CN106868633B - A kind of strontium titanates/dioxide composite nanofiber and preparation method thereof - Google Patents
A kind of strontium titanates/dioxide composite nanofiber and preparation method thereof Download PDFInfo
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- CN106868633B CN106868633B CN201710134054.0A CN201710134054A CN106868633B CN 106868633 B CN106868633 B CN 106868633B CN 201710134054 A CN201710134054 A CN 201710134054A CN 106868633 B CN106868633 B CN 106868633B
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- 239000002131 composite material Substances 0.000 title claims abstract description 24
- 239000002121 nanofiber Substances 0.000 title claims abstract description 17
- 229910052712 strontium Inorganic materials 0.000 title claims abstract description 10
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 title claims abstract description 10
- 238000002360 preparation method Methods 0.000 title claims description 8
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims abstract description 50
- 229910002370 SrTiO3 Inorganic materials 0.000 claims abstract description 21
- 239000000835 fiber Substances 0.000 claims abstract description 18
- 238000010041 electrostatic spinning Methods 0.000 claims abstract description 4
- 239000004408 titanium dioxide Substances 0.000 claims abstract description 3
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 claims description 15
- 238000009987 spinning Methods 0.000 claims description 12
- 239000000243 solution Substances 0.000 claims description 10
- 239000005030 aluminium foil Substances 0.000 claims description 6
- 230000015572 biosynthetic process Effects 0.000 claims description 6
- 239000000203 mixture Substances 0.000 claims description 6
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 claims description 6
- 229920000036 polyvinylpyrrolidone Polymers 0.000 claims description 6
- 239000001267 polyvinylpyrrolidone Substances 0.000 claims description 6
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 5
- 239000013078 crystal Substances 0.000 claims description 4
- RXSHXLOMRZJCLB-UHFFFAOYSA-L strontium;diacetate Chemical compound [Sr+2].CC([O-])=O.CC([O-])=O RXSHXLOMRZJCLB-UHFFFAOYSA-L 0.000 claims description 4
- FPCJKVGGYOAWIZ-UHFFFAOYSA-N butan-1-ol;titanium Chemical compound [Ti].CCCCO.CCCCO.CCCCO.CCCCO FPCJKVGGYOAWIZ-UHFFFAOYSA-N 0.000 claims description 3
- 238000010438 heat treatment Methods 0.000 claims description 3
- 239000011259 mixed solution Substances 0.000 claims description 3
- 239000002243 precursor Substances 0.000 claims description 3
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 claims 2
- 229960000583 acetic acid Drugs 0.000 claims 1
- 239000012362 glacial acetic acid Substances 0.000 claims 1
- 230000001699 photocatalysis Effects 0.000 abstract description 13
- 238000000034 method Methods 0.000 abstract description 9
- 239000000463 material Substances 0.000 abstract description 5
- 229910002367 SrTiO Inorganic materials 0.000 abstract description 3
- STZCRXQWRGQSJD-GEEYTBSJSA-M methyl orange Chemical compound [Na+].C1=CC(N(C)C)=CC=C1\N=N\C1=CC=C(S([O-])(=O)=O)C=C1 STZCRXQWRGQSJD-GEEYTBSJSA-M 0.000 abstract description 3
- 229940012189 methyl orange Drugs 0.000 abstract description 3
- 239000002957 persistent organic pollutant Substances 0.000 abstract description 3
- RBTBFTRPCNLSDE-UHFFFAOYSA-N 3,7-bis(dimethylamino)phenothiazin-5-ium Chemical compound C1=CC(N(C)C)=CC2=[S+]C3=CC(N(C)C)=CC=C3N=C21 RBTBFTRPCNLSDE-UHFFFAOYSA-N 0.000 abstract 1
- 229960000907 methylthioninium chloride Drugs 0.000 abstract 1
- 238000013033 photocatalytic degradation reaction Methods 0.000 abstract 1
- 230000000694 effects Effects 0.000 description 5
- 238000011160 research Methods 0.000 description 5
- 239000003054 catalyst Substances 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- 238000007146 photocatalysis Methods 0.000 description 4
- 230000003197 catalytic effect Effects 0.000 description 3
- 238000006731 degradation reaction Methods 0.000 description 3
- HEDRZPFGACZZDS-UHFFFAOYSA-N Chloroform Chemical compound ClC(Cl)Cl HEDRZPFGACZZDS-UHFFFAOYSA-N 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 2
- 230000015556 catabolic process Effects 0.000 description 2
- 238000006555 catalytic reaction Methods 0.000 description 2
- 230000007812 deficiency Effects 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 239000006185 dispersion Substances 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- -1 hydroxyl radical free radical Chemical class 0.000 description 2
- 239000001048 orange dye Substances 0.000 description 2
- 239000011941 photocatalyst Substances 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 235000021419 vinegar Nutrition 0.000 description 2
- 239000000052 vinegar Substances 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 1
- 238000009303 advanced oxidation process reaction Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000000711 cancerogenic effect Effects 0.000 description 1
- 231100000315 carcinogenic Toxicity 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000006056 electrooxidation reaction Methods 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 231100000086 high toxicity Toxicity 0.000 description 1
- 230000001678 irradiating effect Effects 0.000 description 1
- 230000031700 light absorption Effects 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- XNGIFLGASWRNHJ-UHFFFAOYSA-N o-dicarboxybenzene Natural products OC(=O)C1=CC=CC=C1C(O)=O XNGIFLGASWRNHJ-UHFFFAOYSA-N 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 238000010525 oxidative degradation reaction Methods 0.000 description 1
- 238000006385 ozonation reaction Methods 0.000 description 1
- 150000003071 polychlorinated biphenyls Chemical class 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 239000002351 wastewater Substances 0.000 description 1
Classifications
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- D—TEXTILES; PAPER
- D01—NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
- D01F—CHEMICAL FEATURES IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS; APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OF CARBON FILAMENTS
- D01F9/00—Artificial filaments or the like of other substances; Manufacture thereof; Apparatus specially adapted for the manufacture of carbon filaments
- D01F9/08—Artificial filaments or the like of other substances; Manufacture thereof; Apparatus specially adapted for the manufacture of carbon filaments of inorganic material
-
- 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
- B01J23/002—Mixed oxides other than spinels, e.g. perovskite
-
- 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
- B01J23/02—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the alkali- or alkaline earth metals or beryllium
- B01J23/04—Alkali metals
-
- 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
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/39—Photocatalytic properties
-
- 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
- B01J35/58—Fabrics or filaments
-
- D—TEXTILES; PAPER
- D01—NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
- D01D—MECHANICAL METHODS OR APPARATUS IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS
- D01D1/00—Treatment of filament-forming or like material
- D01D1/02—Preparation of spinning solutions
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Textile Engineering (AREA)
- Mechanical Engineering (AREA)
- General Chemical & Material Sciences (AREA)
- Catalysts (AREA)
- Inorganic Compounds Of Heavy Metals (AREA)
Abstract
The present invention prepares strontium titanates/titanium dioxide (Rutile Type) composite nano-fiber material of 100-200nm using a step method of electrostatic spinning, and method is easy, strong operability.Gained fiber size is controllable, it is good to be distributed uniform and continuity.SrTiO prepared by the present invention3/TiO2(Rutile Type) composite nano fiber compares single TiO2(Rutile Type) and single SrTiO3Have very big raising in terms of photocatalytic activity, photocatalytic degradation persistent organic pollutants for example methyl orange, methylene blue, in terms of have important application prospect.
Description
Technical field
The invention belongs to new function material field more particularly to a kind of SrTiO3/TiO2Composite nano fiber and its preparation
Method.
Background technique
The fast development of modern industry seriously threatens the mankind's containing toxic, carcinogenic contaminant waste water a large amount of discharges
Health.Advanced oxidation processes include the methods of electrochemical oxidation process, Fenton oxidation method, Ozonation, photocatalytic oxidation pair
High stability, the removal of high toxicity organic pollutant are especially effective in water, have been increasingly becoming domestic and international colleges and universities and scientific research institution
One of direction of research.Photocatalytic oxidation is one of high-level oxidation technology, it refers to by irradiating conductor photocatalysis
Agent transits to conduction band after exciting the electronics in its valence band, and forms photohole and electricity in valence band and conduction band respectively
Son generates the extremely strong hydroxyl radical free radical of oxidability, thus by pollutant oxidative degradation in water.With it is inexhaustible, with it not
The solar energy exhausted is that research of the photocatalysis technology that gets up of Power evelopment in terms of pollutant abatement technology field and energy development is non-
It is often active.It is many to be difficult to the organic pollutant removed with other methods, such as chloroform, phthalic acid ester, Polychlorinated biphenyls all may be used
To be removed using the technology, and removal rate is up to 100%.Therefore, the light as the core high activity of photocatalysis technology
The research and development of catalyst naturally become one of the hot spot of many scientific research personnel research.
It is well known that TiO2Have many advantages, such as high catalytic activity, stronger photostability and nontoxic as photochemical catalyst.
But it is directed to how to improve modified TiO2Especially Rutile Type TiO2In terms of photocatalytic activity as photochemical catalyst, there is document report
The TiO of road Rutile Type2It combines to be formed with hetero-junctions photocatalyst with CuS, list can be made up to a certain extent
The deficiency of semiconductor material improves photocatalytic activity；However, not being able to satisfy photocatalytic activity demand still.
Summary of the invention
It is an object of the present invention in view of the deficiencies of the prior art, it is fine provide a kind of strontium titanates/titanium dioxide composite Nano
Dimension and preparation method thereof.
The purpose of the present invention is what is be achieved through the following technical solutions: a kind of SrTiO3/TiO2Composite nano fiber, it is described
Composite nano fiber diameter is 180~220nm, and draw ratio is 80~100, by the TiO of Rutile Type2Monocrystalline and SrTiO3Monocrystalline
Composition, SrTiO3Monocrystalline and TiO2Crystal formation hetero-junctions.
A kind of preparation method of strontium titanates/dioxide composite nanofiber, comprising the following steps:
(1) 2.2g polyvinylpyrrolidone (PVP) is distributed to 8ml N,N-dimethylformamide (DMF) and 2ml ice vinegar
In the mixed solution of acid composition, after being uniformly dispersed, the clear solution of stable homogeneous is obtained；2g butyl titanate is added, dispersion is equal
After even, 15.9mg strontium acetate is added, is uniformly dispersed, forms the spinning solution of stable homogeneous.
(2) spinning is carried out using spinning solution prepared by step 1, and is received by aluminium foil roller receiver, before obtaining fiber
Drive body；Wherein, shower nozzle caliber 0.5mm, flow velocity 0.6ml/h.Spinning voltage is 15kV, and the aluminium foil roller of syringe needle and ground connection connects
Distance 15cm between device is received, the ambient humidity during electrostatic spinning is 40% or less；
(3) Precursors of Fibers is first passed through into 80 DEG C of dry 6h, then rises to 700 DEG C again with 5 DEG C/min heating rate, kept
This temperature is sintered 2h, obtains SrTiO3/TiO2Composite nano fiber.
The beneficial effects of the present invention are: the present invention realizes SrTiO by one-step method3With Rutile Type TiO2Between it is different
The building of matter knot improves Rutile Type TiO2Photocatalytic activity, sun light utilization efficiency effectively improves, during light-catalyzed reaction
The service life of photo-generate electron-hole is long.On the other hand, it is sintered by 700 DEG C, Fiber Aspect Ratio reaches 80~100, greatly widens
Application of the catalysis material in every field.
Detailed description of the invention
Fig. 1 is the XRD diagram of 1 product of embodiment；
Fig. 2 is the high-resolution transmission plot (a.b) and scanning electron microscope (SEM) photograph (c) of ST-3 composite fibre；
Fig. 3 is the degradation effect figure of methyl orange dye；
Fig. 4 is the optical absorption figure of 1 product of embodiment；
Fig. 5 is the repeated experiment result figure of ST-3 composite fibre.
Specific embodiment
A kind of preparation method of strontium titanates/dioxide composite nanofiber, comprising the following steps:
(1) 2.2g polyvinylpyrrolidone (PVP) is distributed to 8ml N,N-dimethylformamide (DMF) and 2ml ice vinegar
In the mixed solution of acid composition, after being uniformly dispersed, the clear solution of stable homogeneous is obtained；2g butyl titanate is added, dispersion is equal
It after even, be added strontium acetate (5.3mg-ST1,15.9mg-ST3,26.5mg-ST5,53mg-ST10), be uniformly dispersed, formed
The spinning solution of stable homogeneous.
(2) spinning is carried out using spinning solution prepared by step 1, and is received by aluminium foil roller receiver, before obtaining fiber
Drive body；Wherein, shower nozzle caliber 0.5mm, flow velocity 0.6ml/h.Spinning voltage is 15kV, and the aluminium foil roller of syringe needle and ground connection connects
Distance 15cm between device is received, the ambient humidity during electrostatic spinning is 40% or less；
(3) Precursors of Fibers is first passed through into 80 DEG C of dry 6h, then rises to 700 DEG C again with 5 DEG C/min heating rate, kept
This temperature is sintered 2h, obtains SrTiO3/TiO2Composite nano fiber.
The XRD of the different obtained products of additional amount strontium acetate is as shown in Figure 1, it can be seen from the figure that the product of synthesis
In include Rutile Type TiO2And SrTiO3；Fig. 2 is the high-resolution transmission plot of ST-3 composite fibre, and a can from Fig. 2
Out, composite fibre by Rutile Type TiO2Monocrystalline and SrTiO3Monocrystalline composition, b can be seen that the crystalline substance of two kinds of crystal from Fig. 2
Lattice fringe spacing is respectively 0.324 and 0.275nm, SrTiO3Monocrystalline and TiO2Crystal formation hetero-junctions.Therefore, compared to existing
Two step method doping mode, the hetero-junctions for the composite fibre that the present invention constructs not only exists only in fiber surface, but is covered with
Whole fiber, the separation for the photo-generate electron-hole pair that is highly advantageous to.C can be seen that the composite fibre diameter of synthesis and be from Fig. 2
180~220nm, draw ratio are 80~100.
Using methyl orange dye to the product ST-1, ST-3, ST-5, ST-10 of the present embodiment and simple Rutile Type
TiO2And SrTiO3Carry out catalytic performance detection, testing result as shown in figure 3, irradiation after forty minutes, ST-1, ST-3, ST-5,
The TiO of ST-10 and simple Rutile Type2And SrTiO3Degradation rate be respectively 62%, 93%, 79%, 43%, 47%,
44%；According to test result, SrTiO is utilized3Modified rutile phase TiO2The activity of obtained composite nano-fiber photocatalyst is bright
It is aobvious to be higher than single rutile TiO2Nanofiber and single SrTiO3Nanofiber, this is urged due principally in complex light
Changing material, there is hetero-junctions roles, because hetero-junctions is conducive to the separation of photo-generate electron-hole pairs.We can also simultaneously
To see with SrTiO3The increase of concentration, what photocatalytic activity was presented is downward trend after first increasing, this shows strontium titanates
Additional amount when reaching a certain appropriate amount, photochemical catalyst can just have highest catalytic activity.When only a small amount of strontium titanates
When addition, the heterojunction structure effect of formation is unobvious, therefore photocatalytic activity raising is few；When strontium titanates additional amount is excessive
When, it will lead to excessive SrTiO3It is covered on TiO2Surface, the TiO made2Active site largely reduce, eventually lead to reduction
Its photocatalytic activity.
Further, as shown in Figure 4, SrTiO3Modified rutile phase TiO2Change of the series of samples obtained afterwards to light absorption
Change very little, it means that it is living that the present invention is not based on (extending light absorbing range) the Lai Tigao photocatalysis of existing technological means
Property, but by constructing a large amount of SrTiO3Rutile Type TiO2Nano heterojunction is realized.
Fig. 5 is the repeated experiment result figure of ST-3 composite fibre, it can be seen from the figure that after 5 recyclings,
The degradation capability of ST-3 composite fibre is basically unchanged.
Claims (1)
1. a kind of SrTiO3/TiO2The preparation method of composite nano fiber, the composite nano fiber diameter is 180 ~ 220nm, long
Diameter ratio is 80 ~ 100, by the TiO of Rutile Type2Monocrystalline and SrTiO3Monocrystalline composition, SrTiO3Monocrystalline and TiO2Crystal formation is heterogeneous
Knot;Characterized by comprising the following steps:
(1) 2.2g polyvinylpyrrolidone (PVP) is distributed to 8ml N,N-dimethylformamide (DMF) and 2ml glacial acetic acid
In the mixed solution of composition, after being uniformly dispersed, the clear solution of stable homogeneous is obtained；2g butyl titanate is added, is uniformly dispersed
Afterwards, 15.9mg strontium acetate is added, is uniformly dispersed, forms the spinning solution of stable homogeneous;
(2) spinning is carried out using the spinning solution of step (1) preparation, and is received by aluminium foil roller receiver, before obtaining fiber
Drive body；Wherein, shower nozzle caliber 0.5mm, flow velocity 0.6ml/h;Spinning voltage is 15kV, and the aluminium foil roller of syringe needle and ground connection connects
Distance 15cm between device is received, the ambient humidity during electrostatic spinning is 40% or less；
(3) Precursors of Fibers is first passed through into 80 DEG C of dry 6h, then rises to 700 DEG C again with 5 DEG C/min heating rate, keeps this
Temperature is sintered 2h, obtains strontium titanates/titanium dioxide (SrTiO3/TiO2) composite nano fiber.
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| CN108212136B (en) * | 2018-01-30 | 2020-08-04 | 河北工业大学 | Preparation method of flower-shaped directional SrTiO3 |
| CN108772080B (en) * | 2018-06-29 | 2020-12-01 | 台州职业技术学院 | Preparation method of one-dimensional nanowire composite photocatalyst with nano heterojunction |
| CN110280248B (en) * | 2019-07-18 | 2022-03-01 | 哈尔滨工业大学 | Preparation method of nickel titanate/titanium dioxide nano composite material |
| CN111250074B (en) * | 2020-02-23 | 2021-02-12 | 北京科技大学 | Method for synthesizing MOF derivative semiconductor heterojunction material by solvothermal method |
| CN111996618B (en) * | 2020-08-13 | 2022-04-15 | 苏州大学 | Vanadium-doped strontium titanate nanofiber and preparation method and application thereof |
| CN113559842A (en) * | 2021-07-29 | 2021-10-29 | 辽宁大学 | Strontium titanate/bismuth molybdate heterojunction nanofiber photocatalyst and preparation method and application thereof |
| CN113713814A (en) * | 2021-09-06 | 2021-11-30 | 齐鲁工业大学 | Au/SrTiO3/TiO2Hollow nano-sphere photocatalytic material, and preparation method and application thereof |
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| US9102570B2 (en) * | 2011-04-22 | 2015-08-11 | Cornell University | Process of making metal and ceramic nanofibers |
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| CN102072927A (en) * | 2010-11-12 | 2011-05-25 | 吉林大学 | Preparation method for fast-response and wide-range ceramic-based nano-fiber humidity sensor |
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| Title |
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| 原位水热合成SrTiO3/TiO2复合纳米纤维及光催化性能;李跃军等;《高等学校化学学报》;20111130;第32卷(第11期);第2490-2497页 |
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