CN116791103A - Method for synthesizing ammonia by electrocatalytic nitric oxide - Google Patents
Method for synthesizing ammonia by electrocatalytic nitric oxide Download PDFInfo
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- CN116791103A CN116791103A CN202310531016.4A CN202310531016A CN116791103A CN 116791103 A CN116791103 A CN 116791103A CN 202310531016 A CN202310531016 A CN 202310531016A CN 116791103 A CN116791103 A CN 116791103A
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- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 title claims abstract description 114
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 title claims abstract description 111
- 229910021529 ammonia Inorganic materials 0.000 title claims abstract description 57
- 238000000034 method Methods 0.000 title claims abstract description 37
- 230000002194 synthesizing effect Effects 0.000 title claims abstract description 14
- 230000009467 reduction Effects 0.000 claims abstract description 30
- 239000007788 liquid Substances 0.000 claims abstract description 28
- 238000010521 absorption reaction Methods 0.000 claims abstract description 19
- 239000000243 solution Substances 0.000 claims description 29
- KCXVZYZYPLLWCC-UHFFFAOYSA-N EDTA Chemical compound OC(=O)CN(CC(O)=O)CCN(CC(O)=O)CC(O)=O KCXVZYZYPLLWCC-UHFFFAOYSA-N 0.000 claims description 18
- 239000003792 electrolyte Substances 0.000 claims description 14
- 238000006243 chemical reaction Methods 0.000 claims description 11
- 230000015572 biosynthetic process Effects 0.000 claims description 9
- 230000001105 regulatory effect Effects 0.000 claims description 9
- 238000003786 synthesis reaction Methods 0.000 claims description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 9
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 8
- 239000007864 aqueous solution Substances 0.000 claims description 8
- 239000006260 foam Substances 0.000 claims description 8
- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 claims description 8
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 6
- 229910052802 copper Inorganic materials 0.000 claims description 6
- 239000010949 copper Substances 0.000 claims description 6
- 239000012528 membrane Substances 0.000 claims description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 4
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 claims description 4
- 229910052799 carbon Inorganic materials 0.000 claims description 4
- 229910052759 nickel Inorganic materials 0.000 claims description 4
- 239000007789 gas Substances 0.000 claims description 3
- JVXHQHGWBAHSSF-UHFFFAOYSA-L 2-[2-[bis(carboxylatomethyl)amino]ethyl-(carboxylatomethyl)amino]acetate;hydron;iron(2+) Chemical compound [H+].[H+].[Fe+2].[O-]C(=O)CN(CC([O-])=O)CCN(CC([O-])=O)CC([O-])=O JVXHQHGWBAHSSF-UHFFFAOYSA-L 0.000 claims description 2
- 230000002378 acidificating effect Effects 0.000 claims description 2
- 235000003891 ferrous sulphate Nutrition 0.000 claims description 2
- 239000011790 ferrous sulphate Substances 0.000 claims description 2
- 229910017053 inorganic salt Inorganic materials 0.000 claims description 2
- 229910000359 iron(II) sulfate Inorganic materials 0.000 claims description 2
- 239000012266 salt solution Substances 0.000 claims description 2
- 238000009738 saturating Methods 0.000 claims description 2
- 239000000126 substance Substances 0.000 abstract description 5
- -1 ammonium ions Chemical class 0.000 abstract description 4
- 239000003337 fertilizer Substances 0.000 abstract description 3
- 238000004519 manufacturing process Methods 0.000 abstract description 3
- 239000003513 alkali Substances 0.000 abstract description 2
- 230000008878 coupling Effects 0.000 abstract description 2
- 238000010168 coupling process Methods 0.000 abstract description 2
- 238000005859 coupling reaction Methods 0.000 abstract description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 17
- 238000005868 electrolysis reaction Methods 0.000 description 14
- 229910052757 nitrogen Inorganic materials 0.000 description 8
- 239000010406 cathode material Substances 0.000 description 7
- 230000008901 benefit Effects 0.000 description 6
- GQPLMRYTRLFLPF-UHFFFAOYSA-N Nitrous Oxide Chemical compound [O-][N+]#N GQPLMRYTRLFLPF-UHFFFAOYSA-N 0.000 description 4
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical group [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 4
- 239000010936 titanium Substances 0.000 description 4
- 229910052719 titanium Inorganic materials 0.000 description 4
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 3
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 3
- 239000003054 catalyst Substances 0.000 description 3
- 239000012153 distilled water Substances 0.000 description 3
- 239000003546 flue gas Substances 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- CJTCBBYSPFAVFL-UHFFFAOYSA-N iridium ruthenium Chemical compound [Ru].[Ir] CJTCBBYSPFAVFL-UHFFFAOYSA-N 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- 238000004064 recycling Methods 0.000 description 3
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 2
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 239000013064 chemical raw material Substances 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000005265 energy consumption Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000004615 ingredient Substances 0.000 description 2
- 230000000813 microbial effect Effects 0.000 description 2
- 239000001272 nitrous oxide Substances 0.000 description 2
- 238000007747 plating Methods 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- HJPBEXZMTWFZHY-UHFFFAOYSA-N [Ti].[Ru].[Ir] Chemical group [Ti].[Ru].[Ir] HJPBEXZMTWFZHY-UHFFFAOYSA-N 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 238000010668 complexation reaction Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- ZOMNIUBKTOKEHS-UHFFFAOYSA-L dimercury dichloride Chemical class Cl[Hg][Hg]Cl ZOMNIUBKTOKEHS-UHFFFAOYSA-L 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 239000002638 heterogeneous catalyst Substances 0.000 description 1
- 239000002815 homogeneous catalyst Substances 0.000 description 1
- 239000000543 intermediate Substances 0.000 description 1
- 239000013067 intermediate product Substances 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 125000004433 nitrogen atom Chemical group N* 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 239000011368 organic material Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
- 230000006798 recombination Effects 0.000 description 1
- 239000003507 refrigerant Substances 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/27—Ammonia
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/50—Processes
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
- C25B11/03—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form perforated or foraminous
- C25B11/031—Porous electrodes
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/055—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the substrate or carrier material
- C25B11/057—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the substrate or carrier material consisting of a single element or compound
- C25B11/061—Metal or alloy
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/055—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the substrate or carrier material
- C25B11/057—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the substrate or carrier material consisting of a single element or compound
- C25B11/065—Carbon
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- Materials Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
The invention discloses a method for synthesizing ammonia by electrocatalytic nitrogen monoxide, which comprises the steps of absorbing nitrogen monoxide by using absorption liquid, and then performing electrocatalytic reduction on the absorption liquid of the nitrogen monoxide as catholyte through an electrolytic cell to generate ammonia; the method can effectively and highly selectively convert nitric oxide into ammonium ions, can be used in the production industry of chemical fertilizers, can be used for adding alkali solution to separate out the ammonium ions subsequently to obtain ammonia with higher purity, and can be used for preparing ammonia by adopting a method of liquid absorption coupling electrocatalytic reduction device.
Description
Technical Field
The invention relates to a method for synthesizing ammonia by electrocatalytic reduction of nitric oxide, in particular to a method for realizing recycling utilization by using high selectivity conversion of harmful ingredient nitric oxide in porous membrane electrode electrocatalytic reduction flue gas into high economic benefit ammonia. Belongs to the technical field of nitrogen oxide flue gas recycling treatment.
Background
Nitric oxide is an important link in microbial nitrogen circulation, is an intermediate product of microbial ammonia synthesis, is an important basic chemical raw material, is mainly used as a chemical fertilizer, a refrigerant and a chemical raw material, is one of chemical products with the largest yield in the world, is an ideal energy storage carrier, and plays an important role in global economy, and ammonia is mainly prepared by directly combining nitrogen and hydrogen in the presence of a catalyst in a Haber method in industry. The method has mature process, but needs high-temperature and high-pressure conditions, and has high investment and operation cost. At present, an attempt is continuously made to synthesize ammonia by electrocatalytic nitrogen reduction, and the method has the advantages that the method can be carried out under the conditions of normal temperature and normal pressure, but because of the chemical inertness of nitrogen, two nitrogen atoms of the nitrogen exist in the form of a nitrogen-nitrogen triple bond, the difficulty of bond breaking is high, the bond energy is very high, and the problems of low activity, low selectivity caused by hydrogen evolution reaction competition and the like exist in the current electrocatalytic nitrogen reduction. Nitric oxide, however, is the oxidation product of nitrogen at high temperatures, and has no poorly cleavable nitrogen-nitrogen triple bonds, but rather relatively weak nitrogen-oxygen bonds. Therefore, the nitrogen monoxide is used as a reducing substance to synthesize ammonia, so that the energy consumption of reduction can be greatly reduced, and the method has certain advantages in the speed and selectivity of synthesizing ammonia.
Electrocatalytic has been applied to degradation of structurally stable organic materials and molecular recombination reactions as an effective method for promoting chemical reactions. The technology has the advantages that the technology can be carried out at normal temperature and normal pressure, thereby greatly saving energy. As one of the important intermediates for the denitration reaction, the study of nitric oxide catalysis helps to understand the complex reaction mechanism thereof. The main products of this reaction are ammonia, nitrogen, nitrous oxide and hydrogen. Where ammonia is produced at a lower potential, nitrogen and nitrous oxide require relatively higher potentials. The current research on electrochemical reduction of nitric oxide mainly uses noble metals such as palladium, platinum, silver and other catalysts, and the selectivity is relatively low. Copper and nickel catalysts have many advantages of heterogeneous and homogeneous catalysts such as high catalytic selectivity, activity, clear structure, and extremely high atomic utilization. Thus, the conversion of the atmospheric pollutant nitric oxide into economically beneficial ammonia in a low cost, sustainable manner is of great importance.
Disclosure of Invention
Aiming at the defects of the prior art, the invention aims to improve the low-cost and high-efficiency electrocatalytic method for reducing nitric oxide to synthesize ammonia, and the method has high efficiency and high selectivity for reducing nitric oxide to synthesize ammonia, can be performed under the conditions of normal temperature and normal pressure, has mild conditions, low energy consumption, simple operation and environment-friendly process, and improves a new way for degrading and recycling the harmful ingredient nitric oxide in industrial flue gas.
In order to achieve the above object, the present invention provides a method for electrocatalytic reduction of nitric oxide to ammonia, wherein nitric oxide is absorbed by liquid complexation to obtain an absorption liquid containing nitric oxide, and the absorption liquid is used as an electrolyte of a cathode chamber to realize electrocatalytic synthesis of ammonia by an external power supply.
The aim of the invention can be achieved by the following technical scheme:
the method for synthesizing ammonia by electrocatalytic reduction of nitric oxide is characterized by comprising the following steps of: the electrocatalytic reaction is carried out in an H-type electrolytic cell, the H-type electrolytic cell comprises an anode chamber and a cathode chamber, the two electrode chambers are separated by a proton membrane, and an anode electrode and a cathode electrode are connected with a power supply; the nitric oxide absorption liquid is used as a cathode electrolyte, the inorganic salt aqueous solution is used as an anode electrolyte, and the ammonia is synthesized through electrocatalytic reduction.
The method for synthesizing ammonia by electrocatalytic nitrogen monoxide reduction is characterized by comprising the following steps of: the nitric oxide absorption liquid is formed by absorbing and saturating nitric oxide gas by the absorption liquid, the absorption liquid is water, ferrous salt water solution or ferrous complex water solution, and the pH value of the nitric oxide absorption liquid is regulated to be acidic.
The method for synthesizing ammonia by electrocatalytic nitrogen monoxide reduction is characterized by comprising the following steps of: the pH of the nitric oxide absorbing liquid is adjusted to 1-3, preferably 2.
The method for synthesizing ammonia by electrocatalytic nitrogen monoxide reduction is characterized by comprising the following steps of: the aqueous ferrous salt solution is an aqueous ferrous sulfate solution with a concentration of 5-20mmol/L, preferably 10mmol/L.
The method for synthesizing ammonia by electrocatalytic nitrogen monoxide reduction is characterized by comprising the following steps of: the ferrous complex aqueous solution is an ethylenediamine tetraacetic acid ferrous salt aqueous solution.
The method for synthesizing ammonia by electrocatalytic nitrogen monoxide reduction is characterized by comprising the following steps of: the concentration of the aqueous solution of ferrous ethylenediamine tetraacetate is 5-20mmol/L, preferably 10mmol/L.
The method for synthesizing ammonia by electrocatalytic nitrogen monoxide reduction is characterized by comprising the following steps of: the anode electrolyte is Na 2 SO 4 The concentration of the solution is 0.5-2 mol/L, preferably 1mol/L.
The method for synthesizing ammonia by electrocatalytic nitrogen monoxide reduction is characterized by comprising the following steps of: the cathode electrode adopts foam copper, foam nickel or carbon felt.
Compared with the prior art, the invention has the beneficial effects that:
the method can effectively and highly selectively convert nitric oxide into ammonium ions, can be used in the production industry of chemical fertilizers, can be used for adding alkali liquor for precipitation in the follow-up process of the ammonium ions to obtain ammonia with higher purity, and can be used for preparing ammonia by adopting a liquid absorption coupling electrocatalytic reduction method.
Detailed Description
The present invention will be described in further detail with reference to the following examples in order to make the objects, technical solutions and advantages of the present invention more apparent. The specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
The invention adopts absorption liquid to absorb nitric oxide gas, the nitrosyl complex after saturation absorption is put into a cathode chamber in an H-type electrolytic cell, the nitrosyl complex is electrified by an electrochemical workstation, electrocatalytic reduction is carried out under the overpotential condition, and ammonia generated by reduction is measured by an ultraviolet spectrophotometer. The ammonia selectivity was calculated by calculating the relationship between the decrease in the nitrosyl complex concentration and the ammonia production amount.
In the embodiment of the invention, the absorption liquid is 100mL of 10mmol Ÿ L -1 Fe (II) EDTA solution, or 10mmol Ÿ L for 100mL -1 FeSO 4 A solution. In the embodiment of the invention, the Fe (II) EDTA (NO) solution refers to 10mmolŸL -1 Fe (II) EDTA solution absorbs NO to saturation. In the embodiment of the invention, fe (NO) SO 4 Solution, means 10mmol Ÿ L -1 FeSO 4 The solution absorbs NO to saturation.
The concentration of Fe (II) EDTA (NO) is measured by a spectrophotometer, the electrocatalytic reaction is carried out in an H-type electrolytic cell in the embodiment of the invention, the H-type electrolytic cell comprises an anode chamber and a cathode chamber, the anode chamber and the cathode chamber are separated by a proton membrane, a three-electrode system is adopted, saturated calomel is used as a reference electrode, the anode electrode is titanium ruthenium iridium plating, the electrode substrate is titanium electrode, the surface of the titanium electrode is loaded with ruthenium iridium bimetallic active components, and the mass ratio of ruthenium iridium is 4:1, the total plating amount of ruthenium iridium on the titanium electrode is 1.2mg/cm 2 The titanium electrode size was 3 cm ×3 cm. The cathode electrode is made of foam copper, foam nickel or carbon felt with the size of 1 cm multiplied by 1 cm, and the cathode electrode is soaked in acetone and 0.1M HCl respectively for 24 h, then soaked in distilled water for 24 h, and ultrasonically cleaned for later use. Proton membrane is required to be in H 2 O 2 (30%), distilled water, 0.5M H 2 SO 4 And distilled water are boiled for 1 h in turn for standby.
Example 1: 100mL of Fe (II) EDTA (NO) solution is taken as cathode electrode liquid, and 100mL of 1mol Ÿ L is taken as cathode material -1 Na 2 SO 4 The solution is anode electrolyte, the initial pH of the catholyte is regulated to be 2, a three-electrode system is adopted to perform electrocatalytic reduction on the nitrosyl complex, constant voltage electrolysis is set, the voltage is-1V, the electrolysis temperature is 298K, ammonia is generated in a cathode chamber, and the ammonia selectivity is 39.42%.
Example 2: 100mL of Fe (II) EDTA (NO) solution is taken as cathode electrode liquid, and 100mL of 1mol Ÿ L is taken as cathode material -1 Na 2 SO 4 The solution is anode electrolyte, the initial pH of the catholyte is regulated to be 2, a three-electrode system is adopted to perform electrocatalytic reduction on the nitrosyl complex, constant voltage electrolysis is set, the voltage is-1V, the electrolysis temperature is 298K, ammonia is generated in a cathode chamber, and the ammonia selectivity is 33.55%.
Example 3: with carbon felt as cathode material, 100mL Fe (II) EDTA (NO) solution as cathode electrode liquid, 100 mL1 mol Ÿ L -1 Na 2 SO 4 The solution is anode electrolyte, the initial pH of the catholyte is regulated to be 2, a three-electrode system is adopted to perform electrocatalytic reduction on the nitrosyl complex, constant voltage electrolysis is set, the voltage is-1V, the electrolysis temperature is 298K, ammonia is generated in a cathode chamber, and the ammonia selectivity is 22.91%.
Example 4: 100mL of Fe (II) EDTA (NO) solution is taken as cathode electrode liquid, and 100mL of 1mol Ÿ L is taken as cathode material -1 Na 2 SO 4 The solution is anode electrolyte, the initial pH of the catholyte is regulated to be 2, a three-electrode system is adopted to perform electrocatalytic reduction on the nitrosyl complex, constant voltage electrolysis is set, the voltage is-1.6V, the electrolysis temperature is 298K, ammonia is generated in a cathode chamber, and the ammonia selectivity is 40.98%.
Example 5: 100mL of Fe (II) EDTA (NO) solution is taken as cathode electrode liquid, and 100mL of 1mol Ÿ L is taken as cathode material -1 Na 2 SO 4 The solution is anode electrolyte, the initial pH of the catholyte is regulated to be 2, a three-electrode system is adopted to perform electrocatalytic reduction on the nitrosyl complex, constant voltage electrolysis is set, the voltage is-1V, the electrolysis temperature is 308K, ammonia is generated in a cathode chamber, and the ammonia selectivity is 42.39%.
Example 6: 100mL Fe (NO) SO with copper foam as cathode material 4 The solution is cathode electrode liquid, 100 mL1 mol Ÿ L -1 Na 2 SO 4 The solution is anode electrolyte, the initial pH of the catholyte is regulated to be 2, a three-electrode system is adopted to perform electrocatalytic reduction on the nitrosyl complex, constant voltage electrolysis is set, the voltage is-1V, the electrolysis temperature is 298K, ammonia is generated in a cathode chamber, and the ammonia selectivity is 40.14%.
Example 7: 100mL Fe (NO) SO with copper foam as cathode material 4 The solution is cathode electrode liquid, 100 mL1 mol Ÿ L -1 Na 2 SO 4 The solution is anode electrolyte, the initial pH of the catholyte is regulated to be 2, a three-electrode system is adopted to perform electrocatalytic reduction on the nitrosyl complex, constant voltage electrolysis is set, the voltage is-1V, the electrolysis temperature is 308K, ammonia is generated in a cathode chamber, and the ammonia selectivity is 40.57%.
Claims (8)
1. A method for synthesizing ammonia by electrocatalytic nitrogen monoxide, which is characterized by comprising the following steps: the electrocatalytic reaction is carried out in an H-type electrolytic cell, the H-type electrolytic cell comprises an anode chamber and a cathode chamber, the two electrode chambers are separated by a proton membrane, and an anode electrode and a cathode electrode are connected with a power supply; the nitric oxide absorption liquid is used as a cathode electrolyte, the inorganic salt aqueous solution is used as an anode electrolyte, and the ammonia is synthesized through electrocatalytic reduction.
2. The method for electrocatalytic nitric oxide synthesis of ammonia according to claim 1, wherein: the nitric oxide absorption liquid is formed by absorbing and saturating nitric oxide gas by the absorption liquid, the absorption liquid is water, ferrous salt water solution or ferrous complex water solution, and the pH value of the nitric oxide absorption liquid is regulated to be acidic.
3. A method for electrocatalytic nitric oxide synthesis of ammonia according to claim 2, wherein: the pH of the nitric oxide absorbing liquid is adjusted to 1-3, preferably 2.
4. The method for electrocatalytic nitrogen monoxide reduction synthesis of ammonia according to claim 2, wherein: the aqueous ferrous salt solution is an aqueous ferrous sulfate solution with a concentration of 5-20mmol/L, preferably 10mmol/L.
5. A method for electrocatalytic nitric oxide synthesis of ammonia according to claim 2, wherein: the ferrous complex aqueous solution is an ethylenediamine tetraacetic acid ferrous salt aqueous solution.
6. A method for electrocatalytic nitric oxide synthesis of ammonia according to claim 2, wherein: the concentration of the aqueous solution of ferrous ethylenediamine tetraacetate is 5-20mmol/L, preferably 10mmol/L.
7. The method for electrocatalytic nitric oxide synthesis of ammonia according to claim 1, wherein: the anode electrolyte is Na 2 SO 4 The concentration of the solution is 0.5-2 mol/L, preferably1mol/L。
8. The method for electrocatalytic nitric oxide synthesis of ammonia according to claim 1, wherein: the cathode electrode adopts foam copper, foam nickel or carbon felt.
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| CN202310531016.4A CN116791103A (en) | 2023-05-12 | 2023-05-12 | Method for synthesizing ammonia by electrocatalytic nitric oxide |
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| CN202310531016.4A CN116791103A (en) | 2023-05-12 | 2023-05-12 | Method for synthesizing ammonia by electrocatalytic nitric oxide |
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