CN113877606A - Non-complete coated core-shell nanoparticle self-driven catalyst and application thereof - Google Patents
Non-complete coated core-shell nanoparticle self-driven catalyst and application thereof Download PDFInfo
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- 239000002105 nanoparticle Substances 0.000 title claims abstract description 54
- 239000003054 catalyst Substances 0.000 title claims abstract description 41
- 239000011258 core-shell material Substances 0.000 title claims abstract description 40
- 239000002957 persistent organic pollutant Substances 0.000 claims abstract description 10
- 229910052802 copper Inorganic materials 0.000 claims description 26
- 239000010949 copper Substances 0.000 claims description 26
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 23
- FOIXSVOLVBLSDH-UHFFFAOYSA-N Silver ion Chemical compound [Ag+] FOIXSVOLVBLSDH-UHFFFAOYSA-N 0.000 claims description 19
- 230000015556 catabolic process Effects 0.000 claims description 15
- 238000006731 degradation reaction Methods 0.000 claims description 15
- 238000006243 chemical reaction Methods 0.000 claims description 12
- 230000000593 degrading effect Effects 0.000 claims description 7
- 238000013329 compounding Methods 0.000 claims description 2
- 238000002360 preparation method Methods 0.000 abstract description 6
- 239000010865 sewage Substances 0.000 abstract description 6
- 239000007864 aqueous solution Substances 0.000 abstract description 3
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 11
- YCKOAAUKSGOOJH-UHFFFAOYSA-N copper silver Chemical compound [Cu].[Ag].[Ag] YCKOAAUKSGOOJH-UHFFFAOYSA-N 0.000 description 10
- 230000003197 catalytic effect Effects 0.000 description 9
- 230000000694 effects Effects 0.000 description 8
- 238000000151 deposition Methods 0.000 description 7
- 238000006555 catalytic reaction Methods 0.000 description 6
- 230000008021 deposition Effects 0.000 description 6
- 229910052709 silver Inorganic materials 0.000 description 6
- 239000004332 silver Substances 0.000 description 6
- 238000010438 heat treatment Methods 0.000 description 4
- 238000002173 high-resolution transmission electron microscopy Methods 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 238000012546 transfer Methods 0.000 description 4
- VYXSBFYARXAAKO-WTKGSRSZSA-N chembl402140 Chemical compound Cl.C1=2C=C(C)C(NCC)=CC=2OC2=C\C(=N/CC)C(C)=CC2=C1C1=CC=CC=C1C(=O)OCC VYXSBFYARXAAKO-WTKGSRSZSA-N 0.000 description 3
- 239000003795 chemical substances by application Substances 0.000 description 3
- 239000011248 coating agent Substances 0.000 description 3
- 238000000576 coating method Methods 0.000 description 3
- 238000001704 evaporation Methods 0.000 description 3
- 230000008020 evaporation Effects 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- 239000000758 substrate Substances 0.000 description 3
- 230000009471 action Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- 239000002086 nanomaterial Substances 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 229910017770 Cu—Ag Inorganic materials 0.000 description 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 1
- OMSFUHVZHUZHAW-UHFFFAOYSA-N [Ag].[Mo] Chemical compound [Ag].[Mo] OMSFUHVZHUZHAW-UHFFFAOYSA-N 0.000 description 1
- 238000000862 absorption spectrum Methods 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000005253 cladding Methods 0.000 description 1
- WUUZKBJEUBFVMV-UHFFFAOYSA-N copper molybdenum Chemical compound [Cu].[Mo] WUUZKBJEUBFVMV-UHFFFAOYSA-N 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- VYXSBFYARXAAKO-UHFFFAOYSA-N ethyl 2-[3-(ethylamino)-6-ethylimino-2,7-dimethylxanthen-9-yl]benzoate;hydron;chloride Chemical compound [Cl-].C1=2C=C(C)C(NCC)=CC=2OC2=CC(=[NH+]CC)C(C)=CC2=C1C1=CC=CC=C1C(=O)OCC VYXSBFYARXAAKO-UHFFFAOYSA-N 0.000 description 1
- 238000005286 illumination Methods 0.000 description 1
- 238000009776 industrial production Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 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
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- 239000011943 nanocatalyst Substances 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 238000002207 thermal evaporation Methods 0.000 description 1
- 238000007738 vacuum evaporation Methods 0.000 description 1
- 239000002699 waste material Substances 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/89—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
- B01J23/8926—Copper and noble 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
- B01J35/20—Catalysts, in general, characterised by their form or physical properties characterised by their non-solid state
- B01J35/23—Catalysts, in general, characterised by their form or physical properties characterised by their non-solid state in a colloidal state
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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
- 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
- B01J35/396—Distribution of the active metal ingredient
- B01J35/397—Egg shell like
-
- 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
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
-
- 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
-
- 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
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- Chemical Kinetics & Catalysis (AREA)
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- General Chemical & Material Sciences (AREA)
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Abstract
The invention discloses a non-completely coated core-shell nanoparticle self-driven catalyst and application thereof. The self-driven catalyst can automatically and efficiently separate electrons and holes in the catalyst at room temperature, the separated electrons and holes can catalyze and degrade organic pollutants in an aqueous solution at room temperature under a lightless condition, the use condition is simple, the preparation cost is low, and the self-driven catalyst can be widely applied to treatment of industrial or domestic sewage and the like under the lightless condition.
Description
Technical Field
The invention relates to preparation and application of a self-driven catalyst, and belongs to the technical field of nano catalyst materials and sewage treatment.
Background
The catalytic reaction is a very important chemical reaction, and has created huge economic benefits and social benefits in chemical industry, pharmacy, energy, environmental protection and other industries at present. The catalytic reaction means that under the action of a catalyst, the reaction rate of the chemical reaction is greatly improved, the reaction process is accelerated, and the method has great significance for the sustainable development of the society. The catalyst is the core of catalytic reaction, and the action in the chemical reaction is to change the rate of the chemical reaction, and the principle is that the catalyst obviously reduces the energy barrier value which needs to be overcome by the chemical reaction, thereby accelerating the separation and transfer efficiency of electrons and holes in the catalytic reaction and achieving the effect of accelerating the progress of the chemical reaction.
In the current industrial production, the problem of sewage treatment is increasingly prominent, and the degradation of organic sewage by adopting a catalyst becomes a hot research topic. The existing catalyst for degrading organic pollutants is driven by light or heating, and the catalyst which has catalysis effect under the conditions of darkness and room temperature is fresh. If the catalyst can degrade organic pollutants at room temperature under the condition of no light, not only can energy be saved, but also convenience can be provided for degrading wastes in places on the earth which are dark for years.
Disclosure of Invention
Based on the problems in the prior art, the invention provides a non-completely coated core-shell nanoparticle self-driven catalyst and application thereof, and aims to enable the provided catalyst to be capable of completing the catalytic degradation effect on organic pollutants at room temperature under the condition of no light.
In order to achieve the purpose, the invention adopts the following technical scheme:
a non-complete coating type core-shell nanoparticle self-driven catalyst is characterized in that: the non-complete coated core-shell nano-particles used as the self-driven catalyst are formed by compounding copper nano-particles and silver nano-particles, wherein the copper nano-particles are partially embedded in the silver nano-particles and partially exposed outside the silver nano-particles. The size of the copper nano-particles is 2-40nm, and the size of the silver nano-particles is 3-40 nm.
The non-completely coated core-shell nano-particles are prepared by the following steps: firstly, preparing silver nanoparticles by a physical or chemical method; then, depositing copper nanoparticles on the surfaces of the silver nanoparticles, wherein the copper nanoparticles can partially enter the silver nanoparticles; the incomplete cladding type core-shell nano-particles are formed by controlling the mass ratio of the deposition amount of the nano-copper to the nano-silver.
The incompletely coated core-shell nano-particles can be used as a self-driven catalyst, active electrons and holes on the surface of the catalyst can be automatically and efficiently separated at room temperature under a dark condition, and the separated electrons and holes can drive a reaction for catalyzing degradation of organic matters, so that organic pollutants in a solution can be catalytically degraded. The principle of degrading organic pollutants by using the self-driven catalyst of the invention is as follows: based on the chemical micro-battery reaction, in a microscopic state, when nano copper and nano silver are contacted, the Fermi level of the copper and the Fermi level of the silver are automatically aligned due to the difference of the Fermi levels of the copper and the silver, so that charge transfer is generated between the copper and the silver, electron holes on the surface of the catalyst are automatically separated, and the separated electrons and holes act on organic dye in an aqueous solution, so that the effect of degrading organic pollutants is achieved.
Compared with the prior art, the invention has the beneficial effects that:
at present, catalysts such as metal nanostructures, semiconductor oxide nanostructures and the like are mainly researched at home and abroad, and catalytic reaction carried out by the catalysts is usually realized by adding specific conditions such as illumination or heating, and the conditions are provided by additional external energy, so that the cost of the catalysts for degrading pollutants is greatly increased. The invention designs a novel non-completely coated core-shell bimetallic nano copper and silver self-driven catalyst by improving the preparation process of copper and silver nano particles. Compared with other traditional catalysts, the self-driven catalyst provided by the invention has good charge transfer capacity, and can realize catalytic degradation of organic dye by transferring electrons and holes between the catalyst and the organic dye at room temperature and in dark environment. The self-driven catalyst of the invention participates in the catalytic degradation of organic matters without the intervention of additional conditions, has simple use conditions, and can be directly used in the fields of sewage treatment, degradation of harmful substances and the like. And the self-driven catalyst has low preparation cost.
Drawings
Fig. 1 is a schematic structural view of an incompletely coated core-shell nanoparticle (fig. 1(a)) and a completely coated core-shell nanoparticle (fig. 1 (b)).
Fig. 2 is a HRTEM high resolution image of the incompletely encapsulated core-shell nanoparticles prepared in example 1.
Fig. 3 is a HRTEM high resolution image of the fully encapsulated core-shell nanoparticles prepared in example 1.
Fig. 4 shows efficiency values of catalytic degradation of dye molecules by the incompletely coated core-shell nanoparticles, the completely coated core-shell nanoparticles, the single copper nanoparticles, the single silver nanoparticles and the copper-silver mixed nanoparticles in the example 1 under room temperature and no light environment.
Fig. 5 is a graph showing the efficiency value of the incompletely coated core-shell nanoparticles in example 1 in the room temperature dark environment for catalytically degrading dye molecules after the electron and hole trapping agents are added.
Detailed Description
The following examples are given for the detailed implementation and specific operation of the present invention, but the scope of the present invention is not limited to the following examples.
Example 1
In the embodiment, a non-complete coated copper-silver core-shell nanoparticle catalyst is prepared by adopting a vacuum evaporation coating mode, and the degradation effect of the catalyst on an R6G aqueous solution under room temperature and no light is tested. The preparation method comprises the following specific steps:
(1) a molybdenum boat was used to insert an evaporation electrode for vacuum thermal evaporation, 0.5g of silver wire was added to the silver-molybdenum boat, and 0.5g of copper wire was added to the copper-molybdenum boat, and a substrate was prepared.
(2) Starting the mechanical pump and the molecular pump to vacuumize the vacuum chamber until the indicated number of the vacuum meter is less than 10-3Pa。
(3) And (3) turning on a silver evaporation electrode power supply, adjusting a heating knob until the deposition rate is 0.03nm/s, controlling the deposition time to be 30s, and forming silver nanoparticles on the surface of the glass substrate.
(4) And (3) turning on a power supply of the copper evaporation electrode, adjusting the heating knob until the deposition rate is 0.03nm/s and the deposition time is controlled to be 30s, and forming the incomplete coating type copper-silver core-shell nano particles on the surface of the glass substrate.
Fig. 2 is an HRTEM high resolution image of the incompletely coated core-shell nanoparticle prepared in this embodiment, and it can be seen from the image that a part of the nano-copper is exposed outside the nano-silver, and the incompletely coated copper-silver core-shell nanoparticle structure is presented.
For comparison, the completely coated core-shell nanoparticles are also prepared in the embodiment, and the preparation method is the same as that of the non-completely coated core-shell nanoparticles, except that the deposition time of the nano-copper is reduced to 15s in the step (4), so that the completely coated copper-silver core-shell nanoparticles can be obtained. Fig. 3 is an HRTEM high resolution diagram of the completely encapsulated core-shell nanoparticle prepared in this embodiment, and it can be seen from the diagram that the nano-copper is completely encapsulated inside the nano-silver, presenting a completely encapsulated copper-silver core-shell nanoparticle structure.
For comparison, this example also prepared copper nanoparticles having a particle size of 2-10nm and silver nanoparticles having a particle size of 2-10 nm.
0.05G of the sample of the incompletely coated core-shell nanoparticles prepared in the example was added to 10mL of rhodamine 6G solution (concentration of 10%-5mol/L), placing the rhodamine 6G solution in a completely dark environment, taking out after placing for 30 minutes, testing the ultraviolet and visible absorption spectrum of the degraded rhodamine 6G solution, calculating the self-driven catalytic efficiency of the sample, and adopting-ln (C)t/C0) The value of (A) represents the degradation efficiency, C0Is the initial dye concentration, CtThe dye concentration after 30min of degradation.
Meanwhile, the self-driven catalytic efficiency of the fully encapsulated core-shell nanoparticles, the copper nanoparticles alone, the silver nanoparticles alone, and the mixture of the copper nanoparticles and the silver nanoparticles prepared in this example were tested by the same methods as described above.
As shown in fig. 4, it can be seen that the catalytic performance of the incompletely coated copper-silver core-shell nanoparticles is significantly better than that of the completely coated copper-silver core-shell nanoparticles, the single copper nanoparticles, the single silver nanoparticles and the copper-silver mixed nanoparticles (composed of the copper nanoparticles and the silver nanoparticles in a mass ratio of 1: 1).
To demonstrate the degradation of the incompletely encapsulated Cu-Ag core-shell nanoparticlesThis example was carried out by adding an electron and a hole-trapping agent (5 mL each, 9.6X 10 each) during the reaction, respectively-4mol/L) proves the self-driven catalytic degradation effect of the incompletely coated core-shell nano particles, and the result is shown in figure 5, after the electron and hole trapping agents are added, the catalytic degradation effect of the incompletely coated core-shell nano particles is obviously inhibited, and the degradation effect of the incompletely coated core-shell nano particles on organic pollutants under the conditions of no light and room temperature is proved.
The results show that the incomplete coated copper-silver core-shell nanoparticle self-driven catalyst can effectively utilize the high-efficiency and stable charge transfer capacity between copper and silver to catalyze and degrade organic pollutants, and represents the great potential of the catalyst in the aspect of industrial sewage treatment.
The present invention is not limited to the above preferred embodiments, and any modifications, equivalent substitutions and improvements made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (4)
1. A non-complete coated core-shell nanoparticle self-driven catalyst is characterized in that: the non-complete coated core-shell nano-particles used as the self-driven catalyst are formed by compounding copper nano-particles and silver nano-particles, wherein the copper nano-particles are partially embedded in the silver nano-particles and partially exposed outside the silver nano-particles.
2. The non-fully encapsulated core-shell nanoparticle self-driving catalyst according to claim 1, characterized in that: the size of the copper nano-particles is 2-40nm, and the size of the silver nano-particles is 3-40 nm.
3. Use of the incompletely encapsulated core-shell nanoparticles according to claim 1 or 2, wherein: the catalyst is used as a self-driven catalyst for catalytically degrading organic pollutants in a solution at room temperature under the dark condition.
4. Use according to claim 3, characterized in that: the incompletely coated core-shell nano-particles can automatically and efficiently separate active electrons and holes on the surface of the catalyst under a dark condition, and the separated electrons and holes can drive a reaction for catalyzing degradation of organic matters.
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Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20100197490A1 (en) * | 2004-12-22 | 2010-08-05 | Brookhaven Science Associates, Llc | Platinum-Coated Non-Noble Metal-Noble Metal Core-Shell Electrocatalysts |
| CN108459003A (en) * | 2018-01-17 | 2018-08-28 | 安徽农业大学 | A kind of preparation method of silver nano-grain coating zinc oxide surface enhanced Raman scattering effect substrate |
| CN110842190A (en) * | 2019-10-11 | 2020-02-28 | 云南大学 | Preparation method of silver-coated copper powder |
| CN111304640A (en) * | 2020-03-10 | 2020-06-19 | 哈尔滨工业大学(深圳)(哈尔滨工业大学深圳科技创新研究院) | Silver-coated copper powder, preparation method thereof and electronic paste |
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- 2021-09-30 CN CN202111157504.0A patent/CN113877606A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20100197490A1 (en) * | 2004-12-22 | 2010-08-05 | Brookhaven Science Associates, Llc | Platinum-Coated Non-Noble Metal-Noble Metal Core-Shell Electrocatalysts |
| CN108459003A (en) * | 2018-01-17 | 2018-08-28 | 安徽农业大学 | A kind of preparation method of silver nano-grain coating zinc oxide surface enhanced Raman scattering effect substrate |
| CN110842190A (en) * | 2019-10-11 | 2020-02-28 | 云南大学 | Preparation method of silver-coated copper powder |
| CN111304640A (en) * | 2020-03-10 | 2020-06-19 | 哈尔滨工业大学(深圳)(哈尔滨工业大学深圳科技创新研究院) | Silver-coated copper powder, preparation method thereof and electronic paste |
Non-Patent Citations (2)
| Title |
|---|
| HESHAM R ET AL.: "Novel synthesis of bimetallic Ag-Cu nanocatalysts for rapid oxidative and reductive degradation of anionic and cationic dyes", APPLIED SURFACE SCIENCE ADVANCES, vol. 3 * |
| HONGLIANG HAO ET AL.: "Epitaxial growth of Ag-Cu bimetallic nanoparticles via thermal evaporation deposition", APPLIED SURFACE SCIENCE, vol. 505, pages 2 * |
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