CN104192957A - Solid electrolyte electrolytic cell device using anion-exchange membrane - Google Patents
Solid electrolyte electrolytic cell device using anion-exchange membrane Download PDFInfo
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Abstract
The invention relates to a solid electrolyte electrolytic cell device using an anion exchange membrane. The solid electrolyte electrolytic cell device comprises an ion exchange membrane as well as an anode chamber and a cathode chamber arranged at both sides of the ion exchange membrane, wherein the anode chamber comprises an anode terminal plate, a porous anode support material and an anode catalytic layer; the cathode chamber comprises a cathode terminal plate and a porous cathode catalytic material and the ion exchange membrane material is the anion exchange membrane. By virtue of the solid electrolyte electrolytic cell device disclosed by the invention, the problem of scaling at an interface between the membrane and the electrode is avoided, the phenomenon of scaling of the ion exchange membrane is greatly retarded, the problem of blocking due to the scaling of the SPE (Solid Polymer Electrolyte) electrolytic cell is avoided and the stability and service life of the sewage treatment device are prolonged. The selection of the cathode catalytic material of the SPE electrolytic cell can be also broadened and the cost of the sewage treatment device can be significantly reduced.
Description
Technical field
The present invention relates to field of environment protection water treatment industry technical field, especially relate to a kind of anion-exchange membrane solid state electrolyte electrolytic cell assembly that adopts.
Background technology
Many biochemical property of industrial waste waters are poor, comprise in addition numerous inorganic and aromatic series hazardous and noxious substances such as a large amount of ammonia, cyanogen, phenols, pyridine, quinoline, are difficult to biochemical degradation.Electrochemistry advanced oxidation is the effective ways of processing this type of trade effluent, electrochemical oxidation utilizes the free radical (as hydroxyl radical free radical direct oxidation) of electrode surface generation or the oxygenant (as hypochlorous acid indirect oxidation) generating, can the efficient oxidation degraded organic pollutants.In addition, negative electrode can be under lower electromotive force, and in negative electrode generation electrical catalyze reduction water, proton produces hydrogen.But greater energy consumption is unanimously the bottleneck that puzzlement electrooxidation technology is applied to wastewater treatment, and due to the open by design of traditional electrolyzer, negative electrode produces hydrogen and cannot effectively reclaim.Canadian Studies personnel adopt the electrolyzer based on SPE proton exchange membrane improvement design to effectively reduce interelectrode distance and reduced energy consumption, evade the cost increase problem that Xiang Yuanshui adds supporting electrolyte, and utilize proton exchange membrane to intercept the anode chamber and the cathode chamber, effectively separate anode producing chlorine and negative electrode institute hydrogen producing (WO2012/167375).But the solid electrolyte adopting in this invention is cationic exchange membrane (the Nafion film etc. of producing as DuPont company), negative electrode adopts containing the cathode catalysis layer of Pt/C and greatly improves electrolyzer cost.Because proton exchange membrane cannot be avoided the migration of positively charged ion from anode to negative electrode, therefore, in electrolytic process, except the proton in anode organic waste water oxidation generation is to cathodic migration, the inorganic cation in waste water is (as Na
+, Ca
2+, Mg
2+deng) also can move to negative electrode, at cathode side and a large amount of OH that produce because producing hydrogen
-ionic bond generates alkali.Therefore, this design of electrolysis cells unavoidably in the fouling of negative electrode generation BS (as Ca (OH)
2, Mg (OH)
2deng), long-play must bring the obstruction of cathode gas diffusion layer and the increase of cathodic polarization, energy consumption is increased and reduce cathode life.Therefore, needing the aspects such as mould material to SPE " zero spacing " electrolyzer and film type, cathode construction, electrode materials and operating method badly improves.
Summary of the invention
The object of the invention is to design a kind of novel employing anion-exchange membrane solid state electrolyte electrolytic cell assembly, address the above problem.
To achieve these goals, the technical solution used in the present invention is as follows:
A kind of anion-exchange membrane solid state electrolyte electrolytic cell assembly that adopts, comprises ion-exchange membrane and anolyte compartment and cathode compartment in described ion-exchange membrane both sides;
Described anolyte compartment comprises anode end plate, porous anode propping material and anode catalyst layer, a side towards described ion-exchange membrane on described anode end plate is provided with anode flow field groove, the feed-water end of described anode flow field groove is provided with anode water-in, and the water side of described anode flow field groove is provided with anode water outlet; Described anode catalyst layer and the sealing of described porous anode propping material are arranged between described anode end plate and described ion-exchange membrane; Described anode catalyst layer, between described ion-exchange membrane and described porous anode propping material, and is close on described porous anode propping material; Described porous anode propping material is provided with anode collector, and described anode collector sealing is stretched out outside described anode end plate and described ion-exchange membrane;
Described cathode compartment comprises cathode end plate and porous cathode catalytic material, a side towards described ion-exchange membrane in described cathode end plate is provided with cathode flow field groove, the feed-water end of described cathode flow field groove is provided with negative electrode water-in, and the water side of described cathode flow field groove is provided with negative electrode water outlet; Described porous cathode catalytic material sealing is arranged between described cathode end plate and described ion-exchange membrane; Described porous cathode catalytic material is provided with cathode current collector, and described cathode current collector sealing is stretched out outside described cathode end plate and described ion-exchange membrane;
Described ion exchange membrane material is anion-exchange membrane.
Described porous sun propping material is corrosion resistant wire establishment net, and its order number is 50-400 order, and diameter wiry is 10-500 micron, and the thickness of wire cloth is 100-1000 micron;
Described anode catalyst layer is RuO
2-TiO
2, PbO
2, SnO
2-Sb
2o
3, Nb
2o
5-SnO
2, SnO
2-In
2o
3, IrO
2-Ta
2o
5, or rare-earth oxide/Sb
2o
5-SnO
2in one or more mixture.
Described corrosion resistant wire comprises tungsten filament, titanium silk, molybdenum filament or niobium silk.
Described corrosion resistant wire establishment net is titanium foam net, and the thickness of described titanium foam net is 300 microns-2000 microns;
Or described corrosion resistant wire establishment net is POROUS TITANIUM PLATE, and the thickness of described POROUS TITANIUM PLATE is 500 microns-3000 microns, and porosity is greater than 40%.
Described cathode end plate is that nickel or stainless steel nickel plating are made;
The design of described cathode flow field groove is consistent with described anode flow field groove, for horizontal or longitudinally snakelike, pectination groove arrange, groove width 1-3 millimeter, groove depth 0.5-2.0 millimeter, the parallel setting of two or three flow path groove, flow field conduit starts to finish to water outlet from water-in;
Described porous cathode catalytic material is the cathode for hydrogen evolution electrocatalysis material being applicable in alkaline water electrolytic cell.
Described cathode for hydrogen evolution electrocatalysis material comprises Ni, Raney Ni, Ni-S, Ni-Mo, or Ni-Mo-S.
Described cathode compartment is closely connected with described anolyte compartment, is only intercepted separately by described ion-exchange membrane, and the thickness of described ion exchange membrane material is 50 microns-150 microns
Also comprise silicon sealing-ring, between described anode end plate and described ion-exchange membrane, seal by described silica gel sealing ring, between described cathode end plate and described ion-exchange membrane, also seal by described silica gel sealing ring.
The object of the invention is to provide a kind of based on a kind of novel design and improvement based on anionic solid state electrolyte " zero spacing " electrolytic cell assembly, solve the fouling blockage problem that the replacement of the expensive cathode material of SPE electrolyzer in international monopoly PCT (WO2012/167375) causes with negative electrode product alkali, finally obtain a kind of SPE electrolytic cell assembly of novel low energy consumption high-efficiency electrochemicial oxidation organic wastewater with difficult degradation thereby.
The invention provides a kind of efficient, economic treatment process that changes traditional organic wastewater with difficult degradation thereby, and the energy in efficient recovery waste water.The present invention utilizes " zero spacing " electrolyzer based on ion-exchange membrane, under the condition of impressed voltage 2.5-4V, the efficient mineralising of anode is decomposed Persistent organic pollutants and ammonia nitrogen in organic waste water, the proton that negative electrode can produce organic substance decomposing also originates in hydrogen under the effect of nickel-base catalyst, is reclaimed the energy.Unique distinction of the present invention is to utilize anion-exchange membrane to replace cationic exchange membrane, and introduce circulating water flow at negative electrode, slow down greatly the scale formation of ion-exchange membrane cathode side, avoided negative electrode because positively charged ion produces the problem that alkali causes that electrode stops up, improved the stability of waste disposal plant.
Beneficial effect of the present invention can be summarized as follows:
(1) in the present invention, adopting anion-exchange membrane to replace after cationic exchange membrane, there is reduction generation hydrogen at negative electrode and produces OH simultaneously in water
-, being delivered to anode side by anion-exchange membrane from cathode side, the proton that oxidation operation in anode side waste water produces is combined and is generated water, thereby has avoided film and electrode interface fouling in electrolyzer to obtain problem; Slow down greatly the scale formation of ion-exchange membrane, the problem of having avoided the fouling of SPE electrolyzer to stop up, stability and the life-span of improving waste disposal plant.
(2) in addition, in the present invention, adopt anion-exchange membrane to replace after cationic exchange membrane, selection to SPE electric tank cathode catalytic material also can be widened, for example can adopt catalyst based and collector of Ni base, Fe etc. to replace the noble metal catalysts such as the Pt in cationic SPE electrolyzer, replace graphite bi-polar plate etc. with Ti base bipolar plates, can significantly reduce the cost of waste disposal plant.
Brief description of the drawings
Fig. 1 is the structural representation of the main apparent direction of SPE electrooxidation system of the present invention
Fig. 2 is the stretch-out view of SPE electrooxidation system of the present invention.
Wherein: 1. anode end plate 1,2. anode flow field groove 2; 3. silica gel sealing ring 3; 4. porous anode propping material 4; 5. anode catalyst layer 5; 6. anode collector 6; 7. ion-exchange membrane 7; 8. cathode current collector 8; 9. porous cathode catalytic material 9; 10. cathode flow field groove 10; 11. cathode end plate 11; 101. anode water-ins 101 (waste water); 102. anode water outlets 102 (processing water); 201. negative electrode water-ins 201 (tap water); 202. negative electrode water outlets 202.
Embodiment
In order to make technical problem solved by the invention, technical scheme and beneficial effect clearer, below in conjunction with drawings and Examples, the present invention is further elaborated.Should be appreciated that specific embodiment described herein, only in order to explain the present invention, is not intended to limit the present invention.
One as depicted in figs. 1 and 2 adopts anion-exchange membrane solid state electrolyte electrolytic cell assembly, comprises ion-exchange membrane 7 and anolyte compartment and cathode compartment in described ion-exchange membrane 7 both sides; Described anolyte compartment comprises anode end plate 1, porous anode propping material 4 and anode catalyst layer 5, a side towards described ion-exchange membrane 7 on described anode end plate 1 is provided with anode flow field groove 2, the feed-water end of described anode flow field groove 2 is provided with anode water-in 101, and the water side of described anode flow field groove 2 is provided with anode water outlet 102; Described anode catalyst layer 5 and 4 sealings of described porous anode propping material are arranged between described anode end plate 1 and described ion-exchange membrane 7; Described anode catalyst layer 5, between described ion-exchange membrane 7 and described porous anode propping material 4, and is close on described porous anode propping material 4; Described porous anode propping material 4 is provided with anode collector 6, and described anode collector 6 sealings are stretched out outside described anode end plate 1 and described ion-exchange membrane 7; Described cathode compartment comprises cathode end plate 11 and porous cathode catalytic material 9, a side towards described ion-exchange membrane 7 in described cathode end plate 11 is provided with cathode flow field groove 10, the feed-water end of described cathode flow field groove 10 is provided with negative electrode water-in 201, and the water side of described cathode flow field groove 10 is provided with negative electrode water outlet 202; Described porous cathode catalytic material 9 sealings are arranged between described cathode end plate 11 and described ion-exchange membrane 7; Described porous cathode catalytic material 9 is provided with cathode current collector 8, and described cathode current collector 8 sealings are stretched out outside described cathode end plate 11 and described ion-exchange membrane 7; Described ion-exchange membrane 7 materials are anion-exchange membrane.
。
In the embodiment being more preferably, described porous sun propping material is corrosion resistant wire establishment net, and its order number is 50-400 order, and diameter wiry is 10-500 micron, and the thickness of wire cloth is 100-1000 micron; Described anode catalyst layer 5 is RuO
2-TiO
2, PbO
2, SnO
2-Sb
2o
3, Nb
2o
5-SnO
2, SnO
2-In
2o
3, IrO
2-Ta
2o
5, or rare-earth oxide/Sb
2o
5-SnO
2in one or more mixture.
In the embodiment being more preferably, described corrosion resistant wire comprises tungsten filament, titanium silk, molybdenum filament or niobium silk.
In the embodiment being more preferably, described corrosion resistant wire establishment net is titanium foam net, and the thickness of described titanium foam net is 300 microns-2000 microns; Or described corrosion resistant wire establishment net is POROUS TITANIUM PLATE, and the thickness of described POROUS TITANIUM PLATE is 500 microns-3000 microns, and porosity is greater than 40%.
In the embodiment being more preferably, described cathode end plate 11 is made for nickel or stainless steel nickel plating; 10 designs of described cathode flow field groove are consistent with described anode flow field groove 2, for horizontal or longitudinally snakelike, comb Installed groove arrange, groove width 1-3 millimeter, groove depth 0.5-2.0 millimeter, two or three flow path groove walks abreast and flow field conduit is set starts to finish to water outlet from water-in; Described porous cathode catalytic material 9 is for being applicable to the cathode for hydrogen evolution electrocatalysis material in alkaline water electrolytic cell.
In the embodiment being more preferably, described cathode for hydrogen evolution electrocatalysis material comprises Ni, Raney Ni, Ni-S, Ni-Mo, or Ni-Mo-S.
In the embodiment being more preferably, described cathode compartment is closely connected with described anolyte compartment, is only intercepted separately by described ion-exchange membrane 7, and the thickness of described ion-exchange membrane 7 materials is 50 microns-150 microns
In the embodiment being more preferably, described employing anion-exchange membrane solid state electrolyte electrolytic cell assembly also comprises silicon sealing-ring, between described anode end plate 1 and described ion-exchange membrane 7, seal by described silica gel sealing ring 3, between described cathode end plate 11 and described ion-exchange membrane 7, also seal by described silica gel sealing ring 3.
In certain specific embodiment:
(1) in the present invention, anolyte compartment is made up of anode end plate 1, anode flow field groove 10, silica gel sealing ring 3, anode collector 6, porous anode propping material 4, anode catalyst layer 5, wherein porous sun propping material is the corrosion resistant wire establishment such as tungsten filament, titanium silk, molybdenum filament, niobium silk net, its order number is 50-400 order, diameter wiry is 10-500 micron, and the thickness of wire cloth is 100 microns-1000 microns; As with titanium foam net as anode support material, its thickness is about 300 microns-2000 microns; As done support material by POROUS TITANIUM PLATE, its thickness is 500-3000 micron, and porosity is greater than 40%; Anode catalyst layer 5 is RuO
2-TiO
2, PbO
2, SnO
2-Sb
2o
3, Nb
2o
5-SnO
2, SnO
2-In
2o
3, IrO
2-Ta
2o
5, or rare-earth oxide/Sb
2o
5-SnO
2in one or more mixture.
(2) in the present invention, negative electrode is by cathode end plate 11, cathode flow field groove 10, silica gel sealing ring 3, porous cathode catalytic material 9, and cathode current collector 8 five parts form; Cathode end plate 11 is that the materials such as nickel or stainless steel nickel plating are made, cathode flow field 10 designs are consistent with anode flow field, for horizontal or longitudinal snakelike, Shu Installed groove is arranged, groove width 1-3 millimeter, groove depth 0.5-2.0 millimeter, two or three flow path groove is parallel to be arranged, and flow field conduit starts to finish to water outlet from water-in; Porous cathode catalytic material 9 is the cathode for hydrogen evolution electrocatalysis material being applicable in alkaline water electrolytic cell, as Ni, and Raney Ni, Ni-S, Ni-Mo, Ni-Mo-S etc.;
(3) cathode compartment of the present invention " zero spacing " electrolyzer is closely connected with anolyte compartment, only intercepted separately by ion-exchange membrane 7, ion-exchange membrane 7 materials used are anion-exchange membrane (as quaternary amine type anion-exchange membrane, season phosphine type anion-exchange membrane etc.), and the thickness of film is that (μ m) for 50-150 micron; On " zero spacing " electrolyzer, the operating voltage that applies is 2-4 volt, and electric tank working current density is 1-20 milliampere/square centimeter;
(4) in the present invention, on SPE anode electrolytic cell, negative plate, respectively have a water-in, water-in is connected with top, flow field in pole plate bottom; SPE anode electrolytic cell, negative electrode respectively have a water outlet, and water outlet is located at pole plate upper side, are connected with flow field end.
(5) organic waste water is with 0.02-0.10ml/cm
2.min flow velocity enters from the import of anionic SPE anode electrolytic cell, under the effect of anode generation electrooxidation, is degraded and mineralising, processes water and discharges from anode export;
(6) negative electrode water inlet is tap water or anodizing water, and the hydrogen that negative electrode produces flows out from cathode outlet, and after gas obtains separating, liquid recycle stream enters negative electrode.
Compared with prior art, tool of the present invention has the following advantages:
(1) in the present invention, adopting anion-exchange membrane to replace after cationic exchange membrane, there is reduction generation hydrogen at negative electrode and produces OH simultaneously in water
-, being delivered to anode side by anion-exchange membrane from cathode side, the proton that oxidation operation in anode side waste water produces is combined and is generated water, thereby has avoided film and electrode interface fouling in electrolyzer to obtain problem; The problem of having avoided the fouling of SPE electrolyzer to stop up, stability and the life-span of improving waste disposal plant.
(2) in addition, in the present invention, adopt anion-exchange membrane to replace after cationic exchange membrane, selection to SPE electric tank cathode catalytic material also can be widened, for example can adopt catalyst based and collector of Ni base, Fe etc. to replace the noble metal catalysts such as the Pt in cationic SPE electrolyzer, replace graphite end plate etc. with Ti cardinal extremity plate, can significantly reduce the cost of waste disposal plant.
More than by the detailed description of concrete and preferred embodiment the present invention; but those skilled in the art should be understood that; the present invention is not limited to the above embodiment; within the spirit and principles in the present invention all; any amendment of doing, be equal to replacement etc., within protection scope of the present invention all should be included in.
Claims (8)
1. adopt an anion-exchange membrane solid state electrolyte electrolytic cell assembly, it is characterized in that: comprise ion-exchange membrane and anolyte compartment and cathode compartment in described ion-exchange membrane both sides;
Described anolyte compartment comprises anode end plate, porous anode propping material and anode catalyst layer, a side towards described ion-exchange membrane on described anode end plate is provided with anode flow field groove, the feed-water end of described anode flow field groove is provided with anode water-in, and the water side of described anode flow field groove is provided with anode water outlet; Described anode catalyst layer and the sealing of described porous anode propping material are arranged between described anode end plate and described ion-exchange membrane; Described anode catalyst layer, between described ion-exchange membrane and described porous anode propping material, and is close on described porous anode propping material; Described porous anode propping material is provided with anode collector, and described anode collector sealing is stretched out outside described anode end plate and described ion-exchange membrane;
Described cathode compartment comprises cathode end plate and porous cathode catalytic material, a side towards described ion-exchange membrane in described cathode end plate is provided with cathode flow field groove, the feed-water end of described cathode flow field groove is provided with negative electrode water-in, and the water side of described cathode flow field groove is provided with negative electrode water outlet; Described porous cathode catalytic material sealing is arranged between described cathode end plate and described ion-exchange membrane; Described porous cathode catalytic material is provided with cathode current collector, and described cathode current collector sealing is stretched out outside described cathode end plate and described ion-exchange membrane; Described ion exchange membrane material is anion-exchange membrane.
2. employing anion-exchange membrane solid state electrolyte electrolytic cell assembly according to claim 1, it is characterized in that: described porous sun propping material is corrosion resistant wire establishment net, its order number is 50-400 order, diameter wiry is 10-500 micron, and the thickness of wire cloth is 100 microns-1000 microns;
Described anode catalyst layer is RuO
2-TiO
2, PbO
2, SnO
2-Sb
2o
3, Nb
2o
5-SnO
2, SnO
2-In
2o
3, IrO
2-Ta
2o
5, or rare-earth oxide/Sb
2o
5-SnO
2in one or more mixture.
3. employing anion-exchange membrane solid state electrolyte electrolytic cell assembly according to claim 2, is characterized in that: described corrosion resistant wire comprises tungsten filament, titanium silk, molybdenum filament or niobium silk.
4. employing anion-exchange membrane solid state electrolyte electrolytic cell assembly according to claim 2, is characterized in that: described corrosion resistant wire establishment net is titanium foam net, and the thickness of described titanium foam net is 300 microns-2000 microns;
Or described corrosion resistant wire establishment net is POROUS TITANIUM PLATE, and the thickness of described POROUS TITANIUM PLATE is 500 microns-3000 microns, and porosity is greater than 40%.
5. employing anion-exchange membrane solid state electrolyte electrolytic cell assembly according to claim 1, is characterized in that: described cathode end plate is that nickel or stainless steel nickel plating are made;
The design of described cathode flow field groove is consistent with described anode flow field groove, for horizontal or longitudinally snakelike, pectination groove arrange, groove width 1-3 millimeter, groove depth 0.5-2.0 millimeter, the parallel setting of two or three flow path groove, flow field conduit starts to finish to water outlet from water-in;
Described porous cathode catalytic material is the cathode for hydrogen evolution electrocatalysis material being applicable in alkaline water electrolytic cell.
6. employing anion-exchange membrane solid state electrolyte electrolytic cell assembly according to claim 5, is characterized in that: described cathode for hydrogen evolution electrocatalysis material comprises Ni Raney Ni, Ni-S, Ni-Mo, or Ni-Mo-S.
7. employing anion-exchange membrane solid state electrolyte electrolytic cell assembly according to claim 1, it is characterized in that: described cathode compartment is closely connected with described anolyte compartment, only intercepted separately by described ion-exchange membrane, the thickness of described ion exchange membrane material is 50 microns-150 microns.
8. employing anion-exchange membrane solid state electrolyte electrolytic cell assembly according to claim 1, it is characterized in that: also comprise silicon sealing-ring, between described anode end plate and described ion-exchange membrane, seal by described silica gel sealing ring, between described cathode end plate and described ion-exchange membrane, also seal by described silica gel sealing ring.
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| CN113135614A (en) * | 2021-03-10 | 2021-07-20 | 中国工程物理研究院材料研究所 | Organic pollutant anodic oxidation treatment device based on proton exchange membrane |
| US11339483B1 (en) | 2021-04-05 | 2022-05-24 | Alchemr, Inc. | Water electrolyzers employing anion exchange membranes |
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| CN113135614A (en) * | 2021-03-10 | 2021-07-20 | 中国工程物理研究院材料研究所 | Organic pollutant anodic oxidation treatment device based on proton exchange membrane |
| US11339483B1 (en) | 2021-04-05 | 2022-05-24 | Alchemr, Inc. | Water electrolyzers employing anion exchange membranes |
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| CN104192957B (en) | 2016-04-06 |
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