CN104689839A - Preparation method for Ag-AgCl/attapulgite nano compound photocatalyst - Google Patents
Preparation method for Ag-AgCl/attapulgite nano compound photocatalyst Download PDFInfo
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- CN104689839A CN104689839A CN201510052636.5A CN201510052636A CN104689839A CN 104689839 A CN104689839 A CN 104689839A CN 201510052636 A CN201510052636 A CN 201510052636A CN 104689839 A CN104689839 A CN 104689839A
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Abstract
The invention relates to a preparation method for an Ag-AgCl/attapulgite nano compound photocatalyst and belongs to the technical field of compound materials and photocatalysis. The preparation method comprises the following steps: with silver nitrate, hydrochloric acid and attapulgite as raw materials, synthesizing the Ag-AgCl/attapulgite nano compound photocatalyst with visible-light response and high activity by adopting a deposition-precipitation method and a photo-reduction method, and carrying out representation on the phase structure and the micro-topography of the photocatalyst by utilizing the technologies such as X-ray powder diffraction (XRD), a scanning electron microscope (SEM), special surface area and porosity analysis (BET), infrared spectrum (IR) and ultraviolet absorption spectrum (UV). The preparation method has the advantages that the catalytic degradation performance of the Ag-AgCl/attapulgite nano compound photocatalyst for methylene blue (MB) is checked under the visible-light condition (lambda is more than or equal to 420nm), and shown by a result, the catalytic performance of the compound material is improved by 11.14 times than that of pure Ag-AgCl when the Ag-AgCl loading rate is 30%.
Description
Technical field
The invention belongs to technical field of composite materials, relate to a kind of preparation of nano-composite catalyst, particularly relate to a kind of preparation method of Ag-AgCl/ palygorskite nano composite photo-catalyst, the present invention has also investigated the catalytic degradation performance of Ag-AgCl/ palygorskite nano composite photo-catalyst for methylene blue (MB) simultaneously.
Background technology
In recent years, along with environmental pollution increasingly sharpens, utilize the photocatalysis technology of semi-conducting material to curb environmental pollution and more and more cause the attention of people, semiconductor catalyst is applied to contaminant degradation and attracts wide attention.Noble metal nano particles is applied to the fields such as photocatalytically degradating organic dye because having surface plasma resonance effect and becomes study hotspot.Being wherein plasma photocatalysis agent with Ag and Ag and silver halide composite nanoparticle, research is relatively many.Ag/AgX(X=Cl, Br, I) plasma resonance photochemical catalyst to dyestuff selective low, processing speed is fast, degradation rate is high, good stability, has good application prospect in treatment of Organic Wastewater field.The Ag-AgCl catalysis material under visible light at present with catalytic performance has been reported, ion-exchange and photoreduction method as being seen in report synthesized different-shape Ag@AgCl plasma resonance photochemical catalyst (
chemistry A:
european Journal, 2010,16(2): 538-544); Support type Ag-AgCl/Al
2o
3photochemical catalyst (artificial lens journal, 2011,40(6): 1563-1568); Ag@AgCl/TiO
2/ SnO
2surface plasma type composite photocatalyst material (
chemical Communications, 2007,41:4291-4293) etc.But, no matter which kind of synthetic method, all wishes obtain the more tiny Ag-AgCl nano particle of particle or make catalyst have larger specific area, to improve photocatalysis efficiency, but the Ag-AgCl nano particle stability that size is less declines, and easily reunites between nanometer.
Attapulgite clay (Attapulgite clay) has another name called palygorskite (palygorskite), be a kind of layer of chain structure containing Shuifu County's magnesium alumino metasilicate clay mineral, in crystal structure, there is a series of nano zeolite duct, make its specific area large, have very strong physical absorption ability.In addition due to law of isomorphism displacement in crystal, crystal defect and room, make attapulgite with surface negative charge, and rely on the cation of Inter layer adsorption to make charge balance.Thus there is the cationic character of exchange adsorption.Gansu Attapulgite Clay stone ore aboundresources, is mainly distributed in Linze, understands the areas such as peaceful, prospective reserves about about 1,000,000,000 tons.Zhangye Linze county attapulgite is of high grade, and reserves are large, are rich in the trace element such as iodine, strontium.Owing to having the zeolite cavity of larger specific area and numerous nano-scales, thus there is a large amount of active centres in attapulgite clay, has stronger mechanical performance and thermal stability, absorption property and catalytic oxidation performance good.Therefore by attapulgite clay and Ag-AgCl Nanocomposites, make Ag-AgCl with plasma load in concave convex rod surface, catalyst is made to have larger specific area, to improve the photocatalysis efficiency of Ag-AgCl, and the photocatalytic oxidation of semiconductor is utilized to decompose the dye molecule of attapulgite clay adsorption.
Summary of the invention
Object of the present invention provides a kind of preparation method of Ag-AgCl/ palygorskite nano composite photo-catalyst.
one,the preparation of Ag-AgCl/ palygorskite nano composite photo-catalyst
By the attapulgite ultrasonic disperse of purification in deionized water, add AgNO
3solution (0.1 ~ 0.3molL
-1) ultrasonic, stir and make it be uniformly dispersed, then add HCl solution (0.1 ~ 0.3molL
-1; ) ultrasonic disperse evenly afterwards stir make it fully react; Filter, spend deionized water, after drying, then irradiate with Metal halogen lamp, part Ag in the AgCl that reaction is generated
+be reduced into Ag, obtain Ag-AgCl/ palygorskite nano composite photo-catalyst.
In the preparation process of nano composite material, by control AgNO
3the mass percent of the addition control Ag-AgCl of solution and HCl solution.Work as AgNO
3control at 1:5 ~ 1:1.2 with the mass ratio of attapulgite; AgNO
3during with the mole proportioning of HCl with 1:1 ~ 1:3, Ag-AgCl mass percent is in the composite 15 ~ 40%.By Ag in the power of Metal halogen lamp and irradiation time control AgCl
+be reduced into the amount of Ag.When power is 400W, when irradiation time is 20 ~ 30min, in Ag-AgCl/ attapulgite composite photo-catalyst, Ag and AgCl is had to coexist.
Two, the structure of Ag-AgCl/ palygorskite nano composite photo-catalyst
For the ease of comparing, we have also prepared pure Ag-AgCl: by AgNO
3solution and HCl solution (AgNO
3with HCl equimolar amounts) hybrid reaction obtains white precipitate, and filter, drying obtains AgCl solid, then irradiates at Metal halogen lamp and makes part Ag
+be reduced into Ag and namely obtain Ag-AgCl.
1, the XRD analysis of composite photo-catalyst
Fig. 1 is the XRD spectra of concave convex rod (a) and Ag-AgCl/ attapulgite composite photo-catalyst (b).As can be seen from a curve, in 2 θ=8.4 °, there is obvious attapulgite (ATP) characteristic diffraction peak at 19.8 °, 26.7 ° and 34.9 ° of places; As can be seen from b curve, 2
θthe diffraction maximum at=27.82 °, 32.23 °, 46. 23 °, 54. 82 °, 57. 48 °, 67.50 ° and 76.67 ° places corresponds respectively to (111), (200), (220) of AgCl, (311), (222), (400) and (420) crystal face (PDF No.85-1355).Simultaneously 2
θthere is the more weak characteristic diffraction peak corresponding to Ag species (111) crystal face (PDF No.89-3722) in=38.20 ° of places, the more weak reason of its diffraction maximum may be due to its particle diameter is too little or amount few caused by, illumination condition lower part Ag is described
+successfully be reduced to elemental silver, in Ag-AgCl/ attapulgite composite photo-catalyst, had the coexisting structure of Ag and AgCl.
2, the Morphology analysis of composite photo-catalyst
Fig. 2 is pure Ag-AgCl(a), the exterior appearance of attapulgite clay (b) and Ag-AgCl/ attapulgite composite photo-catalyst (c) sample.Can see that pure Ag-AgCl is random block structure from Fig. 2 (a), have larger agglomerated microparticles to exist, wherein less as seen Ag simple substance bead, crystallization degree is comparatively complete.It is loose fiber shape structure that Fig. 2 (b) shows attapulgite.From 2(c) the stacking comparatively mixed and disorderly of micro-whisker Ag-AgCl/ attapulgite composite photo-catalyst can be found out, reunite comparatively serious, but greatly take on a new look than pure Ag-AgCl.
3, infrared spectrum analysis
Fig. 3 is pure Ag-AgCl(a), the Fourier transform infrared spectroscopy of attapulgite (b) and Ag-AgCl/ attapulgite composite photo-catalyst (c).All samples is at 3613cm
-1left and right place and 1640cm
-1all there is absworption peak at left and right place, is respectively OH
-stretching vibration absworption peak and the deformation vibration absworption peak of hydrone.This illustrates that undersized composite material surface adsorption activity is higher, the hydrone in easy absorbed air, and this is conducive to absorption degradation thing in Photocatalytic Degradation Process equally.The 3613cm of Fig. 3 b
-1and 3405cm
-1place's absworption peak belongs to the stretching vibration of different hydroxyl in attapulgite structure; 1646cm
-1absworption peak is the flexural vibrations belonging to adsorbed water and intermediary water hydroxyl; 1041,980,474cm
-1it is the characteristic infrared absorption of attapulgite; 1197cm
-1come from the distinctive stretching vibration of (Mg, Al) O key in attapulgite; Fig. 3 c is at 800cm
-1near have obvious background absorption, this absorption can be attributed to the absorption of vibrations of Ag-O.
4, specific surface area analysis
Fig. 4 is the N of concave convex rod and Ag-AgCl/ palygorskite nano composite photo-catalyst
2adsorption-desorption isothermal.According to the BET surface area of the adsorpting data calculation sample of relative pressure between 0.06 ~ 0.30.Result shows, N
2adsorption-desorption isothermal is all in typical IUPAC II type adsorpting characteristic, and have obvious hysteresis loop, known obtained product is mesoporous material.The shape of curve belongs to the IVth class thermoisopleth substantially, two equal corresponding H of curve
3type lag loop.The specific area of composite photo-catalyst is 89.6696 m
2g
-1, be greater than specific area 0.0278 m of pure Ag-AgCl
2g
-1.The specific area that composite photo-catalyst is larger can provide more adsorption site for reactant molecule, is conducive to reactant at the absorption of catalyst surface and mass transfer.
Three, the degradation property of composite photo-catalyst
1, UV absorption spectroanalysis
Fig. 5 is that Ag-AgCl/ attapulgite composite photo-catalyst is to the variation relation figure of the UV-Vis absorption spectrum of methylene blue solution Photocatalytic Degradation Process with light application time.As can be seen from Figure 5, under visible light illumination, along with the increase of light application time; dye solution obviously weakens in absorption peak strength that is visible and ultra-violet (UV) band; illumination 100 min, visible absorbance peak is blue shifted to 651 nm by 664 nm, and this is relevant with the demethylation of methylene blue molecule; Ultraviolet absorption peak is blue shifted to 286 nm by 291 nm, and this is relevant with de-amido effect, illustrates that methylene blue there occurs photocatalytic degradation reaction on composite catalyst.
2, the light-catalyzed reaction of nano-composite catalyst
Light-catalyzed reaction is carried out in the glass reactor (concentric double-layer cylindrical unit) of recirculated cooling water, light source is the metal halide lamp of 500W, 10 mg Ag-AgCl/ palygorskite nano composite photo-catalysts are joined 80 mL methylene blues (MB, 10 mgL
-1) in solution, lucifuge magnetic agitation 30min, to reach adsorption-desorption balance.Pass into cooling water, cover optical filter (light of elimination 420 below nm, to guarantee that the light passed through is for visible ray), then open light source.Stirring is reacted, and pipettes the reactant liquor of 5.0 mL in centrifuge tube, 4000 rmin every 20 min pipettors
-1centrifugal 10 min, Aspirate supernatant, measures centrifuged supernatant with V-1200 type visible spectrophotometer and exists
λ maxthe absorbance at=664 nm places, utilizes working curve (C=5.1316A-0.01831, the R of dyestuff MB
2=0.99914) calculate the concentration of solution, according to formula (1) and (2) calculate respectively composite to the adsorbance of dyestuff (
a t %) and the degradation rate of dyestuff in illumination reaction process (
d t%) can be expressed as:
A t ％=(
c e-
c o )×100%/
c e (1)
D t％=(
c o -
c t )×100% /
c o (2)
Generally, Longmuir-Hinshelwood (L-H) kinetics equation (3) is followed in the reaction of photocatalysis degradation organic contaminant:
(3)
When reactant initial concentration is less, above formula can be reduced to apparent first order reaction kinetic, is represented (4) by the kinetics equation of MB photocatalytic degradation following formula:
ln(
c o /c t )=
kKt=k app t (4)
r(mgL
-1min
-1) be reaction rate;
k(mgL
-1min
-1) be reaction rate constant;
k(Lmg
-1) be the adsorption equilibrium constant;
k app(min
-1) be reaction-rate constant;
c e(mgL
-1) be the original concentration of MB solution;
c o (mgL
-1) equilibrium concentration of rear MB solution has been reacted for adding catalyst dark adsorption;
c t(mgL
-1) be
tthe mass concentration of moment MB solution;
t(min) be the reaction time.
Fig. 6 is the first order kinetics linearity relation of different photochemical catalyst under visible light conditions (mass fraction of Ag-AgCl is different) degradation of methylene blue.The result of Fig. 6 display illustrates, in composite, the mass fraction of Ag-AgCl has a great impact rate of photocatalytic oxidation, along with the increase of the mass fraction of Ag-AgCl, and the change that rate of photocatalytic oxidation is uneven.When the mass fraction of Ag-AgCl is 30%, photocatalytic activity reaches and is 96.04% to the maximum, improves 11.14 times than the catalytic performance of pure Ag-AgCl.When mass ratio increases further, rate of photocatalytic oxidation reduces on the contrary.Reason may be, lower quality than time, the reactivity position that catalyst provides is less, and the concentration that in unit volume solution, photo-generate electron-hole is right is lower, causes catalytic efficiency lower; Along with the increase of mass ratio in catalyst, the particle number participating in light-catalyzed reaction increases, and thus reaction speed is accelerated; And higher quality than time, because excessively strong modification causes light scattering on the one hand, light transmittance is declined, the effective rate of utilization of light reduces, thus cause light degradation rate reduction, may be because excessively strong modification adds the recombination rate of Ag-AgCl/ attapulgite composite material surface electron-hole in solution on the other hand, reduce the activity of catalyst on the contrary.
In sum, the present invention purify attapulgite clay and AgNO
3solution contacts, and makes Ag
+adsorb or be stored in the capillary micropore of attapulgite clay, adding HCl solution and make to adsorb or be stored in Ag in the capillary micropore of attapulgite clay
+be converted into AgCl.Part Ag in the AgCl of generation is made again with photoreduction met hod
+be reduced into Ag under light illumination, thus obtain the attapulgite surface plasma nano composite photo-catalyst of loaded Ag-AgCl, for methylene blue (MB), there is good degradation property, therefore in the contaminant degradations such as methylene blue, have potential application prospect.
Accompanying drawing explanation
The XRD spectra of Fig. 1 concave convex rod and Ag-AgCl/ concave convex rod composite photo-catalyst
The pure Ag-AgCl(a of Fig. 2), the SEM photo of attapulgite (b) and Ag-AgCl/ attapulgite composite photo-catalyst (c)
The IR spectrogram of Fig. 3 Ag-AgCl, concave convex rod and Ag-AgCl/ concave convex rod composite photo-catalyst
The N of Fig. 4 concave convex rod and Ag-AgCl/ concave convex rod composite photo-catalyst
2adsorption-desorption isothermal
The UV absorption spectrum of Fig. 5 Ag-AgCl/ concave convex rod composite photo-catalyst
The first order kinetics linearity relation of different photocatalytic degradation methylene blue under Fig. 6 visible light conditions.
Detailed description of the invention
Below by specific embodiment, the preparation of composite photocatalyst material of the present invention and degradation property are described further.
Embodiment 1
1 g attapulgite is poured in beaker, adds 20ml deionized water, in room temperature ultrasonic disperse 10 min, adds 13 ml 0.1 molL
-1agNO
3solution, at stirring at normal temperature 20 min after ultrasonic 10 min, adds 13 ml 0.1 molL
-1by ultrasonic for mixed solution 10 min after HCl solution, stirring at room temperature 20 min, filters; Clean by deionized water, powder, after 102 DEG C of drying 10 h, irradiates 10 min under 400W Metal halogen lamp, makes part Ag in the AgCl of generation
+be reduced into Ag under light illumination, obtain Ag-AgCl and load to surface plasma nano composite photo-catalyst Ag-AgCl/ attapulgite on attapulgite.In composite, the mass fraction of Ag-AgCl is 15%, reaches 82.61% to the degradation rate of methylene blue.
Embodiment 2
Taking 1 g attapulgite pours in beaker, adds 20ml deionized water, in room temperature ultrasonic disperse 10 min, adds 18 ml 0.1 molL
-1agNO
3solution, at stirring at normal temperature 20 min after ultrasonic 10 min, adds 1 ml 0.2 molL
-1by ultrasonic for mixed solution 10 min after HCl solution, stirring at room temperature 20 min, filters; Clean by deionized water, powder, after 102 DEG C of drying 10 h, irradiates 15 min under 400W Metal halogen lamp, makes part Ag in the AgCl of generation
+be reduced into Ag under light illumination, obtain Ag-AgCl and load to surface plasma nano composite photo-catalyst Ag-AgCl/ attapulgite on attapulgite.In composite, the mass fraction of Ag-AgCl is 20%, reaches 88.47% to the degradation rate of methylene blue.
Embodiment 3
Taking 1 g attapulgite pours in beaker, adds 20ml deionized water, in room temperature ultrasonic disperse 10 min, adds 30 ml 0.1 molL
-1agNO
3solution, at stirring at normal temperature 20 min after ultrasonic 10 min, adds 10 ml 0.3 molL
-1by ultrasonic for mixed solution 10 min after HCl solution, stirring at room temperature 20 min, filters; Clean by deionized water, powder, after 102 DEG C of drying 10 h, irradiates 20 min under 400W Metal halogen lamp, makes part Ag in the AgCl of generation
+be reduced into Ag under light illumination, obtain Ag-AgCl and load to surface plasma nano composite photo-catalyst Ag-AgCl/ attapulgite on attapulgite.In composite, the mass fraction of Ag-AgCl is 30%, reaches 97.31% to the degradation rate of methylene blue.
Embodiment 4
Taking 1 g attapulgite pours in beaker, adds 20ml deionized water, in room temperature ultrasonic disperse 10 min, adds 48 ml 0.1 molL
-1agNO
3solution, at stirring at normal temperature 20 min after ultrasonic 10 min, adds 24 ml 0.2 molL
-1by ultrasonic for mixed solution 10 min after HCl solution, stirring at room temperature 20 min, filters; Clean by deionized water, powder, after 102 DEG C of drying 10 h, irradiates 30 min under 400W Metal halogen lamp, makes part Ag in the AgCl of generation
+be reduced into Ag under light illumination, obtain Ag-AgCl and load to surface plasma nano composite photo-catalyst Ag-AgCl/ attapulgite on attapulgite.In composite, the mass fraction of Ag-AgCl is 40%, reaches 91.44% to the degradation rate of methylene blue.
Claims (6)
- The preparation method of 1.Ag-AgCl/ palygorskite nano composite photo-catalyst, be by purify attapulgite ultrasonic disperse in deionized water, add AgNO 3solution is ultrasonic, stirring makes AgNO 3dispersed, then add HCl solution ultrasonic disperse evenly afterwards stir make itself and AgNO 3abundant reaction; Filter, spend deionized water, dry, then irradiate with Metal halogen lamp, part Ag in the AgCl that reaction is generated +be reduced into Ag, obtain Ag-AgCl/ concave convex rod nano-composite catalyst.
- 2. the preparation method of Ag-AgCl/ concave convex rod nano-composite catalyst as claimed in claim 1, is characterized in that: AgNO 3be 1:5 ~ 1:1.2 with the mass ratio of concave convex rod.
- 3. the preparation method of Ag-AgCl/ concave convex rod nano-composite catalyst as claimed in claim 1, is characterized in that: AgNO 3with the mol ratio 1:1 ~ 1:3 of HCl.
- 4. the preparation method of Ag-AgCl/ concave convex rod nano-composite catalyst as claimed in claim 1, is characterized in that: AgNO 3the concentration of solution is 0.1 ~ 0.3molL -1.
- 5. the preparation method of Ag-AgCl/ concave convex rod nano-composite catalyst as claimed in claim 1, is characterized in that: the concentration of HCl solution is 0.1 ~ 0.3molL -1.
- 6. the preparation method of Ag-AgCl/ concave convex rod nano-composite catalyst as claimed in claim 1, is characterized in that: the power of Metal halogen lamp is 400W, and irradiation time is 10 ~ 30 min.
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105289671A (en) * | 2015-10-31 | 2016-02-03 | 江苏师范大学 | Ag/AgCl loaded sodium nickel phosphate composite photocatalytic material as well as preparation method and application thereof |
| CN106046602A (en) * | 2016-06-30 | 2016-10-26 | 襄阳南洁高分子新型材料有限公司 | Research and development technique of nano silver/silver chloride PVC antibacterial preservative film |
| CN110560027A (en) * | 2019-08-16 | 2019-12-13 | 南京理工大学 | silver halide-biotite composite photocatalyst and preparation method thereof |
| CN110787791A (en) * | 2019-11-15 | 2020-02-14 | 南宁师范大学 | New application of illite/montmorillonite clay, composite photocatalyst prepared from illite/montmorillonite clay and preparation method of composite photocatalyst |
| CN111604068A (en) * | 2020-06-21 | 2020-09-01 | 安徽理工大学 | Ag-AgBr/TiO2Method for preparing nano-rod composite array film |
| CN115254186A (en) * | 2022-08-22 | 2022-11-01 | 江南大学 | Nano-silver/silver chloride/supermolecule perylene bisimide derivative composite photocatalyst and preparation method and application thereof |
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| CN101947464A (en) * | 2010-08-06 | 2011-01-19 | 淮阴工学院 | Preparation method of attapulgite clay composite visible light catalyst |
| CN102407149A (en) * | 2011-11-04 | 2012-04-11 | 武汉理工大学 | Preparation method of Ag-AgBr/attapulgite composited photocatalysis material |
-
2015
- 2015-02-02 CN CN201510052636.5A patent/CN104689839B/en not_active Expired - Fee Related
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101947464A (en) * | 2010-08-06 | 2011-01-19 | 淮阴工学院 | Preparation method of attapulgite clay composite visible light catalyst |
| CN102407149A (en) * | 2011-11-04 | 2012-04-11 | 武汉理工大学 | Preparation method of Ag-AgBr/attapulgite composited photocatalysis material |
Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105289671A (en) * | 2015-10-31 | 2016-02-03 | 江苏师范大学 | Ag/AgCl loaded sodium nickel phosphate composite photocatalytic material as well as preparation method and application thereof |
| CN106046602A (en) * | 2016-06-30 | 2016-10-26 | 襄阳南洁高分子新型材料有限公司 | Research and development technique of nano silver/silver chloride PVC antibacterial preservative film |
| CN110560027A (en) * | 2019-08-16 | 2019-12-13 | 南京理工大学 | silver halide-biotite composite photocatalyst and preparation method thereof |
| CN110560027B (en) * | 2019-08-16 | 2022-08-12 | 南京理工大学 | Silver halide-biotite composite photocatalyst and preparation method thereof |
| CN110787791A (en) * | 2019-11-15 | 2020-02-14 | 南宁师范大学 | New application of illite/montmorillonite clay, composite photocatalyst prepared from illite/montmorillonite clay and preparation method of composite photocatalyst |
| CN110787791B (en) * | 2019-11-15 | 2022-09-30 | 南宁师范大学 | New application of illite/montmorillonite clay, composite photocatalyst prepared from illite/montmorillonite clay and preparation method of composite photocatalyst |
| CN111604068A (en) * | 2020-06-21 | 2020-09-01 | 安徽理工大学 | Ag-AgBr/TiO2Method for preparing nano-rod composite array film |
| CN111604068B (en) * | 2020-06-21 | 2022-10-28 | 安徽理工大学 | Ag-AgBr/TiO 2 Method for preparing nano-rod composite array film |
| CN115254186A (en) * | 2022-08-22 | 2022-11-01 | 江南大学 | Nano-silver/silver chloride/supermolecule perylene bisimide derivative composite photocatalyst and preparation method and application thereof |
| CN115254186B (en) * | 2022-08-22 | 2024-02-27 | 江南大学 | Nano silver/silver chloride/supermolecule perylene imide derivative composite photocatalyst and preparation method and application thereof |
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| CN104689839B (en) | 2017-05-31 |
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