CN112501640B - Battery system for converting nitrate wastewater into ammonia - Google Patents
Battery system for converting nitrate wastewater into ammonia Download PDFInfo
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- CN112501640B CN112501640B CN202011434679.7A CN202011434679A CN112501640B CN 112501640 B CN112501640 B CN 112501640B CN 202011434679 A CN202011434679 A CN 202011434679A CN 112501640 B CN112501640 B CN 112501640B
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- C25B1/00—Electrolytic production of inorganic compounds or non-metals
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Abstract
The invention relates to the field of battery technology and nitrate waste liquid treatment and ammonia synthesis, in particular to a battery system for converting nitrate waste water into ammonia. The invention provides a battery system for converting nitrate wastewater into ammonia, which realizes resource utilization of waste and generates economic benefits.
Description
Technical Field
The invention relates to the field of battery technology and nitrate waste liquid treatment and ammonia synthesis, in particular to a battery system for converting acid salt waste water into ammonia.
Background
In industrial production processes, nitrate is directly or indirectly produced in most industries, and the conventional nitrate removal methods mainly include a reverse osmosis method, an electrodialysis method, an ion exchange method, a catalytic denitrification method, a chemical denitrification method and a biological denitrification method. The nitric acid is reduced and converted into ammonia under the catalysis of an electrochemical method, so that the nitric acid can be removed, valuable ammonia can be generated, and economic benefits are generated.
The metal-water battery replaces the cathode oxygen reduction reaction of the traditional metal-dissolved oxygen battery with the water reduction hydrogen evolution reaction, not only can generate electricity, but also can effectively prepare hydrogen, and realizes hydrogen-electricity integration. Scientists successively invent lithium-water hydrogen production batteries (adv.energy.mater, 2016, 1601390), zinc-water hydrogen production batteries (Angew.chem.2018, 130, 3974-3979) and aluminum-water hydrogen production batteries (Chemeletrochem, 2020, 7.2582-2591), but hydrogen also mainly has the problem of difficult storage and transportation, hydrogen must be cooled to be lower than-253 ℃ to be liquefied, which means that one third of energy of hydrogen fuel is consumed, a storage container needs a special heat insulation and cooling facility, the cost is high, the danger is large, and therefore, the matter which is conveniently stored and transported by electrolytic synthesis has practical application value; compared with the prior art, the ammonia gas can be liquefied at the temperature of minus 10 ℃ by adding a little pressure, the energy loss is small, the ammonia gas is safe and convenient to store and transport, the volume energy density of the liquid ammonia is almost 2 times that of the liquid hydrogen, and a container with the same volume can store more energy.
Disclosure of Invention
In order to solve the technical problems, the invention provides a battery system for converting nitrate wastewater into ammonia, so that the waste is recycled, and economic benefits are generated.
The invention adopts the following technical scheme:
the utility model provides a turn into battery system of ammonia with nitrate waste water, battery system includes battery anode, battery negative pole and electrolyte, battery anode is active metal material, battery negative pole is the electrode with load nitrate reduction catalyst material, the electrolyte is the waste water that contains nitrate, the battery system generates electricity and turns into ammonia with the nitrate in the waste water simultaneously.
The technical scheme is further improved in that the anode of the battery reacts to lose electrons of metal, and the cathode of the battery reacts to reduce nitrate into ammonia by a catalyst.
The technical scheme is further improved in that the battery anode is made of metal, and the metal is one of magnesium, aluminum, zinc, tin, iron and lithium.
The technical scheme is further improved in that the battery anode is made of metal alloy, and the metal alloy is one of magnesium alloy, aluminum alloy, zinc alloy, tin alloy, iron alloy and lithium alloy.
The technical proposal is further improved that the magnesium alloy is a magnesium alloy containing at least one of aluminum, zinc and manganese; the aluminum alloy is an aluminum alloy containing at least one of magnesium, zinc and manganese.
The technical proposal is further improved that the zinc alloy is a zinc alloy containing at least one of magnesium, aluminum and copper; the tin alloy is a tin alloy containing at least one of lithium, magnesium, aluminum and iron.
In a further improvement of the above technical solution, the iron alloy is an iron alloy containing at least one of aluminum and calcium; the lithium alloy is a lithium alloy containing at least one of aluminum, magnesium and boron.
The technical proposal is further improved in that the cathode of the battery is one or more of nickel-based catalyst, ruthenium-based catalyst, copper-based catalyst, single metal catalyst, multi-element metal catalyst or oxide, boride, phosphide and sulfide thereof.
The technical proposal is further improved in that the waste water containing nitrate is strong alkali, and the pH value is more than 11.
The technical proposal is further improved in that the battery anode and the battery cathode are separated by a diaphragm, and the diaphragm comprises one of a bipolar membrane, a proton membrane and a glass sand core.
The invention has the beneficial effects that:
the invention adopts active metal such as magnesium, aluminum, zinc, lithium and alloy thereof as a battery cathode, a nickel-based catalyst, a ruthenium-based catalyst or a copper-based catalyst as an anode, and nitrate-containing wastewater as electrolyte, and the nitrate in the wastewater is converted into ammonia while the battery generates electricity; the electricity generated by the battery system can be stored by connecting a storage battery or be connected into a power grid; the ammonia gas generated by the catalytic reduction of nitrate by the anode can be collected by an evaporation-condensation method and used as a chemical raw material or an ammonia fuel cell fuel, and the nano-scale magnesium hydroxide generated by the cathode can be used as an excellent flame retardant raw material, so that the resource utilization of wastes is realized, and the economic benefit is generated.
Drawings
FIG. 1 is a schematic diagram of a battery system for converting nitrate-containing wastewater into ammonia according to the present invention;
FIG. 2 is a graph of the zinc-nitrate battery performance test-CV for the battery system of FIG. 1 for converting nitrate wastewater to ammonia;
FIG. 3 is a graph of zinc-nitrate cell performance test versus different constant current discharge test performance for the battery system of FIG. 1 for converting nitrate wastewater to ammonia;
FIG. 4 is a graph of magnesium-nitrate battery performance test-CV for the battery system of FIG. 1 for converting nitrate-containing wastewater to ammonia;
FIG. 5 is a graph of aluminum-nitrate battery performance test-CV for the battery system of FIG. 1 for converting nitrate-containing wastewater to ammonia;
FIG. 6 is a graph of magnesium alloy-nitrate battery performance test-CV for the battery system of FIG. 1 for converting nitrate-containing wastewater to ammonia;
FIG. 7 is a graph of the Zinc-nitrate battery performance test-CV for the battery system of FIG. 1 for converting nitrate-containing wastewater to ammonia;
FIG. 8 is a zinc-nitrate constant current of 10mA cm for the battery system of FIG. 1 for converting nitrate-containing wastewater to ammonia -2 A discharge performance test performance diagram;
FIG. 9 is the zinc-nitrate galvanostatic 10mA cm of the battery system of FIG. 1 for conversion of nitrate wastewater to ammonia -2 Discharge synthesis ammonia yield and current conversion efficiency diagram;
fig. 10 is a graph of aluminum-nitrate battery performance test-CV for the battery system of fig. 1 for converting nitrate-containing wastewater to ammonia.
Detailed Description
The technical solution in the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings of the present invention.
As shown in fig. 1 to 10, a battery system for converting nitrate wastewater into ammonia includes a battery anode that is one of a metal or a metal alloy, a battery cathode that is an electrode supporting a nitrate reduction catalyst material, and an electrolyte that is nitrate-containing wastewater, and generates electricity while converting nitrate in the wastewater into ammonia.
As shown in fig. 1, which is a schematic view of the structure of the present invention, wherein 1-cell cathode; 2-a battery anode; 3-battery electrolyte; 4-a separator; 5-ammonia gas outlet.
Specifically, the reaction at the anode of the battery is a metal electron loss (A-e) - →A + ) The reaction of the cathode of the cell is the reduction of nitrate to ammonia (NO) by the catalyst 3 - +8e - +6H 2 O→NH 3 +9OH - )。
Specifically, the battery anode is metal, and the metal is one of magnesium, aluminum, zinc, tin, iron and lithium.
Specifically, the battery anode is made of metal alloy, and the metal alloy is one of magnesium alloy, aluminum alloy, zinc alloy, tin alloy, iron alloy and lithium alloy.
Specifically, the magnesium alloy is a magnesium alloy containing at least one of aluminum, zinc and manganese; the aluminum alloy is an aluminum alloy containing at least one of magnesium, zinc and manganese; the zinc alloy is a zinc alloy containing at least one of magnesium, aluminum and copper; the tin alloy is a tin alloy containing at least one of lithium, magnesium, aluminum and iron; the iron alloy is an iron alloy containing at least one of aluminum and calcium; the lithium alloy is a lithium alloy containing at least one of aluminum, magnesium and boron.
Preferably, the metal of the battery anode is magnesium, aluminum, zinc or metal alloy of aluminum alloy and zinc alloy, and the anode material has higher stability and higher electrode potential.
Specifically, the cathode of the battery is one or more of a nickel-based catalyst, a ruthenium-based catalyst, a copper-based catalyst, a single metal catalyst, a multi-element metal catalyst or an oxide, a boride, a phosphide and a sulfide thereof.
Preferably, the cathode adopts a nickel-based catalyst and a ruthenium-based catalyst, and the catalysts have higher current conversion efficiency of the synthetic ammonia.
Specifically, the nitrate-containing wastewater is strong in alkalinity, and the pH value is greater than 11, so that the converted ammonia is easy to escape and collect.
Preferably, the pH value of the nitrate-containing wastewater is more than or equal to 13, so that ammonia can escape and is convenient to collect.
Specifically, the battery anode and the battery cathode are separated by a diaphragm, wherein the diaphragm comprises one of a bipolar membrane, a proton membrane and a glass sand core, and the purpose of the diaphragm is to prevent or delay ammonia generated by the cathode from diffusing to the anode and being oxidized again on the anode.
The first embodiment is as follows:
the anode of the battery adopts zinc foil, the cathode of the battery adopts an electrode of a copper foam loaded Cu-based nanoparticle catalyst, the battery is assembled, and the discharge performance and the performance of reducing nitrate to generate ammonia are tested.
The test conditions were: the electrode area of the cathode foamy copper-loaded Cu-based nanoparticle catalyst is 5x5mm, the anode is zinc foil, the anolyte is 1M KOH, and the catholyte is1M KOH+1M NaNO 3 The cathode cell and the anode cell were separated by a Nafion proton membrane, and cyclic voltammetry CV and constant current (20 mA/cm) 2 ) And (4) discharge performance.
The battery CV of the test results is shown in FIG. 2, in which the abscissa is voltage, the left side of the ordinate is current density, and the right side is electric power; the constant current discharge performance of the battery is shown in fig. 3, wherein the ordinate represents the discharge time and the abscissa represents the discharge voltage. As can be seen from the graph, the open-circuit voltage of the battery is 0.98V, and the short-circuit current is 103mA/cm 2 Maximum output power of 17mW/cm 2 (ii) a Constant current of 10mA/cm 2 Under the condition, the output voltage is 0.6V, and the current conversion efficiency of the nitrate synthetic ammonia is 7 percent.
Example two:
the battery anode adopts a magnesium sheet, the battery cathode adopts an electrode of a foamed nickel loaded Ru-Ni composite catalyst, the battery is assembled, the discharge performance is tested, and the performance of reducing nitrate to generate ammonia is tested.
The test conditions were: the electrode area of the foamed nickel loaded Ru-Ni composite catalyst of the battery cathode is 5x5mm, the battery anode is a magnesium sheet, the battery anolyte is 1MKOH, and the battery catholyte is 1M KOH +1M NaNO 3 And separating the cathode cell and the anode cell by using a Nafion proton membrane, and testing the cyclic voltammetry CV performance of the cell.
The test result shows that the CV of the battery is shown in figure 4, wherein the abscissa of the graph is voltage, the left side of the ordinate is current density, and the right side of the ordinate is electric power; as can be seen from the graph, the open-circuit voltage of the battery is 1.25V, and the short-circuit current is 1.1mA/cm 2 Maximum output power of 0.5mW/cm 2 。
Example three:
the anode of the battery adopts an aluminum sheet, the cathode of the battery adopts an electrode of a copper foam loaded Cu-based nanoparticle catalyst, the battery is assembled, and the discharge performance and the performance of reducing nitrate to generate ammonia are tested.
The test conditions were: the electrode area of the cathode copper foam loaded Cu-based nanoparticle catalyst is 5x5mm, the anode is aluminum sheet, the anolyte is 1M KOH, and the catholyte is 1M KOH +1M NaNO 3 Nafion protons for cathode cell and anode cellAnd (5) separating the membranes, and testing the cyclic voltammetry CV performance of the battery.
The test result shows that the CV of the battery is as shown in FIG. 5, wherein the abscissa of the graph is voltage, the left side of the ordinate is current density, and the right side of the ordinate is electric power; as can be seen from the graph, the open-circuit voltage of the battery is 1.05V, and the short-circuit current is 120mA/cm 2 Maximum output power 23mW/cm 2 。
Example four:
the anode of the battery adopts magnesium alloy AZ31B, the cathode of the battery adopts an electrode of a foamed nickel loaded Ru-Ni composite catalyst, the battery is assembled, the discharge performance is tested, and the performance of reducing nitrate to generate ammonia is tested.
The test conditions were: the electrode area of the foamed nickel loaded Ru-Ni composite catalyst of the battery cathode is 5x5mm, the battery anode is magnesium alloy AZ31B, the battery anode electrolyte is 1MKOH, and the battery cathode electrolyte is 1M KOH +1M NaNO 3 And separating the cathode cell and the anode cell by using a Nafion proton membrane, and testing the cyclic voltammetry CV performance of the cell.
The test result shows that the CV of the battery is shown as figure 6, wherein the abscissa of the figure is voltage, the left side of the ordinate is current density, and the right side of the ordinate is electric power; as can be seen from the graph, the open-circuit voltage of the battery is 0.28V, and the short-circuit current is 0.15mA/cm 2 。
Example five:
the anode of the battery adopts zinc foil, the cathode of the battery adopts an electrode of a foamed nickel loaded Ru-Ni composite catalyst, the battery is assembled, and the discharge performance and the performance of reducing nitrate to generate ammonia are tested.
The test conditions were: the electrode area of the foamed nickel loaded Ru-Ni composite catalyst of the battery cathode is 5x5mm, the battery anode is a zinc foil, the battery anolyte is 1M KOH, and the battery catholyte is 1M KOH +1M NaNO 3 And separating the cathode cell and the anode cell by using a Nafion proton membrane, and testing the cyclic voltammetry CV performance of the cell.
The test result shows that the CV of the battery is shown in FIG. 7, wherein the abscissa of the graph is voltage, the left side of the ordinate is current density, and the right side of the ordinate is electric power; as can be seen from the figure, the open-circuit voltage of the battery is 1.3V, and the short-circuit current is 80mA/cm 2 Maximum output power of 11mW/cm 2 . As shown in FIG. 8, the constant current is 10mA/cm 2 Under the discharge condition, the battery voltage is stabilized at about 0.52V; as shown in FIG. 9, the current is 10mA/cm at constant current 2 Under the discharge condition, the generation rate of ammonia and the current efficiency thereof are shown in the figure, and the ammonia production time is gradually improved, and the current conversion efficiency of the synthetic ammonia is maintained to be more than 75 percent.
Example six:
the anode of the battery adopts an aluminum sheet, the cathode of the battery adopts an electrode of a foamy copper loaded CuO nano-particle catalyst, the battery is assembled, and the discharge performance and the performance of reducing nitrate to generate ammonia are tested.
The test conditions were: the electrode area of the copper foam loaded Cu-based nanoparticle catalyst at the cathode of the battery is 5x5mm, the anode of the battery is aluminum sheet, and the electrolyte at the anode of the battery is 1M KOH +1M NaNO 3 The cathode electrolyte of the battery is 1M KOH +1M NaNO 3 And separating the cathode cell and the anode cell by using a Nafion proton membrane, and testing the cyclic voltammetry CV performance of the cell.
The test result shows that the battery CV is shown in FIG. 10, wherein the abscissa of the graph is voltage, the left side of the ordinate is current density, and the right side of the ordinate is electric power; as can be seen from the figure, the open-circuit voltage of the battery is 1.05V, and the short-circuit current is 80mA/cm 2 Maximum output power of 14mW/cm 2 。
The invention adopts active metal such as magnesium, aluminum, zinc, lithium and alloy thereof as a battery cathode, a nickel-based catalyst, a ruthenium-based catalyst or a copper-based catalyst as an anode, and nitrate-containing wastewater as electrolyte, and the nitrate in the wastewater is converted into ammonia while the battery generates electricity; the electricity generated by the battery system can be stored by connecting a storage battery or be connected into a power grid; the ammonia gas generated by the catalytic reduction of nitrate by the anode can be collected by an evaporation-condensation method and used as a chemical raw material or an ammonia fuel cell fuel, and the nano-scale magnesium hydroxide generated by the cathode can be used as an excellent flame retardant raw material, so that the resource utilization of wastes is realized, and the economic benefit is generated.
The above-mentioned embodiments only express several embodiments of the present invention, and the description thereof is more specific and detailed, but not construed as limiting the scope of the present invention. It should be noted that various changes and modifications can be made by those skilled in the art without departing from the spirit of the invention, and these changes and modifications are all within the scope of the invention. Therefore, the protection scope of the present patent should be subject to the appended claims.
Claims (4)
1. A battery system for converting nitrate wastewater into ammonia comprises a battery anode, a battery cathode and an electrolyte, and is characterized in that the battery anode is an active metal material, the electrolyte is wastewater containing nitrate, and the battery system generates electricity and converts the nitrate in the wastewater into ammonia; the nitrate-containing wastewater is alkaline;
the battery anode is metal, and the metal is one of aluminum and zinc;
the cathode of the battery is an electrode loaded with a nitrate reduction catalyst material, and the catalyst is one or two of a ruthenium-nickel catalyst and a copper-based catalyst;
the anode and the cathode of the battery are separated by a diaphragm, and the diaphragm comprises one of a bipolar membrane, a proton membrane and a glass sand core and is used for preventing or delaying ammonia generated by the cathode from diffusing to the anode and being oxidized again on the anode.
2. The battery system for converting nitrate-containing wastewater into ammonia according to claim 1, wherein the reaction at the anode of the battery is the loss of electrons from the metal and the reaction at the cathode of the battery is the reduction of nitrate into ammonia.
3. The battery system for converting nitrate-containing wastewater to ammonia according to claim 1, wherein the nitrate-containing wastewater has a pH >11.
4. The battery system for converting nitrate-containing wastewater into ammonia according to claim 1, wherein the copper-based catalyst is a copper oxide catalyst.
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| CN113061918B (en) * | 2021-03-24 | 2022-07-26 | 东莞理工学院 | Hydrogen-electricity integrated device for continuous hydrogen production and application thereof |
| CN113668001A (en) * | 2021-07-27 | 2021-11-19 | 北京化工大学 | Method for synthesizing ammonia by electrocatalysis nitrate radical reduction using hydrogen evolution reaction catalyst |
| CN113789541B (en) * | 2021-10-26 | 2022-09-09 | 苏州科技大学 | Phosphorus and oxygen co-doped copper-based catalyst and preparation method and application thereof |
| CN116161752A (en) * | 2023-03-09 | 2023-05-26 | 东莞理工学院 | Preparation method of composite electrode and application of composite electrode in nitrate-containing wastewater |
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| CN102039125A (en) * | 2009-10-13 | 2011-05-04 | 中国科学院生态环境研究中心 | Preparation and application method of supported bimetallic catalyst for removing nitrate in water |
| CN103236540B (en) * | 2013-05-17 | 2015-06-10 | 重庆大学 | Positive material for magnesium cell, preparation method of positive material and magnesium cell |
| CN105958096A (en) * | 2016-01-20 | 2016-09-21 | 北京师范大学-香港浸会大学联合国际学院 | Improved microalgae biological direct-driven power generation battery |
| CN104928706B (en) * | 2015-06-30 | 2017-07-21 | 福建师范大学 | It is a kind of based on seawater battery technology by nutrient discovery in breeding wastewater into ammonium magnesium phosphate device |
| CN106898788A (en) * | 2015-12-18 | 2017-06-27 | 中国科学院大连化学物理研究所 | A kind of magnesium water battery |
| CN105540954B (en) * | 2016-01-08 | 2018-01-16 | 四川师范大学 | A kind of method that chemical denitrification removes nitrate nitrogen in water removal |
| CN108002518B (en) * | 2017-12-16 | 2023-11-17 | 傲自然成都生物科技有限公司 | Bioelectrochemical system and purification method for purifying nitrate in drinking water |
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