CN105013321A - Method and apparatus for treating sulfur oxides and recovering sulfur using an electro-catalytic converter - Google Patents
Method and apparatus for treating sulfur oxides and recovering sulfur using an electro-catalytic converter Download PDFInfo
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- CN105013321A CN105013321A CN201410449021.1A CN201410449021A CN105013321A CN 105013321 A CN105013321 A CN 105013321A CN 201410449021 A CN201410449021 A CN 201410449021A CN 105013321 A CN105013321 A CN 105013321A
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- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 title claims abstract description 81
- 238000000034 method Methods 0.000 title claims abstract description 60
- XTQHKBHJIVJGKJ-UHFFFAOYSA-N sulfur monoxide Chemical class S=O XTQHKBHJIVJGKJ-UHFFFAOYSA-N 0.000 title claims abstract description 59
- 239000011593 sulfur Substances 0.000 title abstract description 8
- 229910052717 sulfur Inorganic materials 0.000 title abstract description 7
- 229910052815 sulfur oxide Inorganic materials 0.000 title description 6
- 239000007789 gas Substances 0.000 claims abstract description 115
- 239000001301 oxygen Substances 0.000 claims abstract description 29
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 29
- 230000008569 process Effects 0.000 claims abstract description 28
- 239000007787 solid Substances 0.000 claims abstract description 26
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 24
- 239000013078 crystal Substances 0.000 claims abstract description 15
- 238000001816 cooling Methods 0.000 claims abstract description 7
- 239000005864 Sulphur Substances 0.000 claims description 73
- 230000003197 catalytic effect Effects 0.000 claims description 52
- 238000006243 chemical reaction Methods 0.000 claims description 29
- 150000004767 nitrides Chemical class 0.000 claims description 24
- 238000000354 decomposition reaction Methods 0.000 claims description 14
- 239000000758 substrate Substances 0.000 claims description 13
- 239000000428 dust Substances 0.000 claims description 12
- 238000007599 discharging Methods 0.000 claims description 10
- 239000011148 porous material Substances 0.000 claims description 10
- 230000008676 import Effects 0.000 claims description 4
- 238000010926 purge Methods 0.000 claims description 4
- 239000002912 waste gas Substances 0.000 abstract description 17
- 239000003054 catalyst Substances 0.000 abstract description 10
- 238000002485 combustion reaction Methods 0.000 abstract description 7
- 238000006477 desulfuration reaction Methods 0.000 abstract description 4
- 230000023556 desulfurization Effects 0.000 abstract description 4
- TXKMVPPZCYKFAC-UHFFFAOYSA-N disulfur monoxide Inorganic materials O=S=S TXKMVPPZCYKFAC-UHFFFAOYSA-N 0.000 abstract 2
- 238000011084 recovery Methods 0.000 abstract 1
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 44
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 17
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 description 14
- 229910002091 carbon monoxide Inorganic materials 0.000 description 13
- 229910044991 metal oxide Inorganic materials 0.000 description 13
- 238000010586 diagram Methods 0.000 description 12
- 230000005518 electrochemistry Effects 0.000 description 11
- 239000002245 particle Substances 0.000 description 10
- 229930195733 hydrocarbon Natural products 0.000 description 9
- 150000002430 hydrocarbons Chemical class 0.000 description 9
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 8
- -1 used in agricultural Substances 0.000 description 8
- 239000004215 Carbon black (E152) Substances 0.000 description 7
- 230000000694 effects Effects 0.000 description 7
- 238000005516 engineering process Methods 0.000 description 7
- 239000000463 material Substances 0.000 description 7
- 235000019738 Limestone Nutrition 0.000 description 6
- 239000006028 limestone Substances 0.000 description 6
- 229910052751 metal Inorganic materials 0.000 description 6
- 239000002184 metal Substances 0.000 description 6
- 150000004706 metal oxides Chemical class 0.000 description 6
- AKEJUJNQAAGONA-UHFFFAOYSA-N sulfur trioxide Chemical compound O=S(=O)=O AKEJUJNQAAGONA-UHFFFAOYSA-N 0.000 description 6
- 239000003546 flue gas Substances 0.000 description 5
- 229910021526 gadolinium-doped ceria Inorganic materials 0.000 description 5
- 150000002926 oxygen Chemical class 0.000 description 5
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical group O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 4
- 230000008859 change Effects 0.000 description 4
- 229910052757 nitrogen Inorganic materials 0.000 description 4
- 238000002425 crystallisation Methods 0.000 description 3
- 230000008025 crystallization Effects 0.000 description 3
- 238000013461 design Methods 0.000 description 3
- 239000000203 mixture Substances 0.000 description 3
- MGWGWNFMUOTEHG-UHFFFAOYSA-N 4-(3,5-dimethylphenyl)-1,3-thiazol-2-amine Chemical compound CC1=CC(C)=CC(C=2N=C(N)SC=2)=C1 MGWGWNFMUOTEHG-UHFFFAOYSA-N 0.000 description 2
- 208000036366 Sensation of pressure Diseases 0.000 description 2
- GGGMJWBVJUTTLO-UHFFFAOYSA-N [Co]=O.[Sr].[La] Chemical compound [Co]=O.[Sr].[La] GGGMJWBVJUTTLO-UHFFFAOYSA-N 0.000 description 2
- YMVZSICZWDQCMV-UHFFFAOYSA-N [O-2].[Mn+2].[Sr+2].[La+3] Chemical compound [O-2].[Mn+2].[Sr+2].[La+3] YMVZSICZWDQCMV-UHFFFAOYSA-N 0.000 description 2
- WUKWITHWXAAZEY-UHFFFAOYSA-L calcium difluoride Chemical group [F-].[F-].[Ca+2] WUKWITHWXAAZEY-UHFFFAOYSA-L 0.000 description 2
- 229910002092 carbon dioxide Inorganic materials 0.000 description 2
- 239000001569 carbon dioxide Substances 0.000 description 2
- 239000000571 coke Substances 0.000 description 2
- 230000000994 depressogenic effect Effects 0.000 description 2
- LNTHITQWFMADLM-UHFFFAOYSA-N gallic acid Chemical compound OC(=O)C1=CC(O)=C(O)C(O)=C1 LNTHITQWFMADLM-UHFFFAOYSA-N 0.000 description 2
- 230000036541 health Effects 0.000 description 2
- 229910052746 lanthanum Inorganic materials 0.000 description 2
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 2
- 230000003137 locomotive effect Effects 0.000 description 2
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 239000013618 particulate matter Substances 0.000 description 2
- 238000000746 purification Methods 0.000 description 2
- 229910052712 strontium Inorganic materials 0.000 description 2
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 235000002918 Fraxinus excelsior Nutrition 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- 229920001131 Pulp (paper) Polymers 0.000 description 1
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 1
- 239000002250 absorbent Substances 0.000 description 1
- 230000002745 absorbent Effects 0.000 description 1
- 239000003905 agrochemical Substances 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 239000002956 ash Substances 0.000 description 1
- 239000007844 bleaching agent Substances 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 150000001722 carbon compounds Chemical class 0.000 description 1
- 229910000420 cerium oxide Inorganic materials 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 239000003337 fertilizer Substances 0.000 description 1
- 239000010436 fluorite Substances 0.000 description 1
- 239000003721 gunpowder Substances 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000036632 reaction speed Effects 0.000 description 1
- 238000007670 refining Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 229910002076 stabilized zirconia Inorganic materials 0.000 description 1
- 239000012209 synthetic fiber Substances 0.000 description 1
- 229920002994 synthetic fiber Polymers 0.000 description 1
- 239000004753 textile Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 229910001233 yttria-stabilized zirconia Inorganic materials 0.000 description 1
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- Treating Waste Gases (AREA)
- Exhaust Gas Treatment By Means Of Catalyst (AREA)
- Catalysts (AREA)
Abstract
A method and device for treating sulfur oxide and recovering sulfur by electric catalyst converter includes such steps as providing a reactor containing an electric catalyst converter, cooling the waste gas containing sulfur oxide and oxygen to less than 200 deg.C, introducing it to the reactor, introducing it to an airflow channel, contacting it with the cathode of the electric catalyst converter, generating an electromotive force between the anode and the cathode, cooling the sulfur gas, converting it to solid sulfur crystal, and collecting it. By means of the method and the device, the desulfurization of the combustion waste gas and the recovery of the solid sulfur crystals can be simultaneously carried out, and the method and the device have the advantages of simple process, low cost and the like.
Description
Technical field
The present invention relates to and a kind ofly process oxysulfide and reclaim the method and apparatus of sulphur, particularly relate to and a kind ofly utilize electric CC Catalytic Converter process oxysulfide and reclaim the method and apparatus of sulphur.
Background technology
Air-polluting waste gas is caused usually to comprise nitrogen oxide (Nitrogen oxides, NO
x), oxysulfide (Sulfur oxides, SO
x), carbon monoxide (CO), hydrocarbon (Hydrocarbons, HCs), shot-like particle (Particulate matter, PM) etc., wherein, existing research display, comprises the oxysulfide (SO as locomotive, factory, power plant institute discharging waste gas
x), cause significant impact to health, also therefore, for a long time, the equal sustainable development of numerous industrial circle and educational circles effectively can remove the technology of the oxysulfide in waste gas.
Tradition removes the method for waste gas sulphur oxide, most use limestone-based process (maybe can claim boiler method), such as U.S. Patent Bulletin US 5,246, No. 364, about a kind of method reducing the content of sulfur dioxide of flue gas (Flue gases), the method uses a boiler, the tracheae that this boiler comprises a combustion chamber, a hopper be connected with this combustion chamber and connects this combustion chamber and this hopper, one end of this boiler is connected with the conduit of an introducing flue gas, the other end is then an openend, for the ashes that discharge combustion process produces.Wherein, this hopper is for storing lime stone (Limestone) particle, and this limestone particle imports this combustion chamber through the nozzle be connected with this tracheae, is removed by the oxysulfide of this flue gas by this.For another U.S. Patent Bulletin US 6,391, No. 266, it describes a kind of high temperature furnace for sulfur removal technology, itself and aforementioned techniques are similar, this high temperature furnace mainly comprises a boiler and at least one first jet be located in this boiler, and this case utilizes this first jet to provide lime stone, and removes the sulfur dioxide in waste gas.Aforementioned techniques institute according to chemical reaction as follows:
CaCO
3(s)+SO
2(g)→CaSO
3(s)+CO
2(g)
Though as mentioned above, oxysulfide is present in waste gas, the health of human body is had to the possibility of harm, on the other hand, the generation of element sulphur, for many industries, belongs to again a considerable link.The fertilizer such as, used in agricultural, agricultural chemicals; The rubber that automobile industry uses, tire, the synthetic fibers that textile industry uses; The paper pulp that papermaking industry uses, the gunpowder that munitions industry uses; And the bleaching agent etc. that people's livelihood industry uses, invariably relevant with sulphur or sulfide.Also therefore, still there are other prior aries, once the technology of refining elementary sulfur was mentioned, as U.S. Patent Bulletin US 4,427, a kind of flue gas desulfurization process described by No. 642, this technique utilizes semi-coke (Semi-coke) as the absorbent of oxysulfide, makes oxysulfide be decomposed into elementary sulfur and carbon monoxide.
As known from the above, in prior art, as intended removing the oxysulfide in waste gas, boiler method need be used, because boiler method needs to use lime stone as raw material, therefore there is the problem of cost of material; Meanwhile, the solid-state castoff produced in technique, the extra cost of emptier increasing offal treatment and the complicated degree of technique.In addition, as wanted further generting element sulphur, the equipment and the technique that use other is also needed, the inconvenience causing expense to increase and use.
Summary of the invention
Main purpose of the present invention, is to solve existing desulfur technology and has that cost is high, process is complicated and cannot the direct shortcoming such as generting element sulphur.
For reaching above-mentioned purpose, the invention provides and a kind ofly reclaim the method for sulphur with electric CC Catalytic Converter process oxysulfide, including following steps:
Step 1 a: reactor is provided, this reactor comprises a front end, the electric CC Catalytic Converter of one rear end and between this front end and this rear end, a gas channel communicated with each other is formed between this front end and this rear end, this electric CC Catalytic Converter comprises a solid oxide nitride layer, one anode and a negative electrode, this solid oxide nitride layer is between this anode and this negative electrode, this solid oxide nitride layer is one first dense microstructure, this anode is made up of one first porous material and has a reproducibility environment, this negative electrode is made up of one second porous material and is communicated with this gas channel,
Step 2: by a burnt gas containing oxysulfide and oxygen in be cooled to one lower than first temperature of 200 DEG C after, this front end passed into this reactor is communicated with this negative electrode of this electric CC Catalytic Converter to import this gas channel;
Step 3: utilize this reproducibility environment of this electric CC Catalytic Converter and an aerobic environment of this burnt gas in this reactor to make between this anode and this negative electrode and produce an electromotive force, is decomposed into sulphur gas and oxygen to drive the oxysulfide in this burnt gas of promotion to carry out a decomposition reaction in this negative electrode; And
Step 4: this sulphur gas after this reactor is left in cooling, makes this sulphur gas must be converted to solid-state sulphur crystal and be collected.
For reaching above-mentioned purpose, the present invention also provides a kind of and processes oxysulfide and reclaim the electrochemical appliance of sulphur, burnt gas in order to contain oxysulfide and oxygen by one is converted into a Purge gas, include a reactor, one feed unit and a discharging unit, this reactor comprises a front end, the electric CC Catalytic Converter of one rear end and between this front end and this rear end, a gas channel communicated with each other is formed between this front end and this rear end, this electric CC Catalytic Converter comprises an anode, one negative electrode and a solid oxide nitride layer, this anode is made up of one first porous material and has a reproducibility environment, this negative electrode is made up of one second porous material and is communicated with this gas channel, this solid oxide nitride layer is between this anode and this negative electrode, this solid oxide nitride layer is one first dense microstructure, this feed unit for should burnt gas to this reactor, this discharging unit accepts this Purge gas of discharging from this reactor, this feed unit and this discharging unit are connected to this front end and this rear end of this reactor respectively.Wherein, this reproducibility environment of this electric CC Catalytic Converter of this reactor and an aerobic environment of this burnt gas make between this anode and this negative electrode and produce an electromotive force, be decomposed into sulphur gas and oxygen to drive the oxysulfide in this burnt gas of promotion to carry out a decomposition reaction in this negative electrode, and this sulphur gas is cooled after leaving this reactor and is converted to solid-state sulphur crystal and is collected.
Thus, the present invention makes this burnt gas in this electric CC Catalytic Converter, can coordinate the driving of this electromotive force, promotes that this oxysulfide is decomposed into this sulphur gas and this oxygen, and reaches the effect of the sulfur oxides level removing or reduce this burnt gas; Meanwhile, after this sulphur gas leaves this reactor, this solid-state sulphur crystal can be converted to further by cooling, and be convenient to collect.Therefore, real the having concurrently of the present invention reduces the sulfur oxides level of this burnt gas and effect of generting element sulphur, and with regard to chemical reaction, the process that use the present invention carries out desulfurization or generation sulphur is simple not complicated; And from the angle of device structure, electric CC Catalytic Converter of the present invention needn't adopt boiler or high-temperature service, and reaction condition all carries out below 200 DEG C, therefore equipment cost relative moderate.
Describe the present invention below in conjunction with the drawings and specific embodiments, but not as a limitation of the invention.
Accompanying drawing explanation
Fig. 1 is system schematic of the present invention;
Fig. 2, in the first embodiment of the present invention, the three-dimensional appearance schematic diagram of this electric CC Catalytic Converter;
Fig. 3 is the B-B structure cross-sectional schematic of Fig. 2;
Fig. 4 is the enlarged diagram of Fig. 3;
Fig. 5, in the second embodiment of the present invention, the three-dimensional appearance schematic diagram of this electric CC Catalytic Converter;
Fig. 6 is the C-C structure cross-sectional schematic of Fig. 5;
Fig. 7, in the second embodiment of the present invention, the three-dimensional appearance schematic diagram of this electric another aspect of CC Catalytic Converter;
Fig. 8, in the third embodiment of the present invention, the three-dimensional appearance schematic diagram of this electric CC Catalytic Converter;
Fig. 9 is the D-D structure cross-sectional schematic of Fig. 8;
Figure 10, in the fourth embodiment of the present invention, the three-dimensional appearance schematic diagram of this electric another aspect of CC Catalytic Converter;
Figure 11 is the system schematic of fifth embodiment of the invention.
Detailed description of the invention
Detailed description for the present invention and technology contents, the existing accompanying drawing that just coordinates is described as follows:
Refer to shown in Fig. 1, Fig. 1 is system schematic of the present invention, and the present invention is a kind of with electric CC Catalytic Converter process oxysulfide (SO
x) and reclaim the method and apparatus of sulphur, the oxysulfide of indication of the present invention is there is the various gas containing certain density oxysulfide, includes but not limited to waste gas that locomotive discharges, waste gas that plant operation produces and the waste gas that power plant discharges or biogas environment etc.Understand technology of the present invention for convenience, the burnt gas discharged using power plant below and remove its sulphur oxide and reclaim element sulphur as explanation, this burnt gas, except comprising this oxysulfide, also comprises nitrogen oxide (NO usually
x), carbon monoxide (CO), hydrocarbon (Hydrocarbons, HCs) and shot-like particle (Particulate matter, PM).
As shown in Figure 1, of the present invention with electric CC Catalytic Converter process oxysulfide and the device reclaiming sulphur consists predominantly of reactor 10, feed unit 20 and a discharging unit 30, this feed unit 20 accepts a burnt gas 40 and is supplied to this reactor 10.This reactor 10 comprises electric CC Catalytic Converter 11, front end 12 and a rear end 13, and this electric CC Catalytic Converter 11, between this front end 12 and this rear end 13, forms a gas channel communicated with each other between this front end 12 and this rear end 13.In the present invention, this electric CC Catalytic Converter 11 comprises an anode, a negative electrode and a solid oxide nitride layer, concrete structure describe in detail as after.In addition, in other embodiments of the present invention, this feed unit 20 can comprise a heat exchanger, and comprise a dust arrester and an air blast further, namely a dust arrester can be installed additional after this heat exchanger, a such as cyclone, and an air blast is installed again additional after this dust arrester, this discharging unit 30 can comprise a heat exchanger or a radiator or its and combine and a dust arrester.
In the present invention, this anode is made up of one first porous material, and there is a large amount of holes, this hole can be attached with a carbon species, and there is a reproducibility environment, the group that the material of this anode selects the Tao Jin of free metal and fluorite structure metal oxide composition, perovskite structure metal oxide (Perovskite Metal Oxides), fluorite structure metal oxide (Fluorite Metal Oxides), the perovskite structure metal oxide adding metal, the fluorite structure metal oxide adding metal and combination thereof to form.
This solid oxide nitride layer has one first dense microstructure, its material can be fluorite structure metal oxide or perovskite structure metal oxide, such as: gadolinia-doped ceria (the Gadolinia-doped Ceria of the yttria stabilized zirconia of fluorite structure, stabilized zirconia, fluorite structure, GDC), the strontium of doped cerium oxide, perovskite structure and magnesium doped lanthanum gallate (Strontium/magnesium-doped LanthanumGallate, LSGM), doped lanthanum gallate.
This negative electrode is made up of one second porous material, and there is a large amount of holes, its material can be perovskite structure metal oxide, fluorite structure metal oxide, adds the perovskite structure metal oxide of metal or add the fluorite structure metal oxide of metal, such as: the combination of the combination of the lanthanum-strontium-cobalt-oxygen compound of perovskite structure, lanthanum-strontium-manganese oxide, lanthanum-strontium-cobalt-oxygen compound and gadolinia-doped ceria, lanthanum-strontium-manganese oxide and gadolinia-doped ceria.
Refer to shown in Fig. 2 to Fig. 4, be respectively in the first embodiment of the present invention, the three-dimensional appearance schematic diagram of this electric CC Catalytic Converter, the B-B structure cross-sectional schematic of Fig. 2 and the enlarged diagram of Fig. 3, in first embodiment of the invention, this electric CC Catalytic Converter is an electric catalyst honeycomb 11b, this electric catalyst honeycomb 11b is arranged in this reactor 10, and between this front end 12 and this rear end 13, this electric catalyst honeycomb 11b comprises an anode 111b, one negative electrode 112b, one solid oxide nitride layer 113b, a multiple runner 114b and shell 115b, this anode 111b forms a honeycomb skeleton of this electric catalyst honeycomb 11b.This runner 114b is then formed in this honeycomb skeleton, runs through the two ends that this electric catalyst honeycomb 11b is relative, circulates for this burnt gas 40.This shell 115b then covers an outer surface 1111b of this anode 111b, and be one second dense microstructure, this solid oxide nitride layer 113b is attached to an inner surface 1112b of relative this outer surface 1111b of this anode 111b, and the two ends relative on this anode 111b with this shell 115b engage, and seal this anode 111b completely, this solid oxide nitride layer 113b also has one towards the tube wall 1131b of this runner 114b, this negative electrode 112b is attached on this tube wall 1131b, makes this solid oxide nitride layer 113b between this anode 111b and this negative electrode 112b.Structure and the material of only sketching this electric catalyst honeycomb 11b herein form, the structure that detailed description and this electric catalyst honeycomb 11b derive can refer to the U.S. Patent application the 13/666th that applicant in this case applied on November 01st, 2012, No. 593, it is incorporated herein, and should be considered as a part of the present invention.
Please continue to refer to Fig. 5, Fig. 6, be respectively in the second embodiment of the present invention, the three-dimensional appearance schematic diagram of this electric CC Catalytic Converter, the C-C structure cross-sectional schematic of Fig. 5, in second embodiment of the invention, this electric CC Catalytic Converter is an electrochemistry double cell plate 11c, this electrochemistry double cell plate 11c comprises an anode 111c, one negative electrode 112c, an one solid oxide nitride layer 113c and substrate 116c, this substrate 116c has a surperficial 1161c, this surperficial 1161c comprises the bottom surface 1163c of an end face 1162c and this end face relative 1162c, the material of this substrate 116c can be metal or alloy, in the present embodiment, this end face 1162c horizontal direction parallel with this bottom surface 1163c extends and makes this substrate 116c form a tabular, and this surperficial 1161c more comprises one is connected to side 1164c between this end face 1162c and this bottom surface 1163c.In the present embodiment, this reproducibility environment of this anode 111c and this oxidative environment of this negative electrode 112c make between this anode 111c and this negative electrode 112c and produce an electromotive force, this negative electrode 112c is formed contact with this burnt gas 40 one first reacts side 1121c and one second reacts side 1122c, this first reaction side 1121c is to should this end face 1162c of substrate 116c, and this second reaction side 1122c is to should this bottom surface 1163c of substrate 116c.Thus, by driving, this electromotive force promotes that the oxysulfide in this burnt gas 40 and nitrogen oxide with this in this first reaction side 1121c second react side 1122c and carry out a decomposition reaction and form sulphur gas, oxygen and nitrogen, to reach effect of control waste gas.
Please continue to refer to Fig. 7, for in the second embodiment of the present invention, the three-dimensional appearance schematic diagram of this electric another aspect of CC Catalytic Converter, in this aspect, arrange with being separated by for this electrochemistry double cell plate 11c for using a support body 50, make this electrochemistry double cell plate 11c form at least one airflow space 51 to each other, this airflow space 51 with this for this burnt gas flows through this electrochemistry double cell plate 11c first reacts side 1121c and second reacts side 1122c with this and contact.In this aspect, the ornaments direction of this electrochemistry double cell plate 11c is the flow direction this first reaction side 1121c and this second in-plane reacting side 1122c being parallel to this burnt gas, make by this this oxygen-enriched combusting waste gas and this first react side 1121c and this second reacts between the 1122c of side and can have maximum contact area.According to this design, this oxygen-enriched combusting waste gas by the surface of this first reaction side 1121c multiple and this second reaction side 1122c, and more effectively carries out waste gas purification.
Please continue to refer to Fig. 8, Fig. 9, be respectively in the third embodiment of the present invention, the three-dimensional appearance schematic diagram of this electric CC Catalytic Converter, the D-D structure cross-sectional schematic of Fig. 8, the third embodiment of the present invention be by the second embodiment derive, this electrochemistry double cell plate 11d comprises an anode 111d, one negative electrode 112d, an one solid oxide nitride layer 113d and substrate 116d, this substrate 116d has a surperficial 1161d, this surperficial 1161d comprises an end face 1162d, the bottom surface 1163d and one of one relative this end face 1162d is connected to the side 1164d between this end face 1162d and this bottom surface 1163d, wherein, this end face 1162d along a horizontal direction formed respectively multiple upper depressed part 1165d and multiple with this on the adjacent upper protuberance 1166d of depressed part 1165d, and this bottom surface 1163d forms multiple lower concave portion 1167d and multiple lower protuberance 1168d adjacent with this lower concave portion 1167d respectively along this horizontal direction, thus, compare with aforesaid second embodiment, under this electrochemistry double cell plate 11d has the condition of identical length and width, 3rd embodiment will be wavy design because of this substrate 116d, and this first reaction side 1121d of this negative electrode 112d and this second react side 1122d there is larger area, therefore the efficiency processing this burnt gas 40 will be higher.Please continue to refer to Figure 10, for in the fourth embodiment of the present invention, the three-dimensional appearance schematic diagram of this electric another aspect of CC Catalytic Converter, in this aspect, that this electrochemistry double cell plate 11c collocation that this electrochemistry double cell plate 11d made by this substrate 116d by wavy design and this substrate 116c designed by tabular are made uses, and setting interlaced with each other, this electrochemistry double cell plate 11c, multiple passage will be formed between 11d, in this aspect, this oxygen-enriched combusting waste gas enters the direction of this electrochemical appliance as shown in Figure 10, compare with Fig. 7, under identical volume conditions, this burnt gas 40 and this negative electrode 112c in this aspect, the contact area of 112d will be larger, therefore efficiency will be better.
The present invention provides a kind of simultaneously and reclaims the method for sulphur with electric CC Catalytic Converter process oxysulfide, will the method is described and utilize said apparatus process oxysulfide and reclaim the course of reaction of sulphur below.
The method comprises the following steps:
Step 1: this reactor 10 is provided;
Step 2: by this burnt gas 40 in be cooled to one lower than first temperature of 200 DEG C after, this front end 12 passed into this reactor 10 contacts with this negative electrode 112b, 112c, 112d of this electric CC Catalytic Converter 11 to import this gas channel;
Step 3: utilize this reproducibility environment of this electric CC Catalytic Converter 11 and an aerobic environment of this burnt gas 40 in this reactor 10 to make this anode 111b, 111c, 111d and produce an electromotive force between this negative electrode 112b, 112c, 112d, is decomposed into sulphur gas and oxygen to drive the oxysulfide in this burnt gas 40 of promotion to carry out a decomposition reaction in this negative electrode 112b, 112c, 112d; And
Step 4: this sulphur gas after this reactor 10 is left in cooling, makes this sulphur gas must be converted to solid-state sulphur crystal and be collected.
Said method is according to following chemical reaction:
SO
3→SO
2+O
2(a)
2SO
2→S
2(g)+2O
2(b)
4S
2(g)→S
8(g)(c)
Oxysulfide (the SO of this burnt gas 40
x) be mainly sulfur dioxide (SO
2) and the sulfur trioxide (SO of trace
3), as the sulfur trioxide (SO of this burnt gas 40
3) when contacting this negative electrode 112b, 112c, 112d, will to react formula (a) in this negative electrode 112b, 112c, 112d, and produce sulfur dioxide (SO
2) and oxygen, for this oxysulfide (SO
x) in sulfur dioxide (SO
2) or by sulfur trioxide (SO
3) decompose the sulfur dioxide (SO obtained
2), it will to react formula (b) in this negative electrode 112b, 112c, 112d, and produce sulphur gas S
2and oxygen (O
2).Sulphur gas S
2can further combined with being sulphur gas (S in this reactor 10
8), can fully so combine, as shown in reaction equation (c) at less than 200 DEG C reaction conditions of the present invention.Wherein, this decomposition reaction of step 3 is reaction equation (a) and reaction equation (b).As this sulphur gas (S
8) leave this reactor 10 after, cool this sulphur gas (S
8) make its aggegation crystallization be solid-state sulphur crystal and be collected.
In one embodiment of the invention, in step 2, this heat exchanger can be used to allow this burnt gas 40 be cooled to lower than 200 DEG C, so fully reclaim the heat of this burnt gas 40, and be conducive to follow-up temperature control; In another embodiment of the present invention, such as be applied to the exhaust-gas treatment of combustion matchmaker, this feed unit 20 can comprise a dust arrester and an air blast again, namely a dust arrester can be installed additional after this heat exchanger, a such as cyclone, and an air blast is installed again additional after this dust arrester, to compensate the atmospheric pressure lost of this burnt gas 40 by this dust arrester, and this burnt gas 40 is in being cooled to lower than 200 DEG C through this air blast rear.In step 3, it is interval that this burnt gas 40 remains on a reaction temperature between 120 DEG C to 175 DEG C in this gas channel of this electric CC Catalytic Converter 11, if lower than the reaction temperature of 120 DEG C, will hinder generated element sulphur S
2depart from this negative electrode 112b, 112c, 112d form sulphur gas and taken out of this electric CC Catalytic Converter 11, more then above-mentioned disengaging degree is poorer for low temperature, and can impel the generation of the backward reaction of reaction equation (b) higher than the reaction temperature of 175 DEG C and generated sulphur is oxidized to sulfur dioxide (SO
2), more the degree of high temperature then above-mentioned backward reaction is larger; In step 4, this sulphur gas is cooled in this heat exchanger or this radiator or its combination and aggegation crystallization is solid-state sulphur crystal, and use this dust arrester to collect this solid-state sulphur crystal, be cooled to the more low temperature particle of solid-state sulphur crystal that then aggegation crystallization is formed and more greatly and be more easily collected.
Different equilibrium oxygen partial pres-sures (Equilibrium oxygen partial pressure) is produced in this anode 111b, 111c, 111d and this negative electrode 112b, 112c, 112d by this reproducibility environment of this anode 111b, 111c, 111d and this aerobic environment of this burnt gas 40, this negative electrode 112b, 112c, 112d can be impelled and produce electromotive force (Electromotive force between this anode 111b, 111c, 111d, emf), the oxysulfide (SO promoted in this burnt gas 40 is driven
x) carry out this decomposition reaction in this negative electrode 112b, 112c, 112d and form this sulphur gas and oxygen, this electromotive force be produced as according to following principle:
emf＝[(RT)/(4F)]·ln[(P
O2|Cathode)/(P
O2|Anode)] (d)
Wherein, R is gas constant (Gas constant), and T is absolute temperature, and F is Faraday constant (Faradicconstant), P
o2for equilibrium oxygen partial pres-sure.
Referring to Figure 11, is the system schematic of fifth embodiment of the invention, and in this embodiment, this device also includes auxiliary air blender 60 and an air pump 61, and this auxiliary air blender 60 is located between this feed unit 20 and this reactor 10.Though this feed unit 20 in first embodiment of the invention can allow this burnt gas 40 be cooled to lower than 200 DEG C under general burn operation, but the temperature of this burnt gas 40 may change to some extent because of the change of burn operation, further temperature is now needed to regulate, this can supply an auxiliary air 62 by this air pump 61 and mix with this burnt gas 40 to this auxiliary air blender 60, and is fully cooled to this burnt gas 40 mixed lower than 200 DEG C.In addition, although this burnt gas 40 can produce an electromotive force at this aerobic environment, extra this auxiliary air 62 that adds enters this burnt gas 40 and can make its oxygen enrichment and can cause a larger electromotive force more, and promotes decomposition reaction speed.In addition, this air pump 61 is for should can improve the air pressure of this burnt gas 40 mixed to this auxiliary air blender 60 and promote its flow velocity by auxiliary air 62.
The present invention, except having the effect of this solid-state sulphur crystal of above-mentioned collection, can also have the effect of a purifying exhaust air, the mechanism continued purifying exhaust air of the present invention is described.From the above, this burnt gas 40 also includes nitrogen oxide, carbon monoxide, hydrocarbon and shot-like particle composition, the present invention for the purification of this burnt gas 40, mainly can be divided into the removal of nitrogen oxide and carbon monoxide, hydrocarbon, shot-like particle removal two parts carry out.
In nitrogen oxide removal, nitrogen oxide is mainly nitric oxide (NO) and nitrogen dioxide (NO
2), can there is decomposition reaction in this negative electrode 112b, 112c, 112d and produce nitrogen and oxygen in nitric oxide, its reaction equation is following formula (e).
2NO→N
2+O
2(e)
Can there is decomposition reaction in this negative electrode 112b, 112c, 112d and produce nitric oxide in nitrogen dioxide, its reaction equation is following formula (f).
2NO
2→2NO+O
2(f)
Can decomposition reaction be there is in this negative electrode 112b, 112c, 112d again and produce nitrogen and oxygen in its nitric oxide.
In like manner, by this reproducibility environment of this anode 111b, 111c, 111d and this aerobic environment of this burnt gas 40, this negative electrode 112b, 112c, 112d can be impelled and produce electromotive force (Electromotive force between this anode 111b, 111c, 111d, emf), the nitrogen oxide in this burnt gas 40 of promotion is driven to carry out decomposition reaction in this negative electrode 112b, 112c, 112d and form nitrogen and oxygen.
In the reaction of removing carbon monoxide, hydrocarbon and shot-like particle in this burnt gas 40, because this burnt gas 40 is oxygen enrichment state, or add this auxiliary air 62 and make its oxygen enrichment more, it can form innocuous gas by this negative electrode of mat 112b, 112c, 112d catalytic oxidation, carbon monoxide wherein in this burnt gas 40 is oxidable is carbon dioxide, hydrocarbon and shot-like particle (carbon containing (C) material) oxidable be carbon dioxide and water, its reaction equation is respectively as shown in the formula (g) to (i):
2CO+O
2→2CO
2(g)
HCs+O
2→H
2O+CO
2(h)
C+O
2→CO
2(i)
Therefore, the present invention also can pass through electromotive force and drives promotion decomposition reaction to carry out the removal of nitrogen oxide, and can pass through oxidation reaction removal carbon monoxide, hydrocarbon and shot-like particle, and effectively removes the harmful components in this burnt gas 40.
In sum, utilize method and apparatus of the present invention, make this burnt gas in this electric CC Catalytic Converter, coordinate the driving of this electromotive force to promote, this oxysulfide is decomposed into this sulphur gas and this oxygen, reaches the effect of the sulfur oxides level removing or reduce this burnt gas; Meanwhile, after this sulphur gas leaves this reactor, can be exchanged into this solid-state sulphur crystal by cooling, and be convenient to collect.Therefore, real the having concurrently of the present invention reduces the sulfur oxides level of this burnt gas and effect of generting element sulphur, and with regard to chemical reaction, the process that use the present invention carries out desulfurization or generation sulphur is simple not complicated; And from the angle of device structure, electric CC Catalytic Converter of the present invention needn't adopt boiler or high-temperature service, and reaction condition all carries out below 200 DEG C, therefore equipment cost relative moderate.
Certainly; the present invention also can have other various embodiments; when not deviating from the present invention's spirit and essence thereof; those of ordinary skill in the art are when making various corresponding change and distortion according to the present invention, but these change accordingly and are out of shape the protection domain that all should belong to the claim appended by the present invention.
Claims (13)
1. reclaim the method for sulphur with electric CC Catalytic Converter process oxysulfide, it is characterized in that, include following steps:
Step 1 a: reactor is provided, this reactor comprises a front end, the electric CC Catalytic Converter of one rear end and between this front end and this rear end, a gas channel communicated with each other is formed between this front end and this rear end, this electric CC Catalytic Converter comprises a solid oxide nitride layer, one anode and a negative electrode, this solid oxide nitride layer is between this anode and this negative electrode, this solid oxide nitride layer is one first dense microstructure, this anode is made up of one first porous material and has a reproducibility environment, this negative electrode is made up of one second porous material and is communicated with this gas channel,
Step 2: by a burnt gas containing oxysulfide and oxygen in be cooled to one lower than first temperature of 200 DEG C after, this front end passed into this reactor is communicated with this negative electrode of this electric CC Catalytic Converter to import this gas channel;
Step 3: utilize this reproducibility environment of this electric CC Catalytic Converter and an aerobic environment of this burnt gas in this reactor to make between this anode and this negative electrode and produce an electromotive force, is decomposed into sulphur gas and oxygen to drive the oxysulfide in this burnt gas of promotion to carry out a decomposition reaction in this negative electrode; And
Step 4: this sulphur gas after this reactor is left in cooling, makes this sulphur gas must be converted to solid-state sulphur crystal and be collected.
2. according to claim 1ly reclaim the method for sulphur with electric CC Catalytic Converter process oxysulfide, it is characterized in that step 2, is utilize a heat exchanger that this burnt gas is down to this first temperature.
3. according to claim 1ly reclaim the method for sulphur with electric CC Catalytic Converter process oxysulfide, it is characterized in that, step 2 passes into before this reactor in this burnt gas to be mixed into an auxiliary air, this burnt gas is down to this first temperature and promotes the oxygen content of this burnt gas.
4. according to claim 1ly reclaim the method for sulphur with electric CC Catalytic Converter process oxysulfide, it is characterized in that, step 3, it is interval that this burnt gas is in a reaction temperature between 120 DEG C to 175 DEG C in this gas channel of this reactor.
5. according to claim 1ly reclaim the method for sulphur with electric CC Catalytic Converter process oxysulfide, it is characterized in that, step 4, is utilize a heat exchanger or a radiator to cool this sulphur gas.
6. according to claim 1ly reclaim the method for sulphur with electric CC Catalytic Converter process oxysulfide, its feature exists, and in step 4, is utilize a dust arrester to collect this solid-state sulphur crystal.
7. process oxysulfide and reclaim the electrochemical appliance of sulphur, in order to a burnt gas containing oxysulfide and oxygen is converted into a Purge gas, it is characterized in that, include:
One reactor, this reactor comprises a front end, the electric CC Catalytic Converter of a rear end and between this front end and this rear end, and form a gas channel communicated with each other between this front end and this rear end, this electric CC Catalytic Converter comprises:
One anode, this anode is made up of one first porous material and has a reproducibility environment;
One negative electrode, this negative electrode is made up of one second porous material and is communicated with this gas channel; And
One solid oxide nitride layer between this anode and this negative electrode, this solid oxide nitride layer is one first dense microstructure;
One for should burnt gas to the feed unit of this reactor; And
The discharging unit of this Purge gas that one acceptance is discharged from this reactor, this feed unit and this discharging unit are connected to this front end and this rear end of this reactor respectively;
Wherein, this reproducibility environment of this electric CC Catalytic Converter of this reactor and an aerobic environment of this burnt gas make between this anode and this negative electrode and produce an electromotive force, be decomposed into sulphur gas and oxygen to drive the oxysulfide in this burnt gas of promotion to carry out a decomposition reaction in this negative electrode, and this sulphur gas is cooled after leaving this reactor and is converted to solid-state sulphur crystal and is collected.
8. process oxysulfide according to claim 7 reclaim the electrochemical appliance of sulphur, it is characterized in that, this feed unit is a heat exchanger.
9. process oxysulfide according to claim 8 reclaim the electrochemical appliance of sulphur, is characterized in that, this feed unit also comprises one and is located at the dust arrester after this heat exchanger and an air blast.
10. process oxysulfide according to claim 7 reclaim the electrochemical appliance of sulphur, it is characterized in that, have an auxiliary air blender between this feed unit and this reactor, this auxiliary air blender is communicated with an air pump and is mixed into this burnt gas to provide an auxiliary air.
11. process oxysulfides according to claim 7 also reclaim the electrochemical appliance of sulphur, it is characterized in that, this discharging unit comprises a heat exchanger or a radiator or its combination and a dust arrester.
12. process oxysulfides according to claim 7 also reclaim the electrochemical appliance of sulphur, it is characterized in that, this electric CC Catalytic Converter more comprises a honeycomb skeleton be made up of this anode, multiplely to be formed in this skeleton and the runner be communicated with this gas channel, the shell of one outer surface of one this anode of covering, one this solid oxide nitride layer being attached to the relative inner surface of this outer surface of this anode, wherein, this shell is one second dense microstructure, and this solid oxide nitride layer has a tube wall adhered in the face of this runner and for this negative electrode, this solid oxide nitride layer engages with this shell and seals this anode.
13. process oxysulfides according to claim 7 also reclaim the electrochemical appliance of sulphur, it is characterized in that, this electric CC Catalytic Converter more comprises a substrate, this substrate has an outer surface, this outer surface comprises the bottom surface of an end face and this end face relative, this anode at least covers this end face and this bottom surface, and this solid oxide nitride layer covers completely and seals this anode, and this negative electrode then covers this solid oxide nitride layer completely.
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| TW103115760 | 2014-05-02 | ||
| TW103115760A TWI549742B (en) | 2014-05-02 | 2014-05-02 | Method and apparatus for treating sulfur oxides from honeycomb with electric catalyst and recovering sulfur |
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| Publication Number | Publication Date |
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Cited By (1)
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|---|---|---|---|---|
| CN114094242A (en) * | 2021-12-29 | 2022-02-25 | 重庆大学 | Flow type photoelectrochemical cell for treating desulfurization wastewater and reducing carbon dioxide simultaneously |
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| US6331232B1 (en) * | 1996-08-14 | 2001-12-18 | Volvo Car Corporation | Device and method for reduction of oxides of nitrogen |
| CN102335552A (en) * | 2010-07-16 | 2012-02-01 | 国立清华大学 | Electrochemical-catalytic converter controlling exhaust emission and generating electricity |
| CN103100303A (en) * | 2011-11-09 | 2013-05-15 | 黄大仁 | Electric catalyst tube for controlling exhaust emission |
| CN203123723U (en) * | 2012-12-18 | 2013-08-14 | 汪上晓 | Multilayer arranged waste gas purifying reactor |
| TW201412382A (en) * | 2012-09-24 | 2014-04-01 | Ta-Jen Huang | An electro-catalytic honeycomb for controlling exhaust emissions |
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| US20040161596A1 (en) * | 2001-05-31 | 2004-08-19 | Noriyuki Taoka | Porous ceramic sintered body and method of producing the same, and diesel particulate filter |
| JP4103720B2 (en) * | 2003-07-31 | 2008-06-18 | 日産自動車株式会社 | ENGINE EXHAUST PURIFYING APPARATUS AND PARTICLE DEPOSITION STATE JUDGMENT METHOD |
| WO2011102487A1 (en) * | 2010-02-22 | 2011-08-25 | 日立金属株式会社 | Ceramic honeycomb structure and process for producing same |
| TWI390104B (en) * | 2010-03-04 | 2013-03-21 | Nat Univ Tsing Hua | Thermally activated electrochemical-catalytic converter for exhaust emission control with power generation |
| TWI414343B (en) * | 2010-10-29 | 2013-11-11 | Nat Univ Tsing Hua | An oxy catalyst converter for |
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2014
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| US6331232B1 (en) * | 1996-08-14 | 2001-12-18 | Volvo Car Corporation | Device and method for reduction of oxides of nitrogen |
| CN102335552A (en) * | 2010-07-16 | 2012-02-01 | 国立清华大学 | Electrochemical-catalytic converter controlling exhaust emission and generating electricity |
| CN103100303A (en) * | 2011-11-09 | 2013-05-15 | 黄大仁 | Electric catalyst tube for controlling exhaust emission |
| TW201412382A (en) * | 2012-09-24 | 2014-04-01 | Ta-Jen Huang | An electro-catalytic honeycomb for controlling exhaust emissions |
| CN203123723U (en) * | 2012-12-18 | 2013-08-14 | 汪上晓 | Multilayer arranged waste gas purifying reactor |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN114094242A (en) * | 2021-12-29 | 2022-02-25 | 重庆大学 | Flow type photoelectrochemical cell for treating desulfurization wastewater and reducing carbon dioxide simultaneously |
| CN114094242B (en) * | 2021-12-29 | 2023-09-15 | 重庆大学 | Flow type photoelectrochemical cell for treating desulfurization wastewater and simultaneously reducing carbon dioxide |
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|---|---|
| TW201542285A (en) | 2015-11-16 |
| TWI549742B (en) | 2016-09-21 |
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