CN102527370B - Method for synthesizing nanometer zinc-doped tin oxide/zinc stannate heterojunction - Google Patents
Method for synthesizing nanometer zinc-doped tin oxide/zinc stannate heterojunction Download PDFInfo
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- CN102527370B CN102527370B CN 201110451106 CN201110451106A CN102527370B CN 102527370 B CN102527370 B CN 102527370B CN 201110451106 CN201110451106 CN 201110451106 CN 201110451106 A CN201110451106 A CN 201110451106A CN 102527370 B CN102527370 B CN 102527370B
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Abstract
The invention relates to a method for thermally synthesizing a nanometer zinc-doped tin oxide/zinc stannate heterojunction by utilizing a solvent. The method comprises the following steps: 1) selecting a certain amount of tin oxide, zinc nitrate and sodium hydroxide, and respectively dissolving in a mixed solvent of water and absolute ethyl alcohol, thereby obtaining a uniform solution; 2) dropwise adding a NaOH solution into a mixed solution of SnC14 and Zn(NO3)2, stirring, and then placing into a reaction kettle, keeping the temperature at 180 DEG C for 15 hours, and separating, washing and drying the obtained Zn-SnO2; 3) weighting a certain amount of Zn-SnO2, SnC14, Zn(NO3)2 and NaOH, adding into the mixed solvent of water and absolute ethyl alcohol, and continuously and fully stirring; 4) dropwise adding the NaOH solution into a mixed solution of SnC14, Zn(NO3)2 and Zn-SnO2, fully stirring, and then placing into a hydro-thermal reaction kettle, and keeping the temperature at 200 DEG C for 20 hours; and 5) separating, washing and drying, thereby obtaining an end product. The synthesizing technology of the product is simple; the product is 20-30nm spherical grains; the product has the characteristics of a mesoporous structure and has a bigger specific surface area; and the product has an excellent photocatalytic property under an ultraviolet light condition.
Description
Technical field
The present invention relates to a kind of oxide semiconductor nano-powder chemical synthesis process, be specifically related to the method and the product of synthesis of nano zinc-doped tin oxide/zinc stannate hetero-junctions.
Background technology
Zinc stannate (Zn
2SnO
4) be a kind of broad-band gap n type ternary semiconductor with spinel structure, because of it has higher electron mobility and good conductivity, can be used for aspects such as transparency electrode, flammable air-sensitive detection, wet sensitive device, lithium ion battery catalyst and dye-sensitized solar cells, aspect scientific research, caused widely and paid close attention to.Compare Zn with traditional titanium dioxide
2SnO
4Electron mobility and quantum efficiency height, light induced electron and hole-recombination probability are low, and as photochemical catalyst, it has a extensive future.Studies show that nanostructured Zn
2SnO
4Have excellent photocatalysis performance, can effectively degrade NO and HCHO and organic pollution are for indoor gas and the depollution of environment provide new way.
Heterojunction material tends to produce the physics new features that many homogenous materials do not have, and the hetero-junctions with particular nanostructure can be by the bigger advantage of physicochemical properties such as small-size effect, skin effect, quantum confined effect, macro quanta tunnel effect and dielectric confinement effect performance of nano material.Nano-heterogeneous structure causes very big concern at aspects such as luminous, solar cell, photocatalysis.The advantage that the semiconductor nano heterojunction structure shows aspect photocatalysis is: can promote the separation of photo-generated charge carriers, increase the life-span of electric charge carrier and improve the interface charge transfer efficiency.Choose the different Zn-SnO of bandwidth
2With Zn
2SnO
4System is with as Zn
2SnO
4Principal phase, Zn-SnO
2As second phase, adopt solvent method synthesis of nano Zn-SnO
2/ Zn
2SnO
4Hetero-junctions, synthetic product are expected to obtain excellent photocatalytic, however Zn-SnO
2/ Zn
2SnO
4The hetero-junctions synthetic method is not seen relevant report as yet.
Solvent thermal synthesis reaction is (can produce certain pressure) in reactor, as reaction medium, by heating produces high pressure to reaction system, carries out a kind of effective ways of the synthetic and preparation of material with organic solvent.This method can make some very slow thermodynamical reaction realization responses under hydrothermal condition of reaction rate at normal temperatures and pressures rapid, synthetic nano material purity height, productive rate height, crystal structure and grows, controlled amount, and can avoid the impurity and the fault of construction of subsequent techniques introducings such as high-temperature calcination and ball milling.
Summary of the invention
Technical problem to be solved of the present invention is to provide a kind of synthesis of nano zinc-doped tin oxide/zinc stannate hetero-junctions method, and this method technology is simple, easy to operate, the product photocatalysis performance excellence that obtains.
In order to solve the technical problem that the present invention proposes, technical scheme of the present invention is:
A kind of nanometer Zn-SnO
2/ Zn
2SnO
4The synthetic method of hetero-junctions may further comprise the steps:
May further comprise the steps:
(1) configuration amount of substance concentration is the NaOH solution of 2.5mol/L, and solvent is the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:0.8 ~ 1;
(2) configuration SnCl
45H
2O and Zn (NO
3)
26H
2The mixed solution of O, solvent are the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:0.8 ~ 1, wherein SnCl
4Amount of substance concentration be 0.4475~0.4575 mol/L; Zn (NO
3)
2Amount of substance concentration be 0.0425~0.0525 mol/L;
(3) the NaOH solution that step (1) is obtained dropwise is added drop-wise to the SnCl of step (2)
4And Zn (NO
3)
2Mixed solution in, SnCl
4And Zn (NO
3)
2Mixed solution and the volume ratio of the NaOH aqueous solution be 1:2, make SnCl
4Amount of substance concentration is 0.1094 ~ 0.1144mol/L, (Zn (NO
3)
26H
2The amount of substance concentration of O is 0.0106 ~ 0.0156mol/L, and the amount of substance concentration of NaOH is 1.667 mol/L, SnCl
4, Zn (NO
3)
2Be 1:10 with the amount of substance ratio of NaOH, stir, obtain predecessor;
(4) predecessor with step (3) is transferred in the hydrothermal reaction kettle, and making its compactedness is 80%, 180 ℃ ~ 190 ℃ isothermal reactions at least 15 hours;
When (5) treating that the solvent thermal reaction device is reduced to room temperature, the hot product of solvent promptly gets Zn-SnO after centrifugation, cleaning and drying
2Product;
(6) configuration SnCl
45H
2O and Zn (NO
3)
26H
2The mixed solution of O, solvent are the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:0.8 ~ 1, wherein SnCl
4Amount of substance concentration be 0.25mol/L; Zn (NO
3)
2Amount of substance concentration be 0.5 mol/L; Add step (4) Zn-SnO simultaneously
20.0278 ~ 0.0625 mol/L; (7) configuration amount of substance concentration is the NaOH solution of 3.75 mol/L, and solvent is the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:0.8 ~ 1;
(8) the NaOH solution that step (7) is obtained dropwise is added drop-wise to the SnCl of step (6)
4And Zn (NO
3)
2Mixed solution in, SnCl
4And Zn (NO
3)
2Mixed solution and the volume ratio of the NaOH aqueous solution be 1:2, make SnCl
4Amount of substance concentration is 0.0833 mol/L, Zn (NO
3)
26H
2The amount of substance concentration of O is 0.167 mol/L, and the amount of substance concentration of NaOH is 2.5 mol/L, SnCl
4, Zn (NO
3)
2Be 1:10 with the amount of substance ratio of NaOH, guarantee to add step (4) Zn-SnO
2Content be 0.00923 ~ 0.0208 mol/L, stir, obtain predecessor;
(9) predecessor with step (8) is transferred in the hydrothermal reaction kettle, and making its compactedness is 80%, 200 ℃ ~ 210 ℃ isothermal reactions at least 20 hours;
When (10) treating that the solvent thermal reaction device is reduced to room temperature, the hot product of solvent promptly gets nanometer Zn-SnO after centrifugation, cleaning and drying
2/ Zn
2SnO
4Hetero-junctions.
The described solvent of step 3) is deionized water and absolute ethyl alcohol, and volume ratio is 1:0.8 ~ 1, OH in the reactant
-/ (Sn
4++ Zn
2+) molar ratio is 10.
Before the solvent thermal reaction, the compactedness of reactor is 80 %.
Step (4) is followed successively by deionized water and absolute ethyl alcohol with (8) described cleaning process, and the powder after the cleaning is obtaining end product behind dry 10 h under 80 ℃ of temperature.
Press such scheme, step (3) is 2ml ~ 3ml/min with (8) described drop rate,
Press such scheme, step (4) is preferably 80% with (9) described compactedness.Explore by experiment and draw in conjunction with document analysis, compactedness is 80% o'clock, and the suitable pressure of this research system crystal growth and higher productive rate can be provided, and obtains nano heterojunction.
Press such scheme, step (5) with (9) described washing step is: use deionized water and absolute ethanol washing product successively.
Press such scheme, step (5) with (9) described drying steps is: the powder after will cleaning is at 80 ℃ ~ 90 ℃ dry 10h.
Prepare nanometer Zn-SnO according to above-mentioned solvent process for thermosynthesizing
2/ Zn
2SnO
4Hetero-junctions.
The present invention has following beneficial effect:
1, this solvent-thermally synthesizing nano Zn-SnO
2/ Zn
2SnO
4The raw materials used cost of the method for hetero-junctions is low, technology is easy, avoided subsequent techniques such as high-temperature calcination and ball milling to introduce impurity and fault of construction, product purity height easy to operate, that reaction is synthetic, and the synthetic product granular size is controlled.
2, the synthetic nanometer Zn-SnO of this method
2/ Zn
2SnO
4Hetero-junctions has meso-hole structure feature and bigger surface area, and synthetic product has shown excellent photocatalysis performance through under the ultraviolet light methylene blue being tested.
Description of drawings
Fig. 1 is that embodiment 1 gets nanometer 15%Zn-SnO
2/ Zn
2SnO
4Hetero-junctions (mol ratio) FESEM figure;
Fig. 2, the 3rd, embodiment 1 obtains nanometer 15%Zn-SnO
2/ Zn
2SnO
4Hetero-junctions (mol ratio) photocatalysis result (test condition is 15 w uviol lamps, and dominant wavelength 365 nm, photochemical catalyst are 0.2 g).
The specific embodiment
In order to understand the present invention better, further illustrate content of the present invention below in conjunction with example, but content of the present invention not only is confined to the following examples.
Embodiment 1:
The synthetic method of a kind of nanometer zinc-doped tin oxide/zinc stannate hetero-junctions, it comprises the steps:
(1) configuration amount of substance concentration is the NaOH solution of 2.5mol/L, and solvent is the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:1;
(2) configuration SnCl
45H
2O and Zn (NO
3)
26H
2The mixed solution of O, solvent are the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:1, wherein SnCl
4Amount of substance concentration be 0.45mol/L; Zn (NO
3)
2Amount of substance concentration be 0.05mol/L;
(3) the NaOH solution that step (1) is obtained dropwise is added drop-wise to the SnCl of step (2)
4And Zn (NO
3)
2Mixed solution in, SnCl
4And Zn (NO
3)
2Mixed solution and the volume ratio of the NaOH aqueous solution be 1:2, drop rate is 2 ~ 3ml/min, stirs, and obtains predecessor; Above-mentioned predecessor is moved in the hydrothermal reactor, 180 ℃, being incubated at least 15h, to carry out hydro-thermal synthetic.
When (4) treating that the solvent thermal reaction device is reduced to room temperature, the hot product of solvent promptly gets Zn-SnO after centrifugation, cleaning and drying
2Product.
(5) configuration SnCl
45H
2O and Zn (NO
3)
26H
2The mixed solution of O, solvent are the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:1, wherein SnCl
4Amount of substance concentration be 0.25mol/L; Zn (NO
3)
2Amount of substance concentration be 0.5 mol/L; Add step (4) 0.0441 mol/L Zn-SnO simultaneously
2, guarantee Zn-SnO
2Content is the 15%(mol ratio);
(6) configuration amount of substance concentration is the NaOH solution of 3.75 mol/L, and solvent is the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:1;
(7) the NaOH solution that obtains that step (6) is obtained dropwise is added drop-wise to the SnCl of step (5)
4, Zn (NO
3)
2And Zn-SnO
2Suspension in, SnCl
4, Zn (NO
3)
2And Zn-SnO
2Suspension and the volume ratio of NaOH solution be 1:2, drop rate is 2ml/min, stirs, and obtains predecessor; Above-mentioned predecessor is moved in the reactor, 200 ℃, be incubated at least that 20h carries out the solvent thermal synthesis.
When (8) treating that the solvent thermal reaction device is reduced to room temperature, the hot product of solvent promptly gets nanometer 15%Zn-SnO after centrifugation, cleaning and drying
2/ Zn
2SnO
4Hetero-junctions.
The nanometer 15%Zn-SnO that present embodiment is obtained
2/ Zn
2SnO
4The hetero-junctions powder carries out SEM test (see figure 1), and by figure a as can be known: synthetic product is the near-spherical particle, and the particle mean size is 20 ~ 30 nm.
Synthetic product carries out the photocatalysis performance test, and (seeing Fig. 2, Fig. 3), get synthetic product 0.2 g as photochemical catalyst, is that (concentration is 10 to the target degradation product with subunit indigo plant
-5M), the ultraviolet lamp tube of selecting 15 W for use is as ultraviolet source, and its dominant wavelength is 365 nm, and sample is 10 cm apart from the distance of fluorescent tube, and through 120 min illumination, methylene blue is degraded fully; And contrast Zn
2SnO
4With 15%Zn-SnO
2/ Zn
2SnO
4The degradation effect of photochemical catalyst, the result shows nanometer 15%Zn-SnO
2/ Zn
2SnO
4Hetero-junctions has demonstrated excellent photocatalysis performance.
Embodiment 2:
The synthetic method of a kind of nanometer zinc-doped tin oxide/zinc stannate hetero-junctions, it comprises the steps:
(1) configuration amount of substance concentration is the NaOH solution of 2.5mol/L, and solvent is the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:1;
(2) configuration SnCl
45H
2O and Zn (NO
3)
26H
2The mixed solution of O, solvent are the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:1, wherein SnCl
4Amount of substance concentration be 0.4475 mol/L; Zn (NO
3)
2Amount of substance concentration be 0.0525 mol/L;
(3) the NaOH solution that step (1) is obtained dropwise is added drop-wise to the SnCl of step (2)
4And Zn (NO
3)
2Mixed solution in, SnCl
4And Zn (NO
3)
2Mixed solution and the volume ratio of the NaOH aqueous solution be 1:2, drop rate is 2 ~ 3ml/min, stirs, and obtains predecessor; Above-mentioned predecessor is moved in the hydrothermal reactor, 180 ℃, being incubated at least 15h, to carry out hydro-thermal synthetic.
When (4) treating that the solvent thermal reaction device is reduced to room temperature, the hot product of solvent promptly gets Zn-SnO after centrifugation, cleaning and drying
2Product.
(5) configuration SnCl
45H
2O and Zn (NO
3)
26H
2The mixed solution of O, solvent are the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:1, wherein SnCl
4Amount of substance concentration be 0.25mol/L; Zn (NO
3)
2Amount of substance concentration be 0.5 mol/L; Add step (4) 0.0278 mol/L Zn-SnO simultaneously
2, guarantee Zn-SnO
2Content is the 10%(mol ratio);
(6) configuration amount of substance concentration is the NaOH solution of 3.75 mol/L, and solvent is the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:1;
(7) the NaOH solution that obtains that step (6) is obtained dropwise is added drop-wise to the SnCl of step (5)
4, Zn (NO
3)
2And Zn-SnO
2Suspension in, SnCl
4, Zn (NO
3)
2And Zn-SnO
2Suspension and the volume ratio of NaOH solution be 1:2, drop rate is 2 ~ 3ml/min, stirs, and obtains predecessor; Above-mentioned predecessor is moved in the reactor, 200 ℃, be incubated at least that 20h carries out the solvent thermal synthesis.
When (8) treating that the solvent thermal reaction device is reduced to room temperature, the hot product of solvent promptly gets nanometer 10%Zn-SnO after centrifugation, cleaning and drying
2/ Zn
2SnO
4Hetero-junctions.
The nanometer 10%Zn-SnO that present embodiment obtains
2/ Zn
2SnO
4Hetero-junctions, through the FESEM test as can be known, synthetic product is the near-spherical particle, the particle mean size is 20 ~ 30 nm.。
Embodiment 3:
The synthetic method of a kind of nanometer zinc-doped tin oxide/zinc stannate hetero-junctions, it comprises the steps:
(1) configuration amount of substance concentration is the NaOH solution of 2.5mol/L, and solvent is the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:1;
(2) configuration SnCl
45H
2O and Zn (NO
3)
26H
2The mixed solution of O, solvent are the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:1, wherein SnCl
4Amount of substance concentration be 0.4575 mol/L; Zn (NO
3)
2Amount of substance concentration be 0.0425 mol/L;
(3) the NaOH solution that step (1) is obtained dropwise is added drop-wise to the SnCl of step (2)
4And Zn (NO
3)
2Mixed solution in, SnCl
4And Zn (NO
3)
2Mixed solution and the volume ratio of the NaOH aqueous solution be 1:2, drop rate is 2 ~ 3ml/min, stirs, and obtains predecessor; Above-mentioned predecessor is moved in the hydrothermal reactor, 180 ℃, that insulation at least 15 h carry out hydro-thermal is synthetic.
When (4) treating that the solvent thermal reaction device is reduced to room temperature, the hot product of solvent promptly gets Zn-SnO after centrifugation, cleaning and drying
2Product.
(5) configuration SnCl
45H
2O and Zn (NO
3)
26H
2The mixed solution of O, solvent are the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:1, wherein SnCl
4Amount of substance concentration be 0.25mol/L; Zn (NO
3)
2Amount of substance concentration be 0.5 mol/L; Add step (4) 0.0625 mol/L Zn-SnO simultaneously
2, guarantee Zn-SnO
2Content is the 20%(mol ratio);
(6) configuration amount of substance concentration is the NaOH solution of 3.75 mol/L, and solvent is the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:1;
(7) the NaOH solution that obtains that step (6) is obtained dropwise is added drop-wise to the SnCl of step (5)
4, Zn (NO
3)
2And Zn-SnO
2Suspension in, SnCl
4, Zn (NO
3)
2And Zn-SnO
2Suspension and the volume ratio of NaOH solution be 1:2, drop rate is 2 ~ 3ml/min, stirs, and obtains predecessor; Above-mentioned predecessor is moved in the reactor, carry out the solvent thermal synthesis at 200 ℃, insulation at least 20 h.
When (8) treating that the solvent thermal reaction device is reduced to room temperature, the hot product of solvent promptly gets nanometer 10%Zn-SnO after centrifugation, cleaning and drying
2/ Zn
2SnO
4Hetero-junctions.
The nanometer 20%Zn-SnO that present embodiment obtains
2/ Zn
2SnO
4Hetero-junctions, through the FESEM test as can be known, synthetic product is the near-spherical particle, the particle mean size is 20 ~ 30 nm.
Claims (3)
1. the synthetic method of nanometer zinc-doped tin oxide/zinc stannate hetero-junctions is characterized in that it comprises the steps:
(1) configuration amount of substance concentration is the NaOH solution of 2.5mol/L, and solvent is the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:0.8 ~ 1;
(2) configuration SnCl
45H
2O and Zn (NO
3)
26H
2The mixed solution of O, solvent are the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:0.8 ~ 1, wherein SnCl
4Amount of substance concentration be 0.4475~0.4575 mol/L; Zn (NO
3)
2Amount of substance concentration be 0.0425~0.0525 mol/L;
(3) the NaOH solution that step (1) is obtained dropwise is added drop-wise to the SnCl of step (2)
4And Zn (NO
3)
2Mixed solution in, SnCl
4And Zn (NO
3)
2Mixed solution and the volume ratio of the NaOH aqueous solution be 1:2, drop rate is 2mL/min, stirs, and obtains predecessor; Above-mentioned predecessor is moved in the solvent thermal reaction device, 180 ℃, be incubated at least that 15h carries out the solvent thermal synthesis;
When (4) treating that the solvent thermal reaction device is reduced to room temperature, the hot product of solvent promptly gets Zn-SnO after centrifugation, cleaning and drying
2Product;
(5) configuration SnCl
45H
2O and Zn (NO
3)
26H
2The mixed solution of O, solvent are the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:0.8 ~ 1, wherein SnCl
4Amount of substance concentration be 0.25mol/L; Zn (NO
3)
2Amount of substance concentration be 0.5 mol/L; Add step (4) Zn-SnO simultaneously
20.0278 ~ 0.0625 mol/L guarantees Zn-SnO
2Molar content is 10-20%;
(6) configuration amount of substance concentration is the NaOH solution of 3.75 mol/L, and solvent is the mixture of deionized water and absolute ethyl alcohol, volume ratio 1:0.8 ~ 1;
(7) the NaOH solution that step (6) is obtained dropwise is added drop-wise to the SnCl of step (5)
4, Zn (NO
3)
2And Zn-SnO
2Suspension in, SnCl
4, Zn (NO
3)
2And Zn-SnO
2Suspension and the volume ratio of NaOH solution be 1:2, drop rate is 2mL/min, stirs, and obtains predecessor; Above-mentioned predecessor is moved in the reactor, 200 ℃, be incubated at least that 20h carries out the solvent thermal synthesis;
When (8) treating that the solvent thermal reaction device is reduced to room temperature, the hot product of solvent promptly gets nanometer Zn-SnO after centrifugation, cleaning and drying
2/ Zn
2SnO
4Hetero-junctions.
2. the synthetic method of nanometer zinc-doped tin oxide according to claim 1/zinc stannate hetero-junctions is characterized in that: before the solvent thermal reaction, the compactedness of reactor is 80 %.
3. the synthetic method of nanometer zinc-doped tin oxide according to claim 1/zinc stannate hetero-junctions, it is characterized in that: step (4) is followed successively by deionized water with (8) described cleaning process and absolute ethyl alcohol cleans, and the powder after the cleaning is obtaining end product behind dry 10 h under 80 ℃ of temperature.
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CN103265065B (en) * | 2013-04-22 | 2014-12-03 | 中山大学 | Preparation method of graded zinc stannate macroporous materials |
CN104402042A (en) * | 2014-10-22 | 2015-03-11 | 安徽科技学院 | Method for direct synthesis of Mn<+>-doped SnO2 nanocrystals with one-step hydrothermal method |
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CN106115773B (en) * | 2016-06-21 | 2017-12-12 | 广西新晶科技有限公司 | A kind of zinc stannate raw powder's production technology |
CN106492848A (en) * | 2016-11-29 | 2017-03-15 | 洛阳理工学院 | A kind of Basic bismuth bromide and nano-zinc stannate hetero-junctions and preparation method thereof |
CN106512978B (en) * | 2016-11-29 | 2018-12-25 | 洛阳理工学院 | Utilize nanometer Zn2SnO4The method for preparing visible light responsive photocatalyst |
CN107649163A (en) * | 2017-10-16 | 2018-02-02 | 陕西科技大学 | A kind of Zn2SnO4‑xNx/ ZnO photocatalyst and preparation method thereof |
CN107886594A (en) * | 2017-11-07 | 2018-04-06 | 龚土婷 | A kind of drive recorder with alcohol detection function |
CN115318273A (en) * | 2022-08-18 | 2022-11-11 | 电子科技大学长三角研究院(湖州) | Amorphous two-phase heterojunction photocatalyst and in-situ synthesis method thereof |
CN117696045B (en) * | 2024-02-05 | 2024-04-12 | 浙江师范大学杭州校区 | S-type heterojunction catalyst with high-efficiency photocatalysis and piezocatalysis as well as preparation method and application thereof |
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