WO2022056979A1 - Catalyseur à plasma de surface non-métallique et son procédé de préparation et son application - Google Patents
Catalyseur à plasma de surface non-métallique et son procédé de préparation et son application Download PDFInfo
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- 150000002843 nonmetals Chemical class 0.000 title 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
- B01J27/20—Carbon compounds
- B01J27/22—Carbides
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/39—Photocatalytic properties
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/06—Washing
-
- 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
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
- C01B3/042—Decomposition of water
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- 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
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- 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
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- 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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- 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
- C02F2101/32—Hydrocarbons, e.g. oil
- C02F2101/322—Volatile compounds, e.g. benzene
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- 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
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- 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
- C02F2101/345—Phenols
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- 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
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- 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
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- 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
- C02F2101/40—Organic compounds containing sulfur
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
- C02F2103/08—Seawater, e.g. for desalination
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- 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
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
Definitions
- the invention relates to the field of photocatalytic water hydrogen production and the field of photocatalytic environmental protection, in particular to a Ti3C2(MXene)/Cd0.5Zn0.5S catalyst with a special structure assembled by non-metal surface plasmon Ti3C2(MXene) and its application in photocatalytic water (including seawater) hydrogen production, photocatalytic degradation of organic matter in water, removal of volatile organic compounds and odorous organic matter.
- Hydrogen energy as a clean and non-polluting energy source, has attracted more and more people's attention. Hydrogen has the following characteristics: good thermal conductivity, easy recovery, good combustion performance, low loss, environmental friendliness, non-corrosive product water, and high energy per unit mass.
- One of the main factors restricting the development of hydrogen energy is the high cost of hydrogen.
- the main hydrogen production methods include traditional energy hydrogen production (coal hydrogen production, natural gas hydrogen production), renewable energy hydrogen production, water electrolysis hydrogen production and industrial by-product hydrogen.
- the present invention proposes the preparation and application of a non-metallic surface plasmon Ti3C2(MXene)/Cd0.5Zn0.5S photocatalyst.
- the Cd0.5Zn0.5S photocatalyst due to the non-metallic surface plasmon Ti3C2 (MXene) extending the absorption response to sunlight, effectively separates photogenerated electrons and holes, which can strengthen the photocatalytic hydrogen production reaction.
- a preparation method of a non-metallic surface plasma catalyst comprising the following steps: dispersing Cd0.5Zn0.5S and Ti3C2 in water, then performing a hydrothermal reaction in a protective atmosphere, and washing after the reaction to obtain Ti3C2/Cd0.5Zn0 .5S, and dried to obtain a non-metallic surface plasmon catalyst.
- the content of the Ti3C2 in the catalyst is 1-7wt%.
- the content of the Ti3C2 in the catalyst is 5 ⁇ 1wt%.
- the conditions of the hydrothermal reaction are: 150-200° C. for 12-24 hours.
- the preparation of the Ti3C2 take Ti3AlC2, add hydrofluoric acid, the mass ratio of which is 1:10-200, and react for 3 to 4 days, so that the aluminum in the Ti3AlC2 is dissolved; then filter and separate, and wash until neutral. .
- the preparation of the Cd0.5Zn0.5S take equimolar zinc acetate and cadmium acetate, stir in water for 30-60 minutes, add thioacetamide and ethylenediamine, and then add enough water to carry out water Thermal reaction, the reaction conditions are 180-220 DEG C for 12-24 hours, and then washed with deionized water to obtain Cd0.5Zn0.5S.
- non-metallic surface plasmon catalyst prepared by the above method in photocatalytic water production of hydrogen, or photocatalytic degradation of organic substances in water, removal of volatile organic substances and malodorous organic substances.
- the catalyst is dispersed in water and exposed to light for at least 30 minutes; the water is fresh water or sea water.
- Na 2 SO 4 and Na 2 S are used as sacrificial agents in the photocatalytic water-to-hydrogen production, and the illumination wavelength is ⁇ 420 nm.
- the present invention has the following beneficial effects:
- Ti3C2(MXene)/Cd0.5Zn0.5S can reduce the energy required to excite electrons, and the photoresponse extends to the visible light region and the infrared light region, so the present invention proposes a non-metallic surface plasmon Ti3C2(MXene)/Cd0.
- 5Zn0.5S is used in photocatalytic water hydrogen production reaction, especially in the infrared region, it also has good activity.
- Non-metallic surface plasmon Ti3C2(MXene)/Cd0.5Zn0.5S photocatalyst used in photocatalytic water (including seawater) to produce hydrogen, degrade organic compounds in water, remove volatile organic compounds and odorous organic compounds; non-metallic surface plasmon Ti3C2 (MXene) has good electrical conductivity and can form a Schottky barrier with the surface of the semiconductor Cd0.5Zn0.5S.
- the electrons generated on the semiconductor reach the non-metallic surface plasmon Ti3C2 (MXene) through the Schotten interface, so the electrons It is enriched on the non-metal surface plasmon Ti3C2 (MXene), and the holes are enriched on the semiconductor, which inhibits the recombination of electrons and holes.
- Promote photocatalytic water (including seawater) hydrogen production reaction degrade organic compounds in water, and remove volatile organic compounds and odorous organic compounds.
- Fig. 1 is the XRD pattern of Example 1-3Cd0.5Zn0.5S, JCPDS NO.01-089-2943, Ti3C2/Cd0.5Zn0.5S.
- Figure 2 shows the photocatalytic stability of 5wt% Ti3C2/Cd0.5Zn0.5S.
- Figure 3 is the HRTEM pattern of Ti3C2, Cd0.5Zn0.5S, 5wt% Ti3C2/Cd0.5Zn0.5S.
- Figure 4 is a graph showing the effect of different proportions of Ti3C2-Cd0.5Zn0.5S on hydrogen production in seawater and freshwater, respectively.
- Figure 5 is the photocurrent spectra of different ratios of Ti3C2-Cd0.5Zn0.5S.
- Figure 6 is the impedance spectra of different ratios of Ti3C2-Cd0.5Zn0.5S.
- Figure 7 is a static-fluorescence image of different ratios of Ti3C2-Cd0.5Zn0.5S.
- Figure 8 is the effect diagram of 5wt% Ti3C2/Cd0.5Zn0.5S and the reported photocatalyst applied to hydrogen production in seawater.
- Figure 9 is a spectrum of non-metallic surface plasmon effects.
- Figure 10 is the effect diagram of the physical mixing of Ti3C2 and Cd0.5Zn0.5S and the single Cd0.5Zn0.5S hydrogen production in fresh water.
- Figure 11 is a UV diffuse reflectance map of 5% Ti3C2/Cd0.5Zn0.5S and Cd0.5Zn0.5S.
- Figure 12 is a Raman pattern of 5% Ti3C2/Cd0.5Zn0.5S and Cd0.5Zn0.5S.
- Ti3AlC2 Take 1.0 g of Ti3AlC2, add 150 ml of hydrofluoric acid, and react for 4 days to dissolve the aluminum in Ti3AlC2. It is then separated by filtration and washed with deionized water to make the washings neutral. Freeze-dried for 2 days to obtain Ti3C2 powder.
- the photocurrent spectrum of Figure 5 shows that when Ti3C2 and Cd0.5Zn0.5S are used to synthesize new materials, the photogenerated current density can be significantly increased, and a large number of electrons are generated to facilitate the photocatalytic effect.
- the impedance value is mainly determined by the exchange resistance of electrons and holes and the transfer resistance of electrons or holes.
- the reactivity of electrons and holes can be significantly improved, and the mobility of electrons or holes in the material can be improved, which is beneficial to the effect of photocatalysis.
- Figure 7 shows the static-fluorescence graph.
- the fluorescence excitation intensity can evaluate the ability of electron-hole re-polymerization inside the material.
- the tendency of electron-hole re-polymerization is obviously reduced. Thereby, it is beneficial to the effect of photocatalysis.
- Figures 7 and 5, and the experimental results in Figure 6 are consistent, which further verifies the high efficiency of the new materials synthesized by Ti3C2 and Cd0.5ZN0.5S in photocatalysis.
- the solid circle in Fig. 9 is Ti3C2.
- the plasma electric field around Ti3C2 is simulated by finite element calculation. Deepened areas all indicate a strong electric field. This figure proves that non-metallic Ti3C2 also has surface plasmon effects from the theoretical calculation and simulation.
- Figure 11 is a UV diffuse reflectance map to demonstrate that the as-synthesized 5%Ti3C2/Cd0.5Zn0.5S and Cd0.5zn0.5S still have spectral absorption starting from a wavelength of about 510 nm. ability.
- the upward trajectory of the 5%Ti3C2/Cd0.5Zn0.5S spectrum shows an obvious surface plasmon phenomenon compared to the downward trajectory of the Cd0.5Zn0.5S spectrum.
- Figure 12 is the comparison of the Raman spectra of the two. Because the surface plasmon has the effect of Raman enhancement, the newly synthesized 5%Ti3C2/Cd0.5Zn0.5S has a stronger Raman phenomenon than Cd0.5Zn0.5S .
- Example 4 Photocatalytic hydrogen production from water with different percentages of Ti3C2(MXene)/Cd0.5Zn0.5S
- GC7900 online gas chromatograph
- Example 5 Photocatalytic hydrogen production from seawater by Ti3C2(MXene)/Cd0.5Zn0.5S
- Example 6 Photocatalytic degradation of organic matter in water by Ti3C2(MXene)/Cd0.5Zn0.5S
- Example 7 Photocatalytic removal of volatile organic compounds and malodorous organic compounds by Ti3C2(MXene)/Cd0.5Zn0.5S
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Abstract
La présente invention concerne le domaine de la production d'hydrogène photocatalytique à partir de l'eau et le domaine de la protection environnementale photocatalytique. L'invention concerne un catalyseur à plasma de surface non métallique, ainsi qu'un procédé de préparation et une application associée. Le procédé de préparation comprend les étapes suivantes : la dispersion de Cd0.5Zn0.5S et de Ti3C2 dans l'eau, puis la réalisation d'une réaction hydrothermique dans une atmosphère protectrice, le lavage après que la réaction a été achevée pour obtenir du Ti3C2/Cd0.5Zn0.5S, et le séchage pour obtenir le catalyseur à plasma de surface non métallique. Le catalyseur de la présente invention est appliqué à la production d'hydrogène photocatalytique à partir d'eau (comprenant de l'eau de mer), la dégradation de matières organiques dans l'eau et l'élimination des matières organiques volatiles et des matières organiques encrassées, et présente les avantages d'être large dans une plage de photoréponse, étant capable de séparer efficacement des électrons photo-induits et des paires de trous, et ayant une activité photocatalytique élevée.
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| CN202010994915.4A CN112246263B (zh) | 2020-09-21 | 2020-09-21 | 一种非金属表面等离子体催化剂及其制备方法和应用 |
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| WO2022056979A1 true WO2022056979A1 (fr) | 2022-03-24 |
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| PCT/CN2020/121111 WO2022056979A1 (fr) | 2020-09-21 | 2020-10-15 | Catalyseur à plasma de surface non-métallique et son procédé de préparation et son application |
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| CN115282987A (zh) * | 2022-08-18 | 2022-11-04 | 哈尔滨理工大学 | 一种高效人工光合光催化材料及其制备方法 |
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| CN112387264B (zh) * | 2020-11-16 | 2022-02-08 | 西南石油大学 | 一种基于等离子体处理TiO2的方法、改性TiO2光催化剂及应用 |
| CN116273060A (zh) * | 2023-03-01 | 2023-06-23 | 常州大学 | 一种硫化锌镉和碳化钛复合光催化剂的制备方法及应用 |
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| CN112246263B (zh) | 2022-04-22 |
| CN112246263A (zh) | 2021-01-22 |
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