CN110247091A - A method of accelerate electroactive microorganism to carry out extracellular electron transfer process - Google Patents
A method of accelerate electroactive microorganism to carry out extracellular electron transfer process Download PDFInfo
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- CN110247091A CN110247091A CN201910571281.9A CN201910571281A CN110247091A CN 110247091 A CN110247091 A CN 110247091A CN 201910571281 A CN201910571281 A CN 201910571281A CN 110247091 A CN110247091 A CN 110247091A
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- 238000000034 method Methods 0.000 title claims abstract description 33
- 244000005700 microbiome Species 0.000 title claims abstract description 26
- 230000027756 respiratory electron transport chain Effects 0.000 title claims abstract description 13
- 150000001875 compounds Chemical class 0.000 claims abstract description 18
- SZVJSHCCFOBDDC-UHFFFAOYSA-N iron(II,III) oxide Inorganic materials O=[Fe]O[Fe]O[Fe]=O SZVJSHCCFOBDDC-UHFFFAOYSA-N 0.000 claims abstract description 18
- 239000006229 carbon black Substances 0.000 claims abstract description 11
- 239000000446 fuel Substances 0.000 claims abstract description 11
- 230000002906 microbiologic effect Effects 0.000 claims abstract description 9
- 239000010802 sludge Substances 0.000 claims abstract description 6
- 230000001133 acceleration Effects 0.000 claims abstract description 3
- 239000000243 solution Substances 0.000 claims description 11
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonium chloride Substances [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 claims description 6
- 238000006243 chemical reaction Methods 0.000 claims description 6
- 238000002360 preparation method Methods 0.000 claims description 4
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims description 3
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 claims description 3
- 229910021577 Iron(II) chloride Inorganic materials 0.000 claims description 3
- 229910021578 Iron(III) chloride Inorganic materials 0.000 claims description 3
- 235000011114 ammonium hydroxide Nutrition 0.000 claims description 3
- 239000007864 aqueous solution Substances 0.000 claims description 3
- 239000007795 chemical reaction product Substances 0.000 claims description 3
- 238000010438 heat treatment Methods 0.000 claims description 3
- NMCUIPGRVMDVDB-UHFFFAOYSA-L iron dichloride Chemical compound Cl[Fe]Cl NMCUIPGRVMDVDB-UHFFFAOYSA-L 0.000 claims description 3
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical compound Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 claims description 3
- 238000010992 reflux Methods 0.000 claims description 3
- 229910052708 sodium Inorganic materials 0.000 claims description 3
- 239000011734 sodium Substances 0.000 claims description 3
- 229910021642 ultra pure water Inorganic materials 0.000 claims description 3
- 239000012498 ultrapure water Substances 0.000 claims description 3
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 claims description 2
- 238000004090 dissolution Methods 0.000 claims 1
- 230000005540 biological transmission Effects 0.000 abstract description 4
- 239000000126 substance Substances 0.000 abstract description 4
- 238000001556 precipitation Methods 0.000 abstract description 2
- 230000000813 microbial effect Effects 0.000 abstract 1
- TWRXJAOTZQYOKJ-UHFFFAOYSA-L Magnesium chloride Chemical compound [Mg+2].[Cl-].[Cl-] TWRXJAOTZQYOKJ-UHFFFAOYSA-L 0.000 description 6
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 6
- 235000015097 nutrients Nutrition 0.000 description 6
- UXVMQQNJUSDDNG-UHFFFAOYSA-L Calcium chloride Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 description 3
- VMHLLURERBWHNL-UHFFFAOYSA-M Sodium acetate Chemical compound [Na+].CC([O-])=O VMHLLURERBWHNL-UHFFFAOYSA-M 0.000 description 3
- 239000001110 calcium chloride Substances 0.000 description 3
- 229910001628 calcium chloride Inorganic materials 0.000 description 3
- 229940041514 candida albicans extract Drugs 0.000 description 3
- 239000003610 charcoal Substances 0.000 description 3
- 239000012530 fluid Substances 0.000 description 3
- XLYOFNOQVPJJNP-ZSJDYOACSA-N heavy water Substances [2H]O[2H] XLYOFNOQVPJJNP-ZSJDYOACSA-N 0.000 description 3
- 238000009533 lab test Methods 0.000 description 3
- 229910001629 magnesium chloride Inorganic materials 0.000 description 3
- 239000001632 sodium acetate Substances 0.000 description 3
- 235000017281 sodium acetate Nutrition 0.000 description 3
- 239000011780 sodium chloride Substances 0.000 description 3
- 239000006228 supernatant Substances 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- 239000012138 yeast extract Substances 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 230000001404 mediated effect Effects 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- KVYRCBOUKXJXDK-UHFFFAOYSA-N 3,4-dimethylphenazine-1,2-diamine hydrochloride Chemical compound Cl.C1=CC=CC2=NC3=C(C)C(C)=C(N)C(N)=C3N=C21 KVYRCBOUKXJXDK-UHFFFAOYSA-N 0.000 description 1
- RBTBFTRPCNLSDE-UHFFFAOYSA-N 3,7-bis(dimethylamino)phenothiazin-5-ium Chemical compound C1=CC(N(C)C)=CC2=[S+]C3=CC(N(C)C)=CC=C3N=C21 RBTBFTRPCNLSDE-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000000853 adhesive Substances 0.000 description 1
- 230000001070 adhesive effect Effects 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 238000009833 condensation Methods 0.000 description 1
- 230000005494 condensation Effects 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000007306 functionalization reaction Methods 0.000 description 1
- 238000000338 in vitro Methods 0.000 description 1
- 238000011081 inoculation Methods 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229960000907 methylthioninium chloride Drugs 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 125000001820 oxy group Chemical group [*:1]O[*:2] 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 125000004151 quinonyl group Chemical group 0.000 description 1
- 230000010148 water-pollination Effects 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/9075—Catalytic material supported on carriers, e.g. powder carriers
- H01M4/9083—Catalytic material supported on carriers, e.g. powder carriers on carbon or graphite
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/96—Carbon-based electrodes
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/16—Biochemical fuel cells, i.e. cells in which microorganisms function as catalysts
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Electrochemistry (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Life Sciences & Earth Sciences (AREA)
- Microbiology (AREA)
- Sustainable Energy (AREA)
- Sustainable Development (AREA)
- Manufacturing & Machinery (AREA)
- Biochemistry (AREA)
- Inert Electrodes (AREA)
Abstract
The present invention discloses a kind of method for accelerating electroactive microorganism to carry out extracellular electron transfer process, belongs to field of microbial electromechanical technology.The method of the invention is by compound HA@Fe3O4It is doped in the carbon black anode of microbiological fuel cell, constructs microbiological fuel cell, and be inoculated with anaerobic activated sludge, after stable, the electroactive microorganism for being attached to doping anode surface realizes the acceleration of electron stream burst size;Wherein, compound HA@Fe3O4It is 3.33% ~ 10% that mass percent is adulterated in carbon black anode.The method of the invention directly enhances the process rate that electroactive microorganism carries out extracellular electron transmission, hence it is evident that the amount of precipitation for reducing mediator substance helps to realize the practical application of microorganism electrochemical system.
Description
Technical field
The present invention relates to a kind of methods for accelerating electroactive microorganism to carry out extracellular electron transfer process, and in particular to compound
Object HA@Fe3O4The method for accelerating electroactive microorganism to carry out extracellular electron transfer process is mediated, microorganism electrochemical technology is belonged to
Field.
Background technique
Currently, for the modified pass that interacted with to improve it between electroactive microorganism of microorganism electrochemical system anode
Be to promote for example, by using concentrated acid processing or to carry out surface oxygroup functionalization there are many process approach of extracellular electron transmission, with
And the hydrophily of raising anode surface is modified to improve the adhesive ability of electroactive microorganism by Nitrogen element substance, or
It is the interaction relationship that electroactive microorganism and electrode are improved using organic and inorganic medium and electroconductive polymer coating.However
Most effective way is to add dimethyl diaminophenazine chloride, the methylene blue either mediator substance containing quinonyl in anode chamber, can reach rush
The process of extracellular electron transmission is carried out into electroactive microorganism, but these mediators are mostly artificial synthesized and higher cost, it is molten
The problem of Yu Shuihou is easy to be lost, and the stability in use process is poor, is likely to result in secondary pollution.
Summary of the invention
The purpose of the present invention is to provide a kind of methods for accelerating electroactive microorganism to carry out extracellular electron transfer process, should
Method is based on compound HA@Fe3O4Can mediated electron transfer effect, reach modified anode to optimize extracellular electronics transfer
Condition, and then achieve the purpose that promote electroactive microorganism accelerated release in vitro electronics in microorganism electrochemical system.
The invention is realized by the following technical scheme:
A method of accelerate electroactive microorganism to carry out extracellular electron transfer process: by compound HA@Fe3O4It is doped to micro-
In the carbon black anode of biological fuel cell, microbiological fuel cell is constructed, and be inoculated with anaerobic activated sludge, it is attached after stable
Realize the acceleration of electron stream burst size in the electroactive microorganism of doping anode surface;Wherein, compound HA@Fe3O4?
The calculation that mass percent is 3.33% ~ 10%(mass percent is adulterated in carbon black anode are as follows: compound HA Fe3O4Than
Upper compound HA@Fe3O4With the gross mass of carbon black).
Preferably, compound HA@Fe of the present invention3O4The preparation method comprises the following steps: in molar ratio for 1.5:1 ratio will
FeCl3·6H2O and FeCl2·4H2O is dissolved in the aqueous solution of 100mL, and then mixed liquor is put into equipped with reflux condensate device
Vessel in heating to 90 ± 5 DEG C, the sodium humate solution of the ammonia solution of 10mL 25% and 50ml 1% are sequentially added into ferrous solution
In, continuation is heated 30 minutes under the conditions of 90 ± 5 DEG C, in entire reaction process, is stirred, is finally obtained to reaction solution
Reaction product cleaned with ultrapure water to neutrality, it is dry to constant weight, obtain compound HA@Fe3O4, other methods preparation it is compound
Object HA@Fe3O4It can be used for the present invention.
Other parts (such as nutriment, anode plate, structure of reactor, the inoculation of biological fuel cell of the present invention
Source, reactor service condition factor) it is conventional arrangement.
The present invention has the advantage that
(1) the method for the invention is by being put into doped and compounded object HA@Fe in anode in microbiological fuel cell3O4, realize
Accelerate the purpose for mediating electroactive microorganism to carry out extracellular electron transfer process;The electricity improved compared to tradition addition human intermediary's body
The way of son transmitting, the method for the present invention is simple and effective, economic stability, and it is obvious to improve electronics transfer effect.
(2) present invention directly enhances the process rate that electroactive microorganism carries out extracellular electron transmission, hence it is evident that reduces
The amount of precipitation of mediator substance helps to realize the practical application of microorganism electrochemical system.
Specific embodiment
Invention is further described in detail combined with specific embodiments below, but protection scope of the present invention is not limited to
The content.
Compound HA@Fe described in the embodiment of the present invention 1 ~ 33O4The preparation method comprises the following steps: in molar ratio be 1.5:1 ratio
By FeCl3·6H2O and FeCl2·4H2O is dissolved in the aqueous solution of 100mL, is then put into mixed liquor and is filled equipped with reflux condensation mode
It is molten that the vessel in heating set to 90 ± 5 DEG C, by the sodium humate solution of the ammonia solution of 10mL 25% and 50ml 1% sequentially adds iron
In liquid, continuation is heated 30 minutes under the conditions of 90 ± 5 DEG C, in entire reaction process, is stirred to reaction solution, finally
To reaction product cleaned with ultrapure water to neutrality, it is dry to constant weight, obtain compound HA@Fe3O4。
Embodiment 1
Carry out two groups of parallel laboratory tests, two groups of cathode and anode building volumes of starting are the microbiological fuel cell of 56mL, in anode chamber
It is inoculated with the anaerobic activated sludge supernatant in same source, nutrients is the sodium acetate solution of 1g/L, and in addition nutrients prepares base fluid
Containing PBS:50mmol, NH4CL:0.8g/L, NaCl:2.92g/L, CaCl2·2H2O:0.05g/L, MgCl2·6H2O:0.2g/L with
And yeast extract: 0.01g/L;One group of anode is using charcoal black electrode as anode, and another set is using the HA for adulterating 3.33%
Fe3O4Carbon black as anode, two groups of cell cathodes are same electrode.After two groups of batteries are stablized under 1000 Ω perseverance resistance
Carry out discharge test, the results showed that in discharge cycle the anode potential of blank group be -400mV, adulterate 3.33% anode unit be -
455mV;In addition the maximum current density of blank group and power density show are as follows: 356.13 mA m-2/229.56mW m-2, and
The maximum current density and power density of 3.33% doping group anode unit are shown to be 376.57 mA m-2/256.67 mW m-2, with
Blank group increases 5.7% and 11.8% than maximum current density and power density respectively, shows the castering action of electron transfer process
Obviously.
Embodiment 2
Carry out two groups of parallel laboratory tests, two groups of cathode and anode building volumes of starting are the microbiological fuel cell of 56mL, in anode chamber
It is inoculated with the anaerobic activated sludge supernatant in same source, nutrients is the sodium acetate solution of 1g/L, and in addition nutrients prepares base fluid
Containing PBS:50mmol, NH4CL:0.8g/L, NaCl:2.92g/L, CaCl2·2H2O:0.05g/L, MgCl2·6H2O:0.2g/L with
And yeast extract: 0.01g/L;One group of anode is using charcoal black electrode as anode, and another set is using the HA for adulterating 6.67%
Fe3O4Carbon black as anode, two groups of cell cathodes are same electrode.After two groups of batteries are stablized under 1000 Ω perseverance resistance
Carry out discharge test, the results showed that the anode unit that 6.67% is adulterated in discharge cycle is -470mV;Other 6.67% doping group anode
The maximum current density and power density of group are shown to be 392.71mA m-2/279.14 mW m-2, compare maximum current with blank group
Density and power density increase 10.3% and 21.6% respectively.
Embodiment 3
Carry out two groups of parallel laboratory tests, two groups of cathode and anode building volumes of starting are the microbiological fuel cell of 56mL, in anode chamber
It is inoculated with the anaerobic activated sludge supernatant in same source, nutrients is the sodium acetate solution of 1g/L, and in addition nutrients prepares base fluid
Containing PBS:50mmol, NH4CL:0.8g/L, NaCl:2.92g/L, CaCl2·2H2O:0.05g/L, MgCl2·6H2O:0.2g/L with
And yeast extract: 0.01g/L;One group of anode is using charcoal black electrode as anode, and another set is using the HA for adulterating 10.00%
@Fe3O4Carbon black as anode, two groups of cell cathodes are same electrode;After two groups of batteries are stablized under 1000 Ω perseverance resistance
Carry out discharge test, the results showed that the anode unit for adulterating 10.00% is -460mV;The maximum of other 10.00% doping group anode unit
Current density and power density are shown to be 371.71mA m-2/250.09mW m-2, with blank group than maximum current density and power
Density increases 4.4% and 8.9% respectively.
The results show carbon black doped anode compound HA@Fe of embodiment 1 ~ 33O4Afterwards, electroactive microorganism carries out
Extracellular electron transfer process improved efficiency is obvious.
Claims (2)
1. a kind of method for accelerating electroactive microorganism to carry out extracellular electron transfer process, it is characterised in that: by compound HA@
Fe3O4It is doped in the carbon black anode of microbiological fuel cell, constructs microbiological fuel cell, and be inoculated with anaerobic activated sludge, transport
After row is stablized, the electroactive microorganism for being attached to doping anode surface realizes the acceleration of electron stream burst size;Wherein, compound
HA @Fe3O4It is 3.33% ~ 10% that mass percent is adulterated in carbon black anode.
2. the method for accelerating electroactive microorganism to carry out extracellular electron transfer process according to claim 1, it is characterised in that:
Compound HA@Fe3O4The preparation method comprises the following steps: being in molar ratio the ratio of 1.5:1 by FeCl3·6H2O and FeCl2·4H2O dissolution
In the aqueous solution of 100mL, mixed liquor is then put into the vessel in heating equipped with reflux condensate device to 90 ± 5 DEG C, is incited somebody to action
The ammonia solution of 10mL 25% and the sodium humate solution of 50ml 1% sequentially add in ferrous solution, continue to add under the conditions of 90 ± 5 DEG C
Heat 30 minutes, in entire reaction process, reaction solution is stirred, the reaction product finally obtained with ultrapure water clean to
Neutrality, it is dry to constant weight, obtain compound HA@Fe3O4。
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Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN111463441A (en) * | 2020-04-13 | 2020-07-28 | 山东建筑大学 | Aminated Fe3O4@SiO2Nanoparticle and application thereof in polypyrrole-modified microbial fuel cell anode |
CN111682229A (en) * | 2020-06-24 | 2020-09-18 | 中国海洋大学 | Humic acid-Fe composite modified anode, preparation method and application thereof, and seabed microbial fuel cell |
Citations (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN102820473A (en) * | 2012-09-03 | 2012-12-12 | 南开大学 | Preparation method and application of compound positive pole of microbial fuel cell |
CN105489908A (en) * | 2016-01-13 | 2016-04-13 | 中国科学院广州能源研究所 | Application of humic acid composite biochar in microbial fuel cell and preparation method of humic acid composite biochar |
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2019
- 2019-06-28 CN CN201910571281.9A patent/CN110247091A/en active Pending
Patent Citations (2)
Publication number | Priority date | Publication date | Assignee | Title |
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CN102820473A (en) * | 2012-09-03 | 2012-12-12 | 南开大学 | Preparation method and application of compound positive pole of microbial fuel cell |
CN105489908A (en) * | 2016-01-13 | 2016-04-13 | 中国科学院广州能源研究所 | Application of humic acid composite biochar in microbial fuel cell and preparation method of humic acid composite biochar |
Non-Patent Citations (1)
Title |
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SHUNGUI ZHOU,ET AL: ""Influence of Humic Acid Complexation with Metal Ions on Extracellular Electron Transfer Activity"", 《SCIENTIFIC REPORTS》 * |
Cited By (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN111463441A (en) * | 2020-04-13 | 2020-07-28 | 山东建筑大学 | Aminated Fe3O4@SiO2Nanoparticle and application thereof in polypyrrole-modified microbial fuel cell anode |
CN111463441B (en) * | 2020-04-13 | 2022-02-18 | 山东建筑大学 | Aminated Fe3O4@SiO2Nanoparticle and application thereof in polypyrrole-modified microbial fuel cell anode |
CN111682229A (en) * | 2020-06-24 | 2020-09-18 | 中国海洋大学 | Humic acid-Fe composite modified anode, preparation method and application thereof, and seabed microbial fuel cell |
CN111682229B (en) * | 2020-06-24 | 2022-07-15 | 中国海洋大学 | Humic acid-Fe composite modified anode, preparation method and application thereof, and seabed microbial fuel cell |
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