CN117945367A - Method for removing ammonium nitrate from nitric acid solution - Google Patents
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- CN117945367A CN117945367A CN202311756759.8A CN202311756759A CN117945367A CN 117945367 A CN117945367 A CN 117945367A CN 202311756759 A CN202311756759 A CN 202311756759A CN 117945367 A CN117945367 A CN 117945367A
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- PAWQVTBBRAZDMG-UHFFFAOYSA-N 2-(3-bromo-2-fluorophenyl)acetic acid Chemical compound OC(=O)CC1=CC=CC(Br)=C1F PAWQVTBBRAZDMG-UHFFFAOYSA-N 0.000 title claims abstract description 61
- 238000000034 method Methods 0.000 title claims abstract description 31
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 title claims abstract description 29
- 229910017604 nitric acid Inorganic materials 0.000 title claims abstract description 29
- 238000006243 chemical reaction Methods 0.000 claims abstract description 106
- 239000003054 catalyst Substances 0.000 claims abstract description 31
- 238000005984 hydrogenation reaction Methods 0.000 claims abstract description 12
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 7
- 239000001257 hydrogen Substances 0.000 claims abstract description 7
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 4
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 4
- 229910052763 palladium Inorganic materials 0.000 claims description 4
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 3
- 239000002808 molecular sieve Substances 0.000 claims description 3
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 3
- -1 tungsten nitride Chemical class 0.000 claims description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 2
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 claims description 2
- 238000011068 loading method Methods 0.000 claims description 2
- 239000000377 silicon dioxide Substances 0.000 claims description 2
- 229910052721 tungsten Inorganic materials 0.000 claims description 2
- 239000010937 tungsten Substances 0.000 claims description 2
- UONOETXJSWQNOL-UHFFFAOYSA-N tungsten carbide Chemical compound [W+]#[C-] UONOETXJSWQNOL-UHFFFAOYSA-N 0.000 claims description 2
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims 2
- 239000004480 active ingredient Substances 0.000 claims 1
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 claims 1
- 238000000354 decomposition reaction Methods 0.000 abstract description 8
- 239000007800 oxidant agent Substances 0.000 abstract description 4
- 230000001590 oxidative effect Effects 0.000 abstract description 4
- 238000004064 recycling Methods 0.000 abstract description 4
- 239000000243 solution Substances 0.000 description 31
- 238000003756 stirring Methods 0.000 description 22
- 239000007788 liquid Substances 0.000 description 15
- 229910002651 NO3 Inorganic materials 0.000 description 12
- 239000003570 air Substances 0.000 description 12
- 238000001816 cooling Methods 0.000 description 12
- 239000007864 aqueous solution Substances 0.000 description 11
- 229910052757 nitrogen Inorganic materials 0.000 description 7
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 6
- 239000002351 wastewater Substances 0.000 description 5
- 230000003197 catalytic effect Effects 0.000 description 4
- 239000002699 waste material Substances 0.000 description 4
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 3
- 229910010413 TiO 2 Inorganic materials 0.000 description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 235000019253 formic acid Nutrition 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 229910052760 oxygen Inorganic materials 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 2
- IOVCWXUNBOPUCH-UHFFFAOYSA-N Nitrous acid Chemical compound ON=O IOVCWXUNBOPUCH-UHFFFAOYSA-N 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 239000003758 nuclear fuel Substances 0.000 description 2
- 229910052697 platinum Inorganic materials 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 238000009279 wet oxidation reaction Methods 0.000 description 2
- VRZJGENLTNRAIG-UHFFFAOYSA-N 4-[4-(dimethylamino)phenyl]iminonaphthalen-1-one Chemical compound C1=CC(N(C)C)=CC=C1N=C1C2=CC=CC=C2C(=O)C=C1 VRZJGENLTNRAIG-UHFFFAOYSA-N 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 229910052770 Uranium Inorganic materials 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- 238000004176 ammonification Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 229910000420 cerium oxide Inorganic materials 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 230000001877 deodorizing effect Effects 0.000 description 1
- 239000002360 explosive Substances 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 231100001261 hazardous Toxicity 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 239000002901 radioactive waste Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 235000012239 silicon dioxide Nutrition 0.000 description 1
- 238000002798 spectrophotometry method Methods 0.000 description 1
- 239000002915 spent fuel radioactive waste Substances 0.000 description 1
- 239000007858 starting material Substances 0.000 description 1
- 230000001954 sterilising effect Effects 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 235000012222 talc Nutrition 0.000 description 1
- 239000000454 talc Substances 0.000 description 1
- 229910052623 talc Inorganic materials 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
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- Catalysts (AREA)
Abstract
The application discloses a method for removing ammonium nitrate from nitric acid solution, which comprises the following steps: and (3) in the hydrogen atmosphere, contacting the nitric acid solution containing ammonium nitrate with a hydrogenation catalyst for reaction I, and then raising the temperature for reaction II again to obtain the nitric acid solution without ammonium nitrate. The method of the application firstly carries out hydrogenation reaction on the solution under the action of a catalyst, and secondly carries out ammonium nitrate decomposition reaction by raising the temperature of the solution. The method can effectively decompose the ammonium nitrate in the solution without adjusting the pH value of the solution and adding an oxidant, has the ammonium nitrate conversion rate of more than 99 percent, realizes the recycling of nitric acid and has good application prospect.
Description
Technical Field
The application relates to a method for removing ammonium nitrate from a nitric acid solution, and belongs to the field of nuclear waste liquid treatment.
Background
Ammonium nitrate is an important byproduct in the radiochemistry process and exists in the spent fuel post-treatment flow and radioactive waste liquid generated by uranium purification and conversion. Since ammonium nitrate is an explosive hazardous compound, the continuous accumulation of the ammonium nitrate in the waste liquid can bring potential safety hazards to the nuclear fuel circulation, and therefore, the ammonium nitrate in the waste liquid needs to be removed before the waste liquid is further concentrated and treated.
Currently, technologies for treating ammonium ions in wastewater include biochemical, photochemical, electrochemical, catalytic wet oxidation, fenton, and other advanced oxidation technologies. Catalytic wet Oxidation (CWAO) is a green catalytic technology for degrading COD and N, S-containing pollution in high-concentration organic wastewater into harmless components such as CO 2、N2、SO4 2- and H 2 O by using oxygen-enriched matters such as air, oxygen or hydrogen peroxide as an oxidant under the catalysis of a catalyst at a higher temperature (150-280 ℃) and a higher pressure (0.5-20 MPa), and decoloring, deodorizing and sterilizing at the same time. CN114409166a discloses a method for treating ammonium nitrate waste water by catalytic wet oxidation-ammonification, which takes ammonium nitrate waste water, gas containing elemental oxygen and gas containing reducing nitrogen as raw materials, ru/black talcum as catalyst, and reacts for 2 hours at 200 ℃ and 3MPa, and the conversion rate of NH 4 + is 97.3%. CN86102728a discloses a scheme for removing ammonium nitrate from nuclear fuel wastewater, which uses Ru/TiO 2 or Pd/TiO 2 as catalyst, and makes them react for 1h under the action of air at 250 deg.c, and the decomposition conversion rate of ammonium nitrate can be up to above 99%, but the scheme can be implemented only by using specific pH value and specific [ NH 4 +-N/NO3 - -N ] mole ratio of feed liquid, so that its application range is limited.
For the removal of ammonium nitrate from nitric acid systems Anan' ev et al found that formic acid was effective in decomposing ammonium nitrate in nitric acid solutions at 80 ℃, but this process required the consumption of large amounts of formic acid to complete the decomposition of ammonium nitrate (Radiochemistry, vol.47, no.2,2005, pp.157-162), which process took a long time while introducing new material formic acid into the system, affecting the reuse of nitric acid.
Disclosure of Invention
The invention aims to solve the technical problem of removing ammonium nitrate in nitric acid solution and realizing recycling of nitric acid. Therefore, the ammonium nitrate removal method has high reaction efficiency and simple and convenient operation, and does not introduce new substances into the reaction system.
According to one aspect of the present application there is provided a method of removing ammonium nitrate from a nitric acid solution, the method comprising:
and (3) in the hydrogen atmosphere, contacting the nitric acid solution containing ammonium nitrate with a hydrogenation catalyst for reaction I, and then raising the temperature for reaction II again to obtain the nitric acid solution without ammonium nitrate.
Optionally, the pressure of the hydrogen is 1-4 MPa.
Alternatively, the pressure of the hydrogen is independently selected from any of 1MPa, 1.5MPa, 2MPa, 2.5MPa, 3MPa, 3.5MPa, 4MPa, or a range of values therebetween.
Optionally, the content of ammonium nitrate in the nitric acid solution containing ammonium nitrate is 800-1000 ppm.
Optionally, the content of ammonium nitrate in the nitric acid solution without ammonium nitrate is 2-400 ppm.
Optionally, the hydrogenation catalyst is a supported catalyst; the supported catalyst comprises a carrier and an active component supported on the carrier.
Alternatively, the loading of the active component in the supported catalyst is 0.1 to 10wt.%.
Optionally, the active component is selected from at least one of Pd, ru, pt, ir, rh, au.
Optionally, the carrier is at least one selected from activated carbon, alumina, molecular sieve, titanium oxide, cerium oxide, tungsten carbide, tungsten nitride, zirconium oxide and silicon dioxide.
Optionally, the hydrogenation catalyst is used in an amount of 1 to 10% by mass of the nitric acid solution containing ammonium nitrate.
Alternatively, the hydrogenation catalyst is used in an amount such that the mass of the nitric acid solution containing ammonium nitrate is independently selected from any of 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10% or a range between any of the foregoing.
Alternatively, the temperature of reaction I is 20-60 ℃.
Alternatively, the temperature of reaction I is 25-40 ℃.
Alternatively, the temperature of reaction I is independently selected from any value or range of values between any two of 25 ℃, 30 ℃, 35 ℃, 40 ℃.
Optionally, the time of the reaction I is 0.5-4 h.
Optionally, the time of the reaction I is 1-2 h.
Alternatively, the time of reaction I is independently selected from any of 1h, 1.2h, 1.4h, 1.6h, 1.8h, 2h, or a range of values between any two of the foregoing.
Alternatively, the temperature of reaction II is 100 to 250 ℃.
Alternatively, the temperature of reaction II is 100 to 150 ℃.
Alternatively, the temperature of reaction II is independently selected from any value or range of values between any two of 100 ℃, 110 ℃, 120 ℃, 130 ℃, 140 ℃, 150 ℃.
Alternatively, the reaction II takes 1 to 5 hours.
Optionally, the time of the reaction II is 1-3 h.
Alternatively, the time of reaction II is independently selected from any of 1h, 1.5h, 2h, 2.5h, 3h, or a range of values between any two of the foregoing.
In order to solve the technical problems, the technical scheme of the invention is as follows:
the nitrous acid is generated by the hydrogenation of nitric acid, and the decomposition of ammonium nitrate is realized by the reaction of the nitrous acid and the ammonium nitrate. The method comprises the following steps: (1) Introducing hydrogen into a reaction kettle filled with a nitric acid solution of ammonium nitrate, and reacting for 0.5-4 h at 20-60 ℃ under the action of a hydrogenation catalyst; (2) And (3) heating the solution obtained in the step (1) to 100-250 ℃ for reaction for 1-5 h.
The method of the invention firstly carries out hydrogenation reaction on the solution under the action of a catalyst, and secondly carries out ammonium nitrate decomposition reaction by raising the temperature of the solution. The method can effectively decompose the ammonium nitrate in the solution without adjusting the pH value of the solution and adding an oxidant, the conversion rate of the ammonium nitrate can reach more than 99%, the recycling of the nitric acid is realized, and the method has good application prospect.
The application has the beneficial effects that:
1) Compared with the prior art, the method does not need to adjust the pH value of the solution and introduce an oxidant, so as to realize the decomposition of ammonium nitrate.
2) According to the method provided by the application, new substances are not required to be introduced into a reaction system, and the reacted catalyst is easy to separate, so that the recycling of nitric acid is realized.
3) The method provided by the application is simple and convenient to operate, the reaction efficiency is high, and the decomposition conversion rate of ammonium nitrate can reach more than 99%.
Detailed Description
The present application is described in detail below with reference to examples, but the present application is not limited to these examples.
Unless otherwise indicated, all starting materials in the examples of the present application were purchased commercially.
In the application, an indophenol blue spectrophotometry method is adopted to analyze the ammonium nitrate content in the solution.
Example 1
50.0G of an aqueous solution containing 1.0mol/L HNO 3 and 1000ppm NH 4NO3 and 0.5g of a 3% Ru/C catalyst are filled into a 100ml high-pressure reaction kettle, N 2 replaces the air in the reaction, H 2 is introduced into the reaction kettle to 1MPa, the temperature of the reaction system is maintained at 20 ℃, stirring is started, the stirring speed is 400rpm, the reaction is timed for 4 hours, the temperature of the reaction system is increased to 150 ℃, the reaction is timed for 5 hours, cooling is carried out, and the content of ammonium nitrate in the solution is analyzed by taking clear liquid, and the result is shown in Table 1.
Example 2
50.0G of an aqueous solution containing 1.0mol/L HNO 3 and 1000ppm NH 4NO3 and 1.0g of a 3% Pt/SiO 2 catalyst are filled into a 100ml high-pressure reaction kettle, N 2 replaces the air in the reaction, H 2 pressure is introduced into the reaction kettle to 3MPa, after the system temperature is maintained at 25 ℃, stirring is started, the stirring speed is 400rpm, after the reaction is timed for 2 hours, the temperature of the reaction system is increased to 100 ℃, the reaction is timed for 5 hours, cooling is carried out, and the content of ammonium nitrate in the solution is analyzed by taking clear liquid, and the result is shown in Table 1.
Example 3
50.0G of an aqueous solution containing 1.0mol/L HNO 3 and 1000ppm NH 4NO3 and 2.0g of 3% Pd/CeO 2 catalyst are filled into a 100ml high-pressure reaction kettle, N 2 replaces the air in the reaction, H 2 pressure is introduced into the reaction kettle to 2MPa, after the system temperature is maintained at 40 ℃, stirring is started, the stirring speed is 400rpm, after the reaction is timed for 1 hour, the temperature of the reaction system is increased to 200 ℃, the reaction is timed for 4 hours, cooling is carried out, and the content of ammonium nitrate in the solution is analyzed by taking clear liquid, and the result is shown in Table 1.
Example 4
50.0G of an aqueous solution containing 1.0mol/L HNO 3 and 1000ppm NH 4NO3, 0.5g of 3% Ir/Al 2O3 catalyst and N 2 are filled into a 100ml high-pressure reaction kettle to replace air in the reaction, H 2 pressure is introduced into the reaction kettle to 4MPa, after the system temperature is maintained at 60 ℃, stirring is started, the stirring speed is 400rpm, the reaction system temperature is raised to 250 ℃ after the reaction is timed for 0.5H, the reaction is timed for 3H, cooling is carried out, and the clear liquid is taken to analyze the ammonium nitrate content in the solution, and the result is shown in Table 1.
Example 5
50.0G of an aqueous solution containing 1.0mol/L HNO 3 and 1000ppm NH 4NO3 and 1.0g of 3% Au/ZrO 2 catalyst are filled into a 100ml high-pressure reaction kettle, the air in the reaction is replaced by N 2, H 2 pressure is introduced into the reaction kettle to 4MPa, after the system temperature is maintained at 40 ℃, stirring is started, the stirring speed is 400rpm, the reaction is carried out for 1 hour, the temperature of the reaction system is increased to 150 ℃, the reaction is carried out for 3 hours, cooling is carried out, and the content of ammonium nitrate in the solution is analyzed by taking clear liquid, and the result is shown in Table 1.
Example 6
50.0G of an aqueous solution containing 1.0mol/L HNO 3 and 1000ppm NH 4NO3 and 2.0g of 3% Rh/molecular sieve catalyst are filled into a 100ml high-pressure reaction kettle, N 2 replaces the air in the reaction, H 2 pressure is introduced into the reaction kettle to 2MPa, after the system temperature is maintained at 60 ℃, stirring is started, the stirring speed is 400rpm, after the reaction is timed for 1 hour, the temperature of the reaction system is increased to 150 ℃, the reaction is timed for 3 hours, cooling is carried out, and the content of ammonium nitrate in the clear solution is analyzed, so that the results are shown in Table 1.
Example 7
50.0G of an aqueous solution containing 1.0mol/L HNO 3 and 1000ppm NH 4NO3 and 3.0g of a 3% Ru/TiO 2 catalyst are filled into a 100ml high-pressure reaction kettle, the air in the reaction is replaced by N 2, the pressure of H 2 is introduced into the reaction kettle to 4MPa, after the temperature of the system is maintained at 30 ℃, stirring is started, the stirring speed is 400rpm, the reaction is timed for 2 hours, the temperature of the reaction system is increased to 150 ℃, the reaction is timed for 3 hours, cooling is carried out, and the content of ammonium nitrate in the solution is analyzed by taking clear liquid, and the result is shown in Table 1.
Example 8
50.0G of an aqueous solution containing 1.0mol/L HNO 3 and 1000ppm NH 4NO3 and 5.0g of 2.5 percent Ru-0.5 percent Pt)/WC catalyst are filled into a 100ml high-pressure reaction kettle, the air in the reaction is replaced by N 2, H 2 pressure is introduced into the reaction kettle to 4MPa, stirring is started when the system temperature is maintained at 30 ℃, stirring speed is 400rpm, after the reaction is timed for 2 hours, the temperature of the reaction system is increased to 150 ℃, the reaction is timed for 3 hours, cooling and cooling are carried out, and the ammonium nitrate content in the clear solution is analyzed, so that the results are shown in Table 1.
Example 9
50.0G of an aqueous solution containing 1.0mol/L HNO 3 and 1000ppm NH 4NO3 and 5.0g of 2.5% Ru-0.5% Pd/W 2 N catalyst are filled into a 100ml high-pressure reaction kettle, the air in the reaction is replaced by N 2, H 2 pressure is introduced into the reaction kettle to 4MPa, stirring is started until the system temperature is maintained at 40 ℃, the stirring speed is 400rpm, after the reaction is carried out for 2 hours at a timing, the temperature of the reaction system is increased to 150 ℃, the reaction is carried out for 3 hours at a timing, cooling is carried out, and the clear liquid is taken to analyze the ammonium nitrate content in the solution, and the results are shown in Table 1.
Example 10
50.0G of an aqueous solution containing 1.0mol/L HNO 3 and 1000ppm NH 4NO3 and 5.0g of a 3% Pt/ZrO 2-CeO2 catalyst are filled into a 100ml high-pressure reaction kettle, air in the reaction is replaced by N 2, H 2 pressure is introduced into the reaction kettle to 4MPa, after the system temperature is maintained at 30 ℃, stirring is started, stirring speed is 400rpm, after the reaction is timed for 2 hours, the temperature of the reaction system is increased to 150 ℃, the reaction is timed for 3 hours, cooling is carried out, and the content of ammonium nitrate in the solution is analyzed by taking clear liquid, and the result is shown in Table 1.
TABLE 1 reaction results for the different examples
| Examples | Residual concentration of ammonium nitrate in solution | Decomposition conversion rate of ammonium nitrate |
| Example 1 | 2.5ppm | 99.75％ |
| Example 2 | 543.1ppm | 45.69％ |
| Example 3 | 47.6ppm | 95.24％ |
| Example 4 | 236.0ppm | 76.40％ |
| Example 5 | 397.4ppm | 60.26％ |
| Example 6 | 256.7ppm | 74.33％ |
| Example 7 | 23.5ppm | 97.65％ |
| Example 8 | 17.7ppm | 98.23％ |
| Example 9 | 118.8ppm | 88.12％ |
| Example 10 | 95.6ppm | 90.44％ |
| Comparative example 1 | 865.4ppm | 13.46％ |
Comparative example 1
Adding 30mL of aqueous solution containing 1.0mol/L HNO 3 and 1000ppm NH 4NO3 into a 100mL reaction kettle, sealing the reaction system, setting the temperature to 150 ℃, starting heating, starting stirring when the temperature of the reaction system is raised to 150 ℃, stirring at 400rpm, timing for reaction for 120min, cooling, filtering, and taking clear liquid to analyze the ammonium nitrate content in the solution.
While the application has been described in terms of preferred embodiments, it will be understood by those skilled in the art that various changes and modifications can be made without departing from the scope of the application, and it is intended that the application is not limited to the specific embodiments disclosed.
Claims (10)
1. A method for removing ammonium nitrate from a nitric acid solution, the method comprising:
and (3) in the hydrogen atmosphere, contacting the nitric acid solution containing ammonium nitrate with a hydrogenation catalyst for reaction I, and then raising the temperature for reaction II again to obtain the nitric acid solution without ammonium nitrate.
2. The method according to claim 1, wherein the pressure of the hydrogen is 1-4 MPa;
preferably, in the nitric acid solution containing ammonium nitrate, the content of the ammonium nitrate is 800-1000 ppm;
preferably, the content of ammonium nitrate in the nitric acid solution without ammonium nitrate is 2-400 ppm.
3. The process of claim 1, wherein the hydrogenation catalyst is a supported catalyst; the supported catalyst comprises a carrier and an active component supported on the carrier;
Preferably, the loading of the active component in the supported catalyst is 0.1 to 10wt.%.
4. A method according to claim 3, wherein the active ingredient is selected from at least one of Pd, ru, pt, ir, rh, au.
5. A method according to claim 3, wherein the support is selected from at least one of activated carbon, alumina, molecular sieves, titania, ceria, tungsten carbide, tungsten nitride, zirconia, silica.
6. The method according to claim 1, wherein the hydrogenation catalyst is used in an amount of 1 to 10% by mass of the nitric acid solution containing ammonium nitrate.
7. The process according to claim 1, wherein the temperature of reaction I is 20-60 ℃;
preferably, the temperature of reaction I is 25 to 40 ℃.
8. The method according to claim 1, wherein the time of reaction I is 0.5 to 4 hours;
preferably, the time of the reaction I is 1-2 h.
9. The process according to claim 1, wherein the temperature of reaction II is 100-250 ℃;
preferably, the temperature of reaction II is 100 to 150 ℃.
10. The process according to claim 1, wherein the time of reaction II is 1 to 5 hours;
Preferably, the time of the reaction II is 1 to 3 hours.
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| CN202311756759.8A CN117945367A (en) | 2023-12-19 | 2023-12-19 | Method for removing ammonium nitrate from nitric acid solution |
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