CN115072838A - Novel method for generating electricity by treating landfill leachate mixed shale gas flowback wastewater through single-chamber microbial fuel cell - Google Patents
Novel method for generating electricity by treating landfill leachate mixed shale gas flowback wastewater through single-chamber microbial fuel cell Download PDFInfo
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Abstract
A new method for treating old landfill leachate mixed shale gas flowback wastewater by using a single-chamber microbial fuel cell belongs to the technical field of organic wastewater treatment. The invention firstly constructs a single-chamber Microbial Fuel Cell (MFC), prepares different materials as an anode catalyst, utilizes anaerobic activated sludge obtained by culturing aerobic activated sludge of a sewage treatment plant as an anode solution, adds nutrient solution and stabilizes for a plurality of weeks, then replaces an anode chamber anaerobic sludge matrix with mixed wastewater of aged landfill leachate and shale gas flowback wastewater, operates the MFC at room temperature and constant pressure, can remove organic pollutants and ammonia nitrogen in the mixed wastewater, and can recover electric energy. The method has the advantages of simple equipment, convenient operation, energy conservation and no secondary pollution. The catalyst at the anode is H-Co 3 O 4 Under the condition of/Y, the maximum power density of the MFC system reaches 1179mW/m 2 The maximum output voltage is 448mV, the COD removal rate can reach 27.05 percent, and the ammonia nitrogen removal rate can reach 47.88 percent.
Description
Technical Field
The invention relates to a novel method for treating aged landfill leachate mixed shale gas flowback wastewater to generate electricity by using a single-chamber microbial fuel cell, belonging to the technical field of organic wastewater treatment.
Background
With the rapid development of society and the over-development and utilization of resources, the environmental safety problem is particularly prominent in China and even worldwide, and the wastewater treatment becomes the key part of the current environmental safety problem. Old landfill leachate caused by landfill treatment generally pollutes soil, underground water, surface drinking water sources and the surrounding environment; during the hydraulic fracturing exploitation process of shale gas, a large amount of shale gas flowback wastewater is generated, and the shale gas flowback wastewater has the characteristics of high salt content, complex components, environmental toxicity and the like. Old landfill leachate and shale gas flowback wastewater are both organic wastewater which is complex in components and difficult to treat, and the search for more efficiently treating the two types of wastewater and realizing resource utilization becomes an important issue of environmental safety. The existing treatment methods for landfill leachate comprise anaerobic biochemical treatment, membrane treatment, chemical oxidation and the like; the main methods for treating the shale gas flowback wastewater comprise natural evaporation, filtration, ozone oxidation and the like. For example, in the "scientific and technical information" removing refractory substances in old landfill leachate by using the coagulation-precipitation method at the 15 th year 2010 "(comparison document 1), the pollution removal effect of the coagulation-precipitation method on the old landfill leachate is studied, and the results show that the pollution removal effect of the polyaluminium chloride (PAC) on the old landfill leachate is the best, but the removal effect of the coagulation-precipitation method on the pollutants in the old landfill leachate is generally limited, and the following problems exist: (1) the process flow is more complex; (2) the treatment cost is relatively high; (3) the resource utilization rate is not high.
The development trend of treating refractory high-concentration organic wastewater gradually takes biotechnology as the mainstream, wherein, the microbial fuel cell can convert the chemical energy of organic matters into electric energy through a microbial catalytic reaction, and can generate electric energy while degrading the organic matters in the wastewater. Compared with the traditional method, the microbial fuel cell system saves cost, is very environment-friendly and realizes the resource utilization of wastewater. For example, in "Water Research" volume 147 of "organic waste removal of organic and inorganic from a hydro-mechanical free flowing back Water through a multi-batch process of a microbial fuel cell" (reference 2), a microbial fuel cell using sulfur as a circulating medium and NaCl as a catholyte, a multi-batch process of a simulated fracturing flowback fluid is performed, the COD waste liquid value is reduced from 1348 + -112 m/L to 200-300 mg/L, and the power density is 2667 + -529 mW/m 3 . But the method has the following disadvantages: (1) suspended solids in the wastewater need to be pretreated, and the process is complicated; (2) the catholyte has the risk of secondary pollution, and needs to be subjected to desalination treatment after the operation of the battery is finished; (3) compared with actual wastewater, the simulated shale gas flowback wastewater has single component, low organic carbon concentration and low reference value in actual application.
At present, no report related to treatment of old landfill leachate mixed shale gas flowback wastewater by using single-chamber microbial fuel cells exists, and the hydrofluoric acid modified anode catalyst H-Co is prepared by using the single-chamber air cathode microbial fuel cell 3 O 4 And Y, mixed wastewater of aged landfill leachate and shale gas flowback wastewater is used as a treatment object, so that the efficient power generation is realized, a certain pollutant removal effect is achieved, and the application prospect is good.
Disclosure of Invention
The invention aims to provide a novel method for treating old landfill leachate mixed shale gas flowback wastewater by using an MFC (micro-fuel cell) technology, which is low in cost and environment-friendly, so that the wastewater is effectively degraded, and meanwhile, biomass energy in the wastewater can be converted into biological electric energy.
The invention provides a method for treating old landfill leachate mixed shale gas flowback wastewater, which comprises the following steps:
(1) anode catalyst H-Co 3 O 4 Preparation of/Y
Weighing 0.73g of cobalt nitrate hexahydrate, 1.5g of urea and 0.37g of ammonium fluoride, and dissolving in 50mL of distilled water to obtain a solution A; according to Co 3 O 4 Theoretical loading of
Weighing NaY molecular sieve with corresponding mass, adding the NaY molecular sieve into the solution A, magnetically stirring for 2 hours, transferring the NaY molecular sieve into a 100mL reaction kettle, carrying out hydrothermal reaction for 12 hours at 120 ℃, taking out the NaY molecular sieve after the reaction is finished, cooling to room temperature, filtering, carrying out suction filtration and washing on a filter cake with distilled water, drying in a drying oven, grinding, placing the filter cake into a muffle furnace, roasting for 2 hours at 350 ℃, heating at the rate of 5 ℃/min, cooling to room temperature, taking out a sample, grinding againTo obtain Co 3 O 4 /Y；Co 3 O 4 The rest steps are carried out without adding NaY molecular sieve, and Co 3 O 4 Y is prepared consistently; co to be prepared 3 O 4 adding/Y into 10% HF solution, magnetically stirring for 12 hr, centrifuging, washing, drying at 60 deg.C in oven, and grinding to obtain H-Co 3 O 4 /Y。
(2) Construction of single-cell microbial fuel cell
An organic glass is selected to construct a single-chamber Microbial Fuel Cell (MFC) device, the device is designed in a three-section mode as shown in figure 1, and one side of a cathode is designed in a central circular hollow mode, so that the air cathode can be fully contacted with air; the cavity section is in a cylindrical hollow design and is used for containing liquid; the other side is solid, and the inside of the chamber can be observed; the two sections are connected by rubber pads with hollow-out middle parts, so that the sealing and waterproof effects are achieved, the cathode and the anode are connected to an external circuit by adopting 0.5cm titanium wires, the external resistance is 1000 omega, and MFC voltage data are acquired by a parallel data acquisition instrument.
(3) Starting of single-cell microbial fuel cells
Starting the microbial fuel cell by using the cultured anaerobic sludge as a substrate of the anode chamber. The reactor adopts an intermittent operation mode; after three cycles of operation, the output voltage of the MFC can be kept stable for a long time, and the maximum output voltage of each cycle is close, so that the starting of the MFC is finished.
(4) Running microbial fuel cell with aged landfill leachate mixed shale gas flowback wastewater as matrix
Replacing the anode chamber anaerobic sludge matrix with mixed waste liquid of aged landfill leachate and shale gas flowback wastewater, wherein the mixing volume ratio is 2:1, the MFC was run at room temperature and constant pressure and its output voltage was recorded using a data acquisition instrument. Before the operation is started and after the operation is finished, the COD and the ammonia nitrogen concentration of the mixed wastewater are respectively measured.
[ the beneficial effects of the above technical solution of the present invention are as follows ]:
firstly, the method does not need to pretreat the waste water, but directly treats the aged landfill leachate mixed shale gas flowback waste water, and is superior to the comparison document 2; the invention can generate electric energy while removing pollutants in the wastewater, realizes the resource utilization of the wastewater, and is superior to that of the comparison document 1.
Secondly, the comparison document 2 uses simulated shale gas flowback wastewater, so that the practical value is low, and the actual wastewater adopted in the invention has a better application prospect.
Tris, H-Co 3 O 4 the/Y anode catalyst can obviously enhance the electricity generation performance of the single-chamber MFC system and keep a good pollutant removal effect.
Description of the drawings:
FIG. 1 is a schematic diagram of a single-cell microbial fuel cell device, wherein: 1. anode, 2 anode chamber, 3 cathode, 4 wire, 5 resistance box;
FIG. 2 is a plot of single-chamber MFC output voltage versus time for different anode catalysts;
fig. 3 is a plot of the power density of a single-chamber MFC for different anode catalysts.
Detailed Description
The present invention will be further described with reference to the following specific embodiments.
Example 1
A method for generating electricity by treating landfill leachate mixed shale gas flowback wastewater through a single-chamber microbial fuel cell comprises the following specific steps:
(1) anode catalyst H-Co 3 O 4 Preparation of/Y
Weighing 0.73g of cobalt nitrate hexahydrate, 1.5g of urea and 0.37g of ammonium fluoride, and dissolving in 50mL of distilled water to obtain a solution A; according to Co 3 O 4 Weighing a NaY molecular sieve with corresponding mass, adding the NaY molecular sieve into the solution A, magnetically stirring for 2 hours, transferring the NaY molecular sieve into a 100mL reaction kettle, performing hydrothermal reaction for 12 hours at 120 ℃, taking out the NaY molecular sieve after the reaction is finished, cooling to room temperature, filtering, performing suction filtration and washing on a filter cake with distilled water, drying the filter cake in a drying oven, grinding, putting the filter cake into a muffle furnace, roasting for 2 hours at 350 ℃, heating at the rate of 5 ℃/min, cooling to room temperature, taking out a sample, and grinding again to obtain Co 3 O 4 /Y；Co 3 O 4 Is prepared without addition of NaY molecular sieve, the rest steps and Co 3 O 4 Y is prepared consistently; co to be prepared 3 O 4 adding/Y into 10% HF solution, magnetically stirring for 12 hr, centrifuging, washing, drying at 60 deg.C in oven, and grinding to obtain H-Co 3 O 4 /Y。
(2) Electrode pretreatment method
Cutting the carbon cloth, wherein the size of the anode carbon cloth is 1 multiplied by 2cm, and the size of the cathode carbon cloth is 5 multiplied by 5 cm; immersing the cut carbon cloth into absolute ethyl alcohol, ultrasonically cleaning for 15 minutes, then immersing for 30 minutes, and carefully washing with deionized water after immersing; 3) mixing a nitric acid solution with the mass fraction of 10% and a sulfuric acid solution with the mass fraction of 10% according to the volume ratio of 3:1, then immersing carbon cloth in the mixture, ultrasonically cleaning the mixture for 15 minutes, then immersing the mixture for 5 hours, and carefully washing the mixture with deionized water after the immersion is finished; then soaking the carbon cloth in deionized water, ultrasonically cleaning for 15 minutes, then soaking for 30 minutes, and finally carefully cleaning the carbon cloth by using the deionized water; and (3) putting the treated carbon cloth into a 60 ℃ oven for drying, then putting the carbon cloth into a muffle furnace, calcining for 4 hours at 300 ℃, and raising the temperature at the rate of 5 ℃/min.
(3) Fabrication of air cathode
Measuring 1mL of deionized water and 1mL of 60% polytetrafluoroethylene emulsion (PTFE), adding into a 10mL small beaker, then measuring 30mg of carbon black, adding into the small beaker in a small amount for multiple times, and uniformly stirring to obtain a suspension A; slightly brushing the suspension A on a carbon cloth with the thickness of 5 multiplied by 5cm, placing the carbon cloth for air drying for 2 hours, then placing the carbon cloth in a muffle furnace for calcining at 370 ℃ for 25 minutes, after the carbon cloth is cooled, uniformly coating a layer of 60% PTFE on one surface coated with a carbon base layer, air drying until the PTFE becomes white, calcining at 370 ℃ for 12 minutes, after the carbon cloth is cooled, continuously coating a layer of PTFE, calcining, and brushing 4 layers; and (3) transferring 400 mu L of Nafion solution, 200 mu L of isopropanol and 200 mu L of deionized water by using a liquid transfer gun, adding the mixture into a 10mL small beaker, weighing 40mg of 20% platinum-carbon powder, ultrasonically brushing the platinum-carbon powder on the other side of the carbon cloth after 10 minutes, and standing for 24 hours for air drying.
(4) Fabrication of anodes
Weighing 2mg of prepared H-Co 3 O 4 The catalyst/Y is placed in a 10mL small beaker and then a pipette is usedTransferring 200 μ L of anhydrous ethanol, 100 μ L of ethylene glycol and 10 μ L of Nafion solution, adding into a small beaker, placing in an ultrasonic cleaning instrument for ultrasonic treatment for 30min to mix them uniformly, transferring the suspension with a liquid transfer gun, uniformly dripping on a carbon cloth of 1 × 2cm, and drying for later use.
(5) Construction of single-cell microbial fuel cell
The length, width and height of the periphery of the single-chamber MFC are 8.5, 8.5 and 8cm respectively, the cavity is cylindrical with the bottom surface of 4cm in diameter and 4cm in height, and the effective volume is 50 mL; the whole device is made of organic glass, the device is designed in a three-section mode, and one side of the cathode is in a central circular hollow design, so that the air cathode can be fully contacted with air; the cavity section is in a cylindrical hollow design and is used for containing liquid; the other side is solid, and the inside of the chamber can be observed; each section is connected by a rubber pad with a hollow middle part, so that the sealing and waterproof effects are achieved; the top is provided with a small hole for placing a cathode and anode lead, adding liquid and the like; and sequentially placing anode carbon cloth loaded with the prepared catalyst and an air cathode loaded with a platinum carbon catalyst, connecting the cathode and the anode to an external circuit by adopting 0.5cm titanium wires, connecting an external resistor to the external circuit to be 1000 omega, and connecting a data acquisition instrument in parallel to acquire voltage data.
(6) Single cell microbial fuel cell start-up
Mixing a phosphate buffer solution with cultured active anaerobic sludge according to the volume ratio of 1:1 to obtain an anolyte, and adding 1.6g/L of sodium acetate, 0.05g/L of ammonium chloride, 12.5mL/L of trace metal solution and 5mL/L of vitamin solution to maintain the growth of microorganisms in the anolyte, wherein the trace metal solution comprises 6.15g/L of magnesium sulfate, 0.5g/L of manganese sulfate, 1g/L of sodium chloride and 0.1g/L of ferrous sulfate, and the vitamin solution comprises 2mg/L of biological acid, 2mg/L of folic acid, 10mg/L of vitamin B6, 5mg/L of riboflavin and the like; after the chamber is sealed, recording voltage data of the MFC by using a data acquisition instrument; when the voltage data rapidly drop, it indicates that the nutrient substances in the MFC are exhausted, the nutrient substances need to be added again, after a few voltage cycles, if the output voltage can be stabilized for a long time under a higher voltage, and the maximum stable voltage of each cycle is close, it indicates that the MFC is successfully started, and the growth of the biological membrane on the electrode material is mature.
(7) Running microbial fuel cell with aged landfill leachate mixed shale gas flowback wastewater as matrix
Replacing the anode chamber anaerobic sludge matrix with mixed waste liquid of aged landfill leachate and shale gas flowback wastewater, wherein the mixing volume ratio is 2:1, operating the MFC at room temperature and constant pressure, recording the output voltage of the MFC by using a data acquisition instrument, and respectively measuring the COD (chemical oxygen demand) and the ammonia nitrogen concentration of the mixed wastewater before the operation starts and after the operation ends.
Example 2
A method for generating electricity by treating landfill leachate mixed shale gas flowback wastewater through a single-chamber microbial fuel cell comprises the following specific steps:
(1) preparation of anode catalyst
The same procedure as in step (1) of example 1.
(2) Electrode pretreatment
The same procedure as in step (2) of example 1.
(3) Fabrication of cathode
The same procedure as in step (3) of example 1.
(4) Fabrication of anodes
Weighing 2mg of prepared Co 3 O 4 Putting the/Y catalyst into a 10mL small beaker, transferring 200 mu L of absolute ethyl alcohol, 100 mu L of ethylene glycol and 10 mu L of Nafion solution by using a liquid transfer gun, adding the solution into the small beaker, putting the small beaker into an ultrasonic cleaning instrument for ultrasonic treatment for 30min to uniformly mix the solution, transferring the suspension by using the liquid transfer gun, uniformly dripping the suspension on a carbon cloth with the thickness of 1 multiplied by 2cm, and finally drying the suspension for later use.
(5) Construction of single-cell microbial fuel cell
The same procedure as in step (5) of example 1.
(6) Starting of single-cell microbial fuel cells
The same procedure as in step (6) of example 1.
(7) Running microbial fuel cell with aged landfill leachate mixed shale gas flowback wastewater as matrix
The same procedure as in step (7) of example 1.
Example 3
A method for generating electricity by treating landfill leachate mixed shale gas flowback wastewater through a single-chamber microbial fuel cell comprises the following specific steps:
(1) preparation of anode catalyst
The same procedure as in step (1) of example 1.
(2) Electrode pretreatment
Same as step (2) in example 1.
(3) Fabrication of cathode
The same procedure as in step (3) of example 1.
(4) Fabrication of anodes
Weighing 2mg of prepared Co 3 O 4 Putting the catalyst into a 10mL small beaker, then transferring 200 mu L of absolute ethyl alcohol, 100 mu L of ethylene glycol and 10 mu L of Nafion solution by using a liquid transfer gun, adding the solution into the small beaker, putting the small beaker into an ultrasonic cleaning instrument for ultrasonic treatment for 30min to uniformly mix the solution, transferring the suspension by using the liquid transfer gun, uniformly dripping the suspension on a carbon cloth with the thickness of 1 multiplied by 2cm, and finally drying the suspension for later use.
(5) Construction of single-cell microbial fuel cell
The same procedure as in step (5) of example 1.
(6) Starting of single-cell microbial fuel cells
The same procedure as in step (6) of example 1.
(7) Running microbial fuel cell with aged landfill leachate mixed shale gas flowback wastewater as matrix
The same procedure as in step (7) of example 1.
Example 4
A method for generating electricity by treating landfill leachate mixed shale gas flowback wastewater through a single-chamber microbial fuel cell comprises the following specific steps:
(1) preparation of anode catalyst
The same procedure as in step (1) of example 1.
(2) Electrode pretreatment
Same as step (2) in example 1.
(3) Fabrication of the cathode
The same procedure as in step (3) of example 1.
(4) Fabrication of anodes
In this example, the anode was a carbon cloth after pretreatment, and no catalyst was applied by dropping.
(5) Construction of single-cell microbial fuel cell
The same procedure as in step (5) of example 1.
(6) Starting of single-cell microbial fuel cells
Same as in step (6) of example 1.
(7) Running microbial fuel cell with aged landfill leachate mixed shale gas flowback wastewater as matrix
The same procedure as in step (7) of example 1.
Results of the experiment
Example 1 is a suitable method for generating electricity by treating old landfill leachate mixed shale gas flowback wastewater through a single-chamber microbial fuel cell.
The MFC system was started and operated under different anode catalyst conditions with output voltage versus time as shown in FIG. 2, where the anode catalyst was H-Co 3 O 4 Under the condition of/Y, the stable output voltage of the battery is 448mV at most; the maximum power density is 1179mW/m 2 (FIG. 3). Illustrating that the anode catalyst has a large influence on the power generation performance of MFC, H-Co 3 O 4 the/Y anode catalyst can accelerate the transfer rate of anode ions, reduce the ohmic loss of the anode and the activation loss and mass transfer loss, thereby enhancing the electricity generation performance of the microbial fuel cell system.
Tests show that the anode catalyst is blank and Co respectively 3 O 4 、Co 3 O 4 /Y、H-Co 3 O 4 At the time of/Y, the removal rates of COD of the mixed waste liquid in the MFC system are respectively 22.64%, 27.93%, 24.58% and 27.05%; the ammonia nitrogen removal rates were 43.62%, 49.43%, 48.46% and 47.88%, respectively. The constructed single-chamber microbial fuel cell has certain removal effect on pollutants in the aged landfill leachate mixed shale gas flowback wastewater, and the H-Co has certain removal effect 3 O 4 the/Y anode catalyst can greatly improve the electricity generation performance of the MFC.
Claims (2)
1. A method for generating electricity by treating landfill leachate mixed shale gas flowback wastewater through a single-chamber microbial fuel cell is characterized by comprising the following steps of:
(1) anode catalyst H-Co 3 O 4 Preparation of/Y
Weighing 0.73g of cobalt nitrate hexahydrate, 1.5g of urea and 0.37g of ammonium fluoride, and dissolving in 50mL of distilled water to obtain a solution A; according to Co 3 O 4 Weighing a NaY molecular sieve with corresponding mass, adding the NaY molecular sieve into the solution A, magnetically stirring for 2 hours, transferring the solution A into a 100mL reaction kettle, performing hydrothermal reaction for 12 hours at 120 ℃, taking out the solution after the reaction is finished, cooling to room temperature, filtering, performing suction filtration and washing on a filter cake with distilled water, drying the filter cake in a drying oven, grinding the filter cake, placing the filter cake into a muffle furnace, roasting for 2 hours at 350 ℃, heating at the rate of 5 ℃/min, cooling to room temperature, taking out a sample, and grinding again to obtain Co 3 O 4 /Y；Co 3 O 4 The rest steps are carried out without adding NaY molecular sieve, and Co 3 O 4 Y is prepared consistently; co to be prepared 3 O 4 Y is added into 10 percent HF solution, after magnetic stirring for 12 hours, centrifugal washing is carried out, the mixture is moved into a drying oven to be dried and ground at 60 ℃, and then H-Co is prepared 3 O 4 /Y；
(2) Construction and startup of single-cell microbial fuel cell
With H-Co 3 O 4 /Y、Co 3 O 4 /Y、Co 3 O 4 The catalyst is dripped on 1 x 2cm carbon cloth and the carbon cloth is used as an anode, and organic glass is selected to construct a single-chamber microbial fuel cell device, the schematic diagram of the device is shown in figure 1, the device is designed in a three-section mode, and one side of the cathode is designed in a central circular hollow mode, so that the air cathode can be fully contacted with air; the cavity section is in a cylindrical hollow design and is used for containing liquid; the other side is solid, and the inside of the chamber can be observed; each section is connected by a rubber pad with a hollow middle part to play a role of sealing and water proofing, the cathode and the anode are connected to an external circuit by adopting a 0.5cm titanium wire, the external resistance is 1000 omega, and the voltage data of the MFC is acquired by a parallel data acquisition instrument;
starting a microbial fuel cell by using the cultured anaerobic sludge as a substrate of an anode chamber, wherein a reactor adopts an intermittent operation mode; after three cycles of operation, the output voltage of the MFC can be kept stable for a long time, and the maximum output voltage of each cycle is close, so that the starting of the MFC is finished;
(4) running microbial fuel cell with aged landfill leachate mixed shale gas flowback wastewater as matrix
Replacing an anode chamber anaerobic sludge substrate with a mixed waste liquid of aged landfill leachate and shale gas flowback wastewater, wherein the mixing volume ratio is 2:1, operating the MFC at room temperature and constant pressure, and recording the output voltage of the MFC by using a data acquisition instrument; before the operation is started and after the operation is finished, the COD and the ammonia nitrogen concentration of the mixed wastewater are respectively measured.
2. The method for treating the old landfill leachate mixed shale gas flowback wastewater by using the single-chamber microbial fuel cell as claimed in claim 1, wherein in the step 1, Co is prepared by a hydrothermal-roasting method 3 O 4 Y, further treated with 10% HF solution to obtain H-Co 3 O 4 and/Y, and as an anode catalyst for a single-compartment MFC.
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