CN113122882A - Ore pulp battery - Google Patents

Ore pulp battery Download PDF

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Publication number
CN113122882A
CN113122882A CN202110666852.4A CN202110666852A CN113122882A CN 113122882 A CN113122882 A CN 113122882A CN 202110666852 A CN202110666852 A CN 202110666852A CN 113122882 A CN113122882 A CN 113122882A
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reaction tank
anode
cathode
pulp
battery
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CN113122882B (en
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纪效波
陈军
孙伟
胡岳华
侯红帅
邹国强
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Central South University
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Central South University
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    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C1/00—Electrolytic production, recovery or refining of metals by electrolysis of solutions
    • C25C1/06—Electrolytic production, recovery or refining of metals by electrolysis of solutions or iron group metals, refractory metals or manganese
    • C25C1/10—Electrolytic production, recovery or refining of metals by electrolysis of solutions or iron group metals, refractory metals or manganese of chromium or manganese
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C1/00—Electrolytic production, recovery or refining of metals by electrolysis of solutions
    • C25C1/06—Electrolytic production, recovery or refining of metals by electrolysis of solutions or iron group metals, refractory metals or manganese
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C1/00—Electrolytic production, recovery or refining of metals by electrolysis of solutions
    • C25C1/06—Electrolytic production, recovery or refining of metals by electrolysis of solutions or iron group metals, refractory metals or manganese
    • C25C1/08—Electrolytic production, recovery or refining of metals by electrolysis of solutions or iron group metals, refractory metals or manganese of nickel or cobalt
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C1/00—Electrolytic production, recovery or refining of metals by electrolysis of solutions
    • C25C1/16—Electrolytic production, recovery or refining of metals by electrolysis of solutions of zinc, cadmium or mercury
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C7/00—Constructional parts, or assemblies thereof, of cells; Servicing or operating of cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/36—Accumulators not provided for in groups H01M10/05-H01M10/34
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

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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)
  • Manufacturing & Machinery (AREA)
  • General Chemical & Material Sciences (AREA)
  • Manufacture And Refinement Of Metals (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

The invention provides an ore pulp battery, which comprises a reaction tank, a diaphragm, an anode, a cathode, anode slurry, cathode electrolyte and a lead, wherein the diaphragm divides the reaction tank into the cathode reaction tank and the anode reaction tank; one end of the cathode is arranged in the cathode reaction tank, one end of the anode is arranged in the anode reaction tank, and the other end of the cathode is connected with the other end of the anode through a lead to form a closed loop; the diaphragm is an anion exchange membrane; the catholyte is placed in the cathode reaction tank and comprises an acidic metal salt solution, and the metal is at least one of manganese, zinc, iron, cobalt and nickel; placing anode slurry in an anode reaction tank, wherein the anode slurry comprises minerals, conductive carbon and an acid solution, and the pH value is 0-7; the minerals include copper and/or iron minerals. The ore pulp battery provided by the invention can simultaneously realize metal extraction and energy storage/conversion, and effectively solves the problems of high energy consumption, serious environmental pollution, harsh conditions and the like in the traditional metal smelting process.

Description

Ore pulp battery
Technical Field
The invention relates to the technical field of metal extraction and energy storage/conversion, in particular to an ore pulp battery.
Background
With the rapid development of human society, the demand of human resources is increasing. Mining, crushing and metal extraction are all energy intensive processes. Along with the gradual decline of global ore tastes, energy sources are more intensive, and the high-efficiency separation of complex low-grade ores is realized. The development of metal extraction technology is severely restricted by high cost, serious environmental pollution, harsh conditions and the like. Therefore, the development of an efficient and clean metal extraction technology is significant.
Chalcopyrite ore (CuFeS)2) Chalcopyrite is the main copper ore in rock layers, and the mass fraction of copper is as high as 34%. During the process of leaching the chalcopyrite at normal temperature, a layer of sulfur film is generated on the surface of the chalcopyrite, which prevents the chalcopyrite from being leached continuously. Thus, around 80% of copper is obtained by traditional pyrometallurgical processes worldwide. The energy requirements for the pyrometallurgical process for processing chalcopyrite, including mineral processing and flotation processes, require approximately 3.8 kilowatt-hours of energy to produce 1 kilogram of copper from mined ore. Meanwhile, 1 ton of pure copper is produced, and 5.4 tons of greenhouse gas carbon dioxide is emitted. Energy requirements and greenhouse gas emissions are inversely related to the grade of the copper ore. However, the ore grade of copper ores has continued to decline over the past 100 years. On average, the global copper ore grade has dropped from 1.5% -4.0% to about 0.6% from 1900 to 2010. It is predicted that by 2050, the copper ore grade may further decrease to about 0.49%. Therefore, the method for recovering the metal elements such as lithium, copper, nickel, cobalt, manganese and the like from the electronic waste and the low-grade complex tailings by the efficient and environment-friendly hydrometallurgical process has very strong attraction in the aspects of environmental protection and resource recovery.
Disclosure of Invention
In view of the above technical problems in the prior art, the present invention provides a pulp battery, which can simultaneously realize metal extraction and electric energy storage/conversion. Moreover, the ore pulp battery can effectively overcome the problems of high energy consumption, serious environmental pollution, harsh conditions and the like in the traditional wet method/fire method metal extraction process in the process of realizing metal extraction and electric energy storage/conversion.
In order to achieve the purpose, the technical scheme of the invention is as follows:
a pulp battery comprises a reaction tank, a diaphragm, an anode, a cathode, anode slurry, a cathode electrolyte and a lead, wherein the diaphragm divides the reaction tank into a cathode reaction tank and an anode reaction tank; one end of the cathode is arranged in the cathode reaction tank, one end of the anode is arranged in the anode reaction tank, and the other end of the cathode is connected with the other end of the anode through the lead to form a closed loop; the diaphragm is an anion exchange membrane; the catholyte is placed in the cathode reaction tank and comprises an acidic metal salt solution, and the metal is at least one of manganese, zinc, iron, cobalt and nickel; the anode slurry is placed in the anode reaction tank, the anode slurry comprises minerals, conductive carbon and an acid solution, and the pH value is 0-7; the minerals include copper and/or iron minerals. Specifically, the acidic metal salt solution is a mixture of a metal salt solution including, but not limited to, a sulfate, a chloride and a nitrate of a metal and an acid solution selected from one or a mixture of two or more of sulfuric acid, hydrochloric acid and nitric acid.
In some embodiments, the anode slurry comprises 16 to 56wt% of a mineral, 4 to 14wt% of a conductive carbon, and 30 to 80wt% of an acid solution.
In some embodiments, the copper ore is at least one of chalcopyrite, bornite, chalcocite, covellite, enargite, chalcanthite, bismuthate, tetrahedrite, chalcocite, sulfoselenogeite; the iron ore is at least one of pyrite, marcasite, pyrrhotite, maryolite and low-silver pyrite.
In some embodiments, the catholyte further comprises a corrosion inhibitor, the corrosion inhibitor having a concentration of 1 to 1000 ppm. Preferably, the corrosion inhibitor is selected from at least one of cetrimide, sulfenyl benzothiazole and benzotriazole.
In some embodiments, the separator is at least one of 2, 6-dimethyl-1, 4-phenylene ether, polysulfones, polyvinyl alcohol polymers.
In some embodiments, the membrane has a thickness of 5 to 100 μm.
In some embodiments, the conductive carbon is at least one of activated carbon, carbon black, acetylene black, carbon nanotubes, ketjen black, graphene.
In some embodiments, the cathode and the anode are each selected from one of aluminum, lead, zinc, and graphite. Preferably, the cathode and the anode are respectively a cathode plate and an anode plate, the thickness of the cathode plate is 1-5mm, and the thickness of the anode plate is 1-5 mm.
In some embodiments, the side of the reaction tank is a hollow structure with a communication, the reaction tank comprises a water inlet and a water outlet, the water inlet is arranged at the lower part of one side of the reaction tank, and the water outlet is arranged at the upper part of the other side of the reaction tank, which is opposite to the reaction tank, and is used for reducing the reaction temperature in the cathode reaction tank and the anode reaction tank.
In some embodiments, the slurry cell further comprises an anode material storage device, a cathode material storage device and a plurality of conduits; the anode material storage device is communicated with the anode reaction tank through the two guide pipes to form an anode slurry circulation loop, and the top and the bottom of the anode material storage device are respectively provided with a first feeding hole and a first discharging hole; the cathode material storage device is communicated with the cathode reaction tank through two guide pipes to form a cathode electrolyte circulation loop, and the cathode material storage device is also provided with a second feeding hole.
In some embodiments, the bottom of the anode reaction tank and the bottom of the cathode reaction tank are further provided with a second discharge hole and a third discharge hole respectively.
The realization principle of the battery of the invention is as follows:
the diaphragm divides the reaction tank into an anode reaction tank and a cathode reaction tank, and anions can move between the anode reaction tank and the cathode reaction tank through the diaphragm. During charging, the minerals of the anode slurry lose electrons and dissolve to generate metal ions which are dissolved in the solution, the electrons move from the lead to the cathode, the anions move from the cathode reaction tank to the anode reaction tank, and the electrons of the metal ions in the cathode electrolyte are reduced to form metal which is deposited on the surface of the cathode; during discharging, electrons move from the cathode to the anode through a lead based on the potential difference between the anode and the cathode, anions move from the anode reaction tank to the cathode reaction tank, metal deposition on the surface of the cathode loses the electrons to form metal ions which are dissolved in a solution, the electrons of the metal ions in the anode reaction tank form low-valence metal ions, and metal extraction and energy storage/conversion are realized in the charging and discharging process. Along with the continuous progress of the reaction, the minerals in the anode slurry are continuously dissolved, the concentration of the metal ions in the anode reaction tank is continuously increased, and when the reaction reaches a certain degree, the solution containing the high-concentration metal ions in the anode reaction tank can be discharged and collected for further treatment to finish metal smelting/extraction.
Compared with the prior art, the invention has the following beneficial effects:
(1) the ore pulp battery provided by the invention can realize metal extraction and energy storage/conversion at the same time.
(2) The ore pulp battery provided by the invention can effectively solve the problems of high energy consumption, serious environmental pollution, harsh conditions and the like in the traditional pyrometallurgical/hydrometallurgical metal smelting/extracting process.
(3) The ore pulp battery technology provided by the invention can be used for building a factory on site, effectively solving the problems of environmental pollution, cost increase and the like caused by mineral transportation, and effectively saving the cost.
Drawings
Figure 1 is a schematic diagram of the charging of a pulp battery in example 1;
figure 2 is a schematic diagram of the discharge of the pulp battery of example 1;
figure 3 is a schematic diagram of the charging of the ore pulp battery in the embodiment 2;
figure 4 is a schematic diagram of the discharge of the pulp battery of example 2.
The device comprises a reaction tank 1, a diaphragm 2, an anode reaction tank 3, a cathode reaction tank 4, an anode 5, a cathode 6, an anode material tank 7, a cathode material tank 8, a first feed inlet 9, a first discharge outlet 10, a second feed inlet 11, a guide pipe 12, a water inlet 13, a water outlet 14, a second discharge outlet 15, a third discharge outlet 16, a bornite 17 and acetylene black 18.
Detailed Description
In the following description, numerous specific details are set forth in order to provide a thorough understanding of the present invention. This invention may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein, but rather should be construed as broadly as the present invention is capable of modification in various respects, all without departing from the spirit and scope of the present invention.
In the description of the present invention, it should be noted that the terms "center", "upper", "lower", "left", "right", "vertical", "horizontal", "inner", "outer", etc., indicate orientations or positional relationships based on the orientations or positional relationships shown in the drawings, and are only for convenience of description and simplicity of description, but do not indicate or imply that the device or element being referred to must have a particular orientation, be constructed and operated in a particular orientation, and thus, should not be construed as limiting the present invention. Furthermore, the terms "first," "second," and "third" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The terminology used in the description of the invention herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention.
As shown in fig. 1 and 2, a pulp battery comprises a reaction tank 1, a diaphragm 2, an anode 5, a cathode 6, anode slurry, a catholyte and a lead, wherein the diaphragm 2 divides the reaction tank 1 into an anode reaction tank 3 and a cathode reaction tank 4; one end of the cathode 6 is arranged in the cathode reaction tank 4, one end of the anode 5 is arranged in the anode reaction tank 3, and the other end of the cathode 6 is connected with the other end of the anode 5 through a lead to form a closed loop; the diaphragm 2 is a 2, 6-dimethyl-1, 4-phenylene ether film with a thickness of 50 μm; the catholyte is placed in the cathode reaction tank 4, and is a mixture of zinc sulfate solution, sulfuric acid solution and cetrimide, wherein the concentration of zinc sulfate is 100g/L, and the concentration of cetrimide is 200 ppm; the anode slurry is placed in an anode reaction tank 3, the anode slurry is composed of 56wt% of bornite 17, 14wt% of acetylene black 18 and 30wt% of sulfuric acid solution, and the pH value of the anode slurry is 2.
Specifically, the anode 5 is a graphite plate with a thickness of 5mm, and the cathode 6 is a pure zinc plate with a thickness of 5 mm.
The temperature of the materials in the anode reaction tank 3 and the cathode reaction tank 4 is increased during the reaction, so the reaction tank 1 is preferably made of stainless steel, the side and the bottom of the reaction tank 1 are hollow and communicated, a water inlet 13 is arranged at the lower part of one side of the reaction tank, and a water outlet 14 is arranged at the upper part of the other side of the reaction tank opposite to the side provided with the water inlet 13. When the reactor is used, cooling water is introduced into the bottom and the side part of the reaction tank 1 from the water inlet 13 and then flows out from the water outlet 14, and is introduced into the bottom and the side part of the reaction tank 1 from the water inlet 13 after being cooled to form circulation so as to keep the temperature in the reaction tank 1 constant and ensure that the reaction in the anode reaction tank and the reaction in the cathode reaction tank are normally carried out.
Further, a second discharge port 15 and a third discharge port 16 are respectively provided at the bottom of the anode reaction tank 3 and the bottom of the cathode reaction tank 4, so as to facilitate discharging the slurry and the electrolyte.
When the ore pulp battery of the embodiment operates, in the charging process, electrons move from an anode to a cathode through a lead, anions move from a cathode reaction tank to an anode reaction tank through a diaphragm, and the anode reacts as follows:
CuFeS2→Cu1-xFe1-yS2-z+xCu2++yFe2++zS+2(x+y)e- (1)
CuFeS2→Cu2++Fe3++2S+5e- (2)
Cu2S→Cu2-xS+Cu2++2xe- (3)
the cathode reacts as follows:
Zn2++2e-→Zn （4）
during discharge, the anode reacts as follows:
2CuFeS2+6H++2e-→Cu2S+3H2S+2Fe2+ (5)
the cathode reacts as follows:
Zn→Zn2++2e- (6)
example 2
The difference between the present embodiment and embodiment 1 is that the present embodiment further includes an anode material tank 7 and a cathode material tank 8, specifically, as shown in fig. 3 and 4, the anode material tank 7 is communicated with the anode reaction tank 3 through two conduits 12 to form an anode slurry circulation loop, and the top and the bottom of the anode material tank 7 are further provided with a first feed port 9 and a first discharge port 10 respectively; the cathode material tank 8 is communicated with the cathode reaction tank 4 through two guide pipes 12 to form a cathode electrolyte circulation loop, and the top of the cathode material tank 7 is also provided with a second feeding hole 11. When the battery is used, the first discharge hole 10 is closed, anode slurry is filled into the anode material tank from the first feed hole 9, catholyte is filled into the cathode material tank 8 from the second feed hole 11, the anode slurry enters the anode reaction tank 3 from the guide pipe 12, the catholyte enters the cathode reaction tank 4 from the guide pipe 12, and then the first feed hole 9 and the second feed hole 11 are respectively closed. When charging, the power is switched on, and the anode reaction tank reacts:
CuFeS2→Cu1-xFe1-yS2-z+xCu2++yFe2++zS+2(x+y)e-
CuFeS2→Cu2++Fe3++2S+5e-
Cu2S→Cu2-xS+Cu2++2xe-
and (3) carrying out reaction in a cathode reaction tank:
Zn2++2e-→Zn
along with the continuous progress of the reaction, the minerals in the anode reaction tank 3 are continuously consumed, the slurry continuously enters the anode reaction tank 3 from the anode material tank 7 for continuous reaction, and the material generated in the anode reaction tank 3 enters the anode material tank 7 through the guide pipe 12. Similarly, along with the deposition of zinc in the cathode reaction tank 4, the catholyte in the cathode material tank 8 enters the cathode reaction tank from the conduit 12, and the solution obtained by the reaction enters the cathode material pipe 8 through the conduit 12.
During discharging, the anode reaction tank reacts:
2CuFeS2+6H++2e-→Cu2S+3H2S+2Fe2+
and (3) carrying out reaction in a cathode reaction tank:
Zn→Zn2++2e-
the charging and discharging process realizes metal extraction and energy storage/conversion.
After the charging and discharging are completed, the first discharge hole 10 and the third discharge hole 16 are opened, the materials are discharged, and the discharged materials are further processed, so that the metal ions can be further extracted and smelted.
The technical features of the embodiments described above may be arbitrarily combined, and for the sake of brevity, all possible combinations of the technical features in the embodiments described above are not described, but should be considered as being within the scope of the present specification as long as there is no contradiction between the combinations of the technical features.
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 invention. It should be noted that, for a person skilled in the art, several variations and modifications can be made without departing from the inventive concept, which falls within the scope of the present invention. Therefore, the protection scope of the present patent shall be subject to the appended claims.

Claims (10)

1. The ore pulp battery is characterized by comprising a reaction tank, a diaphragm, an anode, a cathode, anode slurry, catholyte and a lead, wherein the diaphragm divides the reaction tank into a cathode reaction tank and an anode reaction tank; one end of the cathode is arranged in the cathode reaction tank, one end of the anode is arranged in the anode reaction tank, and the other end of the cathode is connected with the other end of the anode through the lead to form a closed loop; the diaphragm is an anion exchange membrane; the catholyte is placed in the cathode reaction tank and comprises an acidic metal salt solution, and the metal is at least one of manganese, zinc, iron, cobalt and nickel; the anode slurry is placed in the anode reaction tank, the anode slurry comprises minerals, conductive carbon and an acid solution, and the pH value is 0-7; the minerals include copper and/or iron minerals.
2. The pulp battery as recited in claim 1, wherein the anode slurry includes 16-56wt% minerals, 4-14wt% conductive carbon, and 30-80wt% acid solution.
3. The pulp battery of claim 1, wherein the copper ore is at least one of chalcopyrite, bornite, chalcocite, covellite, enargite, chalcanthite, bismuthatite, tetrahedrite, chalcocite, and selenotherrite; the iron ore is at least one of pyrite, marcasite, pyrrhotite, maryolite and low-silver pyrite.
4. The pulp battery according to claim 1, wherein the catholyte further comprises a corrosion inhibitor, the corrosion inhibitor concentration being 1-1000 ppm.
5. The ore pulp battery as recited in claim 1, wherein the diaphragm is at least one of 2, 6-dimethyl-1, 4-phenylene ether, polysulfones, polyvinyl alcohol polymers.
6. The pulp battery according to claim 1, wherein the conductive carbon is at least one of activated carbon, carbon black, acetylene black, carbon nanotubes, ketjen black, and graphene.
7. The pulp battery as recited in claim 1, wherein the cathode and the anode are each selected from the group consisting of aluminum, lead, zinc, and graphite.
8. The pulp battery according to claim 1, wherein the reaction tank has a hollow structure with a side portion and a bottom portion communicated with each other, the reaction tank includes a water inlet and a water outlet, the water inlet is disposed at a lower portion of one side of the reaction tank, and the water outlet is disposed at an upper portion of the other side of the reaction tank opposite to the side of the reaction tank, and is used for reducing reaction temperatures in the cathode reaction tank and the anode reaction tank.
9. The pulp battery according to any of claims 1-8, further comprising an anode material storage device, a cathode material storage device and a plurality of conduits; the anode material storage device is communicated with the anode reaction tank through the two guide pipes to form an anode slurry circulation loop, and the top and the bottom of the anode material storage device are respectively provided with a first feeding hole and a first discharging hole; the cathode material storage device is communicated with the cathode reaction tank through two guide pipes to form a cathode electrolyte circulation loop, and the cathode material storage device is also provided with a second feeding hole.
10. The pulp battery according to claim 9, characterized in that the bottom of the anode reaction tank and the bottom of the cathode reaction tank are respectively provided with a second discharge hole and a third discharge hole.
CN202110666852.4A 2021-06-16 2021-06-16 Ore pulp battery Active CN113122882B (en)

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CN106400049A (en) * 2016-12-06 2017-02-15 江南大学 Sulfide ore tailing recycling method
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CN111416129A (en) * 2019-01-04 2020-07-14 中国科学院福建物质结构研究所 Acid-base asymmetric electrolyte zinc-quinone battery

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