CN107573921B - A kind of ability of reverse photochromism material and preparation method thereof - Google Patents
A kind of ability of reverse photochromism material and preparation method thereof Download PDFInfo
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Abstract
The present invention provides a kind of ability of reverse photochromism material, general formulas are as follows: Y3Al5‑xGaxO12:yNi2+, wherein 0≤x≤5,0 y≤0.02 <.The present invention passes through transition metal ions Ni2+Adulterated al gallate realizes the colourless ability of reverse photochromism between brownish red, while this photochromic material also has the long-persistence luminous performance of near-infrared.
Description
Technical field
The invention belongs to inorganic functional material technical fields, and in particular to a kind of ability of reverse photochromism material and its preparation side
Method.
Background technique
Long-afterglow material, which refers to, is excited (such as X-ray, ultraviolet light, it is seen that light, electron beam etc.) by the external world, is stopping exciting
It still is able to observe luminous material afterwards, twilight sunset fluorescent lifetime, which can continue to arrive for several seconds, to be differed in several weeks.At present, rear-earth-doped
Aluminate base long persistence luminescent material (such as CaAl2O4:Eu2+,Nd3+,SrAl2O4:Eu2+,Dy3+) and silicate-base long-afterglow material
(such as Sr2MgSi2O7:Eu2+,Dy3+,Ca3MgSi2O8:Eu2+,Dy3+Deng) because of after-glow brightness height, the duration is long, has put into quotient
Industry application.The luminous of these long-afterglow materials is at visible light region.The light of this wave band of 1100-1600nm is to organism blood
Liquid and tissue are relative transparents, are biological second window in this wave-length coverage.It can with the near-infrared luminous material of this wave band
To perform well in living body biological imaging or carry out the detection of molecular targets as biological fluorescent labelling material, and Ni2+Doping
Long-afterglow material just can satisfy this point.In recent years, researcher is just to Ni2+The near-infrared long-afterglow material of doping, which is made, is
The research of system, reported such long-afterglow material are also less.
Off-color material be acknowledged as very with actual application prospect functional material, and photochromic material especially by
The concern of researcher.A kind of photochromic reversible change referred between two kinds of different conditions of substance, wherein at least one side
To variation be due to light radiation cause.Photochromic material causes its suction after the irradiation by a certain electromagnetic wave
It receives spectrum and apparent variation has occurred, and then its body colour is caused to show as another color, then by the electricity of another wavelength
After (or under heat effect) magnetic wave irradiates again, and it is restored to original body colour.This material with light sensitive characteristic military and
Broad application prospect is suffered from civilian: such as optical modulation device, read-write optical information storage and record, molecular switch, memory
Element, protection camouflage, coatings industry, textile, radiant quantity etc..
Currently, studying the most country of photochromic material is the U.S., Japan and France.And study best, it quickly grows
Be organic photochromic material.But organic photochromic material have the shortcomings that it is some intrinsic: such as robustness and stability
Energy is poor, inoxidizability is undesirable, discoloration is strong to medium selectivity, the discoloration duration is short, synthesis process environmental pollution
Greatly.
Inorganic photochromic material stability with higher, very long discoloration duration, good anti-fatigue performance.
In comparison, inorganic photochromic material is very slow in the development of the past few decades, and material category and color also extremely have
Limit, which greatly limits the applications of inorganic photochromic material.
Summary of the invention
In view of this, the technical problem to be solved in the present invention is that providing a kind of ability of reverse photochromism material and its preparation side
Method, the present invention pass through transition metal ions Ni2+Adulterated al gallate realizes the colourless ability of reverse photochromism between brownish red, together
When this photochromic material also there is the long-persistence luminous performance of near-infrared.
The present invention provides a kind of ability of reverse photochromism material, general formulas are as follows: Y3Al5-xGaxO12:yNi2+, wherein x is Ga's
Accounting, 0≤x≤5；Y is the doping content of Ni, 0 y≤0.02 <, it is preferred that x=0,1,2,3,4 or 5,0 < y≤0.02, y=
0.05%, 0.25%, 0.5%, 1% or 2%.
Ability of reverse photochromism material provided by the invention is a kind of with biological second window near-infrared long afterglow property
Photochromic material, photochromic material product body colour after ultraviolet light can slowly become brownish red, using the sun
After light irradiation, and it can be restored to the body colour of script, and this photochromism processes favorable repeatability, fatigue resistance is high.Material
There is near-infrared luminous characteristic after ultraviolet light, biological living imaging can be applied to.This kind of material can answer extensively
It is imaged for biological fluorescent labelling, optical modulation device, read-write optical information storage and record, molecular switch, memory cell, protection
Camouflage, coatings industry, textile, radiant quantity etc..
The present invention also provides a kind of preparation methods of above-mentioned ability of reverse photochromism material, comprising the following steps:
A it) by the compound containing yttrium, the compound containing aluminium, the compound containing gallium, nickeliferous compound mixed grinding, obtains
Hybrid solid powder；
B) under the conditions of air atmosphere by the hybrid solid powder at 1300~1600 DEG C under conditions of carry out roasting 3~
It is ground after 6 hours, obtaining general formula is Y3Al5-xGaxO12:yNi2+Ability of reverse photochromism material, wherein 0≤x≤5,0 < y≤
0.02。
The present invention weighs raw material first, in accordance with the proportion of general formula, by the compound containing yttrium, the compound containing aluminium, the change containing gallium
Object, nickeliferous compound mixed grinding are closed, hybrid solid powder is obtained.
Wherein, the compound containing yttrium is oxide or yttrium nitrate containing yttrium, preferably containing the oxide of yttrium；It is described to contain
The compound of aluminium is oxide or aluminum nitrate containing aluminium, preferably containing the oxide of aluminium.The compound containing gallium is containing gallium
The halide of oxide or gallium, preferably containing the oxide of gallium.The nickeliferous compound be nickeliferous oxide or nickel nitrate,
Preferably nickeliferous oxide.
Then, under the conditions of air atmosphere by the hybrid solid powder at 1300~1600 DEG C under conditions of roast
It is ground after 3~6 hours, obtaining general formula is Y3Al5-xGaxO12:yNi2+Ability of reverse photochromism material, wherein 0≤x≤5,0 < y
≤0.02。
Wherein, the temperature of the roasting is preferably 1400~1500 DEG C, and the time of the roasting is preferably 4~5 hours.
Cost is relatively low needed for preparation method raw material provided by the invention, and method is simple, preparation condition is easy to control.
Compared with prior art, the present invention provides a kind of ability of reverse photochromism material, general formulas are as follows: Y3Al5-xGaxO12:
yNi2+, wherein 0≤x≤5,0 y≤0.02 <.The present invention passes through transition metal ions Ni2+Adulterated al gallate realize it is colourless with
Ability of reverse photochromism between brownish red, while this photochromic material also has the long-persistence luminous performance of near-infrared.
Detailed description of the invention
Fig. 1 is the XRD diagram of product prepared by embodiment 1；
Fig. 2 is that the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 1 is passing through
Cross the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation；
Fig. 3 is that the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 2 is passing through
Cross the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation；
Fig. 4 is that the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 3 is passing through
Cross the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation；
Fig. 5 is that the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 4 is passing through
Cross the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation；
Fig. 6 is that the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 5 is passing through
Cross the diffusing reflection spectrum after ultraviolet 254nm ultraviolet excitation and after sunlight irradiation；
Fig. 7 is that the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 6 is passing through
Cross the diffusing reflection spectrum after ultraviolet 254nm ultraviolet excitation and after sunlight irradiation；
Fig. 8 is that the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 7 is passing through
Cross the diffusing reflection spectrum after ultraviolet 254nm ultraviolet excitation and after sunlight irradiation；
Fig. 9 is that the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 8 is passing through
Cross the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation；
Figure 10 is swashing for the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 8
Luminous spectrum；
Figure 11 is the hair of the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 8
Penetrate spectrum；
Figure 12 is the photochromic material with biological second window near-infrared long afterglow property of the preparation of embodiment 8 in purple
Outer smooth 254nm monitors the attenuation curve of 1420nm after exciting 3 minutes；
Figure 13 is that the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 9 is passing through
Cross the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation；
Figure 14 is that the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 10 exists
Diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation；
Figure 15 is the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 10
Excitation spectrum；
Figure 16 is the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 10
Emission spectrum；
Figure 17 is that the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 10 exists
Ultraviolet light 254nm monitors the attenuation curve of 1420nm after exciting 3 minutes；
Figure 18 is that the photochromic material with biological second window near-infrared long afterglow property prepared by embodiment 11 exists
Diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation.
Specific embodiment
For a further understanding of the present invention, below with reference to embodiment to ability of reverse photochromism material provided by the invention and its
Preparation method is illustrated, and protection scope of the present invention is not limited by the following examples.
Embodiment 1
Raw material Y is accurately weighed in molar ratio for 3:2:3:0.0012O3(analysis is pure), Al2O3(analysis is pure), Ga2O3(analysis
It is pure), NiO (analysis pure) and the H that 0.073g is added3BO3It is as cosolvent, weighed each raw material ground and mixed in mortar is equal
It is even to be placed in corundum crucible, regrinding is taken out after keeping the temperature 4 hours in air environment at 1550 DEG C uniformly obtains solid powder
Product, Y3Al2Ga3O12:0.0005Ni2+。
XRD detection, the result is shown in Figure 1 are carried out to obtained product, Fig. 1 is the XRD diagram of product prepared by embodiment 1.
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.As shown in Fig. 2, Fig. 2 is Ni obtained by embodiment 12+(doping 0.05%) doping
Y3Al2Ga3O12Photochromic material with biological second window near-infrared long afterglow property is passing through 254nm ultraviolet excitation
Diffusing reflection spectrum after being irradiated afterwards with sunlight.Reflectivity changes are bigger, show that the variation of sample body colour is more significant.Ultraviolet excitation
Afterwards, reflectivity is decreased obviously, and shows that sample body colour deepens.Sunlight irradiation back reflection rate obviously rise, indicate sample body colour by
Gradually restore.Ultraviolet light and the multiple interacting radiation of sunlight are able to achieve the reversible change of color sample.
Embodiment 2
Raw material Y is accurately weighed in molar ratio for 3:2:3:0.0052O3(analysis is pure), Al2O3(analysis is pure), Ga2O3(analysis
It is pure), NiO (analysis pure) and the H that 0.073g is added3BO3It is as cosolvent, weighed each raw material ground and mixed in mortar is equal
It is even to be placed in corundum crucible, regrinding is taken out after keeping the temperature 4 hours in air environment at 1550 DEG C uniformly obtains solid powder
Product, Y3Al2Ga3O12:0.0025Ni2+。
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.As shown in figure 3, Fig. 3 be embodiment 2 prepare have biological second window near-infrared it is long more than
The photochromic material of brightness characteristic is in the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation.
Embodiment 3
Raw material Y is accurately weighed in molar ratio for 3:2:3:0.012O3(analysis is pure), Al2O3(analysis is pure), Ga2O3(analysis
It is pure), NiO (analysis pure) and the H that 0.073g is added3BO3It is as cosolvent, weighed each raw material ground and mixed in mortar is equal
It is even to be placed in corundum crucible, regrinding is taken out after keeping the temperature 4 hours in air environment at 1550 DEG C uniformly obtains solid powder
Product, Y3Al2Ga3O12:0.005Ni2+。
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.As shown in figure 4, Fig. 4 be embodiment 3 prepare have biological second window near-infrared it is long more than
The photochromic material of brightness characteristic is in the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation.
Embodiment 4
Raw material Y is accurately weighed in molar ratio for 3:2:3:0.022O3(analysis is pure), Al2O3(analysis is pure), Ga2O3(analysis
It is pure), NiO (analysis pure) and the H that 0.073g is added3BO3It is as cosolvent, weighed each raw material ground and mixed in mortar is equal
It is even to be placed in corundum crucible, regrinding is taken out after keeping the temperature 4 hours in air environment at 1550 DEG C uniformly obtains solid powder
Product, Y3Al2Ga3O12:0.01Ni2+。
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.As shown in figure 5, Fig. 5 be embodiment 4 prepare have biological second window near-infrared it is long more than
The photochromic material of brightness characteristic is in the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation.
Embodiment 5
Raw material Y is accurately weighed in molar ratio for 3:2:3:0.042O3(analysis is pure), Al2O3(analysis is pure), Ga2O3(analysis
It is pure), NiO (analysis pure) and the H that 0.073g is added3BO3It is as cosolvent, weighed each raw material ground and mixed in mortar is equal
It is even to be placed in corundum crucible, regrinding is taken out after keeping the temperature 4 hours in air environment at 1550 DEG C uniformly obtains solid powder
Product, Y3Al2Ga3O12:0.02Ni2+。
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.As shown in fig. 6, Fig. 6 be embodiment 5 prepare have biological second window near-infrared it is long more than
The photochromic material of brightness characteristic is in the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation.
Embodiment 6
Raw material Y is accurately weighed in molar ratio for 3:5:0.0052O3(analysis is pure), Al2O3(analysis is pure), NiO (analysis is pure)
And the H of 0.048g is added3BO3As cosolvent, weighed each raw material ground and mixed in mortar is homogeneously disposed in corundum crucible
In, regrinding is taken out after keeping the temperature 4 hours in air environment at 1500 DEG C uniformly obtains solid powder product, Y3Al5O12:
0.0025Ni2+。
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.As shown in fig. 7, Fig. 7 be embodiment 6 prepare have biological second window near-infrared it is long more than
The photochromic material of brightness characteristic is in the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation.
Embodiment 7
Raw material Y is accurately weighed in molar ratio for 3:4:1:0.0052O3(analysis is pure), Al2O3(analysis is pure), Ga2O3(analysis
It is pure), NiO (analysis pure) and the H that 0.048g is added3BO3It is as cosolvent, weighed each raw material ground and mixed in mortar is equal
It is even to be placed in corundum crucible, regrinding is taken out after keeping the temperature 4 hours in air environment at 1500 DEG C uniformly obtains solid powder
Product, Y3Al4Ga1O12:0.0025Ni2+。
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.As shown in figure 8, Fig. 8 be embodiment 7 prepare have biological second window near-infrared it is long more than
The photochromic material of brightness characteristic is in the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation.
Embodiment 8
Raw material Y is accurately weighed in molar ratio for 3:3:2:0.0052O3(analysis is pure), Al2O3(analysis is pure), Ga2O3(analysis
It is pure), NiO (analysis pure) and the H that 0.048g is added3BO3It is as cosolvent, weighed each raw material ground and mixed in mortar is equal
It is even to be placed in corundum crucible, regrinding is taken out after keeping the temperature 4 hours in air environment at 1500 DEG C uniformly obtains solid powder
Product, Y3Al3Ga2O12:0.0025Ni2+。
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.As shown in figure 9, Fig. 9 be embodiment 8 prepare have biological second window near-infrared it is long more than
The photochromic material of brightness characteristic is in the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation；Figure 10 is
Prepared by embodiment 8 has the excitation spectrum of the photochromic material of biological second window near-infrared long afterglow property；Figure 11 is
Prepared by embodiment 8 has the emission spectrum of the photochromic material of biological second window near-infrared long afterglow property；Figure 12 is
Prepared by embodiment 8 there is the photochromic material of biological second window near-infrared long afterglow property to excite 3 in ultraviolet light 254nm
The attenuation curve of 1420nm is monitored after minute.
Embodiment 9
Raw material Y is accurately weighed in molar ratio for 3:2:3:0.0052O3(analysis is pure), Al2O3(analysis is pure), Ga2O3(analysis
It is pure), NiO (analysis pure) and the H that 0.048g is added3BO3It is as cosolvent, weighed each raw material ground and mixed in mortar is equal
It is even to be placed in corundum crucible, regrinding is taken out after keeping the temperature 4 hours in air environment at 1500 DEG C uniformly obtains solid powder
Product, Y3Al2Ga3O12:0.0025Ni2+。
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.As shown in figure 13, Figure 13 is the long with biological second window near-infrared of the preparation of embodiment 9
The photochromic material of light-decay characteristic is in the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation.
Embodiment 10
Raw material Y is accurately weighed in molar ratio for 3:1:4:0.0052O3(analysis is pure), Al2O3(analysis is pure), Ga2O3(analysis
It is pure), NiO (analysis pure) and the H that 0.048g is added3BO3It is as cosolvent, weighed each raw material ground and mixed in mortar is equal
It is even to be placed in corundum crucible, regrinding is taken out after keeping the temperature 4 hours in air environment at 1500 DEG C uniformly obtains solid powder
Product, Y3Al1Ga4O12:0.0025Ni2+。
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.As shown in figure 14, Figure 14 is the preparation of embodiment 10 with biological second window near-infrared
The photochromic material of long afterglow property is in the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation.Figure
The excitation spectrum of 15 photochromic materials with biological second window near-infrared long afterglow property prepared for embodiment 10；Figure
The emission spectrum of 16 photochromic materials with biological second window near-infrared long afterglow property prepared for embodiment 10；Figure
17 have the photochromic material of biological second window near-infrared long afterglow property in ultraviolet light 254nm for prepared by embodiment 10
The attenuation curve of 1420nm is monitored after excitation 3 minutes.
Embodiment 11
Raw material Y is accurately weighed in molar ratio for 3:5:0.0052O3(analysis is pure), Ga2O3(analysis is pure), NiO (analysis is pure)
And the H of 0.048g is added3BO3As cosolvent, weighed each raw material ground and mixed in mortar is homogeneously disposed in corundum crucible
In, regrinding is taken out after keeping the temperature 4 hours in air environment at 1500 DEG C uniformly obtains solid powder product, Y3Ga5O12:
0.0025Ni2+。
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.As shown in figure 17, Figure 17 is the preparation of embodiment 11 with biological second window near-infrared
The photochromic material of long afterglow property is in the diffusing reflection spectrum after 254nm ultraviolet excitation and after sunlight irradiation.
Embodiment 12
Raw material Y is accurately weighed in molar ratio for 3:2:3:0.032O3(analysis is pure), Al2O3(analysis is pure), Ga2O3(analysis
It is pure), NiO (analysis pure) and the H that 0.073g is added3BO3It is as cosolvent, weighed each raw material ground and mixed in mortar is equal
It is even to be placed in corundum crucible, regrinding is taken out after keeping the temperature 4 hours in air environment at 1550 DEG C uniformly obtains solid powder
Product, Y3Al2Ga3O12:0.015Ni2+。
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.
Embodiment 13
Raw material Y is accurately weighed in molar ratio for 3:2:3:0.062O3(analysis is pure), Al2O3(analysis is pure), Ga2O3(analysis
It is pure), NiO (analysis pure) and the H that 0.073g is added3BO3It is as cosolvent, weighed each raw material ground and mixed in mortar is equal
It is even to be placed in corundum crucible, regrinding is taken out after keeping the temperature 4 hours in air environment at 1550 DEG C uniformly obtains solid powder
Product, Y3Al2Ga3O12:0.03Ni2+。
After the excitation of 254nm ultraviolet light, sample body colour gradually becomes brownish red, then the color sample after sunlight irradiates
It is gradually recovered the color for script again.
The above is only a preferred embodiment of the present invention, it is noted that for the ordinary skill people of the art
For member, various improvements and modifications may be made without departing from the principle of the present invention, these improvements and modifications are also answered
It is considered as protection scope of the present invention.
Claims (6)
1. a kind of ability of reverse photochromism material, which is characterized in that general formula are as follows: Y3Al5-xGaxO12:yNi2+, wherein 0≤x≤5,0
Y≤0.02 <.
2. a kind of preparation method of ability of reverse photochromism material as described in claim 1, which is characterized in that including following step
It is rapid:
A it) by the compound containing yttrium, the compound containing aluminium, the compound containing gallium, nickeliferous compound mixed grinding, is mixed
Solid powder；
B) under the conditions of air atmosphere by the hybrid solid powder at 1300~1600 DEG C under conditions of to carry out roasting 3~6 small
When after grind, obtain general formula be Y3Al5-xGaxO12:yNi2+Ability of reverse photochromism material, wherein 0≤x≤5,0 < y≤
0.02。
3. preparation method according to claim 2, which is characterized in that the compound containing yttrium be oxide containing yttrium or
Yttrium nitrate.
4. preparation method as claimed in claim 2, which is characterized in that the compound containing aluminium is oxide or nitre containing aluminium
Sour aluminium.
5. preparation method as claimed in claim 2, which is characterized in that the compound containing gallium is oxide or gallium containing gallium
Halide.
6. preparation method as claimed in claim 2, which is characterized in that the nickeliferous compound is nickeliferous oxide or nitre
Sour nickel.
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| On the limitary radius of garnet structure compounds Y3Al5-xMxO12 (M = Cr, Co, Mn, Ni, Cu) and Y3Fe5-xCoxO12 (0 <= x <= 2.75) synthesized by sol-gel method;Skaudzius R等;《MATERIALS CHEMISTRY AND PHYSICS》;20120815;第135卷(第2-3期);全文 |
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