF6, NH4RuF7, (NH4)3FeF6, (NH 4)2SiF6, (NH4)3AlF6, NH4SbF6, NH4AsF6, NH4BiF 6, NH4Sb2F11, NH4As2 F11, and NH4Sb3F16. 3. The process of claim 2 wherein the melt ratio of the liquid mixture expressed as HF/NH3 is from about 2.4 to 5. 4. The process of claim 3 wherein the difference between the temperature of the reaction product at the exit of the column and that of the liquid mixture introduced to the inlet of said column is from 1 and 30째 C. 5. The process of claim 4 wherein the ammonium ion source is ammonium acid fluoride. 6. The process of claim 5 wherein the column is a monolith column. 7. The process of claim 5 wherein the exit temperature is sufficiently high such that substantially no liquid melt regarded as waste is generated. 8. The process of claim 7 wherein the pressure in said column is from 10 to 500 psia. 9. The process of claim 8 wherein the temperature of the liquid melt to the inlet of said column is from 90 to 200째 C. 10. The process of claim 5 wherein the melt ratio of the liquid melt to the inlet of said column is from 2.6 to 3.6 and the difference in the melt ratio of the reaction product to that of the initial melt is from 0.01 to 0.5. 11. The process of claim 10 wherein the liquid mixture is cocurrent upflow. 12. The process of claim 10 wherein the liquid mixture is cocurrent downflow. 13. In a process for producing NF3 by contacting gaseous F2, as the fluorine reactant, with an ammonium acid fluoride complex under conditions for generating a reaction product containing NF3, the improvement which comprises: introducing said F2 and said ammonium acid fluoride complex as a liquid melt to a column having a packing selected from the group consisting of random packing and structured packing; effecting reaction of said F2 with said ammonium acid fluoride complex under conditions of plug flow conditions for forming NF3; operating the column under conditions such that the temperature of the reaction product at the exit of said column is higher than the temperature of the liquid melt at the inlet of said column; and, recovering said NF3 from the reaction product. 14. The process of claim 13 wherein the melt ratio of the liquid melt expressed as HF/NH3 into the column is from 2.4 to 5. 15. The process of claim 13 wherein the melt ratio of the reaction product at the exit of the column is higher than the melt ratio of the inlet liquid melt. 16. The process of claim 15 wherein the difference between the melt ratio of the reaction product and that of the liquid melt introduced to the column is from 0.01 to 0.5. 17. The process of claim 16 wherein the conversion of F2 in the reaction with ammonium acid fluoride is at least 95%. 18. In a process for producing NF3 by contacting gaseous F2, reactant, with an ammonium acid fluoride complex under conditions for generating a reaction product containing NF3 and byproduct HF, the improvement which comprises: introducing said F2 and said ammonium acid fluoride complex as a liquid melt mixture having a melt ratio of HF/NH3 from 2.6 to 3.6 to a column selected from the group consisting of random packed column and structured packed column; effecting reaction of said F2 with said ammonium acid fluoride complex under conditions for forming NF3; operating the column under conditions such that the temperature of the reaction product at the exit of said column is from 8 to 20째 C. higher than the temperature of the liquid melt mixture at the inlet of said column; and, recovering NF3 from the reaction product. 19. The process of claim 18 wherein said column is a monolith column.