CN110902721A - Preparation method of rod-like ammonium fluotantalate material - Google Patents
Preparation method of rod-like ammonium fluotantalate material Download PDFInfo
- Publication number
- CN110902721A CN110902721A CN201911240894.0A CN201911240894A CN110902721A CN 110902721 A CN110902721 A CN 110902721A CN 201911240894 A CN201911240894 A CN 201911240894A CN 110902721 A CN110902721 A CN 110902721A
- Authority
- CN
- China
- Prior art keywords
- urea
- rod
- reaction kettle
- tantalum powder
- acetic acid
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
Images
Classifications
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G35/00—Compounds of tantalum
- C01G35/006—Compounds containing, besides tantalum, two or more other elements, with the exception of oxygen or hydrogen
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/70—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data
- C01P2002/72—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data by d-values or two theta-values, e.g. as X-ray diagram
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2004/00—Particle morphology
- C01P2004/01—Particle morphology depicted by an image
- C01P2004/03—Particle morphology depicted by an image obtained by SEM
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Inorganic Compounds Of Heavy Metals (AREA)
Abstract
Rod-shaped (NH)4)2Ta2O3F6The preparation method of the material is characterized by comprising the following steps: the method comprises the following steps of (1) taking metal tantalum powder, 40% by mass of hydrofluoric acid, analytically pure acetic acid, urea and deionized water as raw materials; adopting a hydrothermal method, namely, under the conditions of high temperature and high pressure, the solution containing tantalum ions and fluorine ions and urea are subjected to chemical reaction to generate white rod-shaped (NH)4)2Ta2O3F6The length-diameter ratio of the material is far greater than 10. The invention solves (NH)4)2Ta2O3F6The limitation of difficulty in material preparation; has the following advantages: the selected raw materials are easy to obtain, the experimental equipment is simple, the experimental period is short, and the process flow is easy to control. Prepared rod-like (NH)4)2Ta2O3F6The material has good application prospect in the field of photocatalysis, and can also be used for preparing Ta2O5A precursor of the nano material.
Description
Technical Field
The invention relates to a rod-shaped ammonium fluorotantalate ((NH)4)2Ta2O3F6) A preparation process of a material belongs to the technical field of micro-nano material preparation.
Background
The conversion of solar energy into renewable fuels and useful chemicals is a very promising approach to mitigate and address the world's energy shortages and serious environmental pollution. In contrast to traditional green and valuable chemical development methods, photocatalysis is an effective approach, such as photocatalytic hydrogen production, where semiconductor photocatalysts play a key role. Therefore, the development of efficient and stable semiconductor photocatalysts is still the focus of research in the field.
Tantalum pentoxide (Ta)2O5) Orthorhombic structure, where a =0.6180nm, b =4.0290nm, c =0.3888nm, α = β = γ =90 °. as an n-type wide bandgap semiconductor, its bandgap width is about 4.0eV, with excellent dielectric and optoelectronic properties2O5Has a potential of +3.83eV greater than H+/H2And the potential of the valence band position is-0.17 eV lower than O2/H2Reduction potential of O. This property is such that Ta2O5Becomes a promising material in hydrogen production. In addition, due to Ta2O5The catalyst has the advantages of high photocatalytic activity, excellent chemical stability and the like, and can be widely applied to the fields of pollutant treatment, carbon dioxide reduction and the like. Preparation of Ta2O5There are many methods for photocatalytic materials, such as hydrothermal method, templating method, sol-gel method, etc. Wherein ammonium fluorotantalate ((NH)4)2Ta2O3F6) Ta prepared as precursor2O5The nano material has extremely high photocatalytic activity; for example, Yuxin in the paper "SuperStructure Ta2O5mesocrystals derivedfrom (NH4)2Ta2O3F6In mesocrystals with effective photocatalytic activity ″, ammonium fluorotantalate ((NH) in rod form is used4)2Ta2O3F6) Successfully preparing mesomorphic Ta after calcining for 3 hours in air by 750-plus 900 DEG C2O5A nanosheet photocatalyst. It has a high specific surface area (16.34 m)2g-1) And the photocatalytic hydrogen production speed thereofThe rate can reach 11268.241 mu molg-1h-1Is commercial Ta2O5Photocatalyst (2851.95 mu mol g)-1h-1) 4 times of the total weight of the product.
In addition, the article also shows ammonium fluorotantalate in rod form ((NH)4)2Ta2O3F6) The semiconductor material is also a wide-band-gap semiconductor material, the forbidden band width of the semiconductor material is 4.40eV, the semiconductor material has strong photo-generated electron reduction capability, and the corresponding spectral absorption boundary is 282 nm. The experimental results show that the rod-shaped (NH)4)2Ta2O3F6The photocatalytic hydrogen production rate (3341.39 mu mol g)-1h-1) Far above commercial Ta2O5A photocatalyst; therefore, the method has very wide application prospect in the field of preparing hydrogen by photocatalytic water.
(NH4)2Ta2O3F6Belonging to the Pnma space group, orthorhombic structure, wherein a =10.43 Å, b =5.64 Å, c =14.84 Å = β = γ =90 °. each Ta atom is surrounded by six O or F atoms Ta (O, F)6The octahedral structures are connected to form a double sawtooth-shaped chain structure parallel to the b axis, and ammonium ions are positioned between the chains. Wherein the Ta element is Ta5+Is present in the form of (1). Is currently about (NH)4)2Ta2O3F6The synthesis research of (2) is very few; firstly, taking tantalum ethoxide, ammonium fluoride and ethylene glycol as raw materials, and successfully preparing mesogen (NH) by adopting a steam hydrolysis method4)2Ta2O3F6Nanorod with angular structure of 90%oAnd (4) an angle. Its length is about 8 μm and its diameter is about 800 nm. Secondly, jujuan in the thesis of morphology control of tantalum-based nano materials and research of photocatalytic hydrogen production performance, metal tantalum powder is dissolved in a mixed solution of concentrated nitric acid and hydrofluoric acid, and concentrated ammonia water is gradually added to obtain white precipitate; after centrifugal cleaning and drying, the mixture is moved to a reaction kettle, hydrofluoric acid and water are added, and the reaction is carried out for 24 hours at 180 ℃, thus obtaining (NH)4)2Ta2O3F6A nanotube. Is rich (NH)4)2Ta2O3F6The synthesis method of the invention deepens the understanding of the preparation mechanism, and the invention successfully prepares the rodlike (NH) with high purity, no impurities and uniform appearance by adopting a hydrothermal method4)2Ta2O3F6The material can be applied to the field of photocatalysis or used for preparing Ta2O5A precursor of the nanomaterial; the invention has the advantages of simple preparation method, easily obtained raw materials, short period and the like.
Disclosure of Invention
The purpose of the invention is to solve the problem of original (NH)4)2Ta2O3F6The problems of difficult material preparation, low purity, difficult raw material obtaining, complex steps and the like are solved, and the method provides the (NH) with simple process4)2Ta2O3F6The technical scheme of the material preparation process is as follows: the method is characterized in that metal tantalum powder, hydrofluoric acid with the mass fraction of 40%, analytically pure acetic acid, urea and deionized water are used as raw materials. The method comprises the following steps: (1) hydrofluoric acid and metal tantalum powder are mixed according to a molar ratio (3-12): 1, mixing, and fully stirring until the tantalum powder is completely dissolved; (2) deionized water and acetic acid are mixed according to the volume ratio (0.17-6): 1, uniformly mixing; gradually dripping acetic acid solution into the mixed solution containing tantalum ions and fluorine ions obtained in the step (1) to obtain milky mixed solution; (3) according to the molar ratio of (0.25-2) urea to metal tantalum powder: and 1, weighing urea with corresponding mass, adding the urea into the milky white solution system obtained in the step 3, and uniformly stirring. (4) Transferring the solution system into a lining of a hydrothermal reaction kettle, screwing down the reaction kettle, transferring the reaction kettle into a drying oven, heating to 160-210 ℃, and reacting for 3-48 hours; (5) after the reaction is finished, naturally cooling the reaction kettle to room temperature, then centrifugally separating the product to obtain white precipitate, repeatedly washing the white precipitate with ethanol and water, centrifuging until the filtrate is neutral, and finally drying to obtain white (NH)4)2Ta2O3F6A material.
The working principle of the invention is as follows: first, the metal Ta powder will form H when encountering excessive HF acid2TaF7And hydrogen (as shown in equation (1)); in addition, after the addition of acetic acid, the whole system is acidic:
2Ta(s)+ 14HF(l)=2H2TaF7(l)+5H2(g)(1)
in the hydrothermal synthesis, H2TaF7Urea and water to form white (NH)4)2Ta2O3F6And release CO2Gas (as shown in equation (2)):
2H2TaF7(l)+CO(NH2)2(s)+4H2O(l)= (NH4)2Ta2O3F6 (s)+8HF(l)+CO2(g)(2)
wherein l represents a liquid state, s represents a solid state and g represents a gaseous state; initially precipitated (NH)4)2Ta2O3F6The nano-particles are used as nucleation points and form (NH) through directed assembly4)2Ta2O3F6And (4) nanorods.
The invention has the following advantages: synthetic rod-like (NH)4)2Ta2O3F6High material purity, uniform appearance, simple preparation method, easily obtained raw materials, short period and the like. The material has good photocatalysis application prospect, and can also be used for preparing Ta2O5A precursor of the nano material.
Drawings
FIG. 1 is a rod-like (NH) prepared in example 14)2Ta2O3F6XRD spectrum of the material.
FIG. 2 is a rod-like (NH) prepared in example 14)2Ta2O3F6SEM pictures of the material.
FIG. 3 is a rod-like (NH) prepared in example 24)2Ta2O3F6XRD spectrum of the material.
FIG. 4 is a rod-like (NH) prepared in example 24)2Ta2O3F6SEM pictures of the material.
FIG. 5 is a rod prepared in example 3Form (NH)4)2Ta2O3F6XRD spectrum of the material.
FIG. 6 is a rod-like (NH) prepared in example 34)2Ta2O3F6SEM pictures of the material.
FIG. 7 is a rod-like (NH) prepared in example 44)2Ta2O3F6XRD spectrum of the material.
FIG. 8 is a rod-like (NH) prepared in example 44)2Ta2O3F6SEM pictures of the material.
FIG. 9 is a rod-like (NH) prepared in example 54)2Ta2O3F6XRD spectrum of the material.
FIG. 10 is a rod-like (NH) prepared in example 54)2Ta2O3F6SEM pictures of the material.
FIG. 11 is a rod-like (NH) prepared in example 64)2Ta2O3F6XRD spectrum of the material.
FIG. 12 is a rod-like (NH) prepared in example 64)2Ta2O3F6SEM pictures of the material.
Detailed Description
Example 1:
the method is characterized in that metal tantalum powder, hydrofluoric acid with the mass fraction of 40%, analytically pure acetic acid, urea and deionized water are used as raw materials. The method comprises the following steps: (1) mixing hydrofluoric acid and metal tantalum powder in a molar ratio of 5: 1, mixing, and fully stirring until the metal tantalum powder is dissolved; (2) mixing deionized water and glacial acetic acid according to the volume ratio of 0.75: 1, uniformly mixing; gradually dripping acetic acid solution into the mixed solution containing tantalum ions and fluorine ions obtained in the step (1) to obtain milky mixed solution; (3) according to the molar ratio of urea to metal tantalum powder of 0.5: and 1, weighing urea with corresponding mass, adding the urea into the milky white solution system obtained in the step 3, and uniformly stirring. (4) Transferring the solution system into the inner liner of a hydrothermal reaction kettle, screwing down the reaction kettle, transferring the reaction kettle into an oven, heating to 200 ℃,reacting for 6 hours; (5) after the reaction is finished, naturally cooling the reaction kettle to room temperature, then centrifugally separating the product to obtain white precipitate, repeatedly washing the white precipitate with ethanol and water, centrifuging until the filtrate is neutral, and finally drying to obtain white rod-shaped (NH)4)2Ta2O3F6A material.
The white color (NH) prepared4)2Ta2O3F6The powder was subjected to X-ray diffraction phase analysis (XRD), and the XRD pattern obtained was as shown in FIG. 1. The main characteristic diffraction peaks are all equal to (NH)4)2Ta2O3F6The standard Card (JCPDS Card No. 31-0070) is identical, and no other impurity diffraction peaks exist; the three-strong diffraction peak is positioned at 10.35o、20.79oAnd 25.43oRespectively corresponding to an orthorhombic (NH)4)2Ta2O3F6The (101), (202) and (113) crystal planes of the phases; this shows that (NH) is prepared4)2Ta2O3F6The material is single-phase, high-purity and almost free of other crystal impurity phases.
FIG. 2 shows the preparation of (NH)4)2Ta2O3F6Scanning Electron Microscope (SEM) images of the material. The results show that (NH) is produced4)2Ta2O3F6The material has a rod-like structure, the length of which is 50-80 μm and the width of which is about 5 μm (as shown in FIG. 2 (a)). FIG. 2(b) shows a rod-like (NH)4)2Ta2O3F6The material has an angular framework, and the surface is relatively smooth and compact.
Example 2:
the method is characterized in that metal tantalum powder, hydrofluoric acid with the mass fraction of 40%, analytically pure acetic acid, urea and deionized water are used as raw materials. The method comprises the following steps: (1) mixing hydrofluoric acid and metal tantalum powder in a molar ratio of 5: 1, mixing, and fully stirring until the metal tantalum powder is dissolved; (2) mixing deionized water and glacial acetic acid according to the volume ratio of 0.75: 1, uniformly mixing; gradually dripping acetic acid solution into the tantalum ion and fluorine ion-containing solution obtained in the step (1)Obtaining a milky white mixed solution in the mixed solution; (3) according to the molar ratio of urea to metal tantalum powder of 0.5: and 1, weighing urea with corresponding mass, adding the urea into the milky white solution system obtained in the step 3, and uniformly stirring. (4) Transferring the solution system into the inner liner of a hydrothermal reaction kettle, screwing down the reaction kettle, transferring the reaction kettle into a drying oven, heating to 200 ℃, and reacting for 12 hours; (5) after the reaction is finished, naturally cooling the reaction kettle to room temperature, then centrifugally separating the product to obtain white precipitate, repeatedly washing the white precipitate with ethanol and water, centrifuging until the filtrate is neutral, and finally drying to obtain white rod-shaped (NH)4)2Ta2O3F6A material.
The white color (NH) prepared4)2Ta2O3F6The powder was subjected to X-ray diffraction phase analysis (XRD) and the XRD pattern obtained was as shown in FIG. 3. The main characteristic diffraction peaks are all equal to (NH)4)2Ta2O3F6The standard Card (JCPDS Card No. 31-0070) is identical, and no other impurity diffraction peaks exist; the three-strong diffraction peak is positioned at 10.35o、20.79oAnd 29.46oRespectively corresponding to an orthorhombic (NH)4)2Ta2O3F6The (101), (202) and (213) crystal planes of the phases; in addition, the diffraction peak of the obtained XRD was sharp, indicating that (NH) was produced4)2Ta2O3F6The crystallinity of the material is high. Thus, the white rod (NH) prepared by the method4)2Ta2O3F6The material has good crystallization, high purity and almost no existence of other crystal impurity phases.
FIG. 4 shows the preparation of (NH)4)2Ta2O3F6Scanning Electron Microscope (SEM) images of the material. The results show that (NH) is produced4)2Ta2O3F6The material has a rod-like structure and a length of 50 to 100 μm (see FIG. 4 (a)). FIG. 4(b) shows a rod-like (NH)4)2Ta2O3F6The material has an edge structure with 90 deg. angle and opposite surfacesSmooth and relatively compact, and the diameter of the material is 2-4 mu m.
Example 3:
the method is characterized in that metal tantalum powder, hydrofluoric acid with the mass fraction of 40%, analytically pure acetic acid, urea and deionized water are used as raw materials. The method comprises the following steps: (1) mixing hydrofluoric acid and metal tantalum powder in a molar ratio of 5: 1, mixing, and fully stirring until the metal tantalum powder is dissolved; (2) mixing deionized water and glacial acetic acid according to the volume ratio of 0.75: 1, uniformly mixing; gradually dripping acetic acid solution into the mixed solution containing tantalum ions and fluorine ions obtained in the step (1) to obtain milky mixed solution; (3) according to the molar ratio of urea to metal tantalum powder of 0.5: 1, weighing urea, adding the urea into the milky white solution system obtained in the step (3), and uniformly stirring. (4) Transferring the solution system into the inner liner of a hydrothermal reaction kettle, screwing down the reaction kettle, transferring the reaction kettle into a drying oven, heating to 200 ℃, and reacting for 24 hours; (5) after the reaction is finished, naturally cooling the reaction kettle to room temperature, then centrifugally separating the product to obtain white precipitate, repeatedly washing the white precipitate with ethanol and water, centrifuging until the filtrate is neutral, and finally drying to obtain white rod-shaped (NH)4)2Ta2O3F6A material.
The white color (NH) prepared4)2Ta2O3F6The powder was subjected to X-ray diffraction phase analysis (XRD) and the XRD pattern obtained was as shown in FIG. 5. The main characteristic diffraction peaks are all equal to (NH)4)2Ta2O3F6The standard Card (JCPDS Card No. 31-0070) is identical, and no other impurity diffraction peaks exist; the obtained XRD has sharp diffraction peak, and its three strong diffraction peaks are located at 10.35o、20.79oAnd 29.46oRespectively corresponding to an orthorhombic (NH)4)2Ta2O3F6The (101), (202) and (213) crystal planes of the phases; this indicates that white rods (NH) were prepared4)2Ta2O3F6The material has good crystallization, high purity and almost no existence of other crystal impurity phases.
FIG. 6 shows preparation of (NH)4)2Ta2O3F6Scanning Electron Microscope (SEM) images of the material. The results show that (NH) is produced4)2Ta2O3F6The material has a rod-like structure with a length of about 100 μm; partially rod-shaped (NH)4)2Ta2O3F6A tendency of cluster growth occurs (as shown in fig. 6 (a)). FIG. 6(b) shows a rod-like (NH)4)2Ta2O3F6The edge structure of the material is no longer obvious, the surface is relatively smooth, and the diameter of the material is 4-6 mu m.
Example 4:
the method is characterized in that metal tantalum powder, hydrofluoric acid with the mass fraction of 40%, analytically pure acetic acid, urea and deionized water are used as raw materials. The method comprises the following steps: (1) mixing hydrofluoric acid and metal tantalum powder in a molar ratio of 5: 1, mixing, and fully stirring until the metal tantalum powder is dissolved; (2) mixing deionized water and glacial acetic acid according to the volume ratio of 0.75: 1, uniformly mixing; gradually dripping acetic acid solution into the mixed solution containing tantalum ions and fluorine ions obtained in the step (1) to obtain milky mixed solution; (3) according to the molar ratio of urea to metal tantalum powder of 0.5: 1, weighing urea, adding the urea into the milky white solution system obtained in the step (3), and uniformly stirring. (4) Transferring the solution system into the inner liner of a hydrothermal reaction kettle, screwing down the reaction kettle, transferring the reaction kettle into a drying oven, heating to 180 ℃, and reacting for 3 hours; (5) after the reaction is finished, naturally cooling the reaction kettle to room temperature, then centrifugally separating the product to obtain white precipitate, repeatedly washing the white precipitate with ethanol and water, centrifuging until the filtrate is neutral, and finally drying to obtain white rod-shaped (NH)4)2Ta2O3F6A material.
The white color (NH) prepared4)2Ta2O3F6The powder was subjected to X-ray diffraction phase analysis (XRD) and the XRD pattern obtained was as shown in FIG. 7. The main characteristic diffraction peaks are all equal to (NH)4)2Ta2O3F6The standard Card (JCPDS Card No. 31-0070) is identical, and no other impurity diffraction peaks exist; the diffraction peak of the obtained XRD is sharp, and the three strong diffraction peaks are positioned at 10.35o、20.79oAnd 29.46oRespectively corresponding to an orthorhombic (NH)4)2Ta2O3F6The (101), (202) and (213) crystal planes of the phases; this indicates that white rods (NH) were prepared4)2Ta2O3F6The material has good crystallization, high purity and almost no existence of other crystal impurity phases.
FIG. 8 shows preparation of (NH)4)2Ta2O3F6Scanning Electron Microscope (SEM) images of the material. The results show that (NH) is produced4)2Ta2O3F6The material has a rod-like structure with a length of about 20-40 μm, and is partially rod-like (NH)4)2Ta2O3F6A tendency of cluster growth occurs (as shown in fig. 8 (a)). FIG. 8(b) shows a rod-like (NH)4)2Ta2O3F6The material has an edge structure with an angle of 90 degrees, a relatively smooth and compact surface and a diameter of about 0.5-2.5 μm.
Example 5:
the method is characterized in that metal tantalum powder, hydrofluoric acid with the mass fraction of 40%, analytically pure acetic acid, urea and deionized water are used as raw materials. The method comprises the following steps: (1) mixing hydrofluoric acid and metal tantalum powder in a molar ratio of 5: 1, mixing, and fully stirring until the metal tantalum powder is dissolved; (2) mixing deionized water and glacial acetic acid according to the volume ratio of 0.75: 1, uniformly mixing; gradually dripping acetic acid solution into the mixed solution containing tantalum ions and fluorine ions obtained in the step (1) to obtain milky mixed solution; (3) according to the molar ratio of urea to metal tantalum powder of 0.5: 1, weighing urea, adding the urea into the milky white solution system obtained in the step (3), and uniformly stirring. (4) Transferring the solution system into the inner liner of a hydrothermal reaction kettle, screwing down the reaction kettle, transferring the reaction kettle into a drying oven, heating to 180 ℃, and reacting for 24 hours; (5) after the reaction is finished, naturally cooling the reaction kettle to room temperature, then centrifugally separating the product to obtain white precipitate, repeatedly washing the white precipitate with ethanol and water, centrifuging until the filtrate is neutral, and finally drying to obtain white rod-shaped (NH)4)2Ta2O3F6A material.
The white color (NH) prepared4)2Ta2O3F6The powder was subjected to X-ray diffraction phase analysis (XRD), and the XRD pattern obtained was as shown in FIG. 9. The main characteristic diffraction peaks are all equal to (NH)4)2Ta2O3F6The standard Card (JCPDS Card No. 31-0070) is identical, and no other impurity diffraction peaks exist; the obtained XRD has sharp diffraction peak, and its three strong diffraction peaks are located at 10.35o、20.79oAnd 29.46oRespectively corresponding to an orthorhombic (NH)4)2Ta2O3F6The (101), (202) and (213) crystal planes of the phases; this indicates that white rods (NH) were prepared4)2Ta2O3F6The material has good crystallization, high purity and almost no existence of other crystal impurity phases.
FIG. 10 shows preparation (NH)4)2Ta2O3F6Scanning Electron Microscope (SEM) images of the material. The results show that (NH) is produced4)2Ta2O3F6The material had a rod-like structure with a length of about 40 μm (as shown in FIG. 10 (a)). FIG. 10(b) shows a rod-like (NH)4)2Ta2O3F6The material has an edge structure, is 90 degrees, has a relatively smooth and compact surface, and has a diameter of about 1-2 μm.
Example 6:
the method is characterized in that metal tantalum powder, hydrofluoric acid with the mass fraction of 40%, analytically pure acetic acid, urea and deionized water are used as raw materials. The method comprises the following steps: (1) mixing hydrofluoric acid and metal tantalum powder in a molar ratio of 5: 1, mixing, and fully stirring until the metal tantalum powder is dissolved; (2) mixing deionized water and glacial acetic acid according to the volume ratio of 0.75: 1, uniformly mixing; gradually dripping acetic acid solution into the mixed solution containing tantalum ions and fluorine ions obtained in the step (1) to obtain milky mixed solution; (3) according to the molar ratio of urea to metal tantalum powder of 0.5: 1, weighing urea, adding the urea into the milky white solution system obtained in the step (3), and uniformly stirring. (4) Will be provided withTransferring the solution system into the inner liner of a hydrothermal reaction kettle, screwing down the reaction kettle, transferring the reaction kettle into a drying oven, heating to 160 ℃, and reacting for 6 hours; (5) after the reaction is finished, naturally cooling the reaction kettle to room temperature, then centrifugally separating the product to obtain white precipitate, repeatedly washing the white precipitate with ethanol and water, centrifuging until the filtrate is neutral, and finally drying to obtain white rod-shaped (NH)4)2Ta2O3F6A material.
The white color (NH) prepared4)2Ta2O3F6The powder was subjected to X-ray diffraction phase analysis (XRD), and the XRD pattern obtained was as shown in FIG. 11. The main characteristic diffraction peaks are all equal to (NH)4)2Ta2O3F6The standard Card (JCPDS Card No. 31-0070) is identical, and no other impurity diffraction peaks exist; its three-strong diffraction peak is positioned in 10.35o、20.79oAnd 29.46oRespectively corresponding to an orthorhombic (NH)4)2Ta2O3F6The (101), (202) and (213) crystal planes of the phases; this indicates that white rods (NH) were prepared4)2Ta2O3F6The material is single-phase, has high purity and almost has no other crystal impurity phase.
FIG. 12 shows preparation of (NH)4)2Ta2O3F6Scanning Electron Microscope (SEM) images of the material. The results show that (NH) is produced4)2Ta2O3F6The material has a rod-like structure with a length of about 50 μm; partially rod-shaped (NH)4)2Ta2O3F6A tendency of cluster growth occurs (as shown in fig. 12 (a)). FIG. 12(b) shows a rod-like (NH)4)2Ta2O3F6The edge structure of the material is no longer obvious, and the surface is relatively smooth and compact; in addition, a granular structure of (NH) also appears4)2Ta2O3F6The diameter of the metal wire is about 5 to 10 μm.
Example 7:
using tantalum powder as a baseHydrofluoric acid with the weight fraction of 40%, analytically pure acetic acid, urea and deionized water are used as raw materials. The method comprises the following steps: (1) mixing hydrofluoric acid and metal tantalum powder in a molar ratio of 3: 1, mixing, and fully stirring until the metal tantalum powder is dissolved; (2) deionized water and glacial acetic acid are mixed according to the volume ratio of 6: 1, uniformly mixing; gradually dripping acetic acid solution into the mixed solution containing tantalum ions and fluorine ions obtained in the step (1) to obtain milky mixed solution; (3) according to the mol ratio of 2: 1, weighing urea, adding the urea into the milky white solution system obtained in the step (3), and uniformly stirring. (4) Transferring the solution system into the inner liner of a hydrothermal reaction kettle, screwing down the reaction kettle, transferring the reaction kettle into a drying oven, heating to 160 ℃, and reacting for 48 hours; (5) after the reaction is finished, naturally cooling the reaction kettle to room temperature, then centrifugally separating the product to obtain white precipitate, repeatedly washing the white precipitate with ethanol and water, centrifuging until the filtrate is neutral, and finally drying to obtain white (NH)4)2Ta2O3F6A material.
Example 8:
the method is characterized in that metal tantalum powder, hydrofluoric acid with the mass fraction of 40%, analytically pure acetic acid, urea and deionized water are used as raw materials. The method comprises the following steps: (1) mixing hydrofluoric acid and metal tantalum powder in a molar ratio of 12: 1, mixing, and fully stirring until the metal tantalum powder is dissolved; (2) mixing deionized water and glacial acetic acid according to the volume ratio of 0.17: 1, uniformly mixing; gradually dripping acetic acid solution into the mixed solution containing tantalum ions and fluorine ions obtained in the step (1) to obtain milky mixed solution; (3) according to the molar ratio of urea to metal tantalum powder of 0.25: 1, weighing urea, adding the urea into the milky white solution system obtained in the step (3), and uniformly stirring. (4) Transferring the solution system into the inner liner of a hydrothermal reaction kettle, screwing down the reaction kettle, transferring the reaction kettle into a drying oven, heating to 210 ℃, and reacting for 3 hours; (5) after the reaction is finished, naturally cooling the reaction kettle to room temperature, then centrifugally separating the product to obtain white precipitate, repeatedly washing the white precipitate with ethanol and water, centrifuging until the filtrate is neutral, and finally drying to obtain white (NH)4)2Ta2O3F6A material.
Claims (1)
1. Rod-shaped (NH)4)2Ta2O3F6The preparation method of the material is characterized by comprising the following steps: the method comprises the following steps of (1) taking metal tantalum powder, 40% by mass of hydrofluoric acid, analytically pure acetic acid, urea and deionized water as raw materials; the method comprises the following steps: (1) hydrofluoric acid and metal tantalum powder are mixed according to a molar ratio (3-12): 1, mixing, and fully stirring until the tantalum powder is completely dissolved; (2) deionized water and glacial acetic acid are mixed according to the volume ratio (0.17-6): 1, uniformly mixing; gradually dripping acetic acid solution into the mixed solution containing tantalum ions and fluorine ions obtained in the step (1) to obtain milky mixed solution; (3) according to the molar ratio of (0.25-2) urea to the used metal tantalum powder: 1, weighing urea with corresponding mass, adding the urea into the milky white solution system obtained in the step (2), and uniformly stirring; (4) transferring the solution system into a lining of a hydrothermal reaction kettle, screwing down the reaction kettle, transferring the reaction kettle into a drying oven, heating to 160-210 ℃, and reacting for 3-48 hours; (5) after the reaction is finished, naturally cooling the reaction kettle to room temperature, then centrifugally separating the product to obtain white precipitate, repeatedly washing the white precipitate with ethanol and water, centrifuging until the filtrate is neutral, and finally drying to obtain white (NH)4)2Ta2O3F6A material.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201911240894.0A CN110902721B (en) | 2019-12-06 | 2019-12-06 | Preparation method of rod-like ammonium fluotantalate material |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201911240894.0A CN110902721B (en) | 2019-12-06 | 2019-12-06 | Preparation method of rod-like ammonium fluotantalate material |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN110902721A true CN110902721A (en) | 2020-03-24 |
| CN110902721B CN110902721B (en) | 2022-02-25 |
Family
ID=69822742
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201911240894.0A Active CN110902721B (en) | 2019-12-06 | 2019-12-06 | Preparation method of rod-like ammonium fluotantalate material |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN110902721B (en) |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111905772A (en) * | 2020-07-27 | 2020-11-10 | 山东理工大学 | Preparation method of carbon-coated tantalum oxyfluoride nanosheet |
| CN114351239A (en) * | 2021-12-15 | 2022-04-15 | 中国科学院金属研究所 | Preparation method of porous metal compound array film |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110294495A (en) * | 2019-05-28 | 2019-10-01 | 山东理工大学 | A method of preparing TaO2F nanometer rods |
| CN110357158A (en) * | 2019-05-28 | 2019-10-22 | 山东理工大学 | A kind of three-dimensional sea urchin shape nanostructure TaO2The preparation method of F material |
-
2019
- 2019-12-06 CN CN201911240894.0A patent/CN110902721B/en active Active
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110294495A (en) * | 2019-05-28 | 2019-10-01 | 山东理工大学 | A method of preparing TaO2F nanometer rods |
| CN110357158A (en) * | 2019-05-28 | 2019-10-22 | 山东理工大学 | A kind of three-dimensional sea urchin shape nanostructure TaO2The preparation method of F material |
Non-Patent Citations (3)
| Title |
|---|
| XIN YU等: "Superstructure Ta2O5 mesocrystals derived from (NH4)2Ta2O3F6 mesocrystals with efficient photocatalytic activity", 《DALTON TRANS.》 * |
| 于欣: "五氧化二钽基纳米材料的制备及光催化性能研究", 《中国优秀博硕士学位论文全文数据库(博士)工程科技Ⅰ辑》 * |
| 朱长娟: "钽基纳米材料的形貌控制及光催化制氢性能研究", 《中国优秀博硕士学位论文全文数据库(硕士)工程科技Ⅰ辑》 * |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111905772A (en) * | 2020-07-27 | 2020-11-10 | 山东理工大学 | Preparation method of carbon-coated tantalum oxyfluoride nanosheet |
| CN114351239A (en) * | 2021-12-15 | 2022-04-15 | 中国科学院金属研究所 | Preparation method of porous metal compound array film |
| CN114351239B (en) * | 2021-12-15 | 2024-05-17 | 中国科学院金属研究所 | Preparation method of porous metal compound array film |
Also Published As
| Publication number | Publication date |
|---|---|
| CN110902721B (en) | 2022-02-25 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN102295304B (en) | Preparation method of pseudo-boehmite and microcrystalline corundum abrasive | |
| CN110668452B (en) | Preparation of SiO from fly ash2-Al2O3Method of compounding aerogel materials | |
| Mi et al. | Highly controlled crystallite size and crystallinity of pure and iron-doped anatase-TiO2 nanocrystals by continuous flow supercritical synthesis | |
| CN103240119B (en) | Chirality graphite phase carbon nitride polymer semiconductor photocatalyst | |
| CN110902721B (en) | Preparation method of rod-like ammonium fluotantalate material | |
| CN106732724B (en) | A kind of N doping TiO2The preparation method of hollow nano-material | |
| CN101311376A (en) | Method for preparing strontium titanate nanometer powder of one-dimensional structure | |
| CN106475127A (en) | A kind of nitrogen-doped graphene quantum dot/mesopore titania photocatalyst and preparation method thereof | |
| CN103274461B (en) | Method for modulating titanium dioxide crystalline phases by using fluoride ions | |
| CN104925863A (en) | Preparation method of monoclinic structure vanadium dioxide powder | |
| CN112875755A (en) | Preparation method of bismuth tungstate nano powder | |
| Fang et al. | Rapid microwave-assisted sol-gel synthesis and exceptional visible light photocatalytic activities of Bi12TiO20 | |
| CN100588758C (en) | Preparation for sodium titanate crystal whisker | |
| CN111137921B (en) | Preparation method of tantalum oxyfluoride nanosheet | |
| CN101880057B (en) | Method for preparing high-purity brookite titanium dioxide with controlled appearance | |
| CN101811677B (en) | Method for preparing hollow porous quadruped titanium nitride | |
| CN105883910A (en) | Preparation method and product for perovskite SrTiO3 porous nano particles | |
| Hirano et al. | Direct Synthesis of New Zircon‐Type ZrGeO4 and Zr (Ge, Si) O4 Solid Solutions | |
| CN112850649B (en) | Preparation method of bismuth oxybromide nanosheet | |
| Shaoyou et al. | Effect of ethanol on synthesis and electrochemical property of mesoporous Al-doped titanium dioxide via solid-state reaction | |
| CN110368963B (en) | Ti ion doped TaO2Preparation method of F nano material | |
| CN113336240A (en) | Method for preparing single/double crystal ZSM-5 zeolite based on kaolin mineral regulation and control | |
| Xu et al. | Effect of crystallization degree on optical characteristics of NB2O5 by sol–gel process | |
| CN110681376A (en) | Morphology-adjustable rare earth ion co-doped tungsten oxide nanoparticle and synthesis method thereof | |
| CN111392770B (en) | Shuttle-like titanium dioxide nanocrystal and preparation method thereof |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| SE01 | Entry into force of request for substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| CB03 | Change of inventor or designer information | ||
| CB03 | Change of inventor or designer information |
Inventor after: Li Li Inventor after: Geng Xin Inventor after: Wen Guangwu Inventor after: Xu Yujuan Inventor after: Liu Kaitao Inventor after: Sun Zhiyuan Inventor after: Wang Peng Inventor before: Geng Xin Inventor before: Wen Guangwu Inventor before: Xu Yujuan Inventor before: Liu Kaitao Inventor before: Sun Zhiyuan Inventor before: Wang Peng Inventor before: Li Li |
|
| GR01 | Patent grant | ||
| GR01 | Patent grant |