CN106082420A - A kind of automatic bias pollution control system producing electricity microorganism anode auxiliary hetero-junctions anode - Google Patents

A kind of automatic bias pollution control system producing electricity microorganism anode auxiliary hetero-junctions anode Download PDF

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Publication number
CN106082420A
CN106082420A CN201610429023.3A CN201610429023A CN106082420A CN 106082420 A CN106082420 A CN 106082420A CN 201610429023 A CN201610429023 A CN 201610429023A CN 106082420 A CN106082420 A CN 106082420A
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anode
chamber
quasiconductor
cathode
microorganism
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CN106082420B (en
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柳丽芬
于婷婷
杨凤林
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Dalian University of Technology
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Dalian University of Technology
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    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/72—Treatment of water, waste water, or sewage by oxidation
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/70—Treatment of water, waste water, or sewage by reduction
    • 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
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00—Nature of the contaminant
    • C02F2101/10—Inorganic compounds
    • C02F2101/16—Nitrogen compounds, e.g. ammonia
    • C02F2101/163—Nitrates
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2305/00—Use of specific compounds during water treatment
    • C02F2305/02—Specific form of oxidant
    • C02F2305/023—Reactive oxygen species, singlet oxygen, OH radical
    • 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

Abstract

The invention provides a kind of automatic bias pollution control system producing electricity microorganism anode auxiliary hetero-junctions anode, belong to low energy consumption technical field of waste water processing.Under conditions of without additional illumination and applied voltage, applying quasiconductor catalysis electrode hetero-junctions spontaneous generation electronics, activating oxygen produces free radical, and for oxidizing anode organic pollution, anode produces electronics and conducts to negative electrode also by external circuit, goes back parent pollutant；Meanwhile, microorganism anode produces electronics by external circuit conduction to negative electrode, the reduction reaction of reinforcement negative electrode inorganic pollution.TiO is loaded on carbon cloth2/g‑C3N4As anode 1, load product electricity bacterium graphite granule is as anode 2, and tungsten filament growth in situ tungsten trioxide nano granule is as catalytic cathode；The invention have the advantages that different pollutant are removed in heterojunction semiconductor catalyticing anode, product electricity microorganism anode, quasiconductor catalytic cathode three Room simultaneously, reach low energy consumption and process the target of waste water.

Description

A kind of automatic bias pollution control system producing electricity microorganism anode auxiliary hetero-junctions anode
Technical field
The invention belongs to waste water treatment technology of low energy consumption field, relate to applying automatic bias between heterojunction semiconductor catalysis electrode Generation electronics flows, and activating oxygen produces free radical, and producing electricity microorganism auxiliary provides electronics to urge in quasiconductor catalytic cathode, utilization Polarizing electrode realizes the removal of three kinds of different pollutant from microorganism electrode simultaneously.
Background technology
Along with developing rapidly of modern chemical industry, increasing artificial-synthetic compound enters human lives, at band Many simultaneously also to bring huge negative effect for environment easily；Dyeing waste water is typical case's generation of high pollution industrial wastewater Table, is the environomental pollution source paid close attention in the works of pollutant catabolic gene.
Nitrate is a kind of pollutant being prevalent in natural environment, along with the development of human civilization, subsoil water Pollution of nitrate nitrogen oneself be the environmental problem generally existed in world wide；Excess free enthalpy nitrate can cause cell and group The breathing knitted is destroyed, after nitrate enters human body, it is also possible to be reduced to nitrite in internal organs, make blood red egg in blood Lose oxygen carrying capacity in vain, thus cause anoxia to be poisoned.
Absorption, coagulation, chemical oxidation, electrochemical oxidation and bioanalysis etc. be all in treatment of dyeing wastewater research frequently with Technique.Nitrate dissolubility is high, the characteristic of good stability so that it is have certain difficulty, traditional coagulation-heavy when processing The handling technology of water supply that forms sediment-filter is difficult to remove it；At present, the technology removing nitrate mainly has ion exchange, reverse osmosis, life Thing method etc.., all there are respective pluses and minuses in above method, therefore needs a kind of energy-conservation, sewage treatment process efficiently of design, real Remove while existing organic pollutants and inorganic pollution.
At present the most still without the unsolicited electronic transfer between research and utilization semiconductor catalyst hetero-junctions, activating oxygen be produced from by Base, for oxidizing anode pollutant；Meanwhile, anode produces electronics also by external circuit conduction to negative electrode, reduction cathode contamination Thing；Coupling product electricity microorganism anode generation electronics, by external circuit conduction to negative electrode, can strengthen going back of the reducible pollutant of negative electrode Former reaction.
Summary of the invention
It is an object of the invention to provide a kind of automatic bias Environmental capacity system producing electricity microorganism anode auxiliary hetero-junctions anode System, solves under conditions of without additional illumination and voltage, the problem of variety classes pollutant of simultaneously degrading under the conditions of low energy consumption.
Technical scheme:
A kind of automatic bias pollution control system producing electricity microorganism anode auxiliary hetero-junctions anode, these automatic bias pollutant drop Solution system includes reactor, aerator and computer data acquisition system；Described reactor is divided by cation exchange membrane Being three Room, both sides are anode chamber, and centre is cathode chamber；Left side anode chamber is heterojunction semiconductor catalyticing anode, right side anode chamber For producing electricity microorganism anode, middle cathode chamber is quasiconductor catalytic cathode；Three kinds of different types of polluted-waters are placed in three Room Degrade simultaneously；It is quartz glass outside left side anode chamber and middle cathode chamber；Bottom left side anode chamber and middle cathode chamber all Arranging aeration head, left side anode chamber exposes air, and middle cathode chamber exposes nitrogen, and right side anode chamber maintains anaerobic conditions within；Quasiconductor is different Matter knot catalyticing anode and produce electricity microorganism anode and is connected with catalytic cathode respectively and has external resistance, heterojunction semiconductor catalyticing anode and The resistance connecting external resistance between catalytic cathode is more than product electricity microorganism anode and the resistance being connected external resistance between catalytic cathode, partly leads Bulk heterojunction catalyticing anode is 300-1200 Ω with the resistance being connected external resistance 1 between catalytic cathode, produces electricity microorganism anode and urges Changing the resistance of connection external resistance 2 between negative electrode is 1-100 Ω；The voltage that contaminant degradation system produces passes through computer data acquiring System acquisition.
Described heterojunction semiconductor catalyticing anode is to load two or three conduction band and valence band location on conducting base Different semiconductor catalysts, or semiconductor catalyst is combined with metallic atom, under conditions of without additional illumination and voltage, Between heterojunction semiconductor catalyst, automatic bias produces electric current, such as TiO2/g-C3N4、Cu2O2/TiO2、BiVO4/CdS、BiVO4/g- C3N4/ Fe etc.；Described quasiconductor catalytic cathode is to there is, with heterojunction semiconductor anode, the quasiconductor catalysis that fermi level is poor Agent, such as WO3、ZnO、SnO2Deng；The described electricity microorganism anode that produces is the conducting base that electricity bacterium is produced in load.
It is Recalcitrant chemicals waste water in described left side anode chamber 1, such as rhodamine B, triclosan, berberine etc., right side For the sanitary sewage containing sodium acetate, ammonium chloride etc. for producing electricity bacteria growing in anode chamber 2, it is reducible in middle cathode chamber Pollutant, such as nitrate nitrogen.
The automatic bias pollutant control system producing electricity microorganism anode auxiliary hetero-junctions anode runs: without additional illumination or Voltage, the heterojunction semiconductor catalyticing anode that conduction band positions is relatively born is placed in the anode chamber of left side, the quasiconductor of valence band location corrigendum Catalytic cathode is placed in middle cathode chamber, produces electricity microorganism anode and is placed in the anode chamber of right side, and in the anode chamber of left side, quasiconductor is urged Due to the existence of interior bias between polarizing electrode hetero-junctions and semiconductor cathode, an electronics part for spontaneous generation is raw with oxygen reaction Become O2 -, another part by external circuit conduction to negative electrode reduce hole and electronics between compound, in degraded cathode chamber Reducible pollutant；Meanwhile, h produced by quasiconductor+With absorption at the H of semiconductor surface2O or OH-Reaction generates OH, OH and O2 -For strong oxidizer, the pollutant in oxidative degradation anode chamber；The hole produced also has strong oxidizing property, it is possible to directly Oxidation water pollutant；Product electricity bacterium in the anode chamber of right side produces electronics also can be delivered to catalytic cathode by external circuit, improves The degradation efficiency of the reducible pollutant of above negative electrode；This produces the automatic bias pollutant fall of electricity microorganism anode auxiliary hetero-junctions anode Solution system, degrades three kinds of dissimilar pollutant in three Room simultaneously.
Beneficial effects of the present invention: without additional illumination or voltage, utilize the self power generation between semiconductor catalyst hetero-junctions Son transfer produces oxidative free radical, and oxidizing anode pollutant are carried out with reduction cathode contamination thing simultaneously, and it is micro-that electricity is produced in increase simultaneously Biological anode provides electronics to catalytic cathode, thus improves cathode contamination thing degradation efficiency.
Accompanying drawing explanation
Fig. 1 is a kind of automatic bias pollution control system figure producing electricity microorganism anode auxiliary hetero-junctions anode.
In figure: 1 computer；2 cation exchange membranes；3 heterojunction semiconductor catalyticing anodes；4 aeration heads；5 data collecting cards； 6 external resistances 1；7 external resistances 2；8 quasiconductor catalytic cathode；9 produce electricity microorganism anode；10 expose air；11 expose nitrogen.
Fig. 2 is that heterojunction semiconductor catalyticing anode produces map of current with producing electricity microorganism anode self.
In figure: abscissa express time, unit minute, vertical coordinate represents electric current, unit microampere, square represent three Room, Unglazed, catalyticing anode, round dot represents two Room, unglazed, catalyticing anode, and hollow triangle represents two Room, ultraviolet catalytic anode, Black triangle represents three Room, unglazed, microorganism anode, though the electric current of spontaneous generation is small, can be used for degradation of contaminant.
Fig. 3 is heterojunction semiconductor catalyticing anode rhodamine B degradation efficiency chart.
In figure: abscissa express time, unit minute, vertical coordinate represents clearance, wherein hollow triangle represent two Room, Ultraviolet catalytic anode, black triangle represents three Room, unglazed, microorganism anode, and round dot represents two Room, unglazed, catalyticing anode, Have ultraviolet light irradiate under the conditions of, degradation rate is better than other two kinds of conditions, but adds the cost of additional illumination, and compare two Room without Optical condition, increases microorganism anode, while improving contaminant degradation rate, reduces again energy consumption, it may also be used for sanitary sewage Degraded.
Fig. 4 is catalytic cathode degraded nitrate nitrogen efficiency chart.
In figure: abscissa express time, unit minute, vertical coordinate represents clearance, wherein hollow triangle represent two Room, Ultraviolet catalytic anode, black triangle represents three Room, unglazed, microorganism anode, and round dot represents two Room, unglazed, catalyticing anode, Under the conditions of having ultraviolet light to irradiate, degradation rate is better than other two kinds of conditions.
Detailed description of the invention
The detailed description of the invention of the present invention is described in detail below in conjunction with technical scheme and accompanying drawing.
Embodiment 1
Heterojunction semiconductor catalyticing anode TiO2/g-C3N4Preparation: 27ml butyl titanate mixes with 23ml ethanol, magnetic force Stirring 30min；Add 3.3ml HCl, 2.7ml deionized water；Add appropriate g-C3N4, stir, immerse 20*5cm2Carbon is fine Wei Bu, 105 DEG C of drying, repeatedly after 5 times, under the conditions of 450 DEG C, 5 DEG C of min-1, calcine 2h.
Quasiconductor catalytic cathode WO3Prepared by/W: soaked in ethanol solution 24 hours by tungsten filament, removes tungsten filament impurity Rear 60 DEG C of drying, 500 DEG C of temperature lower calcinations 2 hours, tungsten filament is become light yellow by black.
Produce electricity microorganism anode: graphite granule inoculation Shiva formula bacterium, after one week of biofilm, reactor brings into operation.
The automatic bias pollution control system producing electricity microorganism anode auxiliary hetero-junctions anode runs: TiO2/g-C3N4As half Conductor hetero-junctions catalyticing anode 1 is placed on the left of reactor, and the product electricity microorganism anode of inoculation Shiva formula bacterium graphite granule is placed in instead Answer on the right side of device, WO3/ W negative electrode is placed in the middle of reactor, such as Fig. 1；TiO2/g-C3N4Anode and WO3/ W negative electrode passes through 1000 Ω dispatches from foreign news agency Resistance is connected, and the resistance reason connecting resistance value big is so that TiO2/g-C3N4The electronics of spontaneous generation is mostly used in anode Oxygen activating, produce free radical cracking anode Organic substance；And microorganism anode and WO3/ W negative electrode is connected by 1 Ω external resistance, more Be conducive to the electron transmission that microorganism produces to cathodic reduction nitrate nitrogen.
In anode chamber 1, liquid is 300mL, 10mg L-1RhB, 0.05mol L-1NaOH；Right side anode indoor liquid is (mg L-1)CH3COONa (0.64), NH4Cl (0.057), CaCl2(0.0115), MgSO4(0.012), K2HPO4(0.012)；Cloudy Pole indoor liquid is 300mL 0.05mol L-1Formic acid, 100mg L-1NO3 --N；
Three Room are isolated by cation exchange membrane, are passed through air and provide oxygen, use on the left of heterojunction semiconductor in anode chamber Free radical is produced in electronic activation oxygen；Catalytic cathode indoor are passed through nitrogen, remove the electron acceptor oxygen in cathode chamber so that More electronics is used for reducing nitrate nitrogen；Test under the conditions of following three kinds: two Room, ultraviolet light irradiate the two poles of the earth, three Room, nothing Light, catalyticing anode, increase microorganism anode, two Room, unglazed, catalyticing anode, when quasiconductor spontaneous generation Weak current such as figure 2, degradation of contaminant, as it is shown on figure 3, react four hours, on the left of catalysis, in anode chamber, the degradation rate of rhodamine B is respectively 87.93%, 79.33%, 73.19%；As it is shown on figure 3, react four hours, the degradation rate of negative electrode nitrate nitrogen is respectively 93.80%, 89.97%, 87.08%, the degraded of negative electrode nitrate nitrogen quickly, occurs mainly in front half an hour；Under the conditions of having ultraviolet light to irradiate, fall Solution rate is better than other two kinds of conditions, but adds the cost of additional illumination, and compares two Room no light condition, increases microorganism sun Pole, while improving contaminant degradation rate, reduces again energy consumption, it may also be used for the degraded of sanitary sewage.

Claims (3)

1. the automatic bias pollution control system producing electricity microorganism anode auxiliary hetero-junctions anode, it is characterised in that this self-bias Pressure contaminant degradation system includes reactor, aerator and computer data acquisition system；Described reactor by sun from Proton exchange is divided into three Room, and both sides are anode chamber, and centre is cathode chamber；Left side anode chamber is heterojunction semiconductor catalyticing anode, Right side anode chamber is for producing electricity microorganism anode, and middle cathode chamber is quasiconductor catalytic cathode；Three kinds of different types of polluted-waters It is placed in three Room and degrades simultaneously；It is quartz glass outside left side anode chamber and middle cathode chamber；Left side anode chamber is cloudy with centre Being respectively provided with aeration head bottom room, pole, left side anode chamber exposes air, and middle cathode chamber exposes nitrogen, and right side anode chamber keeps anaerobism bar Part；Heterojunction semiconductor catalyticing anode and product electricity microorganism anode are connected with quasiconductor catalytic cathode respectively external resistance, partly leads The resistance of external resistance it is connected more than producing electricity microorganism anode and quasiconductor between bulk heterojunction catalyticing anode with quasiconductor catalytic cathode The resistance of external resistance, heterojunction semiconductor catalyticing anode and the resistance being connected external resistance 1 between catalytic cathode is connected between catalytic cathode For 300-1200 Ω, producing electricity microorganism anode is 1-100 Ω with the resistance being connected external resistance 2 between quasiconductor catalytic cathode；Pollute The voltage that thing degeneration system produces is gathered by computer data acquisition system.
Automatic bias pollution control system the most according to claim 1, it is characterised in that described heterojunction semiconductor catalysis Anode is to load the semiconductor catalyst that two or three conduction band is different from valence band location on conducting base, or is urged by quasiconductor Agent is combined with metallic atom, and under conditions of without additional illumination and voltage, between heterojunction semiconductor catalyst, automatic bias produces Electric current；Described quasiconductor catalytic cathode is to there is, with heterojunction semiconductor anode, the semiconductor catalyst that fermi level is poor；Institute The electricity microorganism anode that produces stated is the conducting base that electricity bacterium is produced in load.
Automatic bias pollution control system the most according to claim 1 and 2, it is characterised in that in described left side anode chamber For Recalcitrant chemicals waste water, for the sanitary sewage for producing electricity bacteria growing in the anode chamber of right side, it is reducible in middle cathode chamber Pollutant.
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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN107952464A (en) * 2017-12-13 2018-04-24 大连理工大学 A kind of novel photocatalysis material and double photochemical catalyst electrode automatic bias pollution control systems
CN110306203A (en) * 2019-07-09 2019-10-08 郑州大学 A kind of cathode generates the electrochemical appliance and method of the hydrogen peroxide organic wastewater of anode processing simultaneously

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CN105047977A (en) * 2015-08-19 2015-11-11 浙江大学 Photocatalytic and biological composite anode- and biological cathode-coupled fuel cell
CN105110554A (en) * 2015-08-17 2015-12-02 大连理工大学 System for removing nitrate nitrogen in water by virtue of coupling (optical) catalysis and MFC
CN105293688A (en) * 2015-10-22 2016-02-03 大连理工大学 System for removing nitrate nitrogen in water in electro-catalysis mode through coupling biology positive electrode

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Publication number Priority date Publication date Assignee Title
JP2012507828A (en) * 2008-10-30 2012-03-29 エメフシー リミテッド Electrodes for use in bacterial fuel cells and bacterial electrolysis cells, and bacterial fuel cells and bacterial electrolysis cells using such electrodes
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Publication number Priority date Publication date Assignee Title
CN107952464A (en) * 2017-12-13 2018-04-24 大连理工大学 A kind of novel photocatalysis material and double photochemical catalyst electrode automatic bias pollution control systems
CN107952464B (en) * 2017-12-13 2020-09-11 大连理工大学 Novel photocatalytic material and double-photocatalytic-electrode self-bias pollution control system
CN110306203A (en) * 2019-07-09 2019-10-08 郑州大学 A kind of cathode generates the electrochemical appliance and method of the hydrogen peroxide organic wastewater of anode processing simultaneously
CN110306203B (en) * 2019-07-09 2021-08-06 郑州大学 Electrochemical device and method for generating hydrogen peroxide at cathode and simultaneously carrying out anodic treatment on organic wastewater

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