CN117393823B - Biological coupling battery and preparation method and application thereof - Google Patents
Biological coupling battery and preparation method and application thereof Download PDFInfo
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Abstract
The invention relates to a biological coupling battery and a preparation method and application thereof. The bio-coupling battery comprises an electrochemical carbon dioxide reduction module and a microbial electrochemical module, wherein the electrochemical carbon dioxide reduction module is used for quick charge, the microbial electrochemical module is used for durable discharge, so that the battery has the characteristics of quick charge and durable discharge, an extracting agent is used in an extracting chamber of the electrochemical carbon dioxide reduction module to extract a carbon dioxide reduction product, the carbon dioxide reduction product can be metabolized by a bioanode in the microbial electrochemical module to generate bioelectric current, and the bioelectric current can be used as an energy recovery mode or further used as an electric signal for water quality early warning. Based on the invention, a novel multifunctional electrochemical microorganism coupling technology platform can be developed.
Description
Technical Field
The invention relates to the field of energy storage and water environment protection, in particular to a biological coupling battery and a preparation method and application thereof.
Background
Sustainability of economic and social development is one of the currently important issues. To address global warming issues, renewable energy sources that replace fossil fuels are being sought. In this respect, energy storage technologies and devices play a vital role in order to solve the problem of non-uniform production and consumption of renewable energy sources in terms of time and space. Among the various energy storage media, small organic acids (e.g., formic acid) have attracted attention. It is not only safer than hydrogen (H 2), but also has a unique ability to capture and store carbon dioxide (CO 2).
To achieve energy storage, a variety of techniques can be used to produce small molecule organic acids. However, it is known that chemical catalysts have limitations in their manufacture and use, such as severe reliance on precious metals, and the need for extreme reaction conditions. Accordingly, researchers have begun to search for microbial catalysts in order to reduce costs and increase selectivity. However, the current microbial catalytic processes still face challenges such as low conversion rates and poor stability. Therefore, one of the recent focuses is the electrochemical carbon dioxide reduction (CO 2 RR) technology performed at normal temperature and pressure. CO 2 RR can convert CO 2 to small molecule organic acids under mild conditions using electrochemical catalysts. The use of Gas Diffusion Electrodes (GDEs) to overcome the gas-liquid mass transfer limitations is a key technology for CO 2 RR to achieve high rate reduction of CO 2 to produce small molecule organic acids. This means that when we apply CO 2 RR cells containing GDE to energy storage, ultra-fast charging (conversion of electrical energy to chemical energy) is expected. Typically, small molecule organic acids produced by CO 2 RR will dissolve in high concentration salt solutions (e.g., 1M KOH or KHCO 3). Small molecule organic acids dissolved in high concentration salt solutions are not available to conventional microorganisms, greatly limiting the development of CO 2 RR-based electrochemical microbial coupling technologies.
In order to realize energy recovery, the small molecular organic acid obtained by CO 2 RR can be used as an energy carrier and directly used for generating electric energy by a fuel cell. More interestingly, many microorganisms can utilize these small molecule organic acids as a carbon and energy source. Indeed, in microbial electrochemical reactors, small molecule organic acids are often used as substrates for electrochemically active microorganisms (EAB). The power and current density of the microbial electrochemical reactor discharge process is 1 to 2 orders of magnitude lower than the power process of the CO 2 RR cell. That is, bioelectric current is generated using a microbial electrochemical reactor using a small molecule organic acid as a substrate, and a permanent discharge (conversion of chemical energy into electric energy) is possible. In fact, bioelectric currents produced by microbial electrochemical reactors can find practical application in certain contexts where chemical fuel cells are impractical. For example, the microbial electrochemical sensor can track the electron transfer process between the EAB and the electrode under the stress of toxic substances, and the bio-available concentration and the biological reaction of the toxic substances in the water body are characterized by analyzing the electric signals, so that the water quality early warning is realized.
Disclosure of Invention
The invention aims at overcoming the defects of the prior art and provides a biological coupling battery and a preparation method and application thereof, and particularly the biological coupling battery comprises an electrochemical carbon dioxide reduction module and a microbial electrochemical module; the method comprises the steps of carrying out quick charge by using an electrochemical carbon dioxide reduction module and persistent discharge by using a microbial electrochemical module, so that the method has the characteristics of quick charge and persistent discharge, extracting agents are used in an extracting chamber of the electrochemical carbon dioxide reduction module to extract micromolecular organic acid products reduced by carbon dioxide, extracting agents carrying the micromolecular organic acid are directly introduced into the microbial electrochemical module, the products reduced by the carbon dioxide can be metabolized by bioanode in the microbial electrochemical module to generate bioelectric current, the bioelectric current can be used as an energy recovery mode and can also be further used as an electric signal for water quality early warning, and when a monitored water sample is added into a microbial electrochemical reaction solution of the microbial electrochemical module, the electric signal can be used for water quality early warning. The invention provides a quick-charge and durable-discharge biological coupling battery and application thereof in energy storage and water quality early warning. Based on the invention, a novel multifunctional electrochemical microorganism coupling technology platform can be developed.
In order to achieve the above object, the technical scheme of the invention is that the biological coupling battery comprises:
An electrochemical carbon dioxide reduction module;
The preparation method of the gas diffusion electrode comprises the step of coating a catalyst with the function of reducing CO 2 to produce small molecular organic acid on hydrophobic carbon paper or Polytetrafluoroethylene (PTFE) materials. In the invention, a method of coating commercial nano bismuth on commercial hydrophobic carbon paper is adopted to prepare a gas diffusion electrode, and the target small molecular organic acid is formic acid. The anode may catalyze an oxygen evolution reaction under acidic conditions. In the invention, the anode adopts platinized titanium felt.
The extraction chamber is formed by a pair of cation exchange membranes and a cathode exchange membrane, the extraction chamber is filled with ion exchange resin, an extracting agent is used in the extraction chamber to extract a product reduced by carbon dioxide, and the ion exchange resin can be strong acid cation exchange resin, strong alkaline anion exchange resin or a mixed filling of the strong acid cation exchange resin and the strong alkaline anion exchange resin. In the invention, a strong acid cation exchange resin is adopted in the extraction chamber. The extractant may be an inert gas (such as nitrogen, argon, etc.) or a low salinity solution. In the present invention, pure water is used as an extractant.
The cathode chamber is arranged between the cathode and the extracting chamber, catholyte is communicated in the cathode chamber, an anode chamber is also arranged between the anode and the extracting chamber, anolyte is communicated in the anode chamber, and the catholyte is a large amount of anions which can only introduce OH -,CO3 2-, HCO3 -. In the present invention, the catholyte is a KOH solution of 0.5M, 1M and 3M, preferably a KOH solution of 1M. The anolyte can only introduce a large amount of cations, H +. In the invention, 0.5M H 2SO4 solution is adopted as the anolyte.
A microbial electrochemical module;
The microbial electrochemical module is internally provided with a microbial electrochemical reaction solution, the biological anode can metabolize products of carbon dioxide reduction and generate bioelectric current, and the chemical cathode has the function of catalyzing oxygen reduction reaction. In the present invention, a platinum/carbon electrode is used as the chemical cathode.
In one embodiment of the present invention, the product of the reduction of carbon dioxide is a small molecule organic acid.
In one embodiment of the invention, the bio-coupled battery uses the electrochemical carbon dioxide reduction module for rapid charging and uses the microbial electrochemical module for permanent discharging, thus having the characteristics of rapid charging and permanent discharging
In one embodiment of the invention, the charging and discharging processes are as follows, voltage is applied to the electrochemical carbon dioxide reduction module through a direct current power supply, a carbon dioxide reduction product is migrated into an extraction chamber, an extracting agent is used for extracting the carbon dioxide reduction product, the extracting agent carrying the carbon dioxide reduction product is directly introduced into the microbial electrochemical module, the carbon dioxide reduction product can be metabolized by a bioanode in the microbial electrochemical module to generate bioelectric current, the bioelectric current can be used as an energy recovery mode or as an electric signal for water quality early warning, and the bioelectric current generated when a monitored water sample is added into a microbial electrochemical reaction solution of the microbial electrochemical module can be used as an electric signal for water quality early warning.
The invention also provides a preparation method of the biological coupling battery,
The bio-coupled cell includes an electrochemical carbon dioxide reduction module and a microbial electrochemical module.
Providing an electrochemical carbon dioxide reduction module prefabricated body, wherein the electrochemical carbon dioxide reduction module prefabricated body comprises an anode and a cathode, the cathode is a gas diffusion electrode, an extraction chamber arranged between the anode and the cathode, the extraction chamber is formed by a pair of cation exchange membranes and cathode exchange membranes, ion exchange resins are filled in the extraction chamber, an extracting agent is used in the extraction chamber to extract a carbon dioxide reduction product, a cathode chamber arranged between the cathode and the extraction chamber is filled with catholyte, an anode chamber arranged between the anode and the extraction chamber is also arranged, anolyte is communicated in the anode chamber, and anolyte, catholyte and extracting agent are provided;
Providing a microbial electrochemical module preform, and providing a microbial electrochemical reaction solution, wherein the microbial electrochemical reaction solution comprises a bioelectrode liquid and an inoculant.
The method comprises the steps of providing a bioelectrode chamber solution, wherein the bioelectrode chamber solution comprises bioelectrode liquid and an inoculum, the bioelectrode liquid provides necessary nutrient components for the growth of microorganisms, such as artificial configuration solution containing N, P, K, trace elements, vitamins and the like, and the inoculum can be activated sludge from a sewage treatment plant or effluent of a microbial fuel cell for long-term metabolism of small-molecule organic acid to generate electricity. In the invention, the biological anode is prepared by taking the effluent of a microbial fuel cell for generating electricity by long-term metabolism of small molecular organic acid as an inoculum, the inoculum size is 10%, a biological medium containing 50M formate is added for 48 days, the anode biological film is gradually matured, and the judgment basis is that the output current is gradually stable.
The invention further provides an application of the biological coupling battery, the biological coupling battery is applied to energy storage and water quality early warning, voltage is applied to an electrochemical carbon dioxide reduction module through a direct current power supply, electric energy is stored in a mode of reducing carbon dioxide to produce small molecular organic acid, the small molecular organic acid is moved to an extraction chamber under the action of an electric field and is brought out of the electrochemical carbon dioxide reduction module by an extracting agent, the extracting agent carrying the small molecular organic acid is directly connected to the microbial electrochemical module, a biological anode and a chemical cathode of a prefabricated body of the microbial electrochemical module are electrically connected, the biological anode metabolizes the small molecular organic acid in the biological anode to generate biological current, the biological current can be used as an energy recovery mode and can also be further used as an electric signal of the water quality early warning, when a monitored water sample is added into a microbial electrochemical reaction solution of the microbial electrochemical module, the electric signal change of the microbial electrochemical module is analyzed through an electric signal recording device to perform the water quality early warning, if the monitored water sample is free of toxicity, rapid change of the electric signal is caused if the monitored water sample has toxicity, and the early warning signal is triggered. The time of the extractant entering the microbial electrochemical module is controlled, so that the initial concentration of the micromolecular organic acid in the microbial electrochemical module can be controlled, and the discharge time of the microbial electrochemical module is further controlled. In the present invention, the time for the extractant to pass into the microbial electrochemical module described above is set to 1min, 2 min and 3 min, preferably 3 min.
The biological anode and the chemical cathode are electrically connected in series by a small-sized electric appliance such as a fixed-value resistor, a bulb and the like. In the invention, a fixed resistor (1000 ohm) is adopted in an electric connection mode.
The direct current power supply comprises a dry battery, a battery test system, an electrochemical workstation and other power supplies which directly output direct current. The power mode may use a constant voltage or constant current mode. In the present invention, a battery test system is used to apply a voltage of 3.5V, 4V, or 4.5V, preferably 4V, to the electrochemical carbon dioxide reduction module in a constant voltage manner.
The electrical signal recording device comprises a manual electrical signal recording device, such as an ohmmeter, and also comprises an automatic electrical signal recording device, such as a data acquisition system, a battery testing system, an electrochemical workstation and the like. In the invention, a battery test system is adopted for automatic recording.
Compared with the prior art, the biological coupling battery and the preparation method and application thereof have the advantages that the biological coupling battery comprises an electrochemical carbon dioxide reduction module and a microbial electrochemical module, the electrochemical carbon dioxide reduction module is used for quick charge, the microbial electrochemical module is used for durable discharge, therefore, the biological coupling battery has the characteristics of quick charge and durable discharge, an extracting agent is used in an extracting chamber of the electrochemical carbon dioxide reduction module for extracting a small molecular organic acid product reduced by carbon dioxide, the extracting agent carrying the small molecular organic acid is directly introduced into the microbial electrochemical module, the product reduced by carbon dioxide can be metabolized by a biological anode in the microbial electrochemical module to generate bioelectric current, the bioelectric current can be used as an energy recovery mode and can also be further used as an electric signal for water quality early warning, and when a monitored water sample is added into a microbial electrochemical reaction solution of the microbial electrochemical module, the electric signal can be used for water quality early warning. The invention provides a quick-charge and durable-discharge biological coupling battery and application thereof in energy storage and water quality early warning. Based on the invention, a novel multifunctional electrochemical microorganism coupling technology platform can be developed.
Drawings
FIG. 1 is a schematic diagram of a bio-coupled cell based on electrochemical carbon dioxide reduction and microbial electrochemical principles in accordance with one embodiment of the present invention;
FIG. 2 is a schematic diagram of the current variation when a voltage is applied to an electrochemical carbon dioxide reduction module by a DC power source according to an embodiment of the present invention;
FIG. 3 is a schematic diagram showing the voltage change of the microbial electrochemical module when the time for the extractant carrying small molecule organic acid to directly pass through the microbial electrochemical module is set to 1 min, 2 min and 3 min, respectively, according to one embodiment of the present invention;
FIG. 4 is a schematic diagram showing the change of current signals of water quality early warning by using a microbial electrochemical module according to an embodiment of the present invention;
The reference numerals illustrate 1-gas diffusion electrode, 2-catholyte, 3-anion exchange membrane, 4-ion exchange resin, 5-cation exchange membrane, 6-anode, 7-bioanode, 8-chemical cathode, 9-electrical signal, 10-battery test system, 11-extractant.
Detailed Description
The technical scheme of the invention is specifically described below with reference to the accompanying drawings.
Example 1
In this example, a structure of a bio-coupled battery based on electrochemical carbon dioxide reduction and microbial electrochemical principles according to an embodiment of the present invention will be described with reference to fig. 1, which includes:
An electrochemical carbon dioxide reduction module;
an anode 6 and a cathode (gas diffusion electrode) 1 which are arranged on the electrochemical carbon dioxide reduction module, wherein the cathode (gas diffusion electrode) 1 is prepared by a method of coating commercial nano bismuth on commercial hydrophobic carbon paper. In the present invention, the anode 6 is made of platinized titanium felt.
An extraction chamber arranged between the anode and the cathode, wherein the extraction chamber is composed of a pair of cation exchange membranes 5 and a cathode exchange membrane 3, the extraction chamber is filled with ion exchange resin 4, and an extraction agent 11 is used for extracting a product reduced by carbon dioxide, wherein in the invention, a strong acid cation exchange resin is used. In the present invention, pure water is used as an extractant.
The cathode chamber is arranged between the cathode and the extracting chamber, the cathode chamber is communicated with catholyte 2, and the anode chamber is communicated with anolyte. In the present invention, the catholyte is a KOH solution of 0.5M, 1M and 3M, preferably a KOH solution of 1M. In the invention, 0.5M H 2SO4 solution is adopted as the anolyte. The distribution of the small molecular organic acid in the solution can be regulated by regulating the volume of the catholyte. The volume of the anolyte may affect the operational stability. Preferred anolyte (100 mL 0.5M H 2SO4), catholyte (10 mL 1M KOH).
A microbial electrochemical module;
a bioanode 7 and a chemical cathode 8 disposed within the microbial electrochemical module, wherein in the present invention, a platinum/carbon electrode is used as the chemical cathode.
In the invention, the direct current power supply is a battery test system 10, and the change of the electric signal 9 of the microbial electrochemical module is analyzed by an electric signal recording device to perform water quality early warning.
Example 2
In this example, a description will be given of a current change when a voltage is applied to the electrochemical carbon dioxide reduction module by a dc power source in one embodiment of the present invention with reference to fig. 2. The electrochemical carbon dioxide reduction module is firstly applied with voltage 4V through a direct current power supply (a battery test system), electric energy is stored in a mode of reducing carbon dioxide to produce small molecular organic acid, and electrons are required to be consumed for reducing the carbon dioxide to produce the small molecular organic acid, so that current change on an external circuit can be observed. In each period, in the process of applying the voltage of 4V, the small molecular organic acid is migrated to the extraction chamber under the action of an electric field and is carried out of the electrochemical carbon dioxide reduction module by the extracting agent, the extracting agent carrying the small molecular organic acid is directly connected to the microbial electrochemical modules, the number of the microbial electrochemical modules and the time (1 min, 2 min or 3 min) for connecting the microbial electrochemical modules with the extracting agent are needed, and the time for applying the voltage of 4V by the electrochemical carbon dioxide reduction modules in each period exceeds 1 hour in consideration of the switching of operation steps. The time for the microbial electrochemical module to connect with the electrochemical carbon dioxide reduction module via the extractant is defined as the charging time, which is 1 to 3 min. Then, the applied voltage of the electrochemical carbon dioxide reduction module was turned off, and the current was 0 mA. In this embodiment, the number of cycles is 9. The current drops from more than 250 mA for cycle 1 to 156 mA for cycle 5 and further drops to 91 mA for cycle 9. The run time of the electrochemical carbon dioxide reduction module was 164 h, with a run time (total time of 4V voltage applied in 9 cycles) of 12.6 h. Correspondingly, the extract water formate concentration was reduced from 202 mM for cycle 1 to 65 mM for cycle 9.
Example 3
In this example, referring to fig. 3, the voltage change of the microbial electrochemical module is described when the time for directly introducing the extractant carrying the small molecular organic acid into the microbial electrochemical module is set to 1 min, 2 min, and 3 min, respectively, in a specific embodiment of the present invention.
And a 1000 ohm resistor is connected between the chemical cathode and the biological anode of the microbial electrochemical module. The bioelectrode liquid contains ：K2HPO4, 2.6 g L-1; KH2PO4, 4.4 g L-1; NH4Cl, 0.31 g L-1; MgCl2•6H2O, 0.2 g L-1; Na2SO4, 0.05 g L-1; trace elements, 12.5 mL, and vitamin solution, 5 mL. And acquiring the voltage at two ends of the 1000 omega resistor by using a battery test system until the voltage is stable and repeatable, namely the preparation of the biological anode is finished.
The chemical cathode is prepared by coating platinum/carbon on a commercial waterproof breathable film.
And transferring the prepared biological anode and chemical cathode to a microbial electrochemical module. When the voltage of the microbial electrochemical module is reduced to about 0 mV, the extractant containing small molecular organic acid is directly introduced into the microbial electrochemical module at a fixed flow rate. The time for controlling the connection of the microbial electrochemical module and the electrochemical carbon dioxide reduction module through the extractant is respectively 1 min, 2 min and 3 min. Therefore, the initial concentration of the small molecular organic acid in the microbial electrochemical module is different, and the current signal output condition of the microbial electrochemical module is recorded. It can be found that the bio-coupled battery based on electrochemical carbon dioxide reduction and microbial electrochemical principles in the present invention exhibits the characteristics of rapid charge and long-lasting discharge, for example, the electrochemical carbon dioxide reduction module is used to charge the microbial electrochemical module only by 3 min (i.e., the time for controlling the connection of the microbial electrochemical module and the electrochemical carbon dioxide reduction module through the extractant is 3 min), and the discharge process is as long as 25 hours.
Example 4
In this embodiment, referring to fig. 4, a description will be given of a change in a current signal of water quality early warning using a microbial electrochemical module in a specific embodiment of the present invention. When the output voltage of the microbial electrochemical module reaches a stable state, adding formaldehyde solution into the microbial electrochemical module according to a certain volume ratio. When toxic substances are injected, the unitized current signal is found to decrease, i.e., the most readable electrical signal change is produced. For example, after exposure to 0.1% formaldehyde 30 min, the inhibition reached 9.3%.
While the invention has been described in detail, it will be apparent to those skilled in the art that the foregoing description is by way of example only and is not intended to limit the invention.
The above is a preferred embodiment of the present invention, and all changes made according to the technical solution of the present invention belong to the protection scope of the present invention when the generated functional effects do not exceed the scope of the technical solution of the present invention.
Claims (4)
1. A bio-coupled battery, comprising:
An electrochemical carbon dioxide reduction module;
the anode and the cathode are arranged on the electrochemical carbon dioxide reduction module, and the cathode is a gas diffusion electrode;
the extraction chamber consists of a pair of cation exchange membranes and a cathode exchange membrane, and the extraction chamber is filled with ion exchange resin;
A cathode chamber arranged between the cathode and the extracting chamber, wherein a catholyte is communicated in the cathode chamber;
a microbial electrochemical module;
the microbial electrochemical module comprises a microbial electrochemical module, a biological anode and a chemical cathode, wherein the microbial electrochemical module is internally provided with a microbial electrochemical reaction solution;
the bio-coupling battery uses an electrochemical carbon dioxide reduction module to carry out quick charge and uses a microbial electrochemical module to carry out durable discharge, so that the bio-coupling battery has the characteristics of quick charge and durable discharge;
the product of the carbon dioxide reduction is a small molecular organic acid.
2. The bio-coupling battery according to claim 1, wherein the charging and discharging process is as follows, voltage is applied to the electrochemical carbon dioxide reduction module through a direct current power supply, the carbon dioxide reduced product migrates into an extraction chamber, an extracting agent is used for extracting the carbon dioxide reduced product, the extracting agent carrying the carbon dioxide reduced product is directly introduced into the microbial electrochemical module, the carbon dioxide reduced product can be metabolized by a bioanode in the microbial electrochemical module to generate bioelectric current, the bioelectric current can be used as an energy recovery mode, or as an electrical signal of water quality early warning, and the bioelectric current generated when a monitored water sample is added into a microbial electrochemical reaction solution of the microbial electrochemical module can be used for water quality early warning as an electrical signal of water quality early warning.
3. A method for producing a bio-coupled cell according to any one of claim 1 to 2, wherein,
Providing an electrochemical carbon dioxide reduction module prefabricated body, wherein the electrochemical carbon dioxide reduction module prefabricated body comprises an anode and a cathode, the cathode is a gas diffusion electrode, an extraction chamber arranged between the anode and the cathode, the extraction chamber is formed by a pair of cation exchange membranes and cathode exchange membranes, ion exchange resins are filled in the extraction chamber, an extracting agent is used in the extraction chamber to extract a carbon dioxide reduction product, a cathode chamber is arranged between the cathode and the extraction chamber, and a catholyte is filled in the cathode chamber;
Providing a microbial electrochemical module preform, and providing a microbial electrochemical reaction solution, wherein the microbial electrochemical reaction solution comprises a bioelectrode liquid and an inoculant.
4. An application of the biological coupling battery as claimed in any one of claims 1-2 in energy storage and water quality early warning is characterized in that voltage is applied to an electrochemical carbon dioxide reduction module through a direct current power supply to reduce carbon dioxide and generate small molecular organic acid, namely electric energy is stored in a chemical energy form, the small molecular organic acid migrates to an extraction chamber across an anion exchange membrane under the action of an electric field and is carried out of the electrochemical carbon dioxide reduction module by an extracting agent, the extracting agent carrying the small molecular organic acid is directly introduced into a microbial electrochemical module, a biological anode and a chemical cathode of a prefabricated body of the microbial electrochemical module are electrically connected, the small molecular organic acid in the biological anode is metabolized and biological current is generated, the biological current can be used as an energy recovery mode or an electric signal of the water quality early warning, the electric signal of the water quality early warning is recorded through the electric signal, if the monitored water sample is free of toxicity, the electric signal is smooth, the electric signal is changed rapidly, and the water quality early warning signal is triggered if the monitored is toxic.
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| CN113960135A (en) * | 2021-11-09 | 2022-01-21 | 福建农林大学 | A rechargeable microbial electrochemical sensor and its preparation and application in water quality early warning |
| CN116121789A (en) * | 2023-04-17 | 2023-05-16 | 北京林业大学 | A device and method for microbial electrochemical reduction of carbon dioxide to produce acetate and simultaneous in-situ recovery |
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