CN109286026A - A kind of novel (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell system - Google Patents
A kind of novel (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell system Download PDFInfo
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- CN109286026A CN109286026A CN201811065145.4A CN201811065145A CN109286026A CN 109286026 A CN109286026 A CN 109286026A CN 201811065145 A CN201811065145 A CN 201811065145A CN 109286026 A CN109286026 A CN 109286026A
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- 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
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
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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
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/46176—Galvanic cells
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- 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
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- 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
- H01M4/9041—Metals or alloys
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- 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
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- 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
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
- C02F2101/345—Phenols
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- 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
-
- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
The invention belongs to environmental catalysis, purification of water quality and energy recoveries to utilize technical field, it is related to silver/zinc oxide nanometer stick array/nickel foam self-supporting electrode material as anode, cobalt ferrite/carbon nano-fiber electrode or cobalt ferrite/carbon nano-fiber/pvdf membrane and constructs novel photocatalysis fuel cell system as cathode.Cathode Co2+Potentiometric titrations and singlet oxygen are generated by catalysis peroxy-monosulfate, assists promotion system degradation property；Carbon nano-fiber promotes material conductivity and ORR performance, promotes PFC system and produces electricity effect.And CoF2O4Film filtration is introduced system and increases catalysis material and pollutant reaction contact by/carbon nano-fiber/pvdf membrane cathode, increases catalytic activity.And system automatic bias generates electronics and promotes active site Co in cathode material2+Circulation in system reduces Ion release, promotes the reusing of electrode；Whether there is or not realize efficient contaminant degradation under light conditions.
Description
Technical field
The invention belongs to environmental catalysis, purification of water quality and energy recoveries to utilize technical field, be related to silver/zinc oxide nanometer
Stick array/nickel foam self-supporting electrode material is as photocatalysis anode, cobalt ferrite/carbon nano-fiber/carbon fiber cloth electrode or iron
Sour cobalt/carbon nano-fiber/pvdf membrane electrode constructs novel photocatalysis fuel cell system as cathode, and in particular to photoelectricity is urged
Change and potentiometric titrations catalyzing oxidizing degrading.
Background technique
It is increasingly serious due to problem of environmental pollution, how quickly, efficiently, energy savingly realize that the processing of sewage is scientific research
The problem of worker explores always.Based on potentiometric titrations (SO4 ·-) oxidation persistent organic pollutants processing technique be
Grow up a kind of high-level oxidation technology in recent years.Advanced oxygen process oxidability based on sulfate free radical is strong, oxidant
Stability itself is good, activation method is more, pH use scope is wide, and the service life (half-life period 4s) of potentiometric titrations compares hydroxyl
Base free radical (service life is less than 1 μ s) is long, is conducive to contact and degrade with pollutant.Studies have shown that Co2+Activate peroxy-monosulfate
System activity is high, and researcher develops a variety of cobalt compounds, though this kind of compound can efficiently activate peroxy-monosulfate,
It is generally existing Co2+The problems such as the amount of dissolution is big, poor catalyst stability, limits it and is widely applied.It would therefore be highly desirable to develop one kind
Efficiently, stable, reusable active catalyst constructs efficient permonosulphuric acid salt system.
Photocatalytic fuel cell (Photocatalytic Fuel Cell) is to pass through optical electro-chemistry under illumination condition
The solar energy of chemical energy and absorption in organic wastewater is converted into electric energy by reaction, while realizing the purpose of wastewater degradation.Liu
Shanshan etc. is with Bi2MoO6/ ITO is anode, Co3O4/ carbon cloth is that cathode constructs photocatalysis electro-chemical systems, is being added outside
Under 1.5V bias, system phenol removal rate is promoted from 6% to 100% after peroxy-monosulfate addition.(Journal of
Catalysis 355(2017)167–175Contents).But applying bias needs to consume electric energy, and photocatalytic fuel is electric
Cell system can not only be not required to additional electrical energy input, moreover it is possible to realize system electricity production output.And efficient catalytic peroxy-monosulfate is catalyzed
Agent constructs novel PFC system as electrode material, and the research that contaminant degradation efficiently produces electricity simultaneously does not have been reported that also.
Summary of the invention
The object of the present invention is to provide a kind of new catalytic peroxy-monosulfate assisted photo-catalysis fuel cell system, cathodes
To be cobalt ferrite/carbon nano-fiber/carbon fiber cloth electrode (CoF with efficient catalytic permonosulphuric acid reactant salt2O4/CNFs/
) or cobalt ferrite/carbon nano-fiber/pvdf membrane electrode (CoF CC2O4/CNFs/PVDF)；Realize catalysis peroxy-monosulfate fill-in light
Catalysis reaction generates free radicals, and promotes system contaminant degradation effect, while efficiently electricity production；Cathode is realized in automatic bias system
Co2+Circulation, so that Ion release is reduced, it is reusable.
Technical solution of the present invention:
A kind of novel (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell system, including data are adopted
Collecting system, aerating system, the circulatory system and reactor；Reactor is single chamber or dual chamber quartz reactor, and anode is photocatalysis electricity
Pole material, cathode have the membrane electrode material of crown_interception, anode for the electrode material with catalysis peroxy-monosulfate or simultaneously
Forming Fermi with cathode can be very poor；Anode is connect with cathode by external resistance, the electricity production of data collection system real-time monitoring system；
Aerating system is the aeration pump of controllable flow rate, and aeration head is placed in reactor cathode chamber；The circulatory system is when cathode couples membrane electrode
When material, cathodic coating water outlet drives circulating filtration by peristaltic pump, realizes circulation of the sewage in system.
Photochemical catalyst electrode material is silver/zinc oxide nanometer stick array/nickel foam self-supporting electrode material (AgNPs/ ZnO
NRs/NiF), the zinc-oxide nano along zinc oxide crystal layer growth is prepared using crystal layer method and hydro-thermal method on foam nickel base surface
Stick array deposits Nano silver grain in the nanometic zinc oxide rod array surface in situ photo-reduction, AgNPs/ZnO NRs/ is made
NiF。
Electrode material with catalysis peroxy-monosulfate is cobalt ferrite/carbon nano-fiber/carbon fiber cloth electrode (CoF2O4/
CNFs/CC), preparation step is as follows: by CoF2O4/ CNFs powder is dissolved in silicon sol solution or Du Pont's coating solution, CoF2O4/
The concentration of CNFs powder is 0.1-0.5mg/ml；
It is cobalt ferrite/carbon nano-fiber/PVDF carbon fiber with crown_interception and catalysis peroxy-monosulfate membrane electrode material
Cloth membrane electrode, preparation step are as follows: by CoF2O4/ CNFs powder utilizes phase inversion method, and knifing is on carbon cloth, as electricity
Pole；
The compound pvdf membrane electrode of cobalt ferrite/carbon nano-fiber is fixed by plate film assembly, and film goes out water speed by external compacted
Dynamic pump control, film water outlet are recycled to reactor and realize film circulation；
Reaction system peroxy-monosulfate (PMS) additive amount is 0.1-2mM, and cathode material is catalyzed PMS and generates sulfate radical freedom
Base, service hoisting photocatalytic fuel cell degradation effect.
There are unglazed illumination or single-sided electrode to add light, realization contaminant degradation, and system automatic bias generates electronics and promotes
Activity Co in cathode material2+Circulation in system reduces Ion release, promotes the reusing of electrode.
Beneficial effects of the present invention: the present invention using Ag NPs/ZnO NRs/NiF as photocatalysis anode, cobalt ferrite/
Carbon nano-fiber/carbon fiber cloth electrode (CoF2O4/ CNFs/CC) or cobalt ferrite/carbon nano-fiber/PVDF membrane electrode (CoF2O4/
CNFs/PVDF) novel photocatalysis fuel cell system is constructed as cathode.The system realizes automatic bias electricity production and pollutant drop
Solution, while cathode material catalysis peroxy-monosulfate generates potentiometric titrations and assists to promote fuel battery performance；Automatic bias generates
Electronics promotes active site Co in cathode material2+Circulation in system reduces Ion release, promotes the recycling of electrode
Property.
Detailed description of the invention
Fig. 1 is the present invention using Ag NPs/ZnO NRs/NiF as light anode, CoF2O4/ CNF/CC is that cathode building was catalyzed
One sulfate assisted photo-catalysis fuel cell system (outer 2000 Ω of connecting resistance) photocatalytic degradation 20mg/L berberine degradation figure
(a) and system produces electricity (b) figure, replaces anode and cathode material to construct comparison system with carbon nano-fiber cloth respectively.
Fig. 2 is the present invention using Ag NPs/ZnO NRs/NiF as light anode, CoF2O4/ CNF/PVDF film is that cathode building is urged
Change the degradation of peroxy-monosulfate assisted photo-catalysis fuel cell system (outer 2000 Ω of connecting resistance) photocatalytic degradation 20mg/L berberine
Scheme (a) and system produces electricity (b) figure.
Specific embodiment
Below in conjunction with attached drawing and technical solution, a specific embodiment of the invention is further illustrated.
Embodiment 1
Ag NPs/ZnO NRs/NiF is light anode, CoF2O4/ CNF/CC is cathode building catalysis peroxy-monosulfate auxiliary
Photocatalytic fuel cell system degradation berberine:
Ag NPs/ZnO NRs/NiF is light anode, CoF2O4/ CNF/CC is cathode, and saturated calomel electrode is reference electrode
It is connected by conducting wire, external 2000 Ω resistance, cathode bottom aeration.Reaction system is 10 mg/L berberine solution of 100ml, nothing
Half an hour is adsorbed before needing additional electrolyte, reaction to start, it is rear to open the irradiation of 300W xenon lamp while adding 0.05mM PMS, it reacts
40min.Spectrophotometer is utilized to test absorbance at once at interval of 5min sampling 2.5ml.The absorption of reaction and stage of reaction electricity
Data collector whole process is pressed to collect voltage data.
System degradation comparative experimental data is shown in Fig. 1 (a), it can be seen that the degradation of illumination 40min system under 300W xenon lamp
Rate reaches 91%, and under additional 2000 Ω resistance, the cell voltage potential of system is about 0.50V；Respectively in contrast to Ag NPs/ZnO
NRs/NiF is light anode and the carbon-cloth cathode without catalyst, carbon cloth anode and CoF2O4/ CNF/CC is cathode, Ag
NPs/ZnO NRs/NiF is light anode, CoF2O4/ CNF/CC is that cathode building fuel cell system performance is best.
Embodiment 2
Ag NPs/ZnO NRs/NiF is light anode, CoF2O4/ CNF/PVDF film is cathode building catalysis peroxy-monosulfate
Assisted photo-catalysis fuel cell system degradation berberine:
Ag NPs/ZnO NRs/NiF is light anode, CoF2O4/ CNF/PVDF film is cathode, and saturated calomel electrode is reference
Electrode is connected by conducting wire, external 2000 Ω resistance, cathode bottom aeration.Reaction system is that 500ml 10mg/L berberine is molten
Liquid is not necessarily to additional electrolyte, and half an hour is adsorbed in reaction before starting, rear to open the irradiation of 300W xenon lamp while adding 0.05mM PMS,
React 60min；Connect peristaltic pump outside cathodic coating and accelerates circulating system berberine liquid, it is sharp at once at interval of 10min sampling 2.5ml
Absorbance is tested with spectrophotometer.The absorption of reaction and stage of reaction voltage data collector whole process collect voltage data.Figure
2 (a) be degradation experiment figure, and system can reach 86% in 60min degradation rate, and system potential under 2000 Ω extrernal resistances is about
0.7V。
Claims (10)
1. a kind of novel (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell system, which is characterized in that institute
Novel (film) the electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell system stated includes data collection system, aeration
System, the circulatory system and reactor；Reactor is single chamber or dual chamber quartz reactor, and anode is photochemical catalyst electrode material, cathode
There is the membrane electrode material of crown_interception for the electrode material with catalysis peroxy-monosulfate or simultaneously, anode and cathode formation take
Rice can be very poor；Anode is connect with cathode by external resistance, the electricity production of data collection system real-time monitoring system；Aerating system is controllable
The aeration pump of flow velocity, aeration head are placed in reactor cathode chamber；The circulatory system is when cathode coupled film electrode material, and cathodic coating goes out
Water drives circulating filtration by peristaltic pump, realizes circulation of the sewage in system.
2. novel (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell system according to claim 1
System, which is characterized in that the photochemical catalyst electrode material is silver/zinc oxide nanometer stick array/nickel foam self-supporting electrode material,
The nanometic zinc oxide rod array along zinc oxide crystal layer growth is prepared using crystal layer method and hydro-thermal method on foam nickel base surface, in institute
Nanometic zinc oxide rod array surface in situ photo-reduction deposition Nano silver grain is stated, AgNPs/ZnO NRs/NiF is made.
3. novel (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell according to claim 1 or 2
System, which is characterized in that the electrode material with catalysis peroxy-monosulfate is cobalt ferrite/carbon nano-fiber/carbon fiber cloth electrode,
Preparation step is as follows: by CoF2O4/ CNFs powder is dissolved in silicon sol solution or Du Pont's coating solution, CoF2O4/ CNFs powder it is dense
Degree is 0.1-0.5mg/ml.
4. novel (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell according to claim 1 or 2
System, which is characterized in that have crown_interception and catalysis peroxy-monosulfate membrane electrode material be cobalt ferrite/carbon nano-fiber/
PVDF carbon cloth membrane electrode, preparation step are as follows: by CoF2O4/ CNFs powder utilizes phase inversion method, and knifing is in carbon cloth
On, as electrode.
5. novel (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell system according to claim 3
System, which is characterized in that having crown_interception and catalysis peroxy-monosulfate membrane electrode material is cobalt ferrite/carbon nano-fiber/PVDF
Carbon cloth membrane electrode, preparation step are as follows: by CoF2O4/ CNFs powder utilizes phase inversion method, and knifing is made on carbon cloth
For electrode.
6. novel (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell system according to claim 4
System, which is characterized in that cobalt ferrite/carbon nano-fiber/PVDF carbon cloth membrane electrode is fixed by plate film assembly, and film goes out water speed
Degree is controlled by external peristaltic pump, and film water outlet is recycled to reactor and realizes film circulation.
7. novel (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell system according to claim 5
System, which is characterized in that cobalt ferrite/carbon nano-fiber/PVDF carbon cloth membrane electrode is fixed by plate film assembly, and film goes out water speed
Degree is controlled by external peristaltic pump, and film water outlet is recycled to reactor and realizes film circulation.
8. according to claim 1, (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalysis combustion novel described in 2,5,6 or 7
Expect battery system, which is characterized in that reaction system peroxy-monosulfate additive amount is 0.1-2mM, and cathode material is catalyzed PMS and generates sulphur
Acid group free radical, service hoisting photocatalytic fuel cell degradation effect；
There are unglazed illumination or single-sided electrode to add light, realization contaminant degradation, and system automatic bias generates electronics and promotes cathode
Activity Co in material2+Circulation in system reduces Ion release, promotes the reusing of electrode.
9. novel (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell system according to claim 3
System, which is characterized in that reaction system peroxy-monosulfate additive amount is 0.1-2mM, and cathode material is catalyzed PMS and generates sulfate radical freedom
Base, service hoisting photocatalytic fuel cell degradation effect；There are unglazed illumination or single-sided electrode to add light, realization pollutant drop
Solution, and system automatic bias generates electronics and promotes activity Co in cathode material2+Circulation in system reduces Ion release, is promoted
The reusing of electrode.
10. novel (film) electrode catalyst peroxy-monosulfate auxiliary building photocatalytic fuel cell system according to claim 4
System, which is characterized in that reaction system peroxy-monosulfate additive amount is 0.1-2mM, and cathode material is catalyzed PMS and generates sulfate radical freedom
Base, service hoisting photocatalytic fuel cell degradation effect；There are unglazed illumination or single-sided electrode to add light, realization pollutant drop
Solution, and system automatic bias generates electronics and promotes activity Co in cathode material2+Circulation in system reduces Ion release, is promoted
The reusing of electrode.
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| CN109772369A (en) * | 2019-02-27 | 2019-05-21 | 黑龙江大学 | A kind of preparation method of bismuth molybdate/bismuth sulfide/molybdenum disulfide ternary photoelectrocatalysithin thin film material electrodes |
| CN110627186A (en) * | 2019-08-20 | 2019-12-31 | 重庆大学 | Wastewater treatment method for generating singlet oxygen by catalyzing persulfate through modified cobalt oxide |
| CN110756163A (en) * | 2019-10-31 | 2020-02-07 | 上海师范大学 | Nano CoFe2O4Carbon fiber felt composite material and preparation method and application thereof |
| CN111509336A (en) * | 2020-03-18 | 2020-08-07 | 清华大学 | Selective catalytic oxidation synchronous electricity generation photoelectric fuel cell system and application thereof |
| CN112546882A (en) * | 2020-11-18 | 2021-03-26 | 中国科学院生态环境研究中心 | Polypyrrole conductive film and preparation method and application thereof |
| CN113003668A (en) * | 2021-02-02 | 2021-06-22 | 同济大学 | Method for synchronously removing PPCPs (pentatricopeptide repeats) by inactivating urine by using singlet oxygen generated in situ by three-dimensional electrochemical reactor |
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| CN109772369A (en) * | 2019-02-27 | 2019-05-21 | 黑龙江大学 | A kind of preparation method of bismuth molybdate/bismuth sulfide/molybdenum disulfide ternary photoelectrocatalysithin thin film material electrodes |
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| CN110756163A (en) * | 2019-10-31 | 2020-02-07 | 上海师范大学 | Nano CoFe2O4Carbon fiber felt composite material and preparation method and application thereof |
| CN111509336A (en) * | 2020-03-18 | 2020-08-07 | 清华大学 | Selective catalytic oxidation synchronous electricity generation photoelectric fuel cell system and application thereof |
| CN112546882A (en) * | 2020-11-18 | 2021-03-26 | 中国科学院生态环境研究中心 | Polypyrrole conductive film and preparation method and application thereof |
| CN113003668A (en) * | 2021-02-02 | 2021-06-22 | 同济大学 | Method for synchronously removing PPCPs (pentatricopeptide repeats) by inactivating urine by using singlet oxygen generated in situ by three-dimensional electrochemical reactor |
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| CN109286026B (en) | 2022-01-04 |
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