CN109225287B - Preparation method of bismuth-doped tin oxide/bismuth phosphate composite photocatalyst - Google Patents
Preparation method of bismuth-doped tin oxide/bismuth phosphate composite photocatalyst Download PDFInfo
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- 239000011941 photocatalyst Substances 0.000 title claims abstract description 26
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 title claims abstract description 24
- 239000002131 composite material Substances 0.000 title claims abstract description 16
- 229910001887 tin oxide Inorganic materials 0.000 title claims abstract description 14
- SFOQXWSZZPWNCL-UHFFFAOYSA-K bismuth;phosphate Chemical compound [Bi+3].[O-]P([O-])([O-])=O SFOQXWSZZPWNCL-UHFFFAOYSA-K 0.000 title claims abstract description 13
- 238000002360 preparation method Methods 0.000 title claims abstract description 7
- 238000006243 chemical reaction Methods 0.000 claims abstract description 45
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 27
- 239000008367 deionised water Substances 0.000 claims abstract description 24
- 229910021641 deionized water Inorganic materials 0.000 claims abstract description 24
- 238000001035 drying Methods 0.000 claims abstract description 14
- 238000003756 stirring Methods 0.000 claims abstract description 14
- 238000005406 washing Methods 0.000 claims abstract description 13
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims abstract description 7
- 238000001027 hydrothermal synthesis Methods 0.000 claims abstract description 7
- 229910017604 nitric acid Inorganic materials 0.000 claims abstract description 7
- 229910020212 Na2SnO3 Inorganic materials 0.000 claims abstract description 6
- BNIILDVGGAEEIG-UHFFFAOYSA-L disodium hydrogen phosphate Chemical compound [Na+].[Na+].OP([O-])([O-])=O BNIILDVGGAEEIG-UHFFFAOYSA-L 0.000 claims abstract description 6
- 229910000397 disodium phosphate Inorganic materials 0.000 claims abstract description 6
- 238000002156 mixing Methods 0.000 claims abstract description 4
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 6
- 238000000034 method Methods 0.000 claims description 6
- 230000007935 neutral effect Effects 0.000 claims description 5
- 238000001816 cooling Methods 0.000 claims description 4
- 230000000593 degrading effect Effects 0.000 abstract description 9
- 231100000956 nontoxicity Toxicity 0.000 abstract description 3
- 238000000862 absorption spectrum Methods 0.000 abstract description 2
- 239000002957 persistent organic pollutant Substances 0.000 abstract description 2
- 239000002351 wastewater Substances 0.000 description 9
- 230000001699 photocatalysis Effects 0.000 description 8
- PYWVYCXTNDRMGF-UHFFFAOYSA-N rhodamine B Chemical compound [Cl-].C=12C=CC(=[N+](CC)CC)C=C2OC2=CC(N(CC)CC)=CC=C2C=1C1=CC=CC=C1C(O)=O PYWVYCXTNDRMGF-UHFFFAOYSA-N 0.000 description 7
- 229940043267 rhodamine b Drugs 0.000 description 7
- 230000015556 catabolic process Effects 0.000 description 5
- 238000006731 degradation reaction Methods 0.000 description 5
- 238000005516 engineering process Methods 0.000 description 5
- 238000007146 photocatalysis Methods 0.000 description 4
- 229910052724 xenon Inorganic materials 0.000 description 4
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 4
- 238000003760 magnetic stirring Methods 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 229910001868 water Inorganic materials 0.000 description 3
- 239000010842 industrial wastewater Substances 0.000 description 2
- 206010028400 Mutagenic effect Diseases 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 230000000711 cancerogenic effect Effects 0.000 description 1
- 231100000315 carcinogenic Toxicity 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000004043 dyeing Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 238000004134 energy conservation Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 238000005286 illumination Methods 0.000 description 1
- 230000004298 light response Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 231100000243 mutagenic effect Toxicity 0.000 description 1
- 230000003505 mutagenic effect Effects 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 238000007639 printing Methods 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000006798 recombination Effects 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000000725 suspension Substances 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 231100000378 teratogenic Toxicity 0.000 description 1
- 230000003390 teratogenic effect Effects 0.000 description 1
- 238000002834 transmittance Methods 0.000 description 1
- 238000004065 wastewater treatment Methods 0.000 description 1
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- 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
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/14—Phosphorus; Compounds thereof
- B01J27/186—Phosphorus; Compounds thereof with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
-
- 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
-
- B01J35/39—
-
- 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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/10—Heat treatment in the presence of water, e.g. steam
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/308—Dyes; Colorants; Fluorescent agents
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/36—Organic compounds containing halogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/10—Photocatalysts
Abstract
The invention discloses a preparation method of a bismuth-doped tin oxide/bismuth phosphate composite photocatalyst, which is prepared by mixing Bi (NO)3)3·5H2Dissolving O in dilute nitric acid solution to obtain clear and transparent solution A, adding Na2SnO3·4H2Dissolving O in deionized water to obtain solution B, adding dropwise solution B into solution A under stirring to obtain solution C, adding Na2HPO4·12H2Dissolving O in deionized water to obtain a solution D, dropwise adding the solution D into the solution C under the stirring condition, adding deionized water to make the total volume of the mixed system be 30mL, putting the solution into a 50mL high-pressure reaction kettle, putting the high-pressure reaction kettle into a constant-temperature oven at 180 ℃ for hydrothermal reaction for 24h, centrifuging the reaction solution after the high-pressure reaction kettle is cooled to room temperature, washing, and putting the reaction solution into a constant-temperature drying oven at 60 ℃ for drying for 12h to obtain the bismuth-doped tin oxide/bismuth phosphate composite photocatalyst. The composite photocatalyst prepared by the invention has the advantages of wide absorption spectrum range, stable performance, high efficiency, no toxicity and low cost, and can be used for efficiently degrading organic pollutants which are difficult to biodegrade.
Description
Technical Field
The invention belongs to the technical field of synthesis of composite photocatalytic materials, and particularly relates to a preparation method of a bismuth-doped tin oxide/bismuth phosphate composite photocatalyst.
Background
With the progress of society, the industry is continuously developed, and the discharge amount of industrial wastewater is increased. The industrial wastewater has the characteristics of large quantity, multiple types, difficult degradation, large harm and the like, wherein the dye wastewater mainly comes from dye production and printing and dyeing factories, and the high chroma can influence the light transmittance of water bodies and threaten the normal growth of aquatic organisms. The dye wastewater has complex composition, is difficult to degrade in natural environment, has carcinogenic, teratogenic and mutagenic effects on organisms and has great harm. The photocatalysis technology is used as an advanced water treatment technology, and can thoroughly oxidize and degrade pollutants which are difficult to degrade into nontoxic and harmless CO under the irradiation of natural light2And H2O, has the advantages of energy conservation, high efficiency and thorough purification. Therefore, the method can be used for deep degradation of the refractory dye wastewater. At present, the photocatalysis technology is difficult to popularize and apply to actual wastewater treatment, and one key factor is that the degradation performance of most single photocatalysts is poor at present, and the utilization rate of sunlight is not ideal enough. Therefore, modifying the existing photocatalyst by adopting a proper method to improve the photocatalytic performance thereof is the focus of the current research of the photocatalytic technology. SnO2The wide-bandgap n-type semiconductor has the advantages of good thermal stability and chemical stability, no toxicity, low raw material cost, high reduction potential, good electron mobility and the like, is widely applied to gas sensitive materials, catalytic materials, supercapacitors and electrode materials, has a bandgap (Eg) of 3.6eV, can only absorb and utilize ultraviolet light in photocatalysis, and has the problems of high photoproduction electron-hole recombination rate and low photocatalysis efficiency. The method adopts element doping and photocatalyst BiPO4Method for compositely constructing heterojunction to improve SnO2The photocatalytic performance of (a). Research results show that the performance of the composite photocatalyst prepared by the invention for degrading rhodamine B under simulated sunlight is obviously improved, however, no relevant report on the aspect is available at present.
Disclosure of Invention
The invention solves the technical problem of providing a preparation method of a bismuth-doped tin oxide/bismuth phosphate composite photocatalyst capable of effectively degrading rhodamine B dye wastewater.
The invention adopts the following technical scheme for solving the technical problems, and the preparation method of the bismuth-doped tin oxide/bismuth phosphate composite photocatalyst is characterized by comprising the following specific steps of: 1.6007g of Bi (NO)3)3·5H2Dissolving O in 15mL of dilute nitric acid solution with the molar concentration of 1.43mol/L to obtain clear and transparent solution A, and mixing 0.2847g of Na2SnO3·4H2Dissolving O in 5mL deionized water to obtain solution B, adding solution B dropwise into solution A under stirring to obtain solution C, adding 0.0188-0.8237g Na2HPO4·12H2Dissolving O in 5mL of deionized water to obtain a solution D, dropwise adding the solution D into the solution C under the stirring condition, adding deionized water to make the total volume of the mixed system be 30mL, continuously stirring for 30min, then putting the solution into a 50mL high-pressure reaction kettle, putting the high-pressure reaction kettle into a constant-temperature oven at 180 ℃ for hydrothermal reaction for 24h, cooling the high-pressure reaction kettle to room temperature, centrifuging the reaction solution, washing the reaction solution to be neutral by using deionized water, then washing the reaction solution by using absolute ethyl alcohol, and then putting the reaction solution into a constant-temperature drying oven at 60 ℃ for drying for 12h to obtain the bismuth-doped tin oxide/bismuth phosphate composite photocatalyst.
Further preferably, the Na is2SnO3·4H2O and Na2HPO4·12H2The feeding mass ratio of O is 0.2847: 0.0397.
The bismuth-doped tin oxide/bismuth phosphate composite photocatalyst prepared by the invention is a visible light response type photocatalyst, can efficiently degrade rhodamine B dye wastewater under simulated sunlight, has a wide absorption spectrum range, stable performance, high efficiency, no toxicity and low cost, can be used for efficiently degrading organic pollutants which are difficult to biodegrade, and has good market application prospect.
Drawings
FIG. 1 is SnO prepared in examples 1-42、Bi-SnO2、BiPO4And Bi-SnO2/BiPO4The performance curve of the photocatalyst for degrading RhB;
FIG. 2 is SnO prepared in examples 1-42、Bi-SnO2、BiPO4And Bi-SnO2/BiPO4XRD pattern of photocatalyst.
Detailed Description
The present invention is described in further detail below with reference to examples, but it should not be construed that the scope of the above subject matter of the present invention is limited to the following examples, and that all the technologies realized based on the above subject matter of the present invention belong to the scope of the present invention.
Example 1
0.5694g of Na2SnO3·4H2Dissolving O in 5mL of deionized water, and then slowly dropwise adding the O into 15mL of dilute nitric acid solution with the molar concentration of 1.43mol/L under vigorous magnetic stirring to obtain a white turbid solution; adding deionized water to make the total volume of the solution be 30mL, continuously stirring for 30min, placing the solution in a 50mL high-pressure reaction kettle, placing the high-pressure reaction kettle in a constant-temperature oven at 180 ℃ for hydrothermal reaction for 24h, cooling the high-pressure reaction kettle to room temperature, centrifuging the reaction solution, washing the reaction solution to be neutral by using the deionized water, then washing the reaction solution by using absolute ethyl alcohol, and then placing the reaction solution in a constant-temperature drying oven at 60 ℃ for drying for 12h to obtain SnO2The removal rate of RhB of the photocatalyst for degrading rhodamine B dye wastewater for 1.5h under simulated sunlight (500W xenon lamp) is 50.96%.
Example 2
1.6007g of Bi (NO)3)3·5H2Dissolving O in 15mL of dilute nitric acid solution with the molar concentration of 1.43mol/L to prepare a clear and transparent solution A; 0.2847g of Na2SnO3·4H2Dissolving O in 5mL of deionized water, slowly dropwise adding the solution into the solution A under vigorous magnetic stirring to obtain a white turbid solution B, adding deionized water to make the total volume of the solution be 30mL, continuously stirring for 30min, placing the solution in a 50mL high-pressure reaction kettle, placing the solution in a constant-temperature oven at 180 ℃ for hydrothermal reaction for 24h, centrifuging the reaction solution after the high-pressure reaction kettle is cooled to room temperature, washing the reaction solution to be neutral by using the deionized water, then washing the reaction solution by using absolute ethyl alcohol, and then placing the reaction solution in a constant-temperature drying oven at 60 ℃ for drying for 12h to obtain bismuth-doped tin oxide (Bi-SnO)2) The removal rate of RhB of the photocatalyst for degrading rhodamine B dye wastewater for 1.5h under simulated sunlight (500W xenon lamp) is 73.88%.
Example 3
1.6007g of Bi (NO)3)3·5H2Dissolving O in 15mL of dilute nitric acid solution with the molar concentration of 1.43mol/L to prepare a clear and transparent solution A; 1.1814g of Na2HPO4·12H2Dissolving O in 5mL of deionized water, slowly dropwise adding the solution into the solution A under magnetic stirring to obtain a white suspension, adding deionized water to make the total volume of the solution be 30mL, continuously stirring for 30min, placing the solution in a 50mL high-pressure reaction kettle, placing the high-pressure reaction kettle in a constant-temperature oven at 180 ℃ for hydrothermal reaction for 24h, centrifuging the reaction solution after the high-pressure reaction kettle is cooled to room temperature, washing the reaction solution to neutrality with deionized water, then washing with absolute ethyl alcohol, and then placing the reaction solution in a constant-temperature drying oven at 60 ℃ for drying for 12h to obtain BiPO4The removal rate of RhB of the photocatalyst for degrading rhodamine B dye wastewater for 1.5h under simulated sunlight (500W xenon lamp) is 10.13%.
Example 4
1.6007g of Bi (NO)3)3·5H2Dissolving O in 15mL of dilute nitric acid solution with the molar concentration of 1.43mol/L to obtain clear and transparent solution A, and mixing 0.2847g of Na2SnO3·4H2Dissolving O in 5mL deionized water to obtain solution B, adding solution B dropwise into solution A under stirring to obtain solution C, adding Na with different masses (0.0188 g, 0.0397g, 0.1535g, 0.3580g, 0.8237 g) to obtain solution C2HPO4·12H2Dissolving O in 5mL of deionized water to obtain a solution D, dropwise adding the solution D into the solution C under the stirring condition, adding deionized water to make the total volume of the mixed system be 30mL, continuously stirring for 30min, then placing the solution into a 50mL high-pressure reaction kettle, placing the high-pressure reaction kettle in a constant-temperature oven at 180 ℃ for hydrothermal reaction for 24h, cooling the high-pressure reaction kettle to room temperature, centrifuging the reaction solution, washing the reaction solution to be neutral by using the deionized water, then washing the reaction solution by using absolute ethyl alcohol, and then placing the reaction solution in a constant-temperature drying oven at 60 ℃ for drying for 12h to obtain the bismuth-doped tin oxide/bismuth phosphate composite photocatalyst with the molar percentages of 5%, 10%, 30%, 50% and 70% in sequence. The performance of each catalyst for degrading rhodamine B dye wastewater is compared under simulated sunlight (500W xenon lamp). 10% Bi-SnO2/BiPO4The degradation effect is optimal, the degradation rate of RhB under illumination of 1.5h is 99.52 percent, which is compared with SnO2The photocatalyst is 48.56 percent higher than Bi-SnO2Photo catalysisThe agent is 25.64 percent higher than BiPO4The photocatalyst is 89.39% higher.
The foregoing embodiments illustrate the principles, principal features and advantages of the invention, and it will be understood by those skilled in the art that the invention is not limited to the foregoing embodiments, which are merely illustrative of the principles of the invention, and that various changes and modifications may be made therein without departing from the scope of the principles of the invention.
Claims (2)
1. A preparation method of a bismuth-doped tin oxide/bismuth phosphate composite photocatalyst is characterized by comprising the following specific steps: 1.6007g of Bi (NO)3)3·5H2Dissolving O in 15mL of dilute nitric acid solution with the molar concentration of 1.43mol/L to obtain clear and transparent solution A, and mixing 0.2847g of Na2SnO3·4H2Dissolving O in 5mL deionized water to obtain solution B, adding solution B dropwise into solution A under stirring to obtain solution C, adding 0.0188-0.8237g Na2HPO4·12H2Dissolving O in 5mL of deionized water to obtain a solution D, dropwise adding the solution D into the solution C under the stirring condition, adding deionized water to make the total volume of the mixed system be 30mL, continuously stirring for 30min, then putting the solution into a 50mL high-pressure reaction kettle, putting the high-pressure reaction kettle into a constant-temperature oven at 180 ℃ for hydrothermal reaction for 24h, cooling the high-pressure reaction kettle to room temperature, centrifuging the reaction solution, washing the reaction solution to be neutral by using deionized water, then washing the reaction solution by using absolute ethyl alcohol, and then putting the reaction solution into a constant-temperature drying oven at 60 ℃ for drying for 12h to obtain the bismuth-doped tin oxide/bismuth phosphate composite photocatalyst.
2. The method for preparing the bismuth-doped tin oxide/bismuth phosphate composite photocatalyst according to claim 1, wherein the method comprises the following steps: the Na is2SnO3·4H2O and Na2HPO4·12H2The feeding mass ratio of O is 0.2847: 0.0397.
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102489293A (en) * | 2011-11-18 | 2012-06-13 | 陕西科技大学 | Preparation method of tin dioxide/bismuth tungstate composite photocatalyst |
| EP2695663A1 (en) * | 2012-08-10 | 2014-02-12 | Henrik Bauer Beteiligungsgesellschaft mbH | Photocatalytically active material for air purification |
| CN104399504A (en) * | 2014-11-04 | 2015-03-11 | 陕西科技大学 | Fluorine-nitrogen co-doped bismuth phosphate -stannic oxide composite photocatalyst and preparation method thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN102489293A (en) * | 2011-11-18 | 2012-06-13 | 陕西科技大学 | Preparation method of tin dioxide/bismuth tungstate composite photocatalyst |
| EP2695663A1 (en) * | 2012-08-10 | 2014-02-12 | Henrik Bauer Beteiligungsgesellschaft mbH | Photocatalytically active material for air purification |
| CN104399504A (en) * | 2014-11-04 | 2015-03-11 | 陕西科技大学 | Fluorine-nitrogen co-doped bismuth phosphate -stannic oxide composite photocatalyst and preparation method thereof |
Non-Patent Citations (1)
| Title |
|---|
| CTAB-Assisted Hydrothermal Synthesis of Bi2Sn2O7 Photocatalyst and Its Highly Efficient Degradation of Organic Dye under Visible-Light Irradiation;Weicheng Xu等;《International Journal of Photoenergy》;20131231;第1-7页 * |
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