CN105749717A - Preparation method of gas diffusion electrode for electrochemical treatment of SO2 - Google Patents
Preparation method of gas diffusion electrode for electrochemical treatment of SO2 Download PDFInfo
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- CN105749717A CN105749717A CN201610153587.9A CN201610153587A CN105749717A CN 105749717 A CN105749717 A CN 105749717A CN 201610153587 A CN201610153587 A CN 201610153587A CN 105749717 A CN105749717 A CN 105749717A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/77—Liquid phase processes
- B01D53/78—Liquid phase processes with gas-liquid contact
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/48—Sulfur compounds
- B01D53/50—Sulfur oxides
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2259/00—Type of treatment
- B01D2259/12—Methods and means for introducing reactants
Abstract
A preparation method of a gas diffusion electrode for electrochemical treatment of SO2 comprises steps as follows: 1) powdery conductive carbon black is added to absolute ethyl alcohol until the carbon black is completely immersed, a polytetrafluoroethylene emulsion is added, the mixture is subjected to water bath treatment and stirred until clustered substances are formed, the clustered substances are rolled to form a film, and a diffusion layer film is obtained; 2) a stainless steel net current collector is covered with the diffusion layer film, rolling forming is performed, and the film is taken out for standby use after being calcined in a muffle furnace; 3) the powdery carbon black and a little quantity of carbon nanotubes are rolled to form a film with a method in the step 1), and a catalyst layer film is obtained; 4) the other side of the stainless steel net current collector is covered with the catalyst layer film, rolling forming is performed, and a target object is prepared. The preparation method has the advantages as follows: SO2 diffusion mass transfer is reinforced by increasing gas transferring pore channels of the electrode; a process is simple, the cost of raw materials is low, the mechanical strength of the prepared gas diffusion electrode is high, the reusability is good, the SO2 conversion efficiency is high, and the gas diffusion electrode is suitable for engineering application of electrochemical treatment of SO2.
Description
Technical field
The present invention relates to applied chemistry-energy-conserving and emission-cutting technology field, particularly a kind of electrochemical treatments SO2The preparation method of gas-diffusion electrode.
Technical background
Quite a few city of China in winter spring recent years frequently occurs haze weather, SO2It it is one of main matter forming haze.China is to SO2The control indexes of discharge is increasingly strict, the flue gas desulfurization technique of commercial Application (as wet method, dry method semidry method etc.) to discharge polluter that exhaust gas volumn is little, concentration change is big such as small-sized thermal power plant and chemical plant, there is application cost height, the problem such as fluctuation of service.The method of electrochemical control gas pollutant receives the concern of people in recent years due to its many-sided superperformance, and wherein electrochemical method processes SO2It is by SO using electronics as clean inorganic agent2It is converted into the product such as sulphuric acid, sodium bisulfate.
Existing electrochemical treatments technology is mainly by SO2First pass in electrolyte, then apply external electrical field and be oxidized.This belongs to vapor-liquid two phases interfacial reaction, limited mass transfer rate and higher energy consumption in principle and seriously inhibits the efficiency of electrochemical oxidation;The method is to SO2Concentration also there are certain requirements, it is impossible to meet the process requirement of the various low concentration sulfur-containing smoke gas of industrial complicated component, fettered electrochemical treatments SO2Further development and commercial Application.
Summary of the invention
Present invention is generally directed to above-mentioned existing problems, it is provided that a kind of electrochemical treatments SO2The preparation method of gas-diffusion electrode, by increasing the gas transmission duct strengthening SO of electrode2And O2Diffusion mass transfer.O2It is reduced to H by gas-diffusion electrode catalysis under the effect of electricity2O2, the H of generation2O2With can by SO2It is oxidized to H2SO4, the method technique is simple, cost of material is low, and the gas-diffusion electrode mechanical strength prepared is high, and reusability is good, SO2Transformation efficiency high, it is adaptable to SO2The through engineering approaches application of electrochemical treatments.
Technical scheme:
A kind of electrochemical treatments SO2The preparation method of gas-diffusion electrode, step is as follows:
1) powdered conductive white carbon black is added dehydrated alcohol to being totally submerged and being uniformly dispersed, at room temperature it is added dropwise over politef (PTFE) emulsion after ultrasonic agitation 20min, continue ultrasonic agitation 20min, the mixed liquor obtained through 80 DEG C of water-baths and is stirred its roll-in film forming to one-tenth dough, is diffusion tunic;
2) by step 1) gained diffusion tunic covers on stainless (steel) wire collector, and cut into the circle of diameter 6cm after roll-forming, put in Muffle furnace at 340 DEG C, to calcine 20-30min, take out stand-by.
3) Powdered white carbon black and a small amount of multi-walled carbon nano-tubes are added dehydrated alcohol to being totally submerged and being uniformly dispersed, at room temperature it is added dropwise over politef (PTFE) emulsion after ultrasonic agitation 20min, continue ultrasonic agitation 20min, the mixed liquor obtained through 80 DEG C of water-baths and is stirred its roll-in film forming to one-tenth dough, is catalysis tunic;
4) again by step 3) gained catalysis tunic covers step 2) on the another side of gained stainless (steel) wire collector, roll-forming deducts corner excess stock and can be prepared by the circular gas diffusion electrode of diameter 6cm.
Described stainless (steel) wire collector is 60 orders, and thickness is 0.5mm.
Described diffusion layer film thickness is 0.5mm-1mm;Described Catalytic Layer film thickness is 0.5mm-1mm.
Described step 4) in after roll-forming the thickness of gained circular gas diffusion electrode be 0.8mm-1mm.
The mass percent concentration of described PTFE emulsion is 60%;Step 1) in the mass ratio of PTFE emulsion and conductive black be 5:2, step 3) in PTFE emulsion, white carbon black and CNT mass ratio be 5:19:1.
Advantages of the present invention and beneficial effect:
The preparation method of this gas-diffusion electrode, by changing SO2Transmission path in electrochemical reaction and mode, strengthen SO2Diffusion mass transfer, SO2Transformation efficiency, close to 100%, processes 1kgSO2Only power consumption 1.70kW h;Preparation method technique is simple, cost of material is low for this;The gas-diffusion electrode mechanical strength prepared is high, and reusability is good;SO2Transformation efficiency high, consume energy low, non-secondary pollution, be suitable to SO2The through engineering approaches application of electrochemical treatments.
Accompanying drawing explanation
Fig. 1 is that gas-diffusion electrode (CB-CNT-GDE) prepared by the present invention processes SO2Principle schematic.
Fig. 2 is the electrochemical treatments SO of the gas-diffusion electrode (CB-CNT-GDE) prepared of the present invention and common graphite electrode2Efficiency and energy consumption comparison figure.
Fig. 3 is the present invention gas-diffusion electrode (CB-CNT-GDE) prepared and the electrochemical treatments SO being added without the gas-diffusion electrode (CB-GDE) of CNT, the extra gas-diffusion electrode (CB-CNT-AC-GDE) adding activated carbon2Efficiency and energy consumption comparison figure.
Detailed description of the invention
Embodiment 1:
A kind of electrochemical treatments SO2The preparation method of gas-diffusion electrode, step is as follows:
1) 2.0g powdered conductive white carbon black is added 60mL dehydrated alcohol to being totally submerged and being uniformly dispersed, at room temperature it is added dropwise over the ptfe emulsion (density is about 1.45g/mL) that 5g mass fraction is 60% after ultrasonic agitation 20min, continue ultrasonic agitation 20min, the mixed liquor obtained through 80 DEG C of water-baths and is stirred its roll-in film forming to one-tenth dough, obtains diffusion tunic;
2) by step 1) gained diffusion tunic covers on the stainless (steel) wire collector of 60 orders, and cut into the circle of diameter 6cm after roll-forming, put in Muffle furnace 340 DEG C of calcining 20min, take out stand-by.
3) Powdered for 1.9g white carbon black and 0.1g multi-walled carbon nano-tubes are added 60mL dehydrated alcohol to being totally submerged and being uniformly dispersed, at room temperature it is added dropwise over politef (PTFE) emulsion that 0.5g mass fraction is 60% after ultrasonic agitation 20min, continue ultrasonic agitation 20min, the mixed liquor obtained through 80 DEG C of water-baths and is stirred its roll-in film forming to one-tenth dough, is catalysis tunic;
4) again by step 3) gained catalysis tunic covers step 2) on the another side of gained stainless (steel) wire collector, roll-forming deducts corner excess stock and can be prepared by the circular gas diffusion electrode of diameter 6cm.
To SO2Carrying out electrochemical treatments, as shown in Figure 1, wherein negative electrode is the gas-diffusion electrode of the preparation of the present invention to its principle, and anode is platinum electrode (diameter 1mm);Electrolyte: 50mMNa2SO4;Faradaic current: 0.1A is constant;Reaction temperature: 25 DEG C;SO2Flow: 10mL/min, O2Flow: 90mL/min;Response time 180min.Fig. 2 gives the electrochemical treatments SO of gas-diffusion electrode (CB-CNT-GDE) prepared by the present invention and common graphite electrode2Efficiency and energy consumption comparison figure, as shown in Figure 2, use CB-CNT-GDE electrode SO2Transformation efficiency (98%) and the SO of use common graphite electrode in documents and materials2The highest transformation efficiency (96.6%) is suitable, but processes 1kgSO2The energy (1.70kW h) consumed have dropped 33.6% than use common graphite electrode (2.56kW h).This is owing to the use of gas-diffusion electrode changes SO2And O2Transmission path and mode, enhance SO2Gas transmits to the diffusion in solution.
Embodiment 2:
A kind of electrochemical treatments SO2The preparation method of gas-diffusion electrode, step is as follows:
1) 2.0g powdered conductive white carbon black is added 60mL dehydrated alcohol to being totally submerged and being uniformly dispersed, at room temperature it is added dropwise over the ptfe emulsion (density is about 1.45g/mL) that 5g mass fraction is 60% after ultrasonic agitation 20min, continue ultrasonic agitation 20min, the mixed liquor obtained through 80 DEG C of water-baths and is stirred its roll-in film forming to one-tenth dough, obtains diffusion tunic;
2) by step 1) gained diffusion tunic covers on the stainless (steel) wire collector of 60 orders, and cut into the circle of diameter 6cm after roll-forming, put in Muffle furnace 340 DEG C of calcining 20min, take out stand-by.
3) Powdered for 1.9g white carbon black and 0.1g multi-walled carbon nano-tubes are added 60mL dehydrated alcohol to being totally submerged and being uniformly dispersed, at room temperature it is added dropwise over politef (PTFE) emulsion that 0.5g mass fraction is 60% after ultrasonic agitation 20min, continue ultrasonic agitation 20min, the mixed liquor obtained through 80 DEG C of water-baths and is stirred its roll-in film forming to one-tenth dough, is catalysis tunic CB-CNT;With same method, Powdered for 2.0g white carbon black is made catalytic membrane CB again, Powdered for 1.61g white carbon black, 0.1g multi-walled carbon nano-tubes and 0.29g powdered active carbon are made catalytic membrane CB-CNT-AC.
4) by step 3) three kinds of catalysis tunics of gained are respectively overlay in three steps 2) on the another side of gained stainless (steel) wire collector, roll-forming deducts corner excess stock and can be prepared by the circular gas diffusion electrode (CB-CNT-GDE, CB-GDE and CB-CNT-AC-GDE) of three diameter 6cm.
To SO2Carrying out electrochemical treatments, as shown in Figure 1, wherein negative electrode is three kinds of gas-diffusion electrodes to its principle, and anode is platinum electrode (diameter 1mm);Electrolyte: 50mMNa2SO4;Faradaic current: 0.1A is constant;Reaction temperature: 25 DEG C;SO2Flow: 10mL/min, O2Flow: 90mL/min;Response time 180min.Fig. 3 gives the present invention gas-diffusion electrode (CB-CNT-GDE) prepared and the electrochemical treatments SO being added without the gas-diffusion electrode (CB-GDE) of CNT, the extra gas-diffusion electrode (CB-CNT-AC-GDE) adding activated carbon2Efficiency and energy consumption comparison figure, from the figure 3, it may be seen that use CB-CNT-GDE electrode SO2Transformation efficiency (98%), higher than CB-GDE electrode (89.11%) and CB-CNT-GDE electrode (77.18%), processes 1kgSO2The energy (1.70kW h) consumed have dropped 13.3% and 27.0% respectively than use CB-GDE electrode (1.96kW h) and CB-CNT-GDE electrode (2.33kW h).This is owing to the addition of CNT enhances chemical property and the loose structure of gas-diffusion electrode, and the addition of activated carbon inhibits this change.
In various embodiments above, gained diffusion layer film thickness is 0.5mm-1mm;Gained Catalytic Layer film thickness is 0.5mm-1mm;Stainless (steel) wire collector thickness is 0.5mm.Due to diffusion tunic and catalysis tunic roll-in are needed certain pressure to time on stainless (steel) wire, the diffusion tunic and the Catalytic Layer film thickness that are finally compressed on stainless (steel) wire collector two ends are compressed so that in step 4) in after roll-forming gained circular gas diffusion electrode integral thickness be 0.8mm-1mm.
It should be noted that; the above-mentioned description to embodiment is to be understood that for ease of those skilled in the art and apply the present invention; therefore; the invention is not restricted to embodiment here; those skilled in the art's announcement according to the present invention, the improvement made for the present invention and modification all should within protection scope of the present invention.
Claims (5)
1. an electrochemical treatments SO2The preparation method of gas-diffusion electrode, it is characterised in that step is as follows:
1) powdered conductive white carbon black is added dehydrated alcohol to being totally submerged and being uniformly dispersed, at room temperature it is added dropwise over politef (PTFE) emulsion after ultrasonic agitation 20min, continue ultrasonic agitation 20min, the mixed liquor obtained through 80 DEG C of water-baths and is stirred its roll-in film forming to one-tenth dough, is diffusion tunic;
2) by step 1) gained diffusion tunic covers on stainless (steel) wire collector, and cut into the circle of diameter 6cm after roll-forming, put in Muffle furnace at 340 DEG C, to calcine 20-30min, take out stand-by.
3) Powdered white carbon black and a small amount of multi-walled carbon nano-tubes are added dehydrated alcohol to being totally submerged and being uniformly dispersed, at room temperature it is added dropwise over politef (PTFE) emulsion after ultrasonic agitation 20min, continue ultrasonic agitation 20min, the mixed liquor obtained through 80 DEG C of water-baths and is stirred its roll-in film forming to one-tenth dough, is catalysis tunic;
4) again by step 3) gained catalysis tunic covers step 2) on the another side of gained stainless (steel) wire collector, roll-forming deducts corner excess stock and can be prepared by the circular gas diffusion electrode of diameter 6cm.
2. electrochemical treatments SO according to claim 12The preparation method of gas-diffusion electrode, it is characterised in that: described stainless (steel) wire collector is 60 orders, and thickness is 0.5mm.
3. electrochemical treatments SO according to claim 12The preparation method of gas-diffusion electrode, it is characterised in that: described diffusion layer film thickness is 0.5mm-1mm;Described Catalytic Layer film thickness is 0.5mm-1mm.
4. electrochemical treatments SO according to claim 12The preparation method of gas-diffusion electrode, it is characterised in that: described step 4) in after roll-forming the thickness of gained circular gas diffusion electrode be 0.8mm-1mm.
5. electrochemical treatments SO according to claim 12The preparation method of gas-diffusion electrode, it is characterised in that: the mass percent concentration of described PTFE emulsion is 60%;Step 1) in the mass ratio of PTFE emulsion and conductive black be 5:2, step 3) in PTFE emulsion, white carbon black and CNT mass ratio be 5:19:1.
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Cited By (5)
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CN108325350A (en) * | 2018-01-24 | 2018-07-27 | 河海大学 | A kind of flow reactor and its device and method of electrochemical degradation volatile organic contaminant |
CN108842162A (en) * | 2018-06-15 | 2018-11-20 | 重庆大学 | For electrochemical reduction CO2SnO2Nanometer sheet gas-diffusion electrode and method |
CN108866569A (en) * | 2018-07-03 | 2018-11-23 | 青岛理工大学 | A kind of preparation method of teflon heat modification gas-diffusion electrode |
CN111206259A (en) * | 2020-01-14 | 2020-05-29 | 武汉科技大学 | Preparation method of novel carbon black air diffusion cathode sheet capable of efficiently and stably producing hydrogen peroxide |
CN112599790A (en) * | 2020-12-14 | 2021-04-02 | 天津大学仁爱学院 | Cold pressing preparation method of air electrode |
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Cited By (6)
Publication number | Priority date | Publication date | Assignee | Title |
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CN108325350A (en) * | 2018-01-24 | 2018-07-27 | 河海大学 | A kind of flow reactor and its device and method of electrochemical degradation volatile organic contaminant |
CN108842162A (en) * | 2018-06-15 | 2018-11-20 | 重庆大学 | For electrochemical reduction CO2SnO2Nanometer sheet gas-diffusion electrode and method |
CN108866569A (en) * | 2018-07-03 | 2018-11-23 | 青岛理工大学 | A kind of preparation method of teflon heat modification gas-diffusion electrode |
CN111206259A (en) * | 2020-01-14 | 2020-05-29 | 武汉科技大学 | Preparation method of novel carbon black air diffusion cathode sheet capable of efficiently and stably producing hydrogen peroxide |
CN111206259B (en) * | 2020-01-14 | 2021-03-19 | 武汉科技大学 | Preparation method of novel carbon black air diffusion cathode sheet capable of efficiently and stably producing hydrogen peroxide |
CN112599790A (en) * | 2020-12-14 | 2021-04-02 | 天津大学仁爱学院 | Cold pressing preparation method of air electrode |
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