CN103952305A - Method for constructing electro-catalytic bacterial biofilm at anode of microbial electrochemical reactor - Google Patents
Method for constructing electro-catalytic bacterial biofilm at anode of microbial electrochemical reactor Download PDFInfo
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Abstract
The invention relates to a method for constructing an electro-catalytic bacterial biofilm at an anode of a microbial electrochemical reactor. The method comprises the following steps: firstly assembling the microbial electrochemical reactor and connecting with circuits, wherein the first path is formed by connecting a fixed resistor between the anode and a cathode in series, and the second path is formed by connecting a direct current stabilized power supply, an ampere meter, a variable resistor and a working contact of a cycle time relay between the anode and the cathode in series; then injecting a bacterial growth culture medium liquid into an anode chamber, inoculating a bacteria source, conducting the first path to carry out prestart on the microbial anode, measuring the anode potential change to obtain a polarization curve and determining an ultimate current value of the anode; and after electro-catalytic bacterial biofilm is stimulated by using ultimate pulse current to grow, successively obtaining a new ultimate current value again, then stimulating again under the new ultimate pulse current, repeating the steps till no significant growth of the ultimate current exists and finishing construction of the anodic electro-catalytic bacterial biofilm. The electro-catalytic bacterial biofilm can stably run under relatively high working current.
Description
Technical field
The present invention relates to a kind of method that builds electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode, belong to microorganism electrochemical reactor technology field.
Background technology
Microorganism electrochemical reactor comprises microbiological fuel cell, microorganism electrolysis cell and microorganism electrochemical sensor.In microorganism electrochemical reactor, the electro catalytic activity and the operation stability that are attached to the electrocatalysis bacterial biof iotalm of electrode surface are the key parts that determines reactor performance, the electrocatalysis bacterial biof iotalm of stability and high efficiency can improve the energy efficiency of microbiological fuel cell and microorganism electrolysis cell, improves the sensitivity of microorganism electrochemical sensor signal response.Electrocatalysis bacterial biof iotalm is the cell accumulation layer with certain space structure jointly being formed by the electrogenesis bacterium with complete life metabolic function (sometimes also comprising non-electrogenesis bacterium) cell and the outer material of born of the same parents.On the electrode surface of bioelectrochemistry reactor, bacterial biof iotalm has reaction substrate oxygenolysis, and the electronics that oxidising process is discharged is delivered to the electrochemical catalysis function that forms electric current on electrode.
At present, there are two kinds in the method for microorganism electrochemical reactor anode structure electrocatalysis bacterial biof iotalm.The first is the construction process of permanent extrernal resistance pattern, key step has: (1) is inoculated into microbionation source in the anolyte compartment of reactor, and microbionation source comprises taking from cultivates the cultivation bacterium containing electrogenesis bacterium out etc. in environment settling, biological sewage treatment factory containing the mud of electrogenesis bacterium and under laboratory condition; (2) anode is connected by certain certain value external resistance and negative electrode, formed closed circuit, the adaptability growth that utilizes the bacterium that is inoculated into anolyte compartment to carry out on electrode surface, forms electrocatalysis bacterial biof iotalm.
The second is the construction process of permanent electrode potential pattern, key step has: (1) is inoculated into microbionation source in the anolyte compartment of reactor, and microbionation source comprises taking from cultivates the cultivation bacterium containing electrogenesis bacterium out etc. in environment settling, biological sewage treatment factory containing the mud of electrogenesis bacterium and under laboratory condition; (2) utilize potentiostat and reference electrode control anode potential to keep a certain steady state value, the bacterium that makes to be inoculated in anolyte compartment carries out adaptability growth at electrode surface, forms electrocatalysis bacterial biof iotalm.Although the electrochemical control method difference of two kinds of methods, two kinds of methods are in fact all to utilize the adaptability growth of bacterium antianode electromotive force, reach the object that builds electrocatalysis bacterial biof iotalm.
Above two kinds of differences that build the method for electrocatalysis bacterial biof iotalm are: in first method, what bacterium adapted to is the electromotive force of dynamic change.According to current disclosed data, utilize first method to build in electro catalytic activity microbial film process at anode surface, anode potential (with respect to standard hydrogen electrode) all changes conventionally in the scope of approximately+0.5V～-0.3V.In the second approach, what bacterium adapted to is constant anode potential, in biofilm formation process, conventionally anode potential is remained on to some fixed numbers, according to related data, in the second construction process, be all also that a selected constant anode potential is cultivated anode microbial film in the scope of+0.5V～-0.3V (with respect to standard hydrogen electrode) substantially.
The electrocatalysis bacterial biof iotalm of utilizing electromotive force adaptive method to build, ubiquity is not enough as follows: the maximal work electric current that (1) electrode can reach is less, and electrocatalysis efficiency is low; (2) electrocatalysis bacterial biof iotalm is to poor compared with the ability to bear of high workload electric current, in the time that the working current by electrode approaches or exceedes its limiting current, electrode can be by rapid hyperpolarization, more than hyperpolarization can cause anode potential (to be conventionally no more than 10 minutes) at short notice just to move on to+1.2V (with respect to standard hydrogen electrode), high like this anode potential can cause irreversible injury to bacterium itself, cause electrocatalysis bacterial biof iotalm destroyed, lose catalysis.In a word, the electrocatalysis bacterial biof iotalm of utilizing electromotive force adjustment procedure to build, it is less that ubiquity catalytic activity, to the shortcoming of high workload electric current bad adaptability, the electrocatalysis bacterial biof iotalm building, even the in the situation that of nutritive substance abundance, also cannot continous-stable work under the working current that approaches its limiting current level.Therefore, develop the construction process that there is higher catalytic activity and there is the electrocatalysis bacterial biof iotalm of operation stability under compared with high workload electric current, there is important technical meaning and application and popularization value widely for the bioelectrochemistry reactor of exploitation stability and high efficiency.
Summary of the invention
The object of the invention is to, overcome problems of the prior art, a kind of method that builds electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode is provided, can steady running under compared with high workload electric current.
For solving above technical problem, a kind of method that builds electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode of the present invention, in turn include the following steps: (1) assemble microorganism electrochemical reactor, described microorganism electrochemical reactor comprises anolyte compartment and cathode compartment, (2) junction circuit element, circuit element comprises system selector switch, fixed resistor, D.C. regulated power supply, reometer, variohm, cycle time relay and auxiliary DC power supply, the common end of described system selector switch and described anodic bonding, the first selecting side of described system selector switch is connected with described negative electrode with after described fixed resistor series connection, the second selecting side of described system selector switch successively with described D.C. regulated power supply, reometer, after the working contact series connection of variohm and described cycle time relay, be connected with described negative electrode, the coil of described cycle time relay is connected to the two ends of described auxiliary DC power supply by pilot switch, (3) microorganism anode pretrigger, inject bacterial growth media liquid by anode submergence to the anolyte compartment of described microorganism electrochemical reactor, in described anolyte compartment, inoculate the microbial bacteria source containing electrogenesis bacterium again, then described system selector switch is allocated to the first selecting side and connects, anode is connected with cathodic electricity by fixed resistor, microorganism anode is carried out to pretrigger, (4) the anode potential of continuously measured microorganism anode in pre-boot process changes, and anode potential variation is divided into three phases successively, and the first stage is the slow decreasing stage, and anode potential declines and is less than 0.1V altogether in 2～7 days in a high position, subordinate phase is the fast-descending stage, the anode potential 0.2V～0.6V that declined in 10～20 hours, phase III is the smooth change stage, and the amplitude stabilization that anode potential changes reaches more than 10 hours in ± 0.03V, arrives the phase III and is microorganism anode pretrigger and completes when anode potential changes, and the electrocatalysis bacterial biof iotalm Primary Construction of anode completes, (5) disconnect system selector switch, adopt linear sweep voltammetry to measure the polarization curve of microorganism anode, when measurement, taking negative electrode as supporting electrode, saturated calomel electrode is reference electrode, anode potential is scanned to 0V from-0.6V, and the electric current-potential energy diagram obtaining according to scanning is determined the limiting current value of anode, (6) utilize formula R=U/I to calculate the work resistance of required variohm while carrying out pulse current stimulating, the output voltage that wherein U is described D.C. regulated power supply, I is the limiting current value that (5) step records, and then adjusts described variohm to the work resistance calculating, regulate pulse width and the make-and-break time ratio of the make-and-break time setting pulse electric current of cycle time relay, described make-and-break time ratio is (0.5～1) second: 1 second again, then described system selector switch is allocated to the second selecting side and connects, connect described pilot switch simultaneously, make the limit pulsed current setting carry out galvanism to microorganism anode, electrocatalysis bacterial biof iotalm advolution 30～40 hours under above-mentioned galvanism, (7) disconnect described system selector switch, again measure with step method (5) the polarization curve that microorganism anode is new, obtain new higher limiting current value, then under new limit pulsed current, again microorganism anode is carried out to further limit pulse current stimulating by step method (6), so iterative cycles, (8) when after the limit pulse current stimulating repeating, the polarization curve obtaining according to step method is (5) compared with last round of polarization curve, and the growth of limiting current value is lower than 5%, and anode electrocatalysis bacterial biof iotalm of the present invention has built.
With respect to prior art, the present invention has obtained following beneficial effect: (1) circuit of the present invention provides two loops, when system selector switch is allocated to while being connected with the first selecting side, anode is connected with negative electrode by fixed resistor, microorganism anode obtains pretrigger, after three phases, electrocatalysis bacterial biof iotalm Primary Construction completes; When system selector switch is allocated to while being connected with the second selecting side, connect pilot switch simultaneously, the coil of cycle time relay in electricity condition, the break-make that the working contact of cycle time relay circulates, realizes the stimulation of pulse current source to microorganism anode.(2) limit of utilization impulse current system antianode electrocatalysis bacterial biof iotalm stimulates, can realize electrocatalysis bacterial biof iotalm is carried out to high galvanism on the one hand, on the other hand, use pulsed current, the electricity currency is no more than 1 second, otherwise can cause the hyperpolarization of microorganism anode, the electric current break time is not more than 1 second, otherwise do not reach the abundant galvanism to microorganism anode; By regulating suitable dutycycle, can effectively avoid electrocatalysis bacterial biof iotalm because of the damage that anode hyperpolarization causes, make electrocatalysis bacterial biof iotalm under high electric current environment, constantly to produce the adaptability to high electric current.(3) the power of electrocatalysis bacterial biof iotalm catalytic activity shows as the producible catalytic current size of microbial film under certain potential range and ambient condition, and catalytic current is large, and catalytic activity is strong; Limit pulse current stimulating method provided by the invention, than electromotive force adjustment procedure, can be enhanced about more than once the catalytic activity of electrocatalysis bacterial biof iotalm.(4) utilize limit pulse current stimulating method provided by the invention, can accelerate the development process of electrocatalysis bacterial biof iotalm at anode surface, and increase coverage and the biofilm thickness of electrocatalysis bacterial film at anode surface, the work operation stability of electrocatalysis bacterial biof iotalm is strengthened.(5) limit pulse current stimulating method provided by the invention builds electrocatalysis bacterial biof iotalm, be not limited to specific bacterial origin and bacterium monoid, utilize different environment bacterium sources, comprise natural sediment and sludge sewage in varying environment, all can be in bioelectrochemistry reactor, utilize the present invention to construct performance and be better than the electrocatalysis bacterial biof iotalm that electromotive force adjustment procedure obtains.
As preferred version of the present invention, the resistance of described fixed resistor is 500 ohm, and the resistance of described variohm is adjustable within the scope of 0～40000 ohm, and the output voltage of described D.C. regulated power supply is more than 24V.
As preferred version of the present invention, feed composition and the weight content of described bacterial growth media liquid are as follows: Repone K: sodium-chlor: calcium chloride: magnesium chloride: sodium bicarbonate: ammonium chloride: SODIUM PHOSPHATE, MONOBASIC: magnesium sulfate: iron vitriol: tetrahydrate manganese chloride: Sodium Molybdate Dihydrate: yeast water: sodium-acetate: water=(0.05～0.15): (0.05～0.15): (0.05～0.15): (0.05～0.15): (2.0～3.0): (1.0～2.0): (0.5～1.0): (0.05～0.15): (0.001～0.005): (0.001～0.005): (0.001～0.005): (0.05～0.1): (1.6～3.2): 1000.Repone K, sodium-chlor, calcium chloride, magnesium chloride, sodium bicarbonate, ammonium chloride, SODIUM PHOSPHATE, MONOBASIC and magnesium sulfate are constant inorganic salt, on the one hand for supplementing required potassium, sodium, calcium, magnesium, carbon, the nitrogen phosphate and sulfur element of bacterial growth, on the other hand, also there is ionic strength and the conductive capability of regulation culture liquid; As above it is 30 mM～40 mM that proportioning makes nutrient solution keep total ion concentration, and specific conductivity is 1.5 mS/cm～3.0 mS/cm; Wherein sodium bicarbonate and SODIUM PHOSPHATE, MONOBASIC, except being used separately as the inorganic carbon source and phosphorus source of bacterial growth, also have the effect of the pH of buffering nutrient solution.Iron vitriol, tetrahydrate manganese chloride and Sodium Molybdate Dihydrate supplement respectively required trace elements iron, manganese and the molybdenum of nutrient solution.Yeast water is the somatomedin in nutrient solution; Sodium-acetate, as organic substrates, is the required energy substance of bacterial growth, above component and weight ratio can make electrogenesis bacterium limiting current stimulate under at anode advolution preferably.
As preferred version of the present invention, described cathode solution comprises 50 mM K
3fe (CN)
6with 100 mM KH
2pO
4.
As preferred version of the present invention, described microbial bacteria source is the microbial bacteria source containing electrogenesis bacterium in city domestic sewage treatment plant active sludge or fresh water environment settling, and inoculum size is by inoculating 50～100 grams of described active sludge or described settlings in bacterial growth media liquid every liter described.
As preferred version of the present invention, when described step adopts linear sweep voltammetry to measure the polarization curve of microorganism anode in (5), potential scan rate-controlling is below 0.1mV/s.This potential scan speed can be avoided the impact of excessive charging current, can accurately obtain the limiting current value of microorganism anode.
Brief description of the drawings
Below in conjunction with the drawings and specific embodiments, the present invention is further detailed explanation, and accompanying drawing only provides reference and explanation use, non-in order to limit the present invention.
Fig. 1 is the circuit connection diagram of microorganism electrochemical reactor of the present invention.
Fig. 2 is the anode potential variation diagram of microorganism anode in pre-boot process.
Fig. 3 is the electrocatalysis bacterial biof iotalm developing without limit pulse current stimulating.
Fig. 4 is the polarization curve after microorganism anode pretrigger.
Fig. 5 is the polarization curve of microorganism anode after limit pulse current stimulating.
Fig. 6 is the electrocatalysis bacterial biof iotalm developing through limit pulse current stimulating.
In figure: QS1. system selector switch; QS2. pilot switch; R0. fixed resistor; DV1. D.C. regulated power supply; DV2. auxiliary DC power supply; A. reometer; RX. variohm; KT. cycle time relay.
Embodiment
Embodiment mono-
The present invention builds the method for electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode, in turn include the following steps:
(1) assemble microorganism electrochemical reactor, microorganism electrochemical reactor comprises anolyte compartment and cathode compartment.
(2) junction circuit element as shown in Figure 1, circuit element comprises system selector switch QS1, resistance is the fixed resistor R0 of 500 Ω, output voltage is the D.C. regulated power supply DV1 of 24V, reometer A, resistance adjustable variohm RX within the scope of 0～40000 ohm, pilot switch QS2 and on/off time are than (0.1s～10 s): (0.1s～10 are adjustable cycle time relay KT in scope s), common end and the anodic bonding of system selector switch QS1, the first selecting side of system selector switch QS1 is connected with negative electrode with after fixed resistor R0 series connection, the second selecting side of system selector switch QS1 successively with D.C. regulated power supply DV1, reometer A, after the working contact series connection of variohm RX and cycle time relay KT, be connected with negative electrode, the coil of cycle time relay KT is connected to the two ends of auxiliary DC power supply DV2 by pilot switch QS2.
(3) microorganism anode pretrigger, inject bacterial growth media liquid by anode submergence to the anolyte compartment of microorganism electrochemical reactor, inject cathode solution by negative electrode submergence to the cathode compartment of microorganism electrochemical reactor, in anode chamber, inoculate again the microbial bacteria source containing electrogenesis bacterium, then system selector switch QS1 is allocated to the first selecting side and connects and make anode pass through fixed resistor R0 to be connected with cathodic electricity, microorganism anode is carried out to pretrigger.
Feed composition and the weight content of bacterial growth media liquid are as follows: Repone K: sodium-chlor: calcium chloride: magnesium chloride: sodium bicarbonate: ammonium chloride: SODIUM PHOSPHATE, MONOBASIC: magnesium sulfate: iron vitriol: tetrahydrate manganese chloride: Sodium Molybdate Dihydrate: yeast water: sodium-acetate: water=0.08: 0.07: 0.07: 0.08: 2.5: 1.5: 0.7: 0.10:0.003:0.003:0.003:0.08:2.4:1000.Cathode solution comprises 50 mM K
3fe (CN)
6with 100 mM KH
2pO
4.
Microbial bacteria source is the microbial bacteria source containing electrogenesis bacterium in city domestic sewage treatment plant active sludge, and inoculum size is by 80 grams of inoculation of activated-sludge in every liter of bacterial growth media liquid.
(4) the anode potential of continuously measured microorganism anode in pre-boot process changes, and as shown in Figure 2, anode potential variation is divided into three phases successively, and the first stage is the slow decreasing stage, and anode potential declines and is less than 0.1V altogether in 65 hours in a high position; Subordinate phase is the fast-descending stage, the anode potential 0.6V that declined in 20 hours; Phase III is the smooth change stage, the amplitude stabilization that anode potential changes reaches 15 hours in ± 0.03V, arrive the phase III and be microorganism anode pretrigger and complete when anode potential changes, the electrocatalysis bacterial biof iotalm Primary Construction of anode completes, and electrocatalysis bacterial biof iotalm now as shown in Figure 3.
(5) disconnect system selector switch QS1, adopt linear sweep voltammetry to measure the polarization curve of microorganism anode, potential scan rate-controlling is below 0.1mV/s, when measurement taking negative electrode as supporting electrode, saturated calomel electrode is reference electrode, anode potential is scanned to 0V from-0.6V, as shown in Figure 4, electric current-the potential energy diagram obtaining according to scanning is determined the limiting current value of anode, and the electric current that in figure, the vertex of curve is corresponding is the limiting current of microorganism anode.
(6) utilize formula R=U/I to calculate the work resistance of required variohm RX while carrying out pulse current stimulating, wherein U is the output voltage of D.C. regulated power supply DV1, I is the limiting current value that (5) step records, and then adjusts variohm RX to the work resistance calculating; The pulse width and the make-and-break time ratio that regulate again the make-and-break time setting pulse electric current of cycle time relay KT, make-and-break time ratio is 1 second: 1 second; Then system selector switch QS1 is allocated to and the second selecting side is connected, connects pilot switch QS2 simultaneously, make the limit pulsed current setting carry out galvanism to microorganism anode, electrocatalysis bacterial biof iotalm advolution 40 hours under above-mentioned galvanism.
(7) disconnect system selector switch QS1, again measure with step method (5) the polarization curve that microorganism anode is new, obtain new higher limiting current value, then under new limit pulsed current, again microorganism anode is carried out to further limit pulse current stimulating by step method (6), so iterative cycles; Figure 5 shows that the 1. time to the 5. polarization curve contrast of time microorganism anode after class time limit pulse current stimulating, each limiting current value of taking turns all increases than last round of.
(8) when after the limit pulse current stimulating repeating, the polarization curve obtaining according to step method is (5) compared with last round of polarization curve, the growth of limiting current value is lower than 5%, as curve in Fig. 5 4. with curve 5. as shown in, be that limiting current is no longer significantly improved, anode electrocatalysis bacterial biof iotalm of the present invention has built, and the electrocatalysis bacterial biof iotalm developing through limit pulse current stimulating as shown in Figure 6.
Embodiment bis-
The present invention builds the method for electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode, in turn include the following steps:
(1) fill microorganism electrochemical reactor, microorganism electrochemical reactor comprises anolyte compartment and cathode compartment.
(2) junction circuit element as shown in Figure 1, circuit element comprises system selector switch QS1, resistance is the fixed resistor R0 of 500 Ω, output voltage is the D.C. regulated power supply DV1 of 24V, reometer A, resistance adjustable variohm RX within the scope of 0～40000 ohm, pilot switch QS2 and on/off time are than (0.1s～10 s): (0.1s～10 are adjustable cycle time relay KT in scope s), common end and the anodic bonding of system selector switch QS1, the first selecting side of system selector switch QS1 is connected with negative electrode with after fixed resistor R0 series connection, the second selecting side of system selector switch QS1 successively with D.C. regulated power supply DV1, reometer A, after the working contact series connection of variohm RX and cycle time relay KT, be connected with negative electrode, the coil of cycle time relay KT is connected to the two ends of auxiliary DC power supply DV2 by pilot switch QS2.
(3) microorganism anode pretrigger, inject bacterial growth media liquid by anode submergence to the anolyte compartment of microorganism electrochemical reactor, inject cathode solution by negative electrode submergence to the cathode compartment of microorganism electrochemical reactor, in anode chamber, inoculate again the microbial bacteria source containing electrogenesis bacterium, then system selector switch QS1 is allocated to the first selecting side and connects and make anode pass through fixed resistor R0 to be connected with cathodic electricity, microorganism anode is carried out to pretrigger.
Feed composition and the weight content of bacterial growth media liquid are as follows: Repone K: sodium-chlor: calcium chloride: magnesium chloride: sodium bicarbonate: ammonium chloride: SODIUM PHOSPHATE, MONOBASIC: magnesium sulfate: iron vitriol: tetrahydrate manganese chloride: Sodium Molybdate Dihydrate: yeast water: sodium-acetate: water=0.05: 0.05: 0.05: 0.05: 2.0: 1.0: 0.5: 0.05:0.001:0.001:0.001:0.05:1.6:1000.Cathode solution comprises 50 mM K
3fe (CN)
6with 100 mM KH
2pO
4.
Microbial bacteria source is the microbial bacteria source containing electrogenesis bacterium in fresh water environment settling, and inoculum size is by inoculating 50 grams of settlings in every liter of bacterial growth media liquid.
(4) the anode potential of continuously measured microorganism anode in pre-boot process changes, and anode potential variation is divided into three phases successively, and the first stage is the slow decreasing stage, and anode potential declines and is less than 0.1V altogether in 2 days in a high position; Subordinate phase is the fast-descending stage, the anode potential 0.2V that declined in 10 hours; Phase III is the smooth change stage, and the amplitude stabilization that anode potential changes reaches 10 hours in ± 0.03V, arrives the phase III and is microorganism anode pretrigger and completes when anode potential changes, and the electrocatalysis bacterial biof iotalm Primary Construction of anode completes.
(5) disconnect system selector switch QS1, adopt linear sweep voltammetry to measure the polarization curve of microorganism anode, potential scan rate-controlling is below 0.1mV/s, when measurement taking negative electrode as supporting electrode, saturated calomel electrode is reference electrode, anode potential is scanned to 0V from-0.6V, and the electric current-potential energy diagram obtaining according to scanning is determined the limiting current value of anode, and the electric current that in figure, the vertex of curve is corresponding is the limiting current of microorganism anode.
(6) utilize formula R=U/I to calculate the work resistance of required variohm RX while carrying out pulse current stimulating, wherein U is the output voltage of D.C. regulated power supply DV1, I is the limiting current value that (5) step records, and then adjusts variohm RX to the work resistance calculating; The pulse width and the make-and-break time ratio that regulate again the make-and-break time setting pulse electric current of cycle time relay KT, make-and-break time ratio is 0.5 second: 1 second; Then system selector switch QS1 is allocated to and the second selecting side is connected, connects pilot switch QS2 simultaneously, make the limit pulsed current setting carry out galvanism to microorganism anode, electrocatalysis bacterial biof iotalm advolution 30 hours under above-mentioned galvanism.
(7) disconnect system selector switch QS1, again measure with step method (5) the polarization curve that microorganism anode is new, obtain new higher limiting current value, then under new limit pulsed current, again microorganism anode is carried out to further limit pulse current stimulating by step method (6), so iterative cycles, each limiting current value of taking turns all increases than last round of.
(8) when after the limit pulse current stimulating repeating, the polarization curve obtaining according to step method is (5) compared with last round of polarization curve, the growth of limiting current value is lower than 5%, and limiting current is no longer significantly improved, and anode electrocatalysis bacterial biof iotalm of the present invention has built.
Embodiment tri-
The present invention builds the method for electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode, in turn include the following steps:
(1) fill microorganism electrochemical reactor, microorganism electrochemical reactor comprises anolyte compartment and cathode compartment.
(2) junction circuit element as shown in Figure 1, circuit element comprises system selector switch QS1, resistance is the fixed resistor R0 of 500 Ω, output voltage is the D.C. regulated power supply DV1 of 24V, reometer A, resistance adjustable variohm RX within the scope of 0～40000 ohm, pilot switch QS2 and on/off time are than (0.1s～10 s): (0.1s～10 are adjustable cycle time relay KT in scope s), common end and the anodic bonding of system selector switch QS1, the first selecting side of system selector switch QS1 is connected with negative electrode with after fixed resistor R0 series connection, the second selecting side of system selector switch QS1 successively with D.C. regulated power supply DV1, reometer A, after the working contact series connection of variohm RX and cycle time relay KT, be connected with negative electrode, the coil of cycle time relay KT is connected to the two ends of auxiliary DC power supply DV2 by pilot switch QS2.
(3) microorganism anode pretrigger, inject bacterial growth media liquid by anode submergence to the anolyte compartment of microorganism electrochemical reactor, inject cathode solution by negative electrode submergence to the cathode compartment of microorganism electrochemical reactor, in anode chamber, inoculate again the microbial bacteria source containing electrogenesis bacterium, then system selector switch QS1 is allocated to the first selecting side and connects and make anode pass through fixed resistor R0 to be connected with cathodic electricity, microorganism anode is carried out to pretrigger.
Feed composition and the weight content of bacterial growth media liquid are as follows, Repone K: sodium-chlor: calcium chloride: magnesium chloride: sodium bicarbonate: ammonium chloride: SODIUM PHOSPHATE, MONOBASIC: magnesium sulfate: iron vitriol: tetrahydrate manganese chloride: Sodium Molybdate Dihydrate: yeast water: sodium-acetate: water=0.15: 0.15: 0.15: 0.15: 3.0: 2.0: 1.0: 0.15:0.005:0.005:0.005:0.1:3.2:1000.Cathode solution comprises 50 mM K
3fe (CN)
6with 100 mM KH
2pO
4.
Microbial bacteria source is the microbial bacteria source containing electrogenesis bacterium in city domestic sewage treatment plant active sludge, and inoculum size is by 100 grams of inoculation of activated-sludge in every liter of bacterial growth media liquid.
(4) the anode potential of continuously measured microorganism anode in pre-boot process changes, and anode potential variation is divided into three phases successively, and the first stage is the slow decreasing stage, and anode potential declines and is less than 0.1V altogether in 7 days in a high position; Subordinate phase is the fast-descending stage, the anode potential 0.6V that declined in 20 hours; Phase III is the smooth change stage, and the amplitude stabilization that anode potential changes reaches 12 hours in ± 0.03V, arrives the phase III and is microorganism anode pretrigger and completes when anode potential changes, and the electrocatalysis bacterial biof iotalm Primary Construction of anode completes.
(5) disconnect system selector switch QS1, adopt linear sweep voltammetry to measure the polarization curve of microorganism anode, potential scan rate-controlling is below 0.1mV/s, when measurement taking negative electrode as supporting electrode, saturated calomel electrode is reference electrode, anode potential is scanned to 0V from-0.6V, and the electric current-potential energy diagram obtaining according to scanning is determined the limiting current value of anode, and the electric current that in figure, the vertex of curve is corresponding is the limiting current of microorganism anode.
(6) utilize formula R=U/I to calculate the work resistance of required variohm RX while carrying out pulse current stimulating, wherein U is the output voltage of D.C. regulated power supply DV1, I is the limiting current value that (5) step records, and then adjusts variohm RX to the work resistance calculating; The pulse width and the make-and-break time ratio that regulate again the make-and-break time setting pulse electric current of cycle time relay KT, make-and-break time ratio is 1 second: 1 second; Then system selector switch QS1 is allocated to and the second selecting side is connected, connects pilot switch QS2 simultaneously, make the limit pulsed current setting carry out galvanism to microorganism anode, electrocatalysis bacterial biof iotalm advolution 40 hours under above-mentioned galvanism.
(7) disconnect system selector switch QS1, again measure with step method (5) the polarization curve that microorganism anode is new, obtain new higher limiting current value, then under new limit pulsed current, again microorganism anode is carried out to further limit pulse current stimulating by step method (6), so iterative cycles, each limiting current value of taking turns all increases than last round of.
(8) when after the limit pulse current stimulating repeating, the polarization curve obtaining according to step method is (5) compared with last round of polarization curve, the growth of limiting current value is lower than 5%, and limiting current is no longer significantly improved, and anode electrocatalysis bacterial biof iotalm of the present invention has built.
Embodiment tetra-
The present invention builds the method for electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode, in turn include the following steps:
(1) fill microorganism electrochemical reactor, microorganism electrochemical reactor comprises anolyte compartment and cathode compartment.
(2) junction circuit element as shown in Figure 1, circuit element comprises system selector switch QS1, resistance is the fixed resistor R0 of 500 Ω, output voltage is the D.C. regulated power supply DV1 of 24V, reometer A, resistance adjustable variohm RX within the scope of 0～40000 ohm, pilot switch QS2 and on/off time are than (0.1s～10 s): (0.1s～10 are adjustable cycle time relay KT in scope s), common end and the anodic bonding of system selector switch QS1, the first selecting side of system selector switch QS1 is connected with negative electrode with after fixed resistor R0 series connection, the second selecting side of system selector switch QS1 successively with D.C. regulated power supply DV1, reometer A, after the working contact series connection of variohm RX and cycle time relay KT, be connected with negative electrode, the coil of cycle time relay KT is connected to the two ends of auxiliary DC power supply DV2 by pilot switch QS2.
(3) microorganism anode pretrigger, inject bacterial growth media liquid by anode submergence to the anolyte compartment of microorganism electrochemical reactor, inject cathode solution by negative electrode submergence to the cathode compartment of microorganism electrochemical reactor, in anode chamber, inoculate again the microbial bacteria source containing electrogenesis bacterium, then system selector switch QS1 is allocated to the first selecting side and connects and make anode pass through fixed resistor R0 to be connected with cathodic electricity, microorganism anode is carried out to pretrigger.
Feed composition and the weight content of bacterial growth media liquid are as follows: Repone K: sodium-chlor: calcium chloride: magnesium chloride: sodium bicarbonate: ammonium chloride: SODIUM PHOSPHATE, MONOBASIC: magnesium sulfate: iron vitriol: tetrahydrate manganese chloride: Sodium Molybdate Dihydrate: yeast water: sodium-acetate: water=0.05: 0.15: 0.05: 0.15: 2.5: 1.0: 1.0: 0.15:0.001:0.005:0.001:0.1:2.0:1000.Cathode solution comprises 50 mM K
3fe (CN)
6with 100 mM KH
2pO
4.
Microbial bacteria source is the microbial bacteria source containing electrogenesis bacterium in fresh water environment settling, and inoculum size is by inoculating 70 grams of settlings in every liter of bacterial growth media liquid.
(4) the anode potential of continuously measured microorganism anode in pre-boot process changes, and anode potential variation is divided into three phases successively, and the first stage is the slow decreasing stage, and anode potential declines and is less than 0.1V altogether in 3 days in a high position; Subordinate phase is the fast-descending stage, the anode potential 0.4V that declined in 16 hours; Phase III is the smooth change stage, and the amplitude stabilization that anode potential changes reaches 13 hours in ± 0.03V, arrives the phase III and is microorganism anode pretrigger and completes when anode potential changes, and the electrocatalysis bacterial biof iotalm Primary Construction of anode completes.
(5) disconnect system selector switch QS1, adopt linear sweep voltammetry to measure the polarization curve of microorganism anode, potential scan rate-controlling is below 0.1mV/s, when measurement taking negative electrode as supporting electrode, saturated calomel electrode is reference electrode, anode potential is scanned to 0V from-0.6V, and the electric current-potential energy diagram obtaining according to scanning is determined the limiting current value of anode, and the electric current that in figure, the vertex of curve is corresponding is the limiting current of microorganism anode.
(6) utilize formula R=U/I to calculate the work resistance of required variohm RX while carrying out pulse current stimulating, wherein U is the output voltage of D.C. regulated power supply DV1, I is the limiting current value that (5) step records, and then adjusts variohm RX to the work resistance calculating; The pulse width and the make-and-break time ratio that regulate again the make-and-break time setting pulse electric current of cycle time relay KT, make-and-break time ratio is 0.7 second: 1 second; Then system selector switch QS1 is allocated to and the second selecting side is connected, connects pilot switch QS2 simultaneously, make the limit pulsed current setting carry out galvanism to microorganism anode, electrocatalysis bacterial biof iotalm advolution 35 hours under above-mentioned galvanism.
(7) disconnect system selector switch QS1, again measure with step method (5) the polarization curve that microorganism anode is new, obtain new higher limiting current value, then under new limit pulsed current, again microorganism anode is carried out to further limit pulse current stimulating by step method (6), so iterative cycles, each limiting current value of taking turns all increases than last round of.
(8) when after the limit pulse current stimulating repeating, the polarization curve obtaining according to step method is (5) compared with last round of polarization curve, the growth of limiting current value is lower than 5%, and limiting current is no longer significantly improved, and anode electrocatalysis bacterial biof iotalm of the present invention has built.
Embodiment five
The present invention builds the method for electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode, in turn include the following steps:
(1) fill microorganism electrochemical reactor, microorganism electrochemical reactor comprises anolyte compartment and cathode compartment.
(2) junction circuit element as shown in Figure 1, circuit element comprises system selector switch QS1, resistance is the fixed resistor R0 of 500 Ω, output voltage is the D.C. regulated power supply DV1 of 24V, reometer A, resistance adjustable variohm RX within the scope of 0～40000 ohm, pilot switch QS2 and on/off time are than (0.1s～10 s): (0.1s～10 are adjustable cycle time relay KT in scope s), common end and the anodic bonding of system selector switch QS1, the first selecting side of system selector switch QS1 is connected with negative electrode with after fixed resistor R0 series connection, the second selecting side of system selector switch QS1 successively with D.C. regulated power supply DV1, reometer A, after the working contact series connection of variohm RX and cycle time relay KT, be connected with negative electrode, the coil of cycle time relay KT is connected to the two ends of auxiliary DC power supply DV2 by pilot switch QS2.
(3) microorganism anode pretrigger, inject bacterial growth media liquid by anode submergence to the anolyte compartment of microorganism electrochemical reactor, inject cathode solution by negative electrode submergence to the cathode compartment of microorganism electrochemical reactor, in anode chamber, inoculate again the microbial bacteria source containing electrogenesis bacterium, then system selector switch QS1 is allocated to the first selecting side and connects and make anode pass through fixed resistor R0 to be connected with cathodic electricity, microorganism anode is carried out to pretrigger.
Feed composition and the weight content of bacterial growth media liquid are as follows: Repone K: sodium-chlor: calcium chloride: magnesium chloride: sodium bicarbonate: ammonium chloride: SODIUM PHOSPHATE, MONOBASIC: magnesium sulfate: iron vitriol: tetrahydrate manganese chloride: Sodium Molybdate Dihydrate: yeast water: sodium-acetate: water=0.09: 0.08: 0.07: 0.09: 2.4: 1.8: 0.9: 0.07:0.002:0.003:0.005:0.07:1.9:1000.Cathode solution comprises 50 mM K
3fe (CN)
6with 100 mM KH
2pO
4.
Microbial bacteria source is the microbial bacteria source containing electrogenesis bacterium in city domestic sewage treatment plant active sludge, and inoculum size is by 90 grams of inoculation of activated-sludge in every liter of bacterial growth media liquid.
(4) the anode potential of continuously measured microorganism anode in pre-boot process changes, and anode potential variation is divided into three phases successively, and the first stage is the slow decreasing stage, and anode potential declines and is less than 0.1V altogether in 4 days in a high position; Subordinate phase is the fast-descending stage, the anode potential 0.5V that declined in 18 hours; Phase III is the smooth change stage, and the amplitude stabilization that anode potential changes reaches 18 hours in ± 0.03V, arrives the phase III and is microorganism anode pretrigger and completes when anode potential changes, and the electrocatalysis bacterial biof iotalm Primary Construction of anode completes.
(5) disconnect system selector switch QS1, adopt linear sweep voltammetry to measure the polarization curve of microorganism anode, potential scan rate-controlling is below 0.1mV/s, when measurement taking negative electrode as supporting electrode, saturated calomel electrode is reference electrode, anode potential is scanned to 0V from-0.6V, and the electric current-potential energy diagram obtaining according to scanning is determined the limiting current value of anode, and the electric current that in figure, the vertex of curve is corresponding is the limiting current of microorganism anode.
(6) utilize formula R=U/I to calculate the work resistance of required variohm RX while carrying out pulse current stimulating, wherein U is the output voltage of D.C. regulated power supply DV1, I is the limiting current value that (5) step records, and then adjusts variohm RX to the work resistance calculating; The pulse width and the make-and-break time ratio that regulate again the make-and-break time setting pulse electric current of cycle time relay KT, make-and-break time ratio is 0.9 second: 1 second; Then system selector switch QS1 is allocated to and the second selecting side is connected, connects pilot switch QS2 simultaneously, make the limit pulsed current setting carry out galvanism to microorganism anode, electrocatalysis bacterial biof iotalm advolution 30 hours under above-mentioned galvanism.
(7) disconnect system selector switch QS1, again measure with step method (5) the polarization curve that microorganism anode is new, obtain new higher limiting current value, then under new limit pulsed current, again microorganism anode is carried out to further limit pulse current stimulating by step method (6), so iterative cycles, each limiting current value of taking turns all increases than last round of.
(8) when after the limit pulse current stimulating repeating, the polarization curve obtaining according to step method is (5) compared with last round of polarization curve, the growth of limiting current value is lower than 5%, and limiting current is no longer significantly improved, and anode electrocatalysis bacterial biof iotalm of the present invention has built.
Embodiment six
The present invention builds the method for electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode, in turn include the following steps:
(1) fill microorganism electrochemical reactor, microorganism electrochemical reactor comprises anolyte compartment and cathode compartment.
(2) junction circuit element as shown in Figure 1, circuit element comprises system selector switch QS1, resistance is the fixed resistor R0 of 500 Ω, output voltage is the D.C. regulated power supply DV1 of 24V, reometer A, resistance adjustable variohm RX within the scope of 0～40000 ohm, pilot switch QS2 and on/off time are than (0.1s～10 s): (0.1s～10 are adjustable cycle time relay KT in scope s), common end and the anodic bonding of system selector switch QS1, the first selecting side of system selector switch QS1 is connected with negative electrode with after fixed resistor R0 series connection, the second selecting side of system selector switch QS1 successively with D.C. regulated power supply DV1, reometer A, after the working contact series connection of variohm RX and cycle time relay KT, be connected with negative electrode, the coil of cycle time relay KT is connected to the two ends of auxiliary DC power supply DV2 by pilot switch QS2.
(3) microorganism anode pretrigger, inject bacterial growth media liquid by anode submergence to the anolyte compartment of microorganism electrochemical reactor, inject cathode solution by negative electrode submergence to the cathode compartment of microorganism electrochemical reactor, in anode chamber, inoculate again the microbial bacteria source containing electrogenesis bacterium, then system selector switch QS1 is allocated to the first selecting side and connects and make anode pass through fixed resistor R0 to be connected with cathodic electricity, microorganism anode is carried out to pretrigger.
Feed composition and the weight content of bacterial growth media liquid are as follows: Repone K: sodium-chlor: calcium chloride: magnesium chloride: sodium bicarbonate: ammonium chloride: SODIUM PHOSPHATE, MONOBASIC: magnesium sulfate: iron vitriol: tetrahydrate manganese chloride: Sodium Molybdate Dihydrate: yeast water: sodium-acetate: water=0.15: 0.05: 0.15: 0.08: 2.0: 2.0: 0.5: 0.08:0.003:0.004:0.005:0.05:3.2:1000.Cathode solution comprises 50 mM K
3fe (CN)
6with 100 mM KH
2pO
4.
Microbial bacteria source is the microbial bacteria source containing electrogenesis bacterium in city domestic sewage treatment plant active sludge, and inoculum size is by 90 grams of inoculation of activated-sludge in every liter of bacterial growth media liquid.
(4) the anode potential of continuously measured microorganism anode in pre-boot process changes, and anode potential variation is divided into three phases successively, and the first stage is the slow decreasing stage, and anode potential declines and is less than 0.1V altogether in 4 days in a high position; Subordinate phase is the fast-descending stage, the anode potential 0.5V that declined in 16 hours; Phase III is the smooth change stage, and the amplitude stabilization that anode potential changes reaches 10 hours in ± 0.03V, arrives the phase III and is microorganism anode pretrigger and completes when anode potential changes, and the electrocatalysis bacterial biof iotalm Primary Construction of anode completes.
(5) disconnect system selector switch QS1, adopt linear sweep voltammetry to measure the polarization curve of microorganism anode, potential scan rate-controlling is below 0.1mV/s, when measurement taking negative electrode as supporting electrode, saturated calomel electrode is reference electrode, anode potential is scanned to 0V from-0.6V, and the electric current-potential energy diagram obtaining according to scanning is determined the limiting current value of anode, and the electric current that in figure, the vertex of curve is corresponding is the limiting current of microorganism anode.
(6) utilize formula R=U/I to calculate the work resistance of required variohm RX while carrying out pulse current stimulating, wherein U is the output voltage of D.C. regulated power supply DV1, I is the limiting current value that (5) step records, and then adjusts variohm RX to the work resistance calculating; The pulse width and the make-and-break time ratio that regulate again the make-and-break time setting pulse electric current of cycle time relay KT, make-and-break time ratio is 0.6 second: 1 second; Then system selector switch QS1 is allocated to and the second selecting side is connected, connects pilot switch QS2 simultaneously, make the limit pulsed current setting carry out galvanism to microorganism anode, electrocatalysis bacterial biof iotalm advolution 34 hours under above-mentioned galvanism.
(7) disconnect system selector switch QS1, again measure with step method (5) the polarization curve that microorganism anode is new, obtain new higher limiting current value, then under new limit pulsed current, again microorganism anode is carried out to further limit pulse current stimulating by step method (6), so iterative cycles, each limiting current value of taking turns all increases than last round of.
(8) when after the limit pulse current stimulating repeating, the polarization curve obtaining according to step method is (5) compared with last round of polarization curve, the growth of limiting current value is lower than 5%, and limiting current is no longer significantly improved, and anode electrocatalysis bacterial biof iotalm of the present invention has built.
The foregoing is only the present invention's better possible embodiments, non-ly therefore limit to scope of patent protection of the present invention.In addition to the implementation, the present invention can also have other embodiments.All employings are equal to the technical scheme of replacement or equivalent transformation formation, all drop in the protection domain of requirement of the present invention.The present invention can pass through or adopt existing techniques in realizing without the technical characterictic of describing, and does not repeat them here.
Claims (6)
1. a method that builds electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode, is characterized in that, in turn includes the following steps: (1) assemble microorganism electrochemical reactor, described microorganism electrochemical reactor comprises anolyte compartment and cathode compartment, (2) junction circuit element, circuit element comprises system selector switch, fixed resistor, D.C. regulated power supply, reometer, variohm, cycle time relay and auxiliary DC power supply, the common end of described system selector switch and described anodic bonding, the first selecting side of described system selector switch is connected with described negative electrode with after described fixed resistor series connection, the second selecting side of described system selector switch successively with described D.C. regulated power supply, reometer, after the working contact series connection of variohm and described cycle time relay, be connected with described negative electrode, the coil of described cycle time relay is connected to the two ends of described auxiliary DC power supply by pilot switch, (3) microorganism anode pretrigger, inject bacterial growth media liquid by anode submergence to the anolyte compartment of described microorganism electrochemical reactor, in described anolyte compartment, inoculate the microbial bacteria source containing electrogenesis bacterium again, then described system selector switch is allocated to the first selecting side and connects, anode is connected with cathodic electricity by fixed resistor, microorganism anode is carried out to pretrigger, (4) the anode potential of continuously measured microorganism anode in pre-boot process changes, and anode potential variation is divided into three phases successively, and the first stage is the slow decreasing stage, and anode potential declines and is less than 0.1V altogether in 2～7 days in a high position, subordinate phase is the fast-descending stage, the anode potential 0.2V～0.6V that declined in 10～20 hours, phase III is the smooth change stage, and the amplitude stabilization that anode potential changes reaches more than 10 hours in ± 0.03V, arrives the phase III and is microorganism anode pretrigger and completes when anode potential changes, and the electrocatalysis bacterial biof iotalm Primary Construction of anode completes, (5) disconnect system selector switch, adopt linear sweep voltammetry to measure the polarization curve of microorganism anode, when measurement, taking negative electrode as supporting electrode, saturated calomel electrode is reference electrode, anode potential is scanned to 0V from-0.6V, and the electric current-potential energy diagram obtaining according to scanning is determined the limiting current value of anode, (6) utilize formula R=U/I to calculate the work resistance of required variohm while carrying out pulse current stimulating, the output voltage that wherein U is described D.C. regulated power supply, I is the limiting current value that (5) step records, and then adjusts described variohm to the work resistance calculating, regulate pulse width and the make-and-break time ratio of the make-and-break time setting pulse electric current of cycle time relay, described make-and-break time ratio is (0.5～1) second: 1 second again, then described system selector switch is allocated to the second selecting side and connects, connect described pilot switch simultaneously, make the limit pulsed current setting carry out galvanism to microorganism anode, electrocatalysis bacterial biof iotalm advolution 30～40 hours under above-mentioned galvanism, (7) disconnect described system selector switch, again measure with step method (5) the polarization curve that microorganism anode is new, obtain new higher limiting current value, then under new limit pulsed current, again microorganism anode is carried out to further limit pulse current stimulating by step method (6), so iterative cycles, (8) when after the limit pulse current stimulating repeating, the polarization curve obtaining according to step method is (5) compared with last round of polarization curve, and the growth of limiting current value is lower than 5%, and anode electrocatalysis bacterial biof iotalm of the present invention has built.
2. a kind of method that builds electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode according to claim 1, it is characterized in that: the resistance of described fixed resistor is 500 ohm, the resistance of described variohm is adjustable within the scope of 0～40000 ohm, and the output voltage of described D.C. regulated power supply is more than 24V.
3. a kind of method that builds electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode according to claim 1, it is characterized in that, feed composition and the weight content of described bacterial growth media liquid are as follows: Repone K: sodium-chlor: calcium chloride: magnesium chloride: sodium bicarbonate: ammonium chloride: SODIUM PHOSPHATE, MONOBASIC: magnesium sulfate: iron vitriol: tetrahydrate manganese chloride: Sodium Molybdate Dihydrate: yeast water: sodium-acetate: water=(0.05～0.15): (0.05～0.15): (0.05～0.15): (0.05～0.15): (2.0～3.0): (1.0～2.0): (0.5～1.0): (0.05～0.15): (0.001～0.005): (0.001～0.005): (0.001～0.005): (0.05～0.1): (1.6～3.2): 1000.
4. a kind of method that builds electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode according to claim 1, is characterized in that: described cathode solution comprises 50 mM K
3fe (CN)
6with 100 mM KH
2pO
4.
5. a kind of method that builds electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode according to claim 1, it is characterized in that: described microbial bacteria source is the microbial bacteria source containing electrogenesis bacterium in city domestic sewage treatment plant active sludge or fresh water environment settling, and inoculum size is by inoculating 50～100 grams of described active sludge or described settlings in bacterial growth media liquid every liter described.
6. a kind of method that builds electrocatalysis bacterial biof iotalm at microorganism electrochemical reactor anode according to claim 1, it is characterized in that: when described step adopts linear sweep voltammetry to measure the polarization curve of microorganism anode in (5), potential scan rate-controlling is below 0.1mV/s.
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| CN113371847A (en) * | 2021-06-11 | 2021-09-10 | 广东省科学院微生物研究所(广东省微生物分析检测中心) | Method for obtaining a large amount of cable bacteria and application of cable bacteria in removing sulfides in black and odorous sediments |
| CN113607793A (en) * | 2021-07-28 | 2021-11-05 | 广东省科学院微生物研究所(广东省微生物分析检测中心) | Method for constructing biological membrane catalytic electrode with high activity |
| CN113607793B (en) * | 2021-07-28 | 2023-11-17 | 广东省科学院微生物研究所(广东省微生物分析检测中心) | Method for constructing biological film catalytic electrode with high activity |
| CN113960135A (en) * | 2021-11-09 | 2022-01-21 | 福建农林大学 | Rechargeable microbial electrochemical sensor, preparation thereof and application thereof in water quality early warning |
| CN113960135B (en) * | 2021-11-09 | 2023-10-31 | 福建农林大学 | Rechargeable microorganism electrochemical sensor, preparation thereof and application thereof in water quality early warning |
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