CN114768480A - Device for removing ammonia nitrogen in citric acid absorbent in farm and treatment process thereof - Google Patents
Device for removing ammonia nitrogen in citric acid absorbent in farm and treatment process thereof Download PDFInfo
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- CN114768480A CN114768480A CN202210589621.2A CN202210589621A CN114768480A CN 114768480 A CN114768480 A CN 114768480A CN 202210589621 A CN202210589621 A CN 202210589621A CN 114768480 A CN114768480 A CN 114768480A
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- citric acid
- ammonia nitrogen
- electrolytic cell
- absorption tower
- absorbent
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- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 title claims abstract description 411
- XKMRRTOUMJRJIA-UHFFFAOYSA-N ammonia nh3 Chemical compound N.N XKMRRTOUMJRJIA-UHFFFAOYSA-N 0.000 title claims abstract description 90
- 230000002745 absorbent Effects 0.000 title claims abstract description 46
- 239000002250 absorbent Substances 0.000 title claims abstract description 46
- 238000000034 method Methods 0.000 title claims abstract description 46
- 239000007788 liquid Substances 0.000 claims abstract description 98
- 238000010521 absorption reaction Methods 0.000 claims abstract description 58
- 239000002699 waste material Substances 0.000 claims abstract description 51
- 239000002912 waste gas Substances 0.000 claims abstract description 29
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 claims description 32
- 239000011248 coating agent Substances 0.000 claims description 16
- 238000000576 coating method Methods 0.000 claims description 16
- 239000011780 sodium chloride Substances 0.000 claims description 16
- 238000005868 electrolysis reaction Methods 0.000 claims description 12
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 11
- 229910052719 titanium Inorganic materials 0.000 claims description 11
- 239000010936 titanium Substances 0.000 claims description 11
- 238000003756 stirring Methods 0.000 claims description 8
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 claims description 7
- HJPBEXZMTWFZHY-UHFFFAOYSA-N [Ti].[Ru].[Ir] Chemical compound [Ti].[Ru].[Ir] HJPBEXZMTWFZHY-UHFFFAOYSA-N 0.000 claims description 6
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 5
- 229910002804 graphite Inorganic materials 0.000 claims description 5
- 239000010439 graphite Substances 0.000 claims description 5
- 229910052741 iridium Inorganic materials 0.000 claims description 5
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 claims description 5
- 229910000831 Steel Inorganic materials 0.000 claims description 4
- 239000010959 steel Substances 0.000 claims description 4
- 238000002156 mixing Methods 0.000 claims description 3
- 239000011259 mixed solution Substances 0.000 claims description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 abstract description 8
- 239000002994 raw material Substances 0.000 abstract description 4
- 229910052757 nitrogen Inorganic materials 0.000 abstract description 3
- 231100000956 nontoxicity Toxicity 0.000 abstract description 2
- 238000004064 recycling Methods 0.000 abstract 1
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 description 27
- 239000000243 solution Substances 0.000 description 22
- 238000001514 detection method Methods 0.000 description 18
- 238000006243 chemical reaction Methods 0.000 description 16
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 14
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 14
- 238000006056 electrooxidation reaction Methods 0.000 description 14
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 13
- 239000000460 chlorine Substances 0.000 description 13
- 229910052801 chlorine Inorganic materials 0.000 description 13
- 239000007789 gas Substances 0.000 description 9
- 235000006408 oxalic acid Nutrition 0.000 description 9
- 244000088401 Pyrus pyrifolia Species 0.000 description 6
- 235000001630 Pyrus pyrifolia var culta Nutrition 0.000 description 6
- 238000005070 sampling Methods 0.000 description 6
- 239000002253 acid Substances 0.000 description 5
- 229910021529 ammonia Inorganic materials 0.000 description 5
- 230000007797 corrosion Effects 0.000 description 5
- 238000005260 corrosion Methods 0.000 description 5
- 238000012544 monitoring process Methods 0.000 description 5
- DPGAAOUOSQHIJH-UHFFFAOYSA-N ruthenium titanium Chemical compound [Ti].[Ru] DPGAAOUOSQHIJH-UHFFFAOYSA-N 0.000 description 5
- 241000282414 Homo sapiens Species 0.000 description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 238000005265 energy consumption Methods 0.000 description 4
- 239000001301 oxygen Substances 0.000 description 4
- 229910052760 oxygen Inorganic materials 0.000 description 4
- 150000003839 salts Chemical class 0.000 description 4
- 125000004122 cyclic group Chemical group 0.000 description 3
- 239000004135 Bone phosphate Substances 0.000 description 2
- 241001465754 Metazoa Species 0.000 description 2
- 230000002378 acidificating effect Effects 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 229910001873 dinitrogen Inorganic materials 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 244000005700 microbiome Species 0.000 description 2
- 210000004400 mucous membrane Anatomy 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 244000144977 poultry Species 0.000 description 2
- 230000036647 reaction Effects 0.000 description 2
- 229920006395 saturated elastomer Polymers 0.000 description 2
- 239000013589 supplement Substances 0.000 description 2
- 206010003445 Ascites Diseases 0.000 description 1
- KZBUYRJDOAKODT-UHFFFAOYSA-N Chlorine Chemical compound ClCl KZBUYRJDOAKODT-UHFFFAOYSA-N 0.000 description 1
- 229910002651 NO3 Inorganic materials 0.000 description 1
- 208000007125 Neurotoxicity Syndromes Diseases 0.000 description 1
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 1
- IOVCWXUNBOPUCH-UHFFFAOYSA-M Nitrite anion Chemical compound [O-]N=O IOVCWXUNBOPUCH-UHFFFAOYSA-M 0.000 description 1
- 208000005374 Poisoning Diseases 0.000 description 1
- 239000003929 acidic solution Substances 0.000 description 1
- 239000008280 blood Substances 0.000 description 1
- 210000004369 blood Anatomy 0.000 description 1
- 210000005013 brain tissue Anatomy 0.000 description 1
- 210000003169 central nervous system Anatomy 0.000 description 1
- 238000011109 contamination Methods 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 239000012895 dilution Substances 0.000 description 1
- 238000010790 dilution Methods 0.000 description 1
- 238000003113 dilution method Methods 0.000 description 1
- 238000004134 energy conservation Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 210000002615 epidermis Anatomy 0.000 description 1
- 235000013373 food additive Nutrition 0.000 description 1
- 239000002778 food additive Substances 0.000 description 1
- 230000007794 irritation Effects 0.000 description 1
- 244000144972 livestock Species 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 150000007524 organic acids Chemical class 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 230000020477 pH reduction Effects 0.000 description 1
- 231100000572 poisoning Toxicity 0.000 description 1
- 230000000607 poisoning effect Effects 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 230000001172 regenerating effect Effects 0.000 description 1
- 230000008929 regeneration Effects 0.000 description 1
- 238000011069 regeneration method Methods 0.000 description 1
- 210000003491 skin Anatomy 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 208000011580 syndromic disease Diseases 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 231100000167 toxic agent Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 239000003440 toxic substance Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
Images
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
- B01D53/1425—Regeneration of liquid absorbents
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
- B01D53/1412—Controlling the absorption process
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
- B01D53/18—Absorbing units; Liquid distributors therefor
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/68—Halogens or halogen compounds
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/77—Liquid phase processes
- B01D53/78—Liquid phase processes with gas-liquid contact
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F9/00—Multistage treatment of water, waste water or sewage
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
- B01D2252/20—Organic absorbents
- B01D2252/205—Other organic compounds not covered by B01D2252/00 - B01D2252/20494
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/40—Nitrogen compounds
- B01D2257/406—Ammonia
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/46104—Devices therefor; Their operating or servicing
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/66—Treatment of water, waste water, or sewage by neutralisation; pH adjustment
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/16—Nitrogen compounds, e.g. ammonia
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
- C02F2103/18—Nature of the water, waste water, sewage or sludge to be treated from the purification of gaseous effluents
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2209/00—Controlling or monitoring parameters in water treatment
- C02F2209/06—Controlling or monitoring parameters in water treatment pH
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- Environmental & Geological Engineering (AREA)
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Abstract
The invention relates to the technical field of treatment of ammonia nitrogen waste gas in a farm, in particular to a device for removing ammonia nitrogen in a citric acid absorbent in the farm and a treatment process thereof, wherein the device comprises a waste liquid tank, a citric acid absorption tower and an electrolytic cell; the recycling of the citric acid absorbent can be realized, and nitrogen is discharged into the air after the ammonia nitrogen waste gas is treated, so that the nitrogen is harmless to the environment; the treatment process is simple, and does not produce secondary pollution; the raw materials are convenient and easy to obtain, and have no toxicity, and the ammonia nitrogen waste gas can be treated in an environment-friendly way.
Description
Technical Field
The invention relates to the technical field of removal of ammonia nitrogen waste gas in farms, in particular to a device for removing ammonia nitrogen in a citric acid absorbent in a farm and a treatment process thereof.
Background
Ammonia is a toxic substance for living organisms, human brain tissue is extremely sensitive to ammonia, and central nervous system poisoning can be caused when the concentration of ammonia in blood reaches 1%; in addition, ammonia can induce ascites syndromes in poultry, affect the mobility of the poultry, and result in a decrease in growth rate and egg production. At present, a method for treating ammonia nitrogen waste gas commonly used in a farm is a solution absorption method, and clear water, a dilute sulfuric acid solution or a dilute oxalic acid solution is usually adopted as an absorbent.
The sulfuric acid as a strong acid has strong oxidizing property and high corrosion to equipment, and can be applied to waste gas treatment after dilution. However, the strong acid dilution process has great potential safety hazard, so that safety problems such as bumping and the like are easily caused, and the operation is inconvenient.
Oxalic acid is a dibasic acid which can effectively absorb waste gas containing ammonia nitrogen, but oxalic acid is a toxic organic acid which has irritation to the skin and mucous membranes of organisms and is very easy to cause poisoning by being absorbed through the epidermis and the mucous membranes. Secondly, oxalic acid absorbs ammonia nitrogen and is easy to generate insoluble salt, the insoluble salt needs to be shoveled away after being crystallized, and the efficiency and the economic benefit are low in the industrial link of treating a large amount of waste gas containing ammonia nitrogen.
The post-treatment process of the waste liquid containing ammonia nitrogen generally comprises a biological nitrification method and a denitrification method, wherein the biological nitrification method and the denitrification method are combined with various microorganisms and can convert the ammonia nitrogen into nitrate, nitrite or nitrogen. The above two methods are limited by the conditions of dissolved oxygen, pH, temperature and the like of the waste liquid, and a complex treatment process is required to achieve the optimal environment for removing ammonia nitrogen. The above processes all destroy the original function of the absorbent with the potential of circulation. And the culture period of the microorganism is long, the requirement on the biological environment is high, the operation cost of the whole process flow is high, and the biological nitrification method and the denitrification method can not be applied to the treatment of waste liquid with a regeneration prospect based on the aspects of environmental protection and green chemical industry.
Disclosure of Invention
In order to overcome the technical problems in the prior art, the method has good waste gas removal effect, can be applied to protecting components with good electrochemical stability, removes easily decomposed components, and achieves the purpose of regenerating the absorbent.
The invention provides a device for removing ammonia nitrogen in a citric acid absorbent in a farm, which comprises a waste liquid tank, a citric acid absorption tower and an electrolytic tank; the liquid inlet of the citric acid absorption tower is communicated with the liquid outlet of the electrolytic cell, and the liquid outlet of the citric acid absorption tower and the liquid inlet of the electrolytic cell are both communicated with the waste liquid tank; and valves are arranged at the liquid outlet of the citric acid absorption tower, the liquid outlet of the electrolytic cell and the liquid outlet of the waste liquid tank.
Furthermore, a cathode and an anode are arranged in the electrolytic cell, the cathode is connected with the positive pole of a power supply, and the anode is connected with the negative pole of the power supply.
Further, the anode is a DSA electrode, and the cathode is a pure titanium plate, a steel plate or a graphite electrode; the distance between the cathode and the anode is 0.5-2 cm.
Further, the anode is an iridium-based coating titanium electrode or a ruthenium-iridium-titanium coating electrode. The iridium-based coating titanium electrode or the ruthenium-iridium-titanium coating electrode has good chlorine evolution, wide applicable pH range, low price and long service life.
Further, a first pH sensor is arranged inside the citric acid absorption tower; a second pH sensor is arranged at a liquid outlet of the citric acid absorption tower; and a third pH sensor is arranged at a liquid outlet of the electrolytic cell. The first pH sensor is arranged to monitor the pH value in the citric acid absorption tower, when the pH value is higher than a set value, the absorption capacity of the citric acid absorbent reaches a saturated state, the citric acid waste liquid needs to be treated, the second pH sensor is used for monitoring the pH value of the citric acid absorbent in the liquid outlet, and when the pH value is lower than the set value, a valve of the citric acid absorption tower can be closed; the third pH sensor can monitor the pH value in the electrolytic cell, when the pH value is smaller than a set value, a valve of a liquid outlet of the electrolytic cell can be opened, the citric acid absorbent which is subjected to electro-oxidation flows back to the citric acid absorption tower to continuously participate in absorbing ammonia nitrogen waste gas of a farm, and thus the monitoring of the reaction process is realized.
Further, the waste liquid tank, the citric acid absorption tower and the electrolytic cell are all in closed working environments.
Further, the concentration of the citric acid solution in the citric acid absorption tower is 0.5-1.5 g/L.
Compared with the prior art, the invention has the beneficial effects that:
(1) citric acid is used as an absorbent, and the citric acid is tribasic acid, so that the absorption capacity of the citric acid for alkaline gases is larger than that of sulfuric acid and oxalic acid, and the ammonia nitrogen waste gas can be efficiently absorbed.
(2) The citric acid solution has stable electrochemical properties, is not easy to decompose under the condition of electrolysis, and can recover the acidity and the alkaline gas absorption capacity by an electrochemical oxidation method.
(3) In the closed reaction environment of the electrolytic cell, reaction raw materials can be utilized to the maximum extent, and gas generated by electrolysis is prevented from escaping into the environment.
(4) The citric acid in the citric acid absorption tower is used for absorbing ammonia nitrogen waste gas of a farm, when the numerical value of the first pH sensor is higher than a set value, a valve of a liquid outlet of the citric acid absorption tower is opened, the citric acid waste gas which has absorbed the ammonia nitrogen waste gas flows to a waste liquid tank, when the numerical value of the second pH sensor is lower than the set value, the valve of the liquid outlet of the citric acid absorption tower is closed, raw materials in the waste liquid tank are mixed with the citric acid waste liquid, the valve of the liquid outlet of the waste liquid tank is opened after the mixture, the solution flows to an electrolytic cell for electrolytic reaction in the electrolytic cell, when the numerical value of the third pH sensor is lower than the set value, the valve of the liquid outlet of the electrolytic cell is opened, and the citric acid after electro-oxidation flows to the citric acid absorption tower to continuously absorb the ammonia nitrogen waste gas of the farm; therefore, the cyclic utilization of the citric acid absorbent is realized, and the corrosion influence of the citric acid on the device is small.
The second purpose of the invention is to provide a treatment process of a device for removing ammonia nitrogen in a citric acid absorbent in a farm, which comprises the following steps:
the method comprises the following steps: the citric acid absorption tower is filled with a citric acid absorbent for absorbing ammonia nitrogen waste gas of a farm, when the pH value in the citric acid absorption tower is higher than 6, a valve of a liquid outlet of the citric acid absorption tower is opened, and the citric acid absorbent enters a waste liquid tank;
step two: when the citric acid absorbent enters the waste liquid tank, adding sodium chloride into the waste liquid tank, and mixing the citric acid absorbent and the sodium chloride to form a mixed solution;
step three: and opening a valve of a liquid outlet of the waste liquid tank, allowing the mixed liquid to enter an electrolytic cell for electrolysis, continuously stirring in the electrolytic process, and when the pH value in the electrolytic cell is monitored to be lower than 3, opening the valve of the liquid outlet of the electrolytic cell, and allowing the citric acid absorbent to flow back to the citric acid absorption tower.
The citric acid solution does not participate in the oxidation reaction due to its electrochemical stability during the electrolysis process. The chemical reactions involved in the electrolytic cell of the invention are:
6NaCl+6H2O＝6NaOH+3H2↑+3Cl2
3Cl2+3H2O＝3HOCl+3HCl
3HOCl+2NH3＝N2↑+3H2O+3HCl
as can be seen from the above chemical reaction formula, 1mol of N is produced2Will generate equal amount of H+OH-, citric acid can be recovered to absorb NH after ammonia nitrogen in the system is consumed3The whole process flow has a cyclic characteristic due to the prior acidity.
Further, the current density of the electrolytic cell is 50-100mA/cm2. Within this range, the greater the current density, the faster the reaction. Beyond the appropriate current density range, there is a risk of decomposition of the acidic solution when the current density is too high, and energy consumption increases; therefore, the stability of a citric acid system can be ensured and the requirements of environmental protection and energy conservation can be met by adjusting the proper current density.
Further, the content of chloride ions in the sodium chloride in the waste liquid tank is 1-5 g/L. When the concentration of the chloride ions is too low, oxygen may be separated out, and the oxygen may compete with the chlorine evolution reaction, thereby increasing energy consumption. When the chloride ion concentration is too high, salt contamination may result and there is a risk of chlorine gas escaping the apparatus.
Further, the temperature of the electrolytic cell is 30-50 ℃.
Compared with the prior art, the invention has the beneficial effects that:
(1) the citric acid solution is a common food additive, is non-toxic, has little influence on the corrosion of an electrolytic cell, and can stably exist under the electrolysis condition of the invention.
(2) The electrooxidation method can selectively and efficiently remove ammonia nitrogen in the citric acid solution, and the technology only needs electric energy, has little pollution and high economic benefit.
(3) The method has simple flow and does not produce secondary pollution; the raw materials are convenient and easy to obtain, and have no toxicity, and the ammonia nitrogen waste gas can be treated in an environment-friendly way.
(4) The method does not need to supplement sodium chloride frequently; in a closed electrolytic cell reaction device, chlorine generated by electrolysis is completely dissolved in a solution to react with ammonia nitrogen, and finally is changed back to a chloride ion form, so that a chlorine source is continuously increased for reaction; the generation amount of the active chlorine can be controlled to maintain the stable operation of the system, and the chlorine is prevented from overflowing the device and harming the health of human beings and animals.
(5) And only nitrogen gas is discharged after the gas generated after electrolysis is collected, so that the method is environment-friendly.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art will be briefly described below, it is obvious that the drawings in the following description are only some embodiments of the present invention, and for those skilled in the art, other drawings can be obtained according to the drawings without creative efforts.
FIG. 1 is a graph showing the relationship between pH and ammonia nitrogen concentration in the first embodiment of the present invention;
FIG. 2 is a graph showing the relationship between pH and ammonia nitrogen concentration in example II of the present invention;
FIG. 3 is a graph showing the relationship between pH and ammonia nitrogen concentration in example III of the present invention;
FIG. 4 is a graph showing the relationship between pH and ammonia nitrogen concentration in the fourth example of the present invention;
FIG. 5 is a graph showing the relationship between pH and ammonia nitrogen concentration in example V of the present invention;
FIG. 6 is a graph showing the relationship between pH and ammonia nitrogen concentration in example six of the present invention;
the relation between the pH reduction amplitude and the ammonia nitrogen removal rate in the citric acid system is fit with different reference curves based on different implementation conditions, and reliable data are provided for monitoring reaction of an ammonia nitrogen removal device in the citric acid absorbent in a farm.
Detailed Description
The technical solutions in the embodiments of the present invention will be described clearly and completely below, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be obtained by a person skilled in the art without making any creative effort based on the embodiments in the present invention, belong to the protection scope of the present invention.
A device for removing ammonia nitrogen in a citric acid absorbent in a farm comprises a waste liquid tank, a citric acid absorption tower and an electrolytic tank; a liquid inlet of the citric acid absorption tower is communicated with a liquid outlet of the electrolytic cell, and both the liquid outlet of the citric acid absorption tower and the liquid inlet of the electrolytic cell are communicated with a waste liquid tank; valves are arranged at the liquid outlet of the citric acid absorption tower, the liquid outlet of the electrolytic cell and the liquid outlet of the waste liquid tank; the waste liquid tank is filled with sodium chloride. The waste liquid tank, the citric acid absorption tower and the electrolytic cell are all closed working environments. Because the electrolytic cell is a closed working environment, the method does not need to supplement sodium chloride frequently; in a closed electrolytic cell reaction device, chlorine generated by electrolysis is completely dissolved in the solution to react with ammonia nitrogen, and finally the chlorine is changed back to a chloride ion form, so that the chlorine source is continuously increased for the reaction; the generation amount of the active chlorine can be controlled to maintain the stable operation of the system, and the chlorine is prevented from overflowing the device and harming the health of human beings and animals.
The electrolytic cell is provided with a cathode and an anode, the cathode is connected with the positive pole of a power supply, and the anode is connected with the negative pole of the power supply.
The anode is a DSA electrode, and the cathode is a pure titanium plate, a steel plate or a graphite electrode; the distance between the cathode and the anode is 0.5-2 cm.
The anode is an iridium-based coating titanium electrode or a ruthenium-iridium-titanium coating electrode. The iridium-based coating titanium electrode or the ruthenium-iridium-titanium coating electrode has good chlorine evolution condition, wider applicable pH range, low price and long service life.
A first pH sensor is arranged inside the citric acid absorption tower; a second pH sensor is arranged at a liquid outlet of the citric acid absorption tower; and a third pH sensor is arranged at a liquid outlet of the electrolytic cell. The first pH sensor is arranged to monitor the pH value in the citric acid absorption tower, when the pH value is higher than a set value, the absorption capacity of the citric acid absorbent reaches a saturated state, the citric acid waste liquid needs to be treated, the second pH sensor is used for monitoring the pH value of the citric acid absorbent in the liquid outlet, and when the pH value is lower than the set value, a valve of the citric acid absorption tower can be closed; the third pH sensor can monitor the pH value in the electrolytic cell, when the pH value is less than a set value, a valve of a liquid outlet of the electrolytic cell can be opened, the citric acid absorbent which is subjected to electric oxidation flows back to the citric acid absorption tower to continue to participate in absorbing ammonia nitrogen waste gas of a farm, and thus the monitoring reaction process is realized.
The concentration of the citric acid solution in the citric acid absorption tower is 0.5-1.5 g/L. The concentration of citric acid determines the absorption capacity of ammonia, and when the concentration of citric acid is too low, the absorption effect on ammonia gas is not obvious, so that the ammonia gas stays in the air of a farm, and the health of livestock and human bodies is harmed; when the concentration of the citric acid is too high, the acidity is too strong, and certain influence is still generated on the equipment such as electrodes, electrolytic cells and the like.
The working principle is as follows: the method comprises the steps that citric acid in a citric acid absorption tower is used for absorbing ammonia nitrogen waste gas of a farm, when the numerical value monitored by a first pH sensor is higher than 6, a valve of a liquid outlet of the citric acid absorption tower is opened, the citric acid waste gas which has absorbed the ammonia nitrogen waste gas flows to a waste liquid tank, when the numerical value monitored by a second pH sensor is lower than 6, the valve of the liquid outlet of the citric acid absorption tower is closed, sodium chloride in the waste liquid tank is mixed with the citric acid waste liquid, the valve of the liquid outlet of the waste liquid tank is opened after mixing, the solution flows to an electrolytic cell for electrolytic reaction in the electrolytic cell, when the numerical value of a third pH sensor is lower than 3, the valve of the liquid outlet of the electrolytic cell is opened, and the citric acid after electro-oxidation flows to the citric acid absorption tower to continuously absorb the ammonia nitrogen waste gas of the farm; therefore, the cyclic utilization of the citric acid absorbent is realized, and the corrosion influence of the citric acid on the device is small.
And (3) analyzing the citric acid waste liquid containing ammonia nitrogen in the citric acid absorption tower, wherein the content of inorganic ammonia nitrogen is about 100 mg/L.
The first embodiment is as follows: 150ml of waste liquid is taken and put into an electrolytic cell, the concentration of citric acid is 0.6g/L, the concentration of sodium chloride is 3g/L, and the pH value is 6.47; the solution in the electrolytic cell is kept at the constant temperature of 30 ℃; ruthenium-titanium coating electrode is used as anode, pure titanium plate is used as cathode, the distance between the two electrodes is 1cm, and the current density is 50mA/cm2And continuously stirring in the electrolytic process, and carrying out electrooxidation treatment for 3 hours.
Sampling is carried out at intervals of 30min, the pH value and the ammonia nitrogen content in the citric acid waste liquid are detected, and the detection results are shown in table 1. The relationship between the pH value and the ammonia nitrogen concentration is shown in figure 1, and a linear equation can be established between the pH value and the ammonia nitrogen concentration: y 0.0440x-0.1578 (R)20.9945). The groove pressure is between 8.25 and 8.50V.
TABLE 1
Example two: 150ml of citric acid waste liquid is taken and placed in an electrolytic cell, the concentration of the citric acid is 1g/L, the concentration of sodium chloride is 4g/L, and the pH value is 6.12; keeping the temperature of the solution in the electrolytic cell at 40 ℃; ruthenium iridium titanium coating electrode is used as an anode, graphite is used as a cathode, the distance between the two electrodes is 1.5cm, and the current density is 70mA/cm2And continuously stirring in the electrolytic process, and carrying out electrooxidation treatment for 3 hours.
Sampling is carried out at intervals of 30min, the pH value and the ammonia nitrogen content in the citric acid waste liquid are detected, and the detection results are shown in table 2. The relationship between the pH value and the ammonia nitrogen concentration is shown in figure 2, and a linear equation can be established between the pH value and the ammonia nitrogen concentration: y 0.0763x-0.2844 (R)20.9942). The groove pressure is between 8.60 and 8.85V
TABLE 2
| Time/min | pH value | Ammonia nitrogen removal rate/%) |
| 0 | 6.12 | 0 |
| 30 | 5.88 | 17.28 |
| 60 | 5.56 | 37.43 |
| 90 | 5.3 | 53.83 |
| 120 | 5.08 | 74.61 |
| 150 | 4.86 | 95.64 (Ammonia nitrogen concentration lower than the detection limit of Nashi detection method) |
| 180 | / | 95.64 (Ammonia nitrogen concentration lower than the detection limit of Nashi detection method) |
Example three: 150ml of citric acid waste liquid is taken and placed in an electrolytic cell, the concentration of the citric acid is 0.8g/L, the concentration of sodium chloride is 5g/L, and the pH value is 6.18; the solution in the electrolytic cell is kept at the constant temperature of 30 ℃; ruthenium-titanium coating electrode is used as anode, pure titanium plate is used as cathode, the distance between the two electrodes is 1.5cm, and current density is 100mA/cm2Continuously stirring in the electrolytic process, and carrying out electrooxidation treatment for 3 h.
Sampling is carried out at intervals of 30min, the pH value and the ammonia nitrogen content in the citric acid waste liquid are detected, and the detection results are shown in table 3. The relationship between the pH value and the ammonia nitrogen concentration is shown in figure 3, and a linear equation can be established between the pH value and the ammonia nitrogen concentration: y 0.0465 x-0.1821 (R)20.9991). The groove pressure is between 8.75 and 8.95V.
TABLE 3
Example four: placing 150ml of citric acid waste liquid in an electrolytic cell, wherein the concentration of citric acid is 0.5g/L, the concentration of sodium chloride is 1g/L, and the pH value is 6.6; keeping the temperature of the solution in the electrolytic cell at 40 ℃; ruthenium-titanium coating electrode is used as anode, steel plate is used as cathode, the distance between the two electrodes is 0.5cm, and current density is 50mA/cm2Continuously stirring in the electrolytic process, and carrying out electrooxidation treatment for 3 h.
Sampling is carried out at intervals of 30min, the pH value and the ammonia nitrogen content in the citric acid waste liquid are detected, and the detection results are shown in table 4. The relationship between the pH value and the ammonia nitrogen concentration is shown in figure 4, and a linear equation can be established between the pH value and the ammonia nitrogen concentration: y-0.397 x-0.2.4972 (R)20.9961). The groove pressure is between 7.10 and 7.65V.
TABLE 4
| Time/min | pH value | Ammonia nitrogen removal rate/%) |
| 0 | 6.6 | 0 |
| 30 | 6.59 | 3.15 |
| 60 | 6.57 | 9.46 |
| 90 | 6.55 | 15.76 |
| 120 | 6.52 | 25.22 |
| 150 | 6.48 | 37.83 |
| 180 | 6.43 | 53.39 |
Example five: 150ml of citric acid waste liquid is taken and placed in an electrolytic cell, the concentration of the citric acid is 1.5g/L, the concentration of sodium chloride is 2g/L, and the pH value is 6.02; keeping the temperature of the solution in the electrolytic cell at 50 ℃; ruthenium-titanium coating electrode is used as anode, graphite is used as cathode, the distance between the two electrodes is 2cm, and the current density is 100mA/cm2Continuously stirring in the electrolytic process, and carrying out electrooxidation treatment for 3 h.
Sampling is carried out at intervals of 30min, the pH value and the ammonia nitrogen content in the citric acid waste liquid are detected, and the detection results are shown in table 5. The relationship between the pH value and the ammonia nitrogen concentration is shown in figure 5, and a linear equation can be established between the pH value and the ammonia nitrogen concentration: y 0.0518 x-0.1791 (R)20.9896). The groove pressure is between 10.15 and 12.00V.
TABLE 5
| Time/min | pH value | Ammonia nitrogen removal rate/%) |
| 0 | 6.02 | 0 |
| 30 | 5.51 | 20.41 |
| 60 | 4.98 | 40.27 |
| 90 | 4.53 | 65.29 |
| 120 | 3.5 | 94.99 |
| 150 | / | 94.99 (Ammonia nitrogen concentration lower than the detection limit of Nashi detection method) |
| 180 | / | 94.99 (Ammonia nitrogen concentration lower than the detection limit of Nashi detection method) |
Example six: 150ml of citric acid waste liquid is taken and placed in an electrolytic cell, the concentration of the citric acid is 0.5g/L, the concentration of sodium chloride is 2g/L, and the pH value is 6.8; the solution in the electrolytic cell is kept at the constant temperature of 30 ℃; the ruthenium-titanium coating electrode is used as an anode, the titanium plate is used as a cathode, the distance between the two electrodes is 2cm, and the current density is 100mA/cm2Continuously stirring in the electrolytic process, and carrying out electrooxidation treatment for 3 h.
Each interval being 30min, sampling is carried out, the pH value and the ammonia nitrogen content in the citric acid waste liquid are detected, and the detection results are shown in Table 6. The relationship between the pH value and the ammonia nitrogen concentration is shown in figure 6, and a linear equation can be established between the pH value and the ammonia nitrogen concentration: y 0.5048 x-2.0082 (R)20.9998). The groove pressure is between 9.75 and 11.90V.
TABLE 6
| Time/min | pH value | Ammonia nitrogen removal rate/%) |
| 0 | 6.8 | 0 |
| 30 | 5.78 | 36.10 |
| 60 | 5.16 | 58.05 |
| 90 | 4.57 | 78.94 |
| 120 | 4.08 | 97.28 |
| 150 | / | 97.28 (Ammonia nitrogen)Concentration lower than the detection limit of Nashi detection method |
| 180 | / | 97.28 (Ammonia nitrogen concentration lower than the detection limit of Nashi detection method) |
Comparative example one: the sulfuric acid is used as an absorbent for the waste gas of the farm, and is not suitable for an electrochemical oxidation method because of strong oxidizing property and high corrosion to equipment, so that the sulfuric acid cannot be recycled, and only the ammonia nitrogen waste gas can be absorbed within the range of the amount of the sulfuric acid which can be absorbed.
Comparative example two: oxalic acid is used as an absorbent for the waste gas of the farm, and ammonia nitrogen is absorbed to generate insoluble salt easily, so that the oxalic acid is not suitable for an electrochemical oxidation method, cannot be recycled, and only can absorb the ammonia nitrogen waste gas within the range of the amount absorbed by the oxalic acid.
It can be seen from examples 1-6 that the larger the distance between the two electrodes, the larger the cell pressure, and the higher the energy consumption.
As can be seen from the comparison among examples 1, 2 and 4, the smaller the distance between the two electrodes is, the more difficult the gas precipitation is caused, and the lower the ammonia nitrogen removal efficiency is.
As can be seen from the comparison of example 5 with example 6, the removal rate of ammonia nitrogen is lower when the temperature of the electrolytic cell is higher in the same electrolysis time.
As is clear from comparison between example 2 and example 4, when the chloride ion concentration is too low, oxygen may be precipitated, and the energy consumption may be increased in competition with the chlorine evolution reaction.
As can be seen from the comparison between examples 1-6 and comparative examples 1-2, the absorbent can not be recycled in any of comparative examples 1-2, and citric acid is used as an acidic absorbent to absorb the alkaline gas NH3, and the pH value is an index considering the absorption capacity of the acidic absorbent; after ammonia nitrogen waste gas is absorbed, the citric acid is electrolyzed, the pH value of the system is reduced, namely the citric acid recovers the absorption capacity and can be recycled. ② only nitrogen gas is discharged after the gas generated after the electrolysis of the citric acid waste liquid is collected, thus being environment-friendly. And thirdly, the citric acid is tribasic acid, has larger absorption capacity for alkaline gas than sulfuric acid and oxalic acid, and can efficiently absorb ammonia nitrogen waste gas. The citric acid solution has stable electrochemical property, is not easy to decompose under the condition of electrolysis, and can recover the acidity and the capability of absorbing alkaline gas by an electrochemical oxidation method.
As can be seen from fig. 1 to 6, different reference curves can be fitted under different conditions, and the linear equation is y ═ nx-m (n, m are constants), which can both show that the ammonia nitrogen removal rate in citric acid is close to 100% when the pH value is less than 3, indicating that the citric acid recovers its absorption capacity and can be recycled.
The foregoing is a more detailed description of the invention in connection with specific preferred embodiments and it is not intended that the invention be limited to these specific details. For those skilled in the art to which the invention pertains, several simple deductions or substitutions can be made without departing from the spirit of the invention, and all shall be considered as belonging to the protection scope of the invention.
Claims (10)
1. The utility model provides an ammonia nitrogen remove device in plant's citric acid absorbent which characterized in that: comprises a waste liquid tank, a citric acid absorption tower and an electrolytic cell; a liquid inlet of the citric acid absorption tower is communicated with a liquid outlet of the electrolytic cell, and both the liquid outlet of the citric acid absorption tower and a liquid inlet of the electrolytic cell are communicated with the waste liquid tank; and a liquid outlet of the citric acid absorption tower, a liquid outlet of the electrolytic cell and a liquid outlet of the waste liquid tank are respectively provided with a valve.
2. The apparatus for removing ammonia nitrogen in citric acid absorbent for farm according to claim 1, wherein: the electrolytic cell is internally provided with a cathode and an anode, the anode is a DSA electrode, and the cathode is a pure titanium plate, a steel plate or a graphite electrode.
3. The apparatus for removing ammonia nitrogen in citric acid absorbent for farm according to claim 2, characterized in that: the distance between the cathode and the anode is 0.5-2 cm.
4. A device for removing ammonia nitrogen in citric acid absorbent for farm according to claim 2, characterized in that: the anode is an iridium-based coating titanium electrode or a ruthenium-iridium-titanium coating electrode.
5. A device for removing ammonia nitrogen in citric acid absorbent in a farm according to claim 1, characterized in that: a first pH sensor is arranged inside the citric acid absorption tower; and a second pH sensor is arranged at a liquid outlet of the citric acid absorption tower.
6. A device for removing ammonia nitrogen in citric acid absorbent in a farm according to claim 1, characterized in that: and a third pH sensor is arranged at a liquid outlet of the electrolytic cell.
7. A device for removing ammonia nitrogen in citric acid absorbent in a farm according to claim 1, characterized in that: the waste liquid tank, the citric acid absorption tower and the electrolytic cell are all closed working environments.
8. A treatment process of a device for removing ammonia nitrogen in a citric acid absorbent in a farm is characterized by comprising the following steps: the method comprises the following steps:
the method comprises the following steps: the citric acid absorption tower is filled with a citric acid absorbent for absorbing ammonia nitrogen waste gas of a farm, when the pH value in the citric acid absorption tower is higher than 6, a valve of a liquid outlet of the citric acid absorption tower is opened, and the citric acid absorbent enters a waste liquid tank;
step two: when the citric acid absorbent enters the waste liquid tank, adding sodium chloride into the waste liquid tank, and mixing the citric acid absorbent and the sodium chloride to form a mixed solution;
step three: and opening a valve of a liquid outlet of the waste liquid tank, allowing the mixed liquid to enter an electrolytic cell for electrolysis, continuously stirring in the electrolytic process, and when the pH value in the electrolytic cell is monitored to be lower than 3, opening the valve of the liquid outlet of the electrolytic cell, and allowing the citric acid absorbent to flow back to the citric acid absorption tower.
9. A treatment process of a device for removing ammonia nitrogen in citric acid absorbent in a farm according to claim 7, characterized in that: the current density of the electrolytic cell is 50-100mA/cm2。
10. A treatment process of a device for removing ammonia nitrogen in citric acid absorbent in a farm according to claim 7, characterized in that: the content of chloride ions in the sodium chloride in the waste liquid tank is 1-5 g/L.
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