CN104617323B - Non-photocatalytic and photocatalytic fuel cell system capable of generating power and degrading pollutants - Google Patents
Non-photocatalytic and photocatalytic fuel cell system capable of generating power and degrading pollutants Download PDFInfo
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- CN104617323B CN104617323B CN201510041639.9A CN201510041639A CN104617323B CN 104617323 B CN104617323 B CN 104617323B CN 201510041639 A CN201510041639 A CN 201510041639A CN 104617323 B CN104617323 B CN 104617323B
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- photocatalytic
- anode
- fuel cell
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- illumination
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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
- H01M8/08—Fuel cells with aqueous electrolytes
-
- 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
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
-
- 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
- C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
-
- 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
-
- 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
- H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
-
- 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
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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
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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
- 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
-
- 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
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
Abstract
The invention discloses a non-photocatalytic and photocatalytic fuel cell system capable of generating power and degrading pollutants, and belongs to the technical field of wastewater treatment and energy recycling. The non-photocatalytic and photocatalytic fuel cell system is characterized in that without and with additional illumination, non-photocatalytic and photocatalytic effects are applied, an anode is coupled to an electrocatalytic cathode, organic wastewater is treated, and electric energy is generated at the same time; without illumination, an anode catalyst reacts with H2O or OH＜-＞ adsorbed onto the surface of the anode catalyst to generate .OH, .OH reacts with oxygen to generate .O2＜-＞, and .OH and .O2＜-＞ are strong oxidants and degrade organic pollutants in the water; carbon fiber cloth is loaded with TiO2/g-C3N4 to serve as the anode, and a platinum nanowire grows in situ to serve as the electrocatalytic cathode; when NaOH is added into an anode chamber and H2SO4 is added into the cathode chamber, the RhB (rhodamine b) removal rate and the electricity production yield are increased. The non-photocatalytic and photocatalytic fuel cell system has the benefits that the same catalyst system has the non-photocatalytic and photocatalytic effects and forms the fuel cell system, electric energy output is realized while organic dye wastewater is efficiently treated, a purpose of energy recycling is achieved, and the illumination is not required.
Description
Technical field
The invention belongs to environmental conservation and pollution control technology field, it is related under conditions of having light and no light, application
No photocatalytic cell system and photocatalysis coupled battery system, produces electricity while processing Recalcitrant chemicals and organic wastewater
Can, and in closure battery system, contaminant degradation rate is higher.
Background technology
Water is Source of life, and water resource is one of irreplaceable natural resourcess, and water pollution increasingly increases short with water resource
Lack, be that global primary environment administers a difficult problem.Artificial-strengthening water purification and process need to consume the energy, and remove difficult degradation
The classical advanced oxidation processes of pollutant, ton water process energy consumption cost is higher, is the restraining factors of water environment protection.The energy is the mankind
Life and the material base of development, increase with population, world energy supplies growing tension.The energy and exploitation is extracted from waste
Using new forms of energy, it has also become the focus of countries in the world research.Need exploitation both can curb environmental pollution, with energy-conservation and can return again
Receive the New Wastewater Treatment Technique of the energy.
Photocatalytic fuel cell is a kind of new photoelectrocatalysiss coupled system, using organic in photocatalysis Decomposition sewage
Thing purify waste water, produce electric energy, solves the problems, such as simultaneously hole and electronics between be combined.Because its have efficient, pollution-free etc.
Advantage and be widely studied.When having the light irradiation more than photocatalyst forbidden energy gap energy, the electrons in valence band transit to
On conduction band, thus forming hole/electronics pair, electronics is excited to form superoxide radical with oxygen, and produced hole h+With suction
It is attached to the h of photocatalyst surface2O or oh-Reaction generates oh, and oh is strong oxidizer, the organic contamination in oxidative degradation water
Thing；The hole producing also has strong oxidizing property, being capable of direct oxidation Organic substance in water [kang i c, zhang qiwu, yin
Shu, et al.improvement in photocatalytic activity of tio2under visible
irradiation through addition of n-tio2[j] .environmental science＆technology,
2008,42 (10): 3622-3626.].Illumination as the important component part of photocatalytic fuel cell, increased operating cost with
Energy consumption.Therefore, whether research illumination has and has very important significance；Looked in research report, all photocatalytic pollutant degradation are equal
Carry out under ultraviolet or visible light conditions, not to photocatalyst system system, whether produce under dark condition oh and
Produce electric energy studied, and whether this product electric system is improve process pollutant efficiency study.
Content of the invention
It is an object of the invention to provide one kind equal degrading organic pollutant produce electricity under having illumination and non-illuminated conditions
Photocatalytic fuel cell system, solve the problems, such as traditional photocatalysis must illumination, and photocatalytic cell system, no light
Do not produce the problem of electricity.
The technical scheme is that
1. reactor design configuration: reactor is divided into anode chamber and cathode chamber, two indoor setting draw-in grooves, and two electrodes are put respectively
Enter wherein, two Room bottoms are respectively provided with aeration head, cation exchange membrane is sandwiched in the middle of two Room, by two Room solution separately, simultaneously facilitate
Proton transfer, accelerates polarization response speed；
2. anode catalyst load: carbon cloth uses soaked in absolute ethyl alcohol post-drying standby, butyl titanate and ethanol
Mixing, adds hydrochloric acid and deionized water under conditions of magnetic agitation, adds g-c3n4, it is in faint yellow for stirring to solution；
Immersion carbon cloth, dries, and repeatedly soaks after drying, by above carbon cloth high-temperature calcination；
3. cathod catalyst: making growth in situ pt nanowire cathodes method is as follows, ethanol immersion carbon fiber 24h, 60 DEG C
Dry for standby, by 17mg h2ptcl6·6h2O and 0.53ml formic acid, add in the glass dish containing 10.6ml ultra-pure water, immersion
Carbon cloth (catalyst loadings 0.4mg cm-2), 40 DEG C, 16h, become colorless to solution, 40 DEG C, 6h is dried；
4. anode indoor liquid is 10mg l-1rhb,0.5mol·l-1na2so4,0.5mol·l-1naoh 350ml；
5. negative electrode indoor liquid is 10mg l-1rhb,0.5mol·l-1na2so4,0.5mol·l-1h2so4250ml；
6. photocatalytic fuel cell system: anode, negative electrode are described in 2,3, when having more than anode photocatalyst forbidden band
During the light irradiation of band-gap energy, the electron transition in valence band is to conduction band, thus forming hole/electronics pair, produced h+With absorption
H in semiconductor surface2O or oh-Reaction generates oh, with o2Reaction generates o2 -, oh and o2 -For strong oxidizer, aoxidize
Organic pollution in degradation water；The hole producing also has strong oxidizing property, being capable of direct oxidation Organic substance in water；Anode light is urged
Change to produce electronics and directly pass through external circuit and conduct to negative electrode, produce reduce while electric energy hole and electronics between be combined,
Improve photocatalytic degradation efficiency；
7. non-photocatalytic fuel cell system: need not be under additional illumination condition, reactor be placed in dark light tight casing
In, loaded optic catalyst anode tio2/g-c3n4React generation oh with water and naoh, generate o with oxygen reaction2 -, oxidation fall
The organic pollution of Xie Shuizhong produces electronics；Electronics reaches negative electrode by external circuit, with negative electrode interior oxygen reaction, promotes photoproduction
Electronics is separated with hole, increases organic removal rate and produces electric energy；
The invention has the advantages that need not be under conditions of additional illumination and power supply, using photocatalytic fuel cell system
System degraded persistent organic pollutants purify waste water, produce electric energy simultaneously, reach the target of energy recovery utilization, and supported catalyst
Agent negative electrode is simple with the manufacture method of anode.
Brief description
Accompanying drawing 1 is in not illumination, the potential energy diagram having under soda acid existence condition.
In figure: abscissa express time, unit min, vertical coordinate represents voltage, unit v；Square, round dot, triangle divide
Do not represent anode potential, cathode potential, cell voltage；Anode adds naoh, provides oh-, negative electrode addition sulphuric acid, accelerate negative electrode and disappear
Consumption electron velocity.
Accompanying drawing 2 is the potential energy diagram no under the conditions of soda acid.
In figure: abscissa express time, unit min, vertical coordinate represents cell voltage, unit v；Initial reaction stage anode and cathode is equal
Aeration, anode 20w UV illumination, it is stable that cell voltage gradually rises up to 0.375v；After 120min, anode stops aeration stopping
Illumination, negative electrode stops aeration.
Accompanying drawing 3 is potential energy diagram not under aeration condition for the not illumination.
In figure: abscissa express time, unit min, vertical coordinate represents cell voltage, unit v；In whole course of reaction,
Anode not aeration, not illumination, negative electrode not aeration.
Accompanying drawing 4 is 20mg l-1Potential energy diagram under the conditions of rhb, no soda acid.
Fig. 4 abscissa express time, unit min, vertical coordinate represents voltage, unit v；Three curves generation respectively from top to bottom
Table cathode potential, cell voltage, anode potential；The equal aeration of initial reaction stage anode and cathode, anode 20w UV illumination, cell voltage
Gradually rise up to 0.30v to tend towards stability；After 120min, anode stops aeration, stops illumination, and negative electrode stops aeration.
Specific embodiment
Describe the specific embodiment of the present invention below in conjunction with technical scheme and accompanying drawing in detail.
Embodiment 1
Anode makes: 27ml butyl titanate is mixed with 23ml ethanol, magnetic agitation 10min；Add 3.3ml hcl,
2.7ml deionized water；Add appropriate g-c3n4, stir, immerse 20*5cm2Carbon cloth, 105 DEG C of drying, repeatedly after 5 times,
5℃·min-1, 450 DEG C, calcine 2h.
Negative electrode is growth in situ pt nano wire carbon cloth, and the two poles of the earth are connected with data collecting card respectively, record anode potential
With cell voltage potential, anode indoor liquid is 10mg l-1rhb,0.5mol·l-1na2so4,0.5mol·l-1naoh 350ml；Cloudy
Pole indoor liquid is 10mg l-1rhb,0.5mol·l-1na2so4,0.5mol·l-1h2so4250ml；Negative and positive are put in the middle of the two poles of the earth
Put cation exchange membrane, anode without illumination, two indoor all aerations, cell voltage potential is slowly declined by 0.65v, is stable at 0.5v,
As shown in figure；Yin, yang the two poles of the earth interior clearance is respectively 88%, 14.49%.
Embodiment 2
Use same cathode and anode with example one, negative electrode indoor liquid is 350ml, 10mg l-1Rhb, positive the two poles of the earth are indoor
Liquid is 250ml, 10mg l-1rhb；Equal aeration in two Room courses of reaction, Anode Ultraviolet light shines (cell voltage potential 0.375v)
After 2h, stop illumination and aeration, though reactor cell potential decreases, while degraded rhb, still produce electricity
(0.31v), as figure two；In positive and negative pole room, rhb clearance is respectively 72% and 16%.
Embodiment 3
Use same cathode and anode with example one, negative and positive the two poles of the earth indoor liquid is identical with example 2, in two Room courses of reaction
Not illumination, not aeration, reactor cell potential maintains 0.212v, such as figure three；In positive and negative pole room, rhb clearance is respectively
65% and 12%
Embodiment 4
The same cathode and anode with example one, negative electrode indoor liquid is 350ml, 20mg l-1Rhb, positive the two poles of the earth indoor liquid
It is 250ml, 20mg l-1rhb；Equal aeration in two Room courses of reaction, after Anode Ultraviolet light shines (cell voltage potential 0.30v) 2h,
Stop illumination and aeration, though reactor cell potential decreases, while degraded rhb, still produce electricity (0.20v), such as
Figure four；Negative and positive the two poles of the earth initial soln electrical conductivity is 501 μ s cm-1, in course of reaction, two Room electrical conductivity all decline；Yin, yang pole room
Interior rhb clearance is respectively 76.7% and 7.4%.
Claims (2)
1. the non-photocatalysis of a kind of product electricity and degradation of contaminant and photocatalytic fuel cell system, in the condition of no additional illumination
Under, no photocatalysiss and issue third contact of a total solar or lunar eclipse catalytic action in illumination condition in anode, and electro-catalysis cathode combination there are, unglazed
Or have under optical condition all can process organic wastewater and produce electric energy it is characterised in that
a)tio2/g-c3n4Catalyst is carried on carbon cloth by sol-gel method is used as anode, on carbon cloth in situ
As electro-catalysis negative electrode, anode is connected the Pt nanowires of growth with negative electrode, is respectively placed in two indoor；
B) anode, under without illumination condition, is carried on the photocatalyst on carbon cloth and the h adsorbing on its surface2O or oh-
Reaction generates oh, generates o with oxygen reaction2 -, oh and o2 -For strong oxidizer, the organic contamination in oxidative degradation water
Thing；When unglazed, jointed anode and negative electrode also produce electric current, degradation of contaminant；
Under having illumination condition, anode photocatalysis are produced electronics and are directly conducted to negative electrode by external circuit, while producing electric energy
Reduce hole and electronics between compound.
2. the non-photocatalysis of a kind of product electricity according to claim 1 and degradation of contaminant and photocatalytic fuel cell system,
In double-chamber fuel cell system, anode interior addition 0.5mol l-1Naoh, negative electrode interior addition 0.5mol l-1h2so4.
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| CN105110554B (en) * | 2015-08-17 | 2017-12-22 | 大连理工大学 | One kind coupling（Light）The system that nitrate nitrogen in water removal is removed in catalysis with MFC |
| CN106082420B (en) * | 2016-06-15 | 2018-11-09 | 大连理工大学 | A kind of automatic bias pollution control system of electricity-producing microorganism anode auxiliary hetero-junctions anode |
| CN106340661A (en) * | 2016-09-26 | 2017-01-18 | 大连理工大学 | Fuel cell system of ternary heterojunction photoelectrocatalysis membrane |
| CN106486687B (en) * | 2016-11-21 | 2019-03-19 | 重庆大学 | Photocatalysis produces hydrogen peroxide and photocatalytic fuel cell coupled system |
| CN106823789B (en) * | 2017-03-14 | 2019-08-09 | 大连理工大学 | Photoelectric coupling promotes vapor phase contaminants decomposing, purifying method |
| CN107081333B (en) * | 2017-05-18 | 2020-09-25 | 大连理工大学 | Water body sandy soil restoration method of photocatalytic fuel cell |
| CN111217424A (en) * | 2020-02-25 | 2020-06-02 | 上海海洋大学 | Desalination system for removing polycyclic aromatic hydrocarbons in seawater |
| 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 |
| CN112086672B (en) * | 2020-09-15 | 2021-12-07 | 中国科学院大连化学物理研究所 | Composite high-temperature proton exchange membrane for fuel cell and preparation method and application thereof |
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| ITPD20060141A1 (en) * | 2006-04-18 | 2007-10-19 | Univ Padova | ELECTROCATALIZERS BASED ON CARBO-NITRURI MONO / PLURI-METALLICI FOR POLYMERIC FUEL CELLS, PEFC AND DMFC TYPE AND FOR H2 ELECTRIC GENERATORS |
| CN103771565B (en) * | 2014-01-02 | 2015-05-20 | 浙江工商大学 | Preparation method of composite electrode of carbon nitride/titanium dioxide nanotube |
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