CN103599787B - The method that efficient visible light catalyst is prepared based on ZnCuAl houghites presoma - Google Patents
The method that efficient visible light catalyst is prepared based on ZnCuAl houghites presoma Download PDFInfo
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Abstract
The present invention is the composite oxides ZnO/CuO/ZnAl that photocatalysis efficiency high is obtained on the basis of ternary houghite special construction2O4, metal ion reaches the mixing of atomic level in its complex.Present invention obtains while increasing specific surface area, having obtained that there is loose structure, catalysis material of good performance and preparation method thereof.The present invention is using zinc nitrate, copper, aluminium, strong base-weak acid salt and highly basic etc. are raw material, it is made into mixing and ball milling after salting liquid and aqueous slkali, ball milling suspension is carried out into hydro-thermal ripening at a certain temperature, ternary ZnCuAl LDHs presomas are obtained, presoma is put into Muffle furnace and is calcined 26 hours at 400 800 DEG C, obtain final product product, specific surface area is more than 72 m2·g‑1.Photochemical catalyst specific surface area of the invention is big, there is meso-hole structure.The abundant raw material of the composite photo-catalyst is prepared, cheap, process is simple is reusable.
Description
Technical field
The invention belongs to advanced material and its preparing technical field, it is related to a kind of by ZnCuAl houghite forerunner's systems
The method of standby efficient visible light catalyst, the catalysis material has photocatalytic degradation high to organic dyestuff under visible light illumination
Activity.
Background technology
Hydrotalcite refers to a series of naturally occurring or artificial synthesized clay with layer structure, is by positively charged
Metal oxide layer and the negatively charged anion of interlayer filling are constituted.Because their main component is usually by two kinds of metals
Hydroxide constitute, therefore be called layered di-hydroxyl composite metal oxidate again（Write a Chinese character in simplified form LDH）, by these compound intercalations
A series of supramolecular materials of assembling are referred to as hydrotalcite intercalation material（I.e. houghite, writes a Chinese character in simplified form LDHs）.Due to opening up for LDHs
Flutterring transformation makes hydrotalcite precursor be calcined metal composite oxide adjustable and the two high degree of dispersion of composition for preparing, therefore, this system
The property of the metal composite oxide obtained by standby approach is substantially better than other traditional methods.Additionally, being calcined through houghite
The metal composite oxide for obtaining due to less crystallite dimension, heat endurance and larger specific surface area higher,
Photocatalysis field causes extensive concern.Preparing photochemical catalyst by LDHs precursor process has easy to operate, environmental protection simultaneously,
The characteristics of working well.
LDHs can occur thermal decomposition behavior, including the removing of intermediary water, interlayer anion, laminate hydroxyl at a certain temperature
The step such as dehydration and cenotype generation.What is lost during 200 DEG C of roastings is the combination water of physical absorption water and interlayer；Temperature is in 250-
At 450 DEG C, laminate hydroxyl decomposes dehydration, while having anionic part decomposition；When temperature reaches 450-550 DEG C, dehydration compared with
Completely, more anion are decomposed, the substantially all removing of hydroxyl, CO3 2-It is completely transformed into CO2, generation crystallinity neatly not high
Stone Derived Mixed Oxides.When temperature has exceeded 600 DEG C, then the metal composite oxide being decomposed to form starts sintering and becomes point
Spar MAl2O4And the pyrolytic of MO, i.e. LDHs.The LDHs also interchangeabilities with interlayer anion, according to LDHs body layers
Some feature anion can be introduced LDHs interlayers by the recognition capability of plate, by Supramolecular Assembling, form many function materials
Material.Can enter LDHs interlayers and formed stable crystal anion must alkalescence condition can stable existence, including it is inorganic, have
Machine ion, the anion of same polyion, miscellaneous polyion and complex.General anionic charge amount is higher, and volume is smaller,
Ability into hydrotalcite layers is stronger.
LDHs has the controllability of the Nomenclature Composition and Structure of Complexes, the element species and proportion of composing of its main layer board, interlayer anion
Species and quantity, two-dimensional channel structure can as needed in wide scope modulation, can so change its chemical property obtain institute
The material for needing.Different M2+And M3+With reference to may be constructed binary, ternary and polynary hydrotalcite structure system.LDHs constitute and
The adjustable denaturation of structure and thus obtained multifunctionality, become the new of the great research potential of a class and application prospect
Material.LDHs also has memory effect, and the Derived Mixed Oxides formed after LDHs roastings are in enough humidity（Or water）With
CO2（Or CO3 2-）Under the conditions of can reuptake water and anion, it is a certain degree of to revert to original layer structure.Hydrotalcite
The laminate of material is octahedra by magnesia and alumina octahedral is constituted, with stronger alkalescence, this ratio table higher with product of roasting
Area is relevant with the abundant exposure at alkali center.These properties of LDHs have for preparing porous, high-specific surface area catalysis material
It is of great significance.
The LDHs derivatives for being applied to photocatalysis field are in the majority with bimetal composite oxide, and ternary and above LDHs spread out
The biological application report in terms of photocatalysis is less.When zinc-containing hydrotalcite is as presoma, in high-temperature calcination process, generation
Zinc oxide has amphotericity, can be by the corrosion of alkaline solution institute, while a large amount of generation high-ratio surface network structures in system
Mesoporous gahnite.The zinc oxide for wherein generating can have dispersion to gahnite nano-particle and intercept as template to be made
With, it is suppressed that the growth of gahnite nano-particle, make its particle diameter smaller, meanwhile, zinc oxide self-generating template is being chosen
Meso-hole structure is left after property corrosion.
In view of photocatalysis characteristic of the zinc-aluminum hydrotalcite as advantage and the spinelle zinc/aluminium composite oxide of presoma, will
Cu bivalent cations are configured to ternary ZnCuAl-LDHs simultaneously after introducing, it is intended to utilize ZnO/CuO/ZnAl2O4Collaboration make
With, it is expected to be obtained on the basis of LDHs special constructions with relatively low cost the composite oxides of photocatalysis efficiency high, make to be combined
Metal ion reaches the mixing of atomic level in body.While increasing specific surface area, can obtain with porous structure material, it is real
Now good photocatalysis performance.
The content of the invention
The purpose of the present invention is directed to the defect of current composite photo-catalyst, obtains one kind and is used as by ZnCuAl-LDHs
Presoma, what is responded under visible light contains zinc oxide, cupric oxide and zinc aluminate（There may be a small amount of cupric aluminate）Spinelle
With the composite photo-catalyst of metal oxidation structure and preparation method thereof, obtained photochemical catalyst under the irradiation of visible ray, to water
Methyl orange has stronger photocatalytic degradation capability in solution.The photochemical catalyst has preparation method simple simultaneously, and raw material is easy to get,
Can repeatedly ringing the features such as.
The present invention is with reagents such as commodity zinc nitrate, copper nitrate, aluminum nitrate, sodium carbonate and sodium hydroxids in technical scheme
Raw material, ternary ZnCuAl-LDHs presomas are obtained using hydro-thermal method, and apparent is aterrimus, are obtained after uniform temperature is calcined
Composite oxides catalysis material, apparent is brown.Its specific step of preparation process includes：
(1) salting liquid (A) is prepared：The ratio between amount with certain material weighs the addition of zinc nitrate, copper nitrate and aluminum nitrate and goes
In ionized water, fully dissolving forms solution (A), maintains certain total concentration of metal ions；
(2) aqueous slkali (B) is prepared：MOH（Highly basic）And MnA（Strong base-weak acid salt, An-It is weak acid root）It is dissolved in deionized water
Solution (B) is formed, wherein [An-] ＞ [Al3+], [OH-] ＞ [Cu2+]+[Zn2+]+[Al3+]；
(3) mixing and ball milling：The solution (B) for taking a certain amount of solution (A) and respective amount volume is quickly mixed and added into ball milling
In the ball grinder of machine, with certain frequency ball milling certain hour；
(4) hydro-thermal reaction：By step（3）Obtained ball milling suspension is transferred to the hydro-thermal reaction of inner liner polytetrafluoroethylene
In kettle, in ripening a few hours under uniform temperature；
(5) suction filtration, washing, dry and collection：Product after ripening is naturally cooled into room temperature, then pours into vacuum
Suction filtration in Suction filtration device, with the multiple filtering and washing of deionized water, the solids of acquisition is dried in being put into drying box, obtained final product after grinding
Zn-Cu-Al houghites, product is aterrimus.
(6) solid that step (5) is obtained is put into corundum crucible, is placed in Muffle furnace and is calcined at a certain temperature
A few hours, product is obtained final product, it is brown, sample is characterized, its specific surface area of sample is obtained under optimum condition more than 72 m2·
g-1。
On the basis of such scheme, in the step (1) amount of the material of control zinc nitrate, copper nitrate and aluminum nitrate it
Than being 1~3:1~3:1~3, i.e. any one ion concentration can not be more than 1.5 times of other two kinds of ion concentrations.Three kinds of metals
The concentration sum of ion is up to 1.5 molL-1, minimum 0.5molL-1。
On the basis of such scheme, the highly basic described in step (2) is at least one of NaOH, KOH, and salt of weak acid is at least
Na2CO3、K2CO3、NaAc（Ac-It is acetate）, one of KAc, NaSCN and KSCN.Wherein weak acid ion concentration is Al3+Concentration
1.0~3.0 times, OH-Concentration is Cu2+、Zn2+And Al3+Three kinds the 1.4~1.8 of ion concentration sum times.
On the basis of such scheme, the respective amount volume that solution (B) is added in step (3) is probably solution (A) volume
1/3rd, 1/2nd and it is equal.
On the basis of such scheme, roasting process wants temperature programming in step (6), room temperature between 400 DEG C, heating rate
More than 5 DEG C of min-1, after 400 DEG C, heating rate is less than or equal to 5 DEG C of min-1。
It is presoma the present invention relates to one kind ternary LDHs derivatives, by after high-temperature roasting, generating high-ratio surface knot
The porous gahnite and zinc oxide of structure, the preparation method of cupric oxide nano composite.The composite photocatalyst material for being obtained
Material particle diameter is small, and specific surface area is big, and pore structure is conducive to the suction-operated to organic molecule.Finally greatly improve to organic molecule
Suction-operated and degradation, are a kind of methods of the good catalysis material of processability.Sample is dropped with methyl orange
Solution activity rating shows that the amount of samples that optimum condition is obtained is 0.5 gL-1, it is 25 mgL to concentration-1Methyl orange is molten
Liquid light-catalyzed reaction 1h under simulated solar irradiation, the percent of decolourization of methyl orange reaches more than 93%.
Brief description of the drawings
Fig. 1 is the XRD of optimum condition sample presoma；
Fig. 2 is the SEM figures of optimum condition sample presoma；
Fig. 3 is that the SEM of product after optimum condition sample presoma is calcined through 500 DEG C schemes；
Fig. 4 is the XRD of product after optimum condition sample presoma is calcined through different temperatures.
Specific embodiment
Embodiment 1：
(1) salting liquid is prepared：It is 3 with zinc nitrate, copper nitrate and aluminum nitrate concentration ratio:1:In 1 addition deionized water,
Fully dissolving forms solution, and its total concentration of metal ions is 0.8 molL-1；
(2) aqueous slkali is prepared：NaOH and NaSCN are dissolved in deionized water respectively, [OH is formed respectively-]=1.28
mol·L-1, [SCN-]=0.56 mol·L-1Aqueous slkali；
(3) mixing and ball milling：Take 100mL solution (A) and the quick ball grinder for being mixed and added into ball mill of 50mL solution (B)
In, ball milling frequency is 20 Hz/min, the min of Ball-milling Time 60；
(4) houghite is prepared：Mixed liquor obtained in step (3) is transferred to the water of 200 mL inner liner polytetrafluoroethylenes
In thermal response kettle, the h of ripening 20 at 100 DEG C.Reactor to be naturally cooled to pour into Vacuum filtration device after room temperature and is taken out
Filter, with deionized water filtering and washing repeatedly, the black precipitate of acquisition is put into drying box in drying 4 h at 80 DEG C, and grinding is
Obtain product；
(5) roasting of sample presoma：Step (4) acquisition product is put into corundum crucible, be placed in Muffle furnace in
3 h are calcined at 600 DEG C, brown photocatalyst product is obtained final product.When temperature programming is by less than 400 DEG C, heating rate is 8 DEG C
min-1, after 400 DEG C, 5 DEG C of min of heating rate-1Carry out.
(6) Photocatalytic activity evaluation：Step (5) acquisition product is weighed a certain amount of, light is transferred to after being fully ground
In catalytic reactor, methyl orange is determined as material, the light-catalyzed reaction 1h under simulated solar irradiation is evaluated with degraded methyl orange
Percent of decolourization.The consumption of course of reaction photochemical catalyst is 0.5 gL-1, methyl orange concentration is 100 mgL-1。
Embodiment 2：
(1) salting liquid is prepared：It is 2 with zinc nitrate, nickel nitrate and aluminum nitrate concentration ratio:1:In 1 addition deionized water,
Fully dissolving forms solution, and its total concentration of metal ions is 0.8 molL-1；
(2) aqueous slkali is prepared：By KOH and K2CO3It is dissolved in deionized water respectively, [OH is formed respectively-]=1.32
mol·L-1, [CO3 2-]=0.6 mol·L-1Aqueous slkali；
(3) mixing and ball milling：Take 100 mL solution (A) and the quick ball milling for being mixed and added into ball mill of 33.3mL solution (B)
In tank, ball milling frequency is 30 Hz/min, the min of Ball-milling Time 50；
(4) houghite is prepared：Mixed liquor obtained in step (3) is transferred to the water of 200 mL inner liner polytetrafluoroethylenes
In thermal response kettle, the h of ripening 30 at 90 DEG C.Suction filtration in Vacuum filtration device is poured into after reactor is naturally cooled into room temperature,
With deionized water filtering and washing repeatedly, the black precipitate of acquisition is obtained final product in being put into drying box in dry 4 h at 80 DEG C, grinding
Product；
(5) roasting of sample presoma：Step (4) acquisition product is put into corundum crucible, be placed in Muffle furnace in
4 h are calcined at 500 DEG C, brown photocatalyst product is obtained final product.When temperature programming is by less than 400 DEG C, heating rate is 7 DEG C
min-1, after 400 DEG C, 5 DEG C of min of heating rate-1Carry out.
(6) with the step (6) in embodiment 1.
Embodiment 3：
(1) salting liquid is prepared：It is 1 with zinc nitrate, nickel nitrate and aluminum nitrate concentration ratio:1:In 1 addition deionized water,
Fully dissolving forms solution, and its total concentration of metal ions is 1.2 molL-1；
(2) aqueous slkali is prepared：NaOH and NaAc are dissolved in deionized water respectively, [OH is formed respectively-]=1.9
mol·L-1, [Ac-]=0.8 mol·L-1Aqueous slkali；
(3) with the step (3) in embodiment 1；
(4) houghite is prepared：Mixed liquor obtained in step (3) is transferred to the water of 200 mL inner liner polytetrafluoroethylenes
In thermal response kettle, the h of ripening 40 at 95 DEG C.Suction filtration in Vacuum filtration device is poured into after reactor is naturally cooled into room temperature,
With deionized water filtering and washing repeatedly, the black precipitate of acquisition is obtained final product in being put into drying box in dry 4 h at 80 DEG C, grinding
Product；
(5) roasting of sample presoma：Step (4) acquisition product is put into corundum crucible, be placed in Muffle furnace in
5 h are calcined at 400 DEG C, brown photocatalyst product is obtained final product.Programmed rate is 6 DEG C of min-1。
(6) with the step (6) in embodiment 1.
Embodiment 4：
(1) salting liquid is prepared：It is 1 with zinc nitrate, nickel nitrate and aluminum nitrate concentration ratio:2:In 1 addition deionized water,
Fully dissolving forms solution, and its total concentration of metal ions is 1.0 molL-1；
(2) aqueous slkali is prepared：By NaOH and Na2CO3It is dissolved in deionized water respectively, [OH is formed respectively-]=1.6
mol·L-1, [CO3 2-]=0.50 mol·L-1Aqueous slkali；
(3) mixing and ball milling：Take 100mL solution (A) and the quick ball grinder for being mixed and added into ball mill of 100mL solution (B)
In, ball milling frequency is 30 Hz/min, the min of Ball-milling Time 45；
(4) houghite is prepared：Mixed liquor obtained in step (3) is transferred to the hydro-thermal of 200mL inner liner polytetrafluoroethylenes
In reactor, the h of ripening 48 at 90 DEG C.Suction filtration in Vacuum filtration device is poured into after reactor is naturally cooled into room temperature, is used
Repeatedly, the black precipitate of acquisition obtains final product product to deionized water filtering and washing in being put into drying box in dry 4 h at 80 DEG C, grinding
Product；
(5) roasting of sample presoma：Step (4) acquisition product is put into corundum crucible, be placed in Muffle furnace in
3 h are calcined at 500 DEG C, brown photocatalyst product is obtained final product.Temperature programming is carried out by embodiment (1).
(6) with the step (6) in embodiment 1
Embodiment 5：
(1) salting liquid is prepared：It is 1 with zinc nitrate, nickel nitrate and aluminum nitrate concentration ratio:3:In 1 addition deionized water,
Fully dissolving forms solution, and its total concentration of metal ions is 1.0 molL-1；
(2) with the step (2) in embodiment 4；
(3) mixing and ball milling：Take 100mL solution (A) and the quick ball grinder for being mixed and added into ball mill of 100mL solution (B)
In, ball milling frequency is 30 Hz/min, the min of Ball-milling Time 50；
(4) houghite is prepared：Mixed liquor obtained in step (3) is transferred to the hydro-thermal of 200mL inner liner polytetrafluoroethylenes
In reactor, the h of ripening 30 at 95 DEG C.Suction filtration in Vacuum filtration device is poured into after reactor is naturally cooled into room temperature, is used
Repeatedly, the black precipitate of acquisition obtains final product product to deionized water filtering and washing in being put into drying box in dry 4 h at 80 DEG C, grinding
Product；
(5) roasting of sample presoma：Step (4) acquisition product is put into corundum crucible, be placed in Muffle furnace in
2 h are calcined at 700 DEG C, brown photocatalyst product is obtained final product.When temperature programming is by less than 400 DEG C, heating rate is 8 DEG C
min-1, after 400 DEG C, 5 DEG C of min of heating rate-1Carry out.
(6) with the step (6) in embodiment 1.
Embodiment 6：
(1) salting liquid is prepared：It is 1 with zinc nitrate, nickel nitrate and aluminum nitrate concentration ratio:1:In 2 addition deionized waters,
Fully dissolving forms solution, and its total concentration of metal ions is 1.5 molL-1；
(2) aqueous slkali is prepared：KOH and NaSCN are dissolved in deionized water respectively, [OH is formed respectively-]=1.9
mol·L-1, [SCN-]=1.0 mol·L-1Aqueous slkali；
(3) mixing and ball milling：Take 100mL solution (A) and the quick ball grinder for being mixed and added into ball mill of 100mL solution (B)
In, ball milling frequency is 40 Hz/min, the min of Ball-milling Time 40；
(4) houghite is prepared：Mixed liquor obtained in step (3) is transferred to the hydro-thermal of 200mL inner liner polytetrafluoroethylenes
In reactor, the h of ripening 25 at 100 DEG C.Suction filtration in Vacuum filtration device is poured into after reactor is naturally cooled into room temperature,
With deionized water filtering and washing repeatedly, the black precipitate of acquisition is obtained final product in being put into drying box in dry 4 h at 80 DEG C, grinding
Product；
(5) roasting of sample presoma：Step (4) acquisition product is put into corundum crucible, be placed in Muffle furnace in
1 h is calcined at 800 DEG C, brown photocatalyst product is obtained final product.Temperature programming is carried out by the step (5) in embodiment 5.
(6) with the step (6) in embodiment 1.
Embodiment 7：
(1) salting liquid is prepared：It is 1 with zinc nitrate, nickel nitrate and aluminum nitrate concentration ratio:1:In 3 addition deionized waters,
Fully dissolving forms solution, and its total concentration of metal ions is 1.4 molL-1；
(2) aqueous slkali is prepared：KOH and NaAc are dissolved in deionized water respectively, [OH is formed respectively-]=1.8 mol·
L-1, [Ac-]=1.5 mol·L-1Aqueous slkali；
(3) mixing and ball milling：Take 100mL solution (A) and the quick ball grinder for being mixed and added into ball mill of 50mL solution (B)
In, ball milling frequency is 35 Hz/min, the min of Ball-milling Time 45；
(4) houghite is prepared：Mixed liquor obtained in step (3) is transferred to the hydro-thermal of 200mL inner liner polytetrafluoroethylenes
In reactor, the h of ripening 48 at 90 DEG C.Suction filtration in Vacuum filtration device is poured into after reactor is naturally cooled into room temperature, is used
Repeatedly, the black precipitate of acquisition obtains final product product to deionized water filtering and washing in being put into drying box in dry 4 h at 80 DEG C, grinding
Product；
(5) roasting of sample presoma：Step (4) acquisition product is put into corundum crucible, be placed in Muffle furnace in
1 h is calcined at 600 DEG C, brown photocatalyst product is obtained final product.Temperature programming is carried out by the step (5) in embodiment 5.
(6) with the step (6) in embodiment 1.
It should be noted that：Above example is only to embody technical characteristic of the invention and provide, and not limits this with this
The scope of patent protection of patent of invention request.
Claims (7)
1. one kind obtains efficient composite oxides nano-photocatalyst material on the basis of ternary houghite special construction
Preparation method, it is characterized by：It is that raw material prepares ZnCuAl- by zinc nitrate, copper nitrate, aluminum nitrate, strong base-weak acid salt and highly basic
Houghite presoma, by obtaining composite oxides after roasting, the composite oxides chemical composition is ZnO, CuO, ZnAl2O4。
Its step of preparation process includes：
(1) salting liquid (A) is prepared：Zinc nitrate, copper nitrate and aluminum nitrate are weighed with the ratio between certain amount of material and adds deionization
In water, fully dissolving forms solution (A), maintains certain total concentration of metal ions；
(2) aqueous slkali (B) is prepared：MOH（Highly basic）And MnA（Strong base-weak acid salt）Formation solution (B) in deionized water is dissolved in, wherein
[An-] ＞ [Al3+], [OH-] ＞ [Cu2+]+[Zn2+]+[Al3+]
(3) mixing and ball milling：The solution (B) for taking a certain amount of solution (A) and respective amount volume is quickly mixed and added into ball mill
In ball grinder, with certain frequency ball milling certain hour；
(4) hydro-thermal reaction：By step（3）Obtained ball milling suspension is transferred in the hydrothermal reaction kettle of inner liner polytetrafluoroethylene,
In ripening a few hours under uniform temperature；
(5) suction filtration, washing, dry and collection：Product after ripening is naturally cooled into room temperature, then pours into vacuum filtration
Suction filtration in device, is washed with deionized water multiple filtering and washing, and the solids of acquisition is dried in being put into drying box, obtained final product after grinding
Zn-Cu-Al houghites, product is aterrimus.
(6) solid that step (5) is obtained is put into corundum crucible, is placed in Muffle furnace that to be calcined number at a certain temperature small
When, product is obtained final product, it is brown, sample is characterized, its specific surface area of sample is obtained under optimum condition more than 72m2·g-1。
2. a kind of preparation method of composite oxides nano-photocatalyst material according to claim 1, it is characterised in that step
Suddenly（1）The amount ratio of the middle material for controlling zinc, copper and the metal ion species of aluminium three is 1~3:1~3:1~3, and maintain three kinds of metals
Total ion concentration is 0.5-1.5 molL-1。
3. a kind of preparation method of composite oxides nano-photocatalyst material according to claim 1, it is characterised in that step
Suddenly（2）Described in An-Concentration is Al3+1.0~3.0 times of concentration, OH-Concentration is Cu 2+、Zn2+And Al3+Three kinds of ions are dense
1.4~1.8 times of degree sum.
4. a kind of preparation method of composite oxides nano-photocatalyst material according to claim 1, it is characterised in that step
Suddenly the highly basic described in (2) is at least one of NaOH, KOH, and strong base-weak acid salt is at least Na2CO3、K2CO3、NaAc、KAc、
One of NaSCN and KSCN.
5. a kind of preparation method of composite oxides nano-photocatalyst material according to claim 1, it is characterised in that step
Suddenly solution (B) and the volume ratio of solution (A) are 1 in (3):3、1:2 and 1:One of 1.
6. a kind of preparation method of composite oxides nano-photocatalyst material according to claim 1, it is characterised in that step
Suddenly be calcined 2-6 hour in the Muffle furnace presoma at 400-800 DEG C by (6).Temperature programming is, less than 400 DEG C, heating rate
More than 5 DEG C of min-1；More than 400 DEG C, heating rate is less than or equal to 5 DEG C of min-1。
7. it is a kind of by ZnCuAl- houghites presoma obtain composite oxides nano-photocatalyst material, it is characterised in that institute
It is that the preparation method as described in claim 1-6 any one is obtained to state catalysis material.
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