CN106040232A - Catalyst for wastewater treatment, method for preparing catalyst, and wastewater treatment equipment comprising catalyst - Google Patents
Catalyst for wastewater treatment, method for preparing catalyst, and wastewater treatment equipment comprising catalyst Download PDFInfo
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- CN106040232A CN106040232A CN201610124275.5A CN201610124275A CN106040232A CN 106040232 A CN106040232 A CN 106040232A CN 201610124275 A CN201610124275 A CN 201610124275A CN 106040232 A CN106040232 A CN 106040232A
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- catalyst
- nano
- pore
- stainless steel
- steel substrate
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- 239000003054 catalyst Substances 0.000 title claims abstract description 108
- 238000000034 method Methods 0.000 title claims abstract description 59
- 238000004065 wastewater treatment Methods 0.000 title abstract description 16
- 239000011148 porous material Substances 0.000 claims abstract description 57
- 239000000758 substrate Substances 0.000 claims abstract description 57
- 229910001220 stainless steel Inorganic materials 0.000 claims abstract description 52
- 239000010935 stainless steel Substances 0.000 claims abstract description 52
- 239000002351 wastewater Substances 0.000 claims abstract description 29
- 239000002082 metal nanoparticle Substances 0.000 claims abstract description 23
- 229910052751 metal Inorganic materials 0.000 claims abstract description 19
- 239000002184 metal Substances 0.000 claims abstract description 19
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 claims description 26
- 230000003647 oxidation Effects 0.000 claims description 26
- 238000007254 oxidation reaction Methods 0.000 claims description 26
- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(1+) nitrate Chemical group [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 claims description 21
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 17
- 239000010865 sewage Substances 0.000 claims description 14
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 13
- 239000002105 nanoparticle Substances 0.000 claims description 13
- 229910052719 titanium Inorganic materials 0.000 claims description 13
- 239000010936 titanium Substances 0.000 claims description 13
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical group [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 12
- 229910000831 Steel Inorganic materials 0.000 claims description 12
- 229910052709 silver Inorganic materials 0.000 claims description 12
- 239000004332 silver Substances 0.000 claims description 12
- 239000010959 steel Substances 0.000 claims description 12
- 239000002253 acid Substances 0.000 claims description 10
- 230000008859 change Effects 0.000 claims description 9
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 8
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 claims description 7
- 229910010062 TiCl3 Inorganic materials 0.000 claims description 7
- 229910003074 TiCl4 Inorganic materials 0.000 claims description 7
- 238000007540 photo-reduction reaction Methods 0.000 claims description 7
- 150000003839 salts Chemical class 0.000 claims description 7
- 239000011260 aqueous acid Substances 0.000 claims description 6
- 239000003638 chemical reducing agent Substances 0.000 claims description 6
- 239000000203 mixture Substances 0.000 claims description 6
- 239000012279 sodium borohydride Substances 0.000 claims description 6
- 229910000033 sodium borohydride Inorganic materials 0.000 claims description 6
- LNTHITQWFMADLM-UHFFFAOYSA-N gallic acid Chemical compound OC(=O)C1=CC(O)=C(O)C(O)=C1 LNTHITQWFMADLM-UHFFFAOYSA-N 0.000 claims description 5
- 239000001301 oxygen Substances 0.000 claims description 5
- 229910052760 oxygen Inorganic materials 0.000 claims description 5
- 230000009467 reduction Effects 0.000 claims description 5
- 238000006722 reduction reaction Methods 0.000 claims description 5
- 239000007864 aqueous solution Substances 0.000 claims description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 4
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 claims description 4
- 229910052757 nitrogen Inorganic materials 0.000 claims description 4
- 239000001509 sodium citrate Substances 0.000 claims description 4
- NLJMYIDDQXHKNR-UHFFFAOYSA-K sodium citrate Chemical compound O.O.[Na+].[Na+].[Na+].[O-]C(=O)CC(O)(CC([O-])=O)C([O-])=O NLJMYIDDQXHKNR-UHFFFAOYSA-K 0.000 claims description 4
- 238000013019 agitation Methods 0.000 claims description 3
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 claims description 2
- 239000012153 distilled water Substances 0.000 claims description 2
- 229940074391 gallic acid Drugs 0.000 claims description 2
- 235000004515 gallic acid Nutrition 0.000 claims description 2
- 239000007788 liquid Substances 0.000 claims description 2
- 239000011734 sodium Substances 0.000 claims description 2
- 229910052708 sodium Inorganic materials 0.000 claims description 2
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 claims 1
- 238000009303 advanced oxidation process reaction Methods 0.000 abstract description 16
- 230000006641 stabilisation Effects 0.000 abstract description 5
- 239000002244 precipitate Substances 0.000 abstract description 4
- 230000007797 corrosion Effects 0.000 abstract description 3
- 238000005260 corrosion Methods 0.000 abstract description 3
- 238000011105 stabilization Methods 0.000 abstract description 2
- 238000002360 preparation method Methods 0.000 description 24
- 238000006243 chemical reaction Methods 0.000 description 16
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 12
- 239000000463 material Substances 0.000 description 10
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 9
- 230000008569 process Effects 0.000 description 9
- 238000005516 engineering process Methods 0.000 description 7
- 239000003795 chemical substances by application Substances 0.000 description 6
- 230000008901 benefit Effects 0.000 description 5
- 238000006555 catalytic reaction Methods 0.000 description 5
- 239000003344 environmental pollutant Substances 0.000 description 5
- 230000002085 persistent effect Effects 0.000 description 5
- 231100000719 pollutant Toxicity 0.000 description 5
- 238000012545 processing Methods 0.000 description 5
- 230000015556 catabolic process Effects 0.000 description 4
- 239000000356 contaminant Substances 0.000 description 4
- 238000006731 degradation reaction Methods 0.000 description 4
- 230000007246 mechanism Effects 0.000 description 4
- 238000013459 approach Methods 0.000 description 3
- 230000033228 biological regulation Effects 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000000724 energy-dispersive X-ray spectrum Methods 0.000 description 3
- 150000003254 radicals Chemical class 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- XJDNKRIXUMDJCW-UHFFFAOYSA-J titanium tetrachloride Chemical compound Cl[Ti](Cl)(Cl)Cl XJDNKRIXUMDJCW-UHFFFAOYSA-J 0.000 description 3
- 238000012876 topography Methods 0.000 description 3
- LRHPLDYGYMQRHN-UHFFFAOYSA-N N-Butanol Chemical compound CCCCO LRHPLDYGYMQRHN-UHFFFAOYSA-N 0.000 description 2
- OUUQCZGPVNCOIJ-UHFFFAOYSA-M Superoxide Chemical compound [O-][O] OUUQCZGPVNCOIJ-UHFFFAOYSA-M 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000004821 distillation Methods 0.000 description 2
- 239000003792 electrolyte Substances 0.000 description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 2
- 239000010931 gold Substances 0.000 description 2
- 229910052737 gold Inorganic materials 0.000 description 2
- -1 hydroxyl radical free radical Chemical class 0.000 description 2
- 238000007654 immersion Methods 0.000 description 2
- 238000011068 loading method Methods 0.000 description 2
- 239000013528 metallic particle Substances 0.000 description 2
- 150000002739 metals Chemical class 0.000 description 2
- 238000006552 photochemical reaction Methods 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- WKBOTKDWSSQWDR-UHFFFAOYSA-N Bromine atom Chemical compound [Br] WKBOTKDWSSQWDR-UHFFFAOYSA-N 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 241000196324 Embryophyta Species 0.000 description 1
- 240000001973 Ficus microcarpa Species 0.000 description 1
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 1
- 206010028980 Neoplasm Diseases 0.000 description 1
- 241001593750 Turcica Species 0.000 description 1
- 238000001467 acupuncture Methods 0.000 description 1
- 238000006065 biodegradation reaction Methods 0.000 description 1
- GDTBXPJZTBHREO-UHFFFAOYSA-N bromine Substances BrBr GDTBXPJZTBHREO-UHFFFAOYSA-N 0.000 description 1
- 229910052794 bromium Inorganic materials 0.000 description 1
- 201000011510 cancer Diseases 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000008199 coating composition Substances 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 230000005284 excitation Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000008187 granular material Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- 230000001699 photocatalysis Effects 0.000 description 1
- 239000012266 salt solution Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 235000015096 spirit Nutrition 0.000 description 1
- 239000003381 stabilizer Substances 0.000 description 1
- 230000001954 sterilising effect Effects 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 239000013076 target substance Substances 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 238000002560 therapeutic procedure Methods 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- YONPGGFAJWQGJC-UHFFFAOYSA-K titanium(iii) chloride Chemical compound Cl[Ti](Cl)Cl YONPGGFAJWQGJC-UHFFFAOYSA-K 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/48—Silver or gold
- B01J23/50—Silver
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/06—Silicon, titanium, zirconium or hafnium; Oxides or hydroxides thereof
- B01J21/063—Titanium; Oxides or hydroxides thereof
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/40—Catalysts, in general, characterised by their form or physical properties characterised by dimensions, e.g. grain size
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
- B01J35/51—Spheres
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/78—Treatment of water, waste water, or sewage by oxidation with ozone
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Hydrology & Water Resources (AREA)
- Life Sciences & Earth Sciences (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Catalysts (AREA)
- Treatment Of Water By Oxidation Or Reduction (AREA)
- Crystallography & Structural Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Toxicology (AREA)
- Physical Water Treatments (AREA)
Abstract
The invention discloses a catalyst for wastewater treatment, and discloses a wastewater treatment catalyst. The catalyst comprises a stainless steel nano-substrate with nano-pores formed on the surface of the catalyst and metal nano-particles loaded into the nano-pores; the metal nano-particles are loaded into the nano-pores; the metal nano-particles are loaded into the nano-pores; the metal nano-particles are loaded into the nano-pores; the metal nano -. The catalyst has excellent corrosion resistance and wear resistance and is stable in pH and temperature changes. In particular, when applied to wastewater treatment based on advanced oxidation processes, wastewater treatment based on advanced oxidation processes is applied, this catalyst increases the rate of wastewater treatment to two or more times compared to existing catalysts, by using the catalyst, the wastewater treatment cost is significantly reduced, and the wastewater treatment cost is significantly reduced. The catalyst can be repeatedly reused without being used for special stabilization after being used, and other existing catalysts are different from other existing catalysts., the catalyst does not leave a precipitate and eliminates the subsequent treatment requirements. The catalyst is easy to prepare, and the catalyst is easy to prepare. In addition, the catalyst can be simply applied to the existing equipment. Thus, the catalyst can be directly used without treating the wastewater. The invention further discloses a method for preparing the catalyst and a wastewater treatment equipment comprising the catalyst. The wastewater treatment equipment comprises the catalyst.
Description
Technical field
The present invention relates to the catalyst for waste water process, for preparing the method for this catalyst and including
The sewage treatment equipment of this catalyst.
Background technology
In recent years, the environment regulations for the wastewater effluent increased has become stricter.Therefore,
Occur in that the demand to the technology economically and efficiently processed for waste water.Existing biological effluent treatment
Technology is not enough in terms of meeting strict regulation, and in terms of processing the waste water of ever-increasing amount also
Unsatisfactory.It is difficult to remove persistent organism and micropollutants completely by biologic treating technique.
Such persistent organism and micropollutants flow into water system and are considered as that aquatic ecosystem is unbalance
Main cause.In this case, exist full compared with prior art based on biological treatment
Foot acupuncture therapy to the strict regulations of effluent, in terms of processing the waste water of ever-increasing amount effectively and can
It is used for removing completely the demand of the advanced technology of persistent organism and micropollutants.
In this, Korean government is planned to carry out studying to propose about the most organic in effluent
The standard of carbon (TOC), and expection quickly proposition effluent quality standard.Therefore, more concerns are
Persistent organism and micropollutants is removed from effluent through concentrating on.But, this polluter
Remove completely and make to need to introduce modern advanced oxidation equipment.Some mechanisms of Korea S and company manage
Waste water treatment plant based on advanced oxidation method, but it is because the intrinsic problem of method, they have fortune
The difficulty of waste water treatment plant of battalion.
Many advanced oxidation methods are applied to waste water at present and process.Such as, Fenton method is at pH 3 to 5
Acid range in the aspect of oxidized waste water most effective.But, the method disadvantageously, waste water
PH should be adjusted to the acid range for reaction, and should increase treated after having aoxidized
The pH of water is with discharge.Fenton method also needs to follow-up process step and removes and during reaction produce
A large amount of precipitate.As another example, it is known that based on ultraviolet light/hydrogen peroxide (UV/H2O2)
Advanced oxidation method.According to the method, ultraviolet light accelerates the decomposition of hydrogen peroxide to improve oxidation stain
The synthesis speed of the OH free radical of thing.Based on UV/H2O2Method be to have removing in terms of pollutant
Effect, but have a problem in that to realize high efficiency, need substantial amounts of hydrogen peroxide.
Another has a problem in that: the use of a large amount of hydrogen peroxide causes financial burden, and causes final effluent
The increase of COD (COD), making it difficult to meet effluent quality standard.
On the contrary, based on ozone (O3As long as) method have the advantage that electric power be available just
Can prepare ozone as required, and by can be to pollutant with ozone direct reaction in the short time
Carry out sterilizing effectively and oxidation.Due to these advantages, method based on ozone has attracted a lot
Pay close attention to.The another advantage of method based on ozone is to make lyophobic dust such as persistent organism
Hydrophiling, and can be by easily biodegradation.Therefore, method based on ozone is environment friend
Alright, therefore it is suitable in the processed and applied requiring high water quality as the technology for Wastewater Pretreatment.
But, because method based on ozone depends on contact with pollutant, so they are only specific in removal
Target substance aspect effective.This causes the selectivity of difference, and limits and can be gone by direct reaction
The amount of the organic substance removed.Other shortcomings of method based on ozone are: the existence of bromine may cause causing
The generation of cancer material, and need to use other energy sources to promote for reducing between organic substance
Connect reaction.
Rustless steel has corrosion resistance and the wearability of excellence, and is not susceptible to compared with other metals
PH and the impact of variations in temperature.It is to say, rustless steel has extraordinary physical and chemical stability.With it
His material based on ferrum is different, and rustless steel is eco-friendly catalysis material, this is because it is not give birth to
Rust, do not leave precipitate.Because this advantage, rustless steel can obtain in various water treatment field
Directly application.To this, Korean Patent No. 0403275 discloses a kind of stainless steel substrate that is administered to
Photocatalytic coating composition, it comprises organosilan, metal-oxide, storage stabilizing agent etc..Separately
Outward, Korean Patent Publication No. 2007-0113551 discloses a kind of at by advanced oxidation method
The equipment complex of reason persistency waste liquid.This equipment complex is catalyzed based on ozone electrolysis and quasiconductor, and wraps
Include surface-coated and have the stainless steel anode of titanium and iridium.
But, prior art only discloses relevant to the coating of the part of metallic particles on stainless steel material
Technology, and do not disclose for by effectively constructing the structure of stainless steel carrier and being loaded in load
Metallic particles on body makes the maximized technology of degraded of pollutant.
Summary of the invention
It is complete the present invention to solve the problem of Conventional waste water treatment technology, and it is contemplated that carries
For a kind of for waste water process catalyst, its durability having had, promote waste water process, can
Carry out after repeatedly re-using and noting be used in use special stabilisation or subsequent treatment, easily prepared,
And can simply directly be applied to existing equipment, the present invention also provides for for preparing this catalyst
Method and the sewage treatment equipment including this catalyst.
One aspect of the present invention provides a kind of catalyst processed for waste water, and described catalyst includes
The rustless steel nanometer base material being formed with nano-pore on surface and the metal nano being loaded in nano-pore
Grain.
According to one embodiment of the invention, metal nanoparticle can be selected from silver with titanium at least
A kind of nano-particle of non-ferrous metal.
According to another embodiment of the present invention, nano-pore can have the average straight of 70nm to 90nm
Footpath and the mean depth of 20nm to 100nm.
According to another embodiment of the present invention, per unit surface area (1 μm of stainless steel substrate2)
Nano-pore quantity can be 160 to 200.
According to another embodiment of the present invention, metal nanoparticle can be average diameter be 15nm extremely
The spheroid of 50nm.
According to another embodiment of the present invention, the average diameter of nano-pore is average straight with nano-particle
The ratio in footpath can be 2:1 to 5:1.
Can be 3:1 according to another embodiment of the present invention, the average diameter of nano-pore and the ratio of the degree of depth
To 1:1.
Another aspect of the present invention provides a kind of method of catalyst prepared and process for waste water, its bag
Include and on the surface of stainless steel substrate, form nano-pore and by electronation or photochemical by anodic oxidation
Learn reduction to be loaded in nano-pore by metal nanoparticle.
According to one embodiment of the invention, can be the temperature of 5 DEG C to 9 DEG C under agitation with 20V
Anodic oxidation is carried out to the voltage of 60V and the electric current of 0.1A to 6A.
According to another embodiment of the present invention, electronation can be carried out by following steps: will not
Rust steel substrate is immersed in containing in slaine and aqueous acid, and adds reducing agent to aqueous solution.
According to another embodiment of the present invention, slaine can be selected from AgNO3、TiCl3And TiCl4
Water solublity non-ferrous metal salt, acid can be to have the acid of at least one oh group or carboxylic group also
Sodium citrate, gallic acid and its mixture can be selected from, reducing agent can be selected from sodium hydroxide,
Sodium borohydride and the highly basic of its mixture.
According to another embodiment of the present invention, metal can be added with the concentration of 0.001M to 0.05M
Salt.
According to another embodiment of the present invention, stainless steel substrate can be immersed 1 hour or shorter
Time.
According to another embodiment of the present invention, photoreduction can be carried out by following steps:
In dark, in a vacuum stainless steel substrate is immersed containing in slaine and aqueous acid, with distillation
Water and nitrogen clean stainless steel substrate, and irradiate cleaned stainless steel substrate with UV-C light.
According to another embodiment of the present invention, slaine can be selected from AgNO3、TiCl3And TiCl4
Water solublity non-ferrous metal salt.
According to another embodiment of the present invention, metal can be added with the concentration of 0.001M to 0.05M
Salt.
According to another embodiment of the present invention, stainless steel substrate can be immersed 6 hours to 12 hours,
And UV-C light can irradiate 0.5 hour to 2 hours.
Another aspect of the present invention provides a kind of sewage treatment equipment based on advanced oxidation method, its bag
Including ozone reactor and UV generator, wherein ozone reactor includes the catalyst processed for waste water.
The catalyst of the present invention has corrosion resistance and the wearability of excellence, and to pH and variations in temperature
The most stable.Especially, when being applied to waste water based on advanced oxidation method and processing, the present invention urges
Agent makes waste water processing speed increase to twice or more compared with existing catalyst.Therefore, according to this
The use of the catalyst of invention makes cost for wastewater treatment significantly reduce.The catalyst of the present invention can repeat
Re-use and not be used in use after carry out special stabilisation.Different from other existing catalyst, this
The catalyst of invention does not leave precipitate, eliminates the demand to subsequent treatment.The catalyst of the present invention is very
Easily preparation.Additionally, the catalyst of the present invention can be simply applied to existing equipment.Therefore, exist
The catalyst of the present invention can be directly used in the case of needing to process waste water.
Accompanying drawing explanation
In conjunction with accompanying drawing, according to the description of embodiments below, these and/or other aspect of the present invention and
Advantage can become obvious and easier to understand, in described accompanying drawing:
Fig. 1 is to illustrate that the catalyst of the present invention is applied to advanced oxidation method based on UV/ozone
(AOP) schematic diagram of the photochemically reactive mechanism occurred time；
Fig. 2 a to 2d is shown respectively in embodiment 1 the nano-pore stainless steel substrate of preparation, embodiment 2.1
By using hydroxide in catalyst that middle use sodium borohydride is prepared by chemical reaction, embodiment 2.1
The catalyst prepared by photochemical reaction in catalyst prepared by the chemical reaction of sodium and embodiment 2.2
Field emission scanning electron microscope (FE-SEM) figure of surface topography；
Fig. 3 a and 3b is catalyst and the supported titanium of the load silver illustrating preparation in embodiment 2 respectively
The figure of the result of the energy dispersive X-ray spectrum of catalyst；
Fig. 4 schematically shows the sewage treatment equipment based on AOP of the present invention；
Fig. 5 is to illustrate the catalyst of preparation in the stainless steel substrate and embodiment 2 prepared in embodiment 1
It is applied to based on UV/O3AOP time COD removal efficiency the figure of change；
Fig. 6 is to illustrate the catalyst of preparation in the stainless steel substrate and embodiment 2 prepared in embodiment 1
It is applied to based on UV/O3AOP time TOC removal efficiency the figure of change；With
Fig. 7 is to be shown in based on UV/O3AOP in reuse the property of catalyst of the period present invention
The figure that can change.
Detailed description of the invention
Should be understood that the term used in description and claims and word should not be construed as having generally
Implication and dictionary meanings, but the concept of term and word can be defined suitably according to the present inventor
The principle describing his/her invention with the best way is understood as having the technical spirit with the present invention
Corresponding concept.Therefore, embodiment described in description and the structure shown in accompanying drawing only with
Illustrative purpose provides, and is not intended to represent all technical spirits of the present invention.It will be understood, therefore, that
These embodiments and structure can be carried out various equivalent and adjustment when submitting the application to.
It is more fully described the present invention now with reference to accompanying drawing and following example part.
The present invention relates to a kind of for waste water process catalyst, for prepare this catalyst method and
Sewage treatment equipment including this catalyst.Specifically, ozone reactor and UV are included when being applied to
During the sewage treatment equipment based on AOP of generator, make with UV's the catalyst stabilization of the present invention
Reaction maximizes, and can promote the formation of hydroxyl radical free radical, and this is conducive to contaminant removal efficiency
Significantly improve.
Especially, the catalyst of the present invention includes stainless steel substrate and the dress being formed with nano-pore on surface
The metal nanoparticle being downloaded in nano-pore.
Fig. 1 is to illustrate that the catalyst of the present invention is applied to advanced oxidation method based on UV/ozone
(AOP) schematic diagram of the photochemically reactive mechanism occurred time.With reference to Fig. 1, based on UV/O3's
AOP is carried out the most in the following manner: the ultraviolet 121 produced by uviol lamp 120 is irradiated to catalysis
In agent 110, exciting electronic to conduction band by luminous energy, present in the electronics excited and water, oxygen is anti-
Should be to form the superoxide radical for degradation of contaminant.When electronics is excited to conduction band, they
Hole is left in valence band.Hole and water molecule reaction formed also with the OH free radical of pollutant reaction.
Metal nanoparticle 130 is the energy excitation of generation after making to be irradiated on catalyst by light
The conduction band (being represented by dotted lines in the drawings) of electronics reduces.According to this mechanism, i.e. use relatively small amount
Energy also is able to excite electronics, can excite further amounts of electronics with same amount of energy, and this causes increasing
The superoxide radical added and OH free radical synthesis speed.Therefore, the making of catalyst according to the invention
It is effective for being used in promotion contaminant degradation aspect.
Metal nanoparticle can be to prepare conventional that of the catalyst processed for waste water in this area
A bit.Such as, metal nanoparticle can be selected from silver and the nanometer of at least one non-ferrous metal of titanium
Grain.
In the present invention, the spatial form of nano-pore formed on stainless steel substrate and layout and gold
The shapes and sizes of metal nano-particle have appreciable impact to the degradation property of catalyst.Nano-pore is permissible
There is the average diameter of 70nm to 90nm and the mean depth of 20nm to 100nm.Stainless steel substrate
Per unit surface area (1 μm2) nano-pore quantity can be 160 to 200 holes.Metal nano
Granule can be average diameter be the spheroid of 15nm to 50nm.
If the average diameter of nano-pore is less than above-mentioned lower limit, then metal nanoparticle can not be by effectively
Be loaded in nano-pore.Meanwhile, if the average diameter of nano-pore is more than the above-mentioned upper limit, the most stainless
The problem that steel substrate may have durability.If the degree of depth of nano-pore is less than above-mentioned lower limit, then gold
Metal nano-particle can not be loaded in nano-pore effectively.Meanwhile, if the degree of depth of nano-pore is big
In the above-mentioned upper limit, the then problem that stainless steel substrate may have durability.
Nano-pore can be with hole, the 160 to 200 of stainless steel substrate/μm2Density formed.Nano-pore
Density the lowest, make the reaction efficiency (i.e. contaminant degradation performance) of catalyst be deteriorated undesirably.
Meanwhile, the density of nano-pore is the highest, causes the reduction of the average diameter of nano-pore undesirably.
The nano-particle being loaded in nano-pore can be average diameter be the spheroid of 15nm to 50nm.
If the diameter of nano-particle is less than 15nm, then they are probably deficiency to the cohesive force of stainless steel substrate
's.Meanwhile, if the diameter of nano-particle is more than 50nm, then they may to the loading in nano-pore
It is inefficient.
Preferably, average diameter and the degree of depth of nano-pore meets predetermined with the average diameter of nano-particle
Relation.When the average diameter of nano-pore is 2:1 to 5:1 with the ratio of the average diameter of nano-particle and receives
When the average diameter of metre hole and the ratio of the degree of depth are 3:1 to 1:1, it is possible to be effectively realized suitable durability
And adhesion.
The catalyst of the present invention can be prepared by the following method.
Specifically, method includes forming nano-pore on the surface of stainless steel substrate by anodic oxidation,
With by electronation or photoreduction, metal nanoparticle is loaded in nano-pore.
Term " anodic oxidation " generally refers to following reaction: wherein base material such as metal base is immersed electrolyte
In solution, anode is connected to base material, make electric current flow into base material, thus, anode produce oxygen with
Substrate surface forms porous coating.In the method for the invention, first, by anodic oxidation stainless
Nano-pore is formed on steel substrate.The 3-dimensional structure of the nano-pore formed on substrate surface can be according to specifically
Anodic oxidation condition and change.In order to realize the detailed construction size of above-mentioned nano-pore, can be at 5 DEG C
Under agitation anode is carried out with the voltage of 20V to 60V and the electric current of 0.1A to 6A to the temperature of 9 DEG C
Oxidation.
Afterwards, metal nanoparticle is loaded into by receiving that anodic oxidation is formed on stainless steel substrate
In metre hole, complete the preparation of catalyst.
In the method for the invention, the method being used for loading metal nanoparticle is segmented in a broad sense
Two kinds of approach.A kind of chemically based reduction of approach.Electronation can be by immersing stainless steel substrate
Carry out containing in slaine and aqueous acid and adding reducing agent to aqueous solution.
Slaine is the salt compound of the metal on stainless steel substrate to be supported on.Slaine is water solublity
Non-ferrous metal salt.The suitably example of slaine includes but not limited to AgNO3、TiCl3And TiCl4。
Acid can be to have at least one oh group or the acid of carboxylic group and can be selected from sodium citrate, not have
Gallate-based and its mixture.Reducing agent can be selected from sodium hydroxide, sodium borohydride and its mixture
Highly basic.
Slaine can be added with the concentration of 0.001M to 0.05M.If the concentration of slaine is less than
0.001M, then cannot ensure the uniformity of desired metal nanoparticle.Meanwhile, if slaine
Concentration is more than 0.05M, then nano-pore structure may be blocked.
Another kind of approach is based on photoreduction.Photoreduction can be carried out by following steps:
In dark, in a vacuum stainless steel substrate is immersed containing in slaine and aqueous acid, with distillation
Water and nitrogen clean stainless steel substrate, and irradiate cleaned stainless steel substrate with UV-C light.
Slaine is identical with those limited in electronation with the concentration of the kind of acid and slaine.
Stainless steel substrate can be immersed in metal salt solution 6 hours to 12 hours.If the immersion time is shorter than
6 hours, then the metal nanoparticle of q.s can not be loaded on substrate surface the nano-pore formed
In.Meanwhile, if the immersion time more than 12 hours, then takes a long time Method Of Accomplishment, this
It is less desirable economically.UV-C light irradiation time can be adjusted to 0.05 hour to 2 hours.
It is shorter than the irradiation time of 0.5 hour and causes the low rate of reduction of metal ion.Meanwhile, 2 hours it are longer than
Irradiation time is less desirable economically.
When being applied to various sewage treatment equipment, the catalyst of the present invention can show the useless of improvement
Water treatmenting performance.Specifically, as visible in the experimental result from following example part, work as application
Catalyst performance in time including the sewage treatment equipment based on AOP of ozone reactor and UV generator
Go out high COD removal efficiency and TOC removal efficiency, and can repeatedly re-use even without
Carry out special stabilisation after a procedure.
Therefore, the present invention also provides for sewage treatment equipment based on advanced oxidation method (AOP), its
Including ozone reactor and UV generator, wherein ozone reactor includes the catalysis processed for waste water
Agent.
Fig. 4 schematically shows the sewage treatment equipment based on AOP of the present invention.With reference to Fig. 4, this
The equipment of invention includes: ozonator 420, and it is suitable for being produced by the air supplied from air tank 410
Raw ozone；Ozone reactor 430, ozone enter wherein and with pending waste water reaction；Send out with UV
Raw device 440, the uviol lamp 441 that it is included in around ozone reactor.As shown in the figure, catalysis
Agent 450 is arranged in ozone reactor 430 and reacts to realize sewage treatment equipment with ozone 431 etc.
The waste water treatment efficiency significantly improved.
The present invention can be illustrated in greater detail with reference to following example.But, these embodiments are to help
Assistant solves the present invention and provides, and is not intended to limit the scope of the present invention.
Embodiment
Embodiment 1: the preparation of nano-pore stainless steel substrate
Rustless steel (304L) thin film is made to carry out anodic oxidation to be formed with nano-pore not on preparation surface
Rust steel substrate.By being scaling up the size (10mm × 10mm) of existing stainless steel substrate by porous
Stainless steel substrate is designed with the size of 50mm × 60mm.Anode is carried out under following treatment conditions
Oxidation.
The water chuck through double jacket reactor in the thermostat of 5 DEG C of temperature is made to circulate continuously.Utilize
Agitator makes the temperature of electrolyte keep constant.The constant voltage of 40V is kept during whole reaction.
Make stainless steel substrate anodic oxidation 10 minutes.
Fig. 2 a illustrates that in embodiment 1, the Flied emission of the surface topography of the nano-pore stainless steel substrate of preparation is swept
Retouch ultramicroscope (FE-SEM) figure.Observe that nano-pore has average diameter and the 55nm of 80nm
Mean depth.The image of Fig. 2 a further discloses the nano-pore every list with nano-pore stainless steel substrate
Bit surface area (1 μm2) density in 160 to 200 holes formed.
Embodiment 2: metal-doped on the surface of stainless steel substrate
With metal, the stainless steel substrate of preparation in embodiment 1 is doped with preparation for waste water process
Catalyst.Silver or titanium is used to carry out as doping metals and by electronation or photoreduction
Doping.
Embodiment 2.1: electronation
The stainless steel substrate of preparation in embodiment 1 is immersed 0.001M to 0.05M AgNO3、TiCl3
Or TiCl4With in 20mL sodium citrate or Galla Turcica (Galla Helepensis) aqueous acid 10 minutes, and be added to
The 10mM sodium hydroxide of 0.5mL or sodium borohydride.
Embodiment 2.2: photoreduction
The most under vacuo the stainless steel substrate of preparation in embodiment 1 is immersed 0.001M extremely
0.05M AgNO3、TiCl3Or TiCl4Aqueous solution in 12 hours, clean 5 with distilled water and nitrogen
To 10 minutes, and irradiate 1 to 2 hour with UV-C.
Fig. 2 b to 2d is shown respectively in embodiment 2.1 use sodium borohydride by prepared by chemical reaction urging
Agent, embodiment 2.1 are used the catalyst prepared by chemical reaction of sodium hydroxide and embodiment
The field emission scanning electron microscope of the surface topography of the catalyst prepared by photochemical reaction in 2.2
(FE-SEM) figure.Fig. 3 a and 3b is the catalyst of the load silver illustrating preparation in embodiment 2 respectively
Figure with the result of the energy dispersive X-ray spectrum (EDX) of the catalyst of supported titanium.Fig. 2 b is extremely
2d and Fig. 3 a to 3b demonstrates silver and the titanium successful doping on nano-pore stainless steel substrate surface.
Embodiment 3: catalyst is applied to the application in sewage treatment equipment based on advanced oxidation method
In this embodiment, have rated the performance characteristic of the catalyst of preparation in embodiment 2.Specifically,
Use the effluent of production of butanol plant emissions from China evaluate catalyst COD removal efficiency and
TOC removal efficiency.Also been evaluated the performance characteristic reusing rear catalyst.
Neutral range is carried out test without single pH regulator.With consolidating of 5 ml/min
The ozone that constant speed rate produces in waste water ozone supply generator.Power and the ripple of 254nm with 5W
Long use UV lamp produces UV light.
Embodiment 3.1:COD removal efficiency
Initial COD concentration is set to 500mg/L.Target COD value is set to less than 100mg/L,
This is the effluent COD standard of China.Fig. 5 be illustrate in embodiment 1 preparation stainless steel substrate and
In embodiment 2, the catalyst of preparation is applied to based on UV/O3AOP time COD removal efficiency change
The figure changed.With reference to Fig. 5, when there is no applications catalyst (A), the COD obtaining 62.35% in 60 minutes
Removal efficiency.By contrast, when use the nano-pore stainless steel substrate (B) of preparation in embodiment 1,
The catalyst (C) being mounted with silver nano-grain of preparation and preparation in embodiment 2 in embodiment 2
When being mounted with catalyst (D) of titanium, obtain the COD of 64.44%, 70.42% and 77.35% respectively
Removal efficiency.According to these as a result, it is possible to find out the catalyst doped with silver nano-grain and doped with
The catalyst of titanium nano-particle shows the removal efficiency significantly improved compared with other situations.At four kinds
Under different condition, the most in the absence of a catalyst with there is nanometer stainless steel substrate (embodiment
1), doped with the catalyst (embodiment 2) of silver nano-grain and the catalysis doped with titanium nano-particle
In the case of agent (embodiment 2), final COD concentration be respectively 148mg/L, 128mg/L, 99mg/L,
And 70mg/L.These results prove that the catalyst of only embodiment 2 meets the effluent COD mark of China
Accurate (100mg/L).
Embodiment 3.2:TOC removal efficiency
Initial TOC concentration is set to 500mg/L.Fig. 6 is to illustrate the rustless steel of preparation in embodiment 1
In base material and embodiment 2, the catalyst of preparation is applied to based on UV/O3AOP time TOC remove effect
The figure of the change of rate.With reference to Fig. 6, when there is no applications catalyst (A), within 60 minutes, obtain 58.06%
TOC removal efficiency.By contrast, when using the nano-pore stainless steel substrate of preparation in embodiment 1
(B) catalyst (C) being mounted with silver nano-grain, prepared in embodiment 2 and embodiment 2
During catalyst (D) being mounted with titanium nano-particle of middle preparation, obtain 65.32% respectively, 73.79%,
With 82.06% TOC removal efficiency.According to these as a result, it is possible to find out doped with silver nano-grain
Catalyst shows going of significantly improving compared with other situations with the catalyst doped with titanium nano-particle
Except efficiency.The use of catalyst causes the TOC removal efficiency bigger than the difference of COD removal efficiency
Difference.
Embodiment 3.3: reuse the performance of rear catalyst
Every kind of catalyst reuses total 100 times.In order to unanimously, experiment is entered at identical conditions
OK.Fig. 7 is to be shown in based on UV/O3AOP in reuse period catalyst performance change
Figure.With reference to Fig. 7, unrelated with reusable number of times, catalyst all shows almost identical removal effect
Rate.Before and after use, the feature of material does not all have significant difference.It is therefore contemplated that catalyst
Can semi-permanently be used.
Claims (18)
1. the catalyst processed for waste water, described catalyst includes being formed with on surface nano-pore
Stainless steel substrate and the metal nanoparticle that is loaded in described nano-pore.
Catalyst the most according to claim 1, wherein, described metal nanoparticle is selected from silver
Nano-particle with at least one non-ferrous metal of titanium.
Catalyst the most according to claim 1, wherein, described nano-pore has 70nm to 90nm
Average diameter and the mean depth of 20nm to 100nm.
Catalyst the most according to claim 1, wherein, the per unit table of described stainless steel substrate
Area (1 μm2) the quantity of nano-pore be 160 to 200.
Catalyst the most according to claim 1, wherein, described metal nanoparticle is average straight
Footpath is the spheroid of 15nm to 50nm.
Catalyst the most according to claim 1, wherein, the average diameter of described nano-pore and institute
The ratio of the average diameter stating nano-particle is 2:1 to 5:1.
Catalyst the most according to claim 1, wherein, the average diameter of described nano-pore is with deep
The ratio of degree is 3:1 to 1:1.
8. the method preparing the catalyst processed for waste water, described method includes passing through anodic oxygen
Change and on the surface of stainless steel substrate, form nano-pore and pass through electronation or photoreduction by metal
Nano-particle is loaded in nano-pore.
Method the most according to claim 8, wherein, the temperature of 5 DEG C to 9 DEG C under agitation with
The voltage of 20V to 60V and the electric current of 0.1A to 6A carry out described anodic oxidation.
Method the most according to claim 8, wherein, carries out described chemistry also by following steps
Former: described stainless steel substrate to be immersed and contains in slaine and aqueous acid, and to described aqueous solution
Add reducing agent.
11. methods according to claim 10, wherein, described slaine is selected from AgNO3、
TiCl3And TiCl4Water solublity non-ferrous metal salt, described acid is to have at least one oh group or carboxyl
The acid of group is also selected from sodium citrate, gallic acid and its mixture, and described reducing agent is selected from hydrogen-oxygen
Change sodium, sodium borohydride and the highly basic of its mixture.
12. methods according to claim 10, wherein, with the concentration of 0.001M to 0.05M
Add described slaine.
13. methods according to claim 10, wherein, immerse 1 by described stainless steel substrate little
Time or shorter time.
14. methods according to claim 8, wherein, carry out described photochemistry by following steps
Reduction: in the dark, in a vacuum by described stainless steel substrate immerse containing slaine and acid water-soluble
In liquid, clean described stainless steel substrate with distilled water and nitrogen, and cleaned not with the irradiation of UV-C light
Rust steel substrate.
15. methods according to claim 14, wherein, described slaine is selected from AgNO3、
TiCl3And TiCl4Water solublity non-ferrous metal salt.
16. methods according to claim 14, wherein, with the concentration of 0.001M to 0.05M
Add described slaine.
17. methods according to claim 14, wherein, immerse 6 by described stainless steel substrate little
Up to 12 hours, and UV-C light irradiated 0.5 hour to 2 hours.
18. 1 kinds of sewage treatment equipments based on advanced oxidation method, described sewage treatment equipment includes smelly
Oxygen reactor and UV generator, wherein said ozone reactor includes according in claim 1 to 7
The catalyst processed for waste water described in any one.
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| KR102209270B1 (en) * | 2018-12-14 | 2021-01-29 | 한국과학기술연구원 | Sulfated transition metal oxide catalysts for electro-fenton reaction system, electrode comprising the same and electro-fenton reaction system using the same |
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| JP2006051457A (en) | 2004-08-13 | 2006-02-23 | Fuji Photo Film Co Ltd | Silver-supported catalyst and its production method, and silver catalyst support type gas diffusion electrode, and electrolytic oxidation method and electrolytic oxidation system using it, |
| KR101480441B1 (en) * | 2013-04-02 | 2015-01-13 | 한국기계연구원 | Method for surface alloying of porous metal using titanium hydride |
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| EP2065407A1 (en) * | 2007-11-30 | 2009-06-03 | Borealis Technology OY | Random propylene copolymer with high comonomer content |
| JP2012517894A (en) * | 2009-03-27 | 2012-08-09 | バイオニア コーポレーション | Nanoporous membrane and method for producing the same |
| US20130172649A1 (en) * | 2011-12-30 | 2013-07-04 | Sivadinarayana Chinta | Supported nano sized zeolite catalyst for alkylation reactions |
| KR101284610B1 (en) * | 2012-04-09 | 2013-07-17 | 한국과학기술원 | Nanofiber with elliptical pore structure, method for fabricating the same and articles comprising the same |
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