CN112723878A - Energy-collecting porous ceramic Pt-BaTiO3Its preparation method and high-efficiency hydrogen production - Google Patents
Energy-collecting porous ceramic Pt-BaTiO3Its preparation method and high-efficiency hydrogen production Download PDFInfo
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- 239000000919 ceramic Substances 0.000 title claims abstract description 88
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 68
- 239000001257 hydrogen Substances 0.000 title claims abstract description 68
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 65
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 42
- 238000002360 preparation method Methods 0.000 title claims abstract description 19
- 229910002113 barium titanate Inorganic materials 0.000 claims abstract description 68
- 230000003197 catalytic effect Effects 0.000 claims abstract description 17
- 239000011159 matrix material Substances 0.000 claims abstract description 6
- 239000011148 porous material Substances 0.000 claims abstract description 5
- 239000008187 granular material Substances 0.000 claims description 18
- 229920002472 Starch Polymers 0.000 claims description 17
- 235000019698 starch Nutrition 0.000 claims description 17
- 239000008107 starch Substances 0.000 claims description 17
- 239000002245 particle Substances 0.000 claims description 16
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 15
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 15
- 238000006555 catalytic reaction Methods 0.000 claims description 15
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 15
- 238000010438 heat treatment Methods 0.000 claims description 14
- 238000002156 mixing Methods 0.000 claims description 14
- 238000003825 pressing Methods 0.000 claims description 14
- 238000009210 therapy by ultrasound Methods 0.000 claims description 13
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 claims description 9
- 238000003306 harvesting Methods 0.000 claims description 9
- WDIHJSXYQDMJHN-UHFFFAOYSA-L barium chloride Chemical compound [Cl-].[Cl-].[Ba+2] WDIHJSXYQDMJHN-UHFFFAOYSA-L 0.000 claims description 8
- 229910001626 barium chloride Inorganic materials 0.000 claims description 8
- 239000003054 catalyst Substances 0.000 claims description 8
- 238000000034 method Methods 0.000 claims description 8
- 238000001816 cooling Methods 0.000 claims description 7
- 238000000465 moulding Methods 0.000 claims description 7
- 230000010287 polarization Effects 0.000 claims description 7
- 238000000498 ball milling Methods 0.000 claims description 6
- IWOUKMZUPDVPGQ-UHFFFAOYSA-N barium nitrate Chemical compound [Ba+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O IWOUKMZUPDVPGQ-UHFFFAOYSA-N 0.000 claims description 6
- 238000005469 granulation Methods 0.000 claims description 6
- 230000003179 granulation Effects 0.000 claims description 6
- XJDNKRIXUMDJCW-UHFFFAOYSA-J titanium tetrachloride Chemical compound Cl[Ti](Cl)(Cl)Cl XJDNKRIXUMDJCW-UHFFFAOYSA-J 0.000 claims description 6
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 5
- QVQLCTNNEUAWMS-UHFFFAOYSA-N barium oxide Chemical compound [Ba]=O QVQLCTNNEUAWMS-UHFFFAOYSA-N 0.000 claims description 4
- 159000000009 barium salts Chemical class 0.000 claims description 4
- DCKVFVYPWDKYDN-UHFFFAOYSA-L oxygen(2-);titanium(4+);sulfate Chemical compound [O-2].[Ti+4].[O-]S([O-])(=O)=O DCKVFVYPWDKYDN-UHFFFAOYSA-L 0.000 claims description 4
- 150000003608 titanium Chemical class 0.000 claims description 4
- 229910000348 titanium sulfate Inorganic materials 0.000 claims description 4
- 229910002621 H2PtCl6 Inorganic materials 0.000 claims description 2
- 239000003513 alkali Substances 0.000 claims description 2
- 229910021529 ammonia Inorganic materials 0.000 claims description 2
- 239000002585 base Substances 0.000 claims description 2
- 239000000203 mixture Substances 0.000 claims 1
- 239000000446 fuel Substances 0.000 abstract description 10
- 229910000510 noble metal Inorganic materials 0.000 abstract description 6
- 229910010293 ceramic material Inorganic materials 0.000 abstract description 5
- JBANFLSTOJPTFW-UHFFFAOYSA-N azane;boron Chemical compound [B].N JBANFLSTOJPTFW-UHFFFAOYSA-N 0.000 abstract description 4
- 239000000243 solution Substances 0.000 description 28
- 238000006243 chemical reaction Methods 0.000 description 11
- 239000000463 material Substances 0.000 description 10
- 238000007789 sealing Methods 0.000 description 10
- XYFCBTPGUUZFHI-UHFFFAOYSA-N Phosphine Natural products P XYFCBTPGUUZFHI-UHFFFAOYSA-N 0.000 description 8
- 239000007789 gas Substances 0.000 description 7
- 229910000085 borane Inorganic materials 0.000 description 6
- 238000005086 pumping Methods 0.000 description 6
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 5
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 5
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 5
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 5
- 235000011114 ammonium hydroxide Nutrition 0.000 description 5
- 229910002091 carbon monoxide Inorganic materials 0.000 description 5
- 238000002474 experimental method Methods 0.000 description 5
- 229910000037 hydrogen sulfide Inorganic materials 0.000 description 5
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 4
- 229910000073 phosphorus hydride Inorganic materials 0.000 description 4
- 239000002574 poison Substances 0.000 description 4
- 231100000614 poison Toxicity 0.000 description 4
- 239000007864 aqueous solution Substances 0.000 description 3
- 125000004429 atom Chemical group 0.000 description 3
- 239000007772 electrode material Substances 0.000 description 3
- 150000002431 hydrogen Chemical class 0.000 description 3
- 238000012545 processing Methods 0.000 description 3
- 230000009471 action Effects 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 239000002803 fossil fuel Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- QDZRBIRIPNZRSG-UHFFFAOYSA-N titanium nitrate Chemical compound [O-][N+](=O)O[Ti](O[N+]([O-])=O)(O[N+]([O-])=O)O[N+]([O-])=O QDZRBIRIPNZRSG-UHFFFAOYSA-N 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 241000282414 Homo sapiens Species 0.000 description 1
- 229910003203 NH3BH3 Inorganic materials 0.000 description 1
- 239000003034 coal gas Substances 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 229940079593 drug Drugs 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 230000005684 electric field Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- XLYOFNOQVPJJNP-ZSJDYOACSA-N heavy water Substances [2H]O[2H] XLYOFNOQVPJJNP-ZSJDYOACSA-N 0.000 description 1
- GPRLSGONYQIRFK-UHFFFAOYSA-N hydron Chemical compound [H+] GPRLSGONYQIRFK-UHFFFAOYSA-N 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 238000003801 milling Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- 230000010355 oscillation Effects 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 239000003209 petroleum derivative Substances 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000010970 precious metal Substances 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 238000003797 solvolysis reaction Methods 0.000 description 1
- 230000004083 survival effect Effects 0.000 description 1
- 238000005979 thermal decomposition reaction Methods 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
- C04B35/46—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates
- C04B35/462—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates based on titanates
- C04B35/465—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates based on titanates based on alkaline earth metal titanates
- C04B35/468—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates based on titanates based on alkaline earth metal titanates based on barium titanates
-
- 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
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/56—Platinum group metals
- B01J23/58—Platinum group metals with alkali- or alkaline earth metals
-
- B01J35/33—
-
- B01J35/60—
-
- 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
- C01B3/06—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents
- C01B3/065—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents from a hydride
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B38/00—Porous mortars, concrete, artificial stone or ceramic ware; Preparation thereof
- C04B38/06—Porous mortars, concrete, artificial stone or ceramic ware; Preparation thereof by burning-out added substances by burning natural expanding materials or by sublimating or melting out added substances
- C04B38/063—Preparing or treating the raw materials individually or as batches
- C04B38/0635—Compounding ingredients
- C04B38/0645—Burnable, meltable, sublimable materials
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B38/00—Porous mortars, concrete, artificial stone or ceramic ware; Preparation thereof
- C04B38/06—Porous mortars, concrete, artificial stone or ceramic ware; Preparation thereof by burning-out added substances by burning natural expanding materials or by sublimating or melting out added substances
- C04B38/063—Preparing or treating the raw materials individually or as batches
- C04B38/0635—Compounding ingredients
- C04B38/0645—Burnable, meltable, sublimable materials
- C04B38/067—Macromolecular compounds
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/02—Processes for making hydrogen or synthesis gas
- C01B2203/0266—Processes for making hydrogen or synthesis gas containing a decomposition step
- C01B2203/0277—Processes for making hydrogen or synthesis gas containing a decomposition step containing a catalytic decomposition step
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/10—Catalysts for performing the hydrogen forming reactions
- C01B2203/1041—Composition of the catalyst
- C01B2203/1047—Group VIII metal catalysts
- C01B2203/1064—Platinum group metal catalysts
- C01B2203/107—Platinum catalysts
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/10—Catalysts for performing the hydrogen forming reactions
- C01B2203/1041—Composition of the catalyst
- C01B2203/1082—Composition of support materials
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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
Abstract
The invention provides an energy-collecting porous ceramic Pt-BaTiO3Its preparation method and high-efficiency hydrogen production. The porous ceramic with the energy collection function comprises BaTiO3The piezoelectric ceramic comprises a piezoelectric porous ceramic matrix and Pt monoatomic atoms uniformly dispersed on the surface of the ceramic matrix and in pore channels, wherein the mass fraction of the Pt monoatomic atoms is 0.01-0.1 wt%. The porous ceramic material with the functions of energy collection, provided by the invention has the advantages of low content of noble metal, high catalytic activity and great reduction of production cost. The energy-collecting porous ceramic can be used for preparing high-purity hydrogen by self-energizing in ammonia borane solution and can be directly used asThe hydrogen fuel cell vehicle provides hydrogen energy.
Description
Technical Field
The invention relates to porous ceramic Pt-BaTiO with energy collection and catalysis functions3The preparation method especially relates to a Pt monoatomic BaTiO3A preparation method of piezoelectric porous ceramics and application thereof in self-powered high-efficiency hydrogen production belong to the field of clean energy materials.
Background
The development of new energy sources in the world is urgent, because the used energy sources such as petroleum, natural gas, coal and petroleum gas are all non-renewable resources, the stock on the earth is limited, and the human beings can not leave the energy sources all the time for survival, so the new energy sources are required to be searched. With the increasing consumption and decreasing reserves of fossil fuels, the resources and energy sources will be exhausted in the whole day, and a new energy-containing body energy source which is rich in reserves and does not depend on the fossil fuels is urgently needed to be found. Hydrogen is just such a new secondary energy source that people expect while the conventional energy crisis appears and new secondary energy sources are developed. However, the electrode material of the hydrogen fuel cell is easily poisoned by impurities such as carbon monoxide, hydrogen sulfide, phosphine, and chloride ions mixed in the hydrogen gas, thereby affecting the service life of the hydrogen fuel cell. Therefore, the preparation of high-purity hydrogen has important application value for developing hydrogen fuel cells and new energy automobile industries. In addition, although the noble metal can be used as a catalyst to produce hydrogen, the noble metal is expensive and has limited resources, thereby limiting the wide application of the noble metal. Therefore, how to prepare high-purity hydrogen by using a material with low quality of precious metal and high catalytic activity is an urgent problem to be solved.
Disclosure of Invention
Most of the existing hydrogen sources are derived from chemical hydrogen production, and the existing hydrogen sources contain gaseous substances such as carbon monoxide, hydrogen sulfide, phosphine, chloride ions and the like which are easy to poison electrode materials of fuel cells. The invention aims to provide porous ceramic Pt-BaTiO with energy collection and catalysis functions3The material, the preparation method thereof and the application thereof in vehicle-mounted self-powered high-efficiency hydrogen production, so as to overcome the defects in the prior hydrogen production technology and overcome the defects of low utilization rate and low catalytic activity of noble metal Pt in the prior art, which result in higher cost.
In order to achieve the purpose, the technical scheme adopted by the invention comprises the following steps:
the porous ceramic Pt-BaTiO with energy collection and catalysis functions3Materials including BaTiO3The piezoelectric ceramic comprises a piezoelectric porous ceramic matrix and Pt monoatomic atoms uniformly dispersed on the surface of the piezoelectric porous ceramic;
wherein the mass fraction of the Pt monoatomic atoms is 0.01 wt% -0.1 wt%;
the BaTiO3The aperture of the piezoelectric porous ceramic matrix is 0.1 mm-1.0 mm.
Preferably, the upper limit of the mass fraction of Pt monoatomic is selected from 0.02 wt%, 0.03 wt%, 0.04 wt%, 0.05 wt%, 0.06 wt%, 0.07 wt%, 0.08 wt%, 0.09 wt%, 0.10 wt%; the lower limit of the mass fraction of Pt monoatomic atoms is selected from 0.01 wt%, 0.02 wt%, 0.03 wt%, 0.04 wt%, 0.05 wt%, 0.06 wt%, 0.07 wt%, 0.08 wt%, 0.09 wt%.
Preferably, the BaTiO3The upper limit of the pore diameter of the piezoelectric porous ceramic is selected from 0.2mm, 0.3mm, 0.4mm, 0.5mm, 0.6mm, 0.7mm, 0.8mm, 0.9mm and 1.0 mm; the BaTiO3The lower limit of the pore diameter of the piezoelectric porous ceramic is selected from 0.01mm, 0.02mm, 0.03mm, 0.04mm, 0.05mm, 0.06mm, 0.07mm, 0.08mm and 0.09 mm.
Optionally, the Pt monoatomic group is also dispersed in the BaTiO3The surfaces of the piezoelectric porous ceramic pore channels.
The porous ceramic Pt-BaTiO with energy collection and catalysis functions3The preparation method of the material comprises the following steps:
(1) preparation of BaTiO3And (3) particle: reacting barium salt and titanium salt with alkali to generate BaTiO3Particles;
(2) and (3) granulation: adding the BaTiO prepared in the step (1)3Respectively adding 0.5-8 wt% of starch and a certain amount of polyvinyl alcohol solution into the granules, and ball-milling and granulating;
(3) preparing a greenware: BaTiO prepared in the step (2)3Adding the granules into a mould with a certain size, and pressing into a greenware by a film pressing machine under the pressure of 10-30 MPa;
(4) pore-forming and degumming: heating the ceramic blank to 350-450 ℃, and keeping the temperature for 1-2 h; continuously heating for degumming treatment;
(5) molding: after degumming, processing for 0.5h-2h at the temperature of 900 ℃ -1150 ℃, and cooling to obtain BaTiO3A porous ceramic;
(6) and (3) polarization treatment: mixing BaTiO3Polarizing the porous ceramic plate for 20-60min at the voltage of 3-5 KV/mm, and standing for 24h to obtain BaTiO3Piezoelectric porous ceramics;
(7) Pt-BaTiO with energy collection and catalysis functions3Preparing porous ceramics: mixing BaTiO3The piezoelectric porous ceramic is arranged in H2PtCl6Carrying out ultrasonic treatment in the solution to obtain the Pt-BaTiO with the energy collecting and catalyzing function3The porous ceramic of (1).
Optionally, the temperature of the degumming treatment is 500-.
Optionally, the barium salt is selected from at least one of barium chloride, barium nitrate and barium oxide.
Optionally, the titanium salt is selected from at least one of titanium sulfate and titanium chloride.
Optionally, the base is selected from at least one of sodium hydroxide, potassium hydroxide, and ammonia.
Alternatively, the BaTiO3The particles are prepared by reacting barium chloride, titanium sulfate and sodium hydroxide.
Optionally, the concentration of the sodium hydroxide is 0.1mol/L to 1.0 mol/L.
Alternatively, the BaTiO3The particles are prepared by reacting barium chloride, titanium chloride and ammonia water.
Optionally, the concentration of the ammonia water is 0.1mol/L-1.0 mol/L.
Optionally, the starch is present in an amount of 0.5-8 wt%.
Optionally, the starch is 0.5 wt% by mass.
Optionally, the starch is 1.0 wt% by mass.
Optionally, the starch is present in an amount of 2.0 wt%.
Optionally, the starch is 3.0 wt% by mass.
Optionally, the starch is 4.0 wt% by mass.
Optionally, the starch is 5.0 wt% by mass.
Optionally, the starch is 6.0 wt% by mass.
Optionally, the starch is 7.0 wt% by mass.
Optionally, the starch is 8.0 wt% by mass.
Optionally, the mass concentration of the polyvinyl alcohol (PVA) solution is 5.0-8.0 wt%.
Optionally, the polyvinyl alcohol (PVA) solution has a mass concentration of 6.0 wt%.
Optionally, the polyvinyl alcohol (PVA) solution has a mass concentration of 7.0 wt%.
Optionally, the temperature of the pore-forming treatment is 350 ℃, 380 ℃, 400 ℃ and 450 ℃;
optionally, the temperature of the degumming treatment is 450 ℃, 500 ℃, 550 ℃ and 600 ℃;
optionally, the ultrasonic treatment time is 30-80 min, and the ultrasonic treatment frequency is 20-60 KHz.
Optionally, the upper limit of the ultrasonic treatment time is 40min, 50min, 60min, 70min, 80 min; the lower limit of the ultrasonic treatment time is 30min, 40min, 50min, 60min and 70 min.
The Pt-BaTiO with the energy collection and catalysis functions3The porous ceramic is applied to self-powered high-efficiency hydrogen production.
Preferably, the frequency of the ultrasonic wave is 10-60 KHz.
Preferably, the upper limit of the frequency of the ultrasonic wave is 20KHz, 30KHz, 40KHz, 50KHz and 60 KHz; the lower limit of the frequency of the ultrasonic wave is 10KHz, 20KHz, 30KHz, 40KHz and 50 KHz.
Preferably, the Pt-BaTiO with energy collection and catalytic functions3The porous ceramic is applied to vehicle-mounted self-powered hydrogen production.
Preferably, the Pt-BaTiO is treated at the temperature of 1-95 DEG C3The hydrogen production reaction system formed by the porous ceramic and the ammonia borane aqueous solution applies mechanical vibration or ultrasonic vibration to realize the preparation of the hydrogen.
Preferably, a self-powered piezoelectric catalytic hydrogen production method comprises the following steps:
(1) putting ammonia borane aqueous solution into a catalytic hydrogen production reactor, and adding Pt-BaTiO into the ammonia borane aqueous solution3A hydrogen production reaction system is formed by the piezoelectric porous ceramic material, and then the reactor is sealed;
(2) adjusting the temperature of the reactor to 1-95 ℃, then pumping the system to vacuum, and adjusting the temperature in the reactor to 20-30 ℃ after the reactor reaches a vacuum state;
(3) and applying ultrasonic waves to a hydrogen production reaction system in the reactor to enable the hydrogen production reaction system to react and produce hydrogen.
The piezoelectric material can convert mechanical energy into electric energy, and the action principle is that the original electrically neutral material generates non-coincidence of positive and negative charge centers under the action of external force by utilizing the asymmetry of the structure of the material, so that two ends or two surfaces of the material are provided with different charges. The mechanical vibration or the ultrasonic vibration realizes the conversion of mechanical energy and electric energy.
The reaction mechanism of the piezoelectric catalytic hydrogen production provided by the invention is that NH is carried out in the presence of a proper catalyst3BH3Hydrogen may be released by solvolysis or thermal decomposition, as shown in formula (I) below:
NH3BH3(aq)+2H2O(l)＝NH4 +(aq)+BO2 -(aq)+3H2(g) formula (I)
In the present invention, Pt-BaTiO3The piezoelectric porous ceramic material is a catalyst with piezoelectric effect. The catalyst generates piezoelectric effect in ultrasonic oscillation, and forms self-establishing electric field in the material to make the electrons move directionally, so that the generated electrons and protons H in water+Reacting to generate hydrogen, generating positive hole and negative hydrogen ion H-The combination produces hydrogen.
The hydrogen prepared by the method is high-purity hydrogen, and does not contain carbon monoxide, hydrogen sulfide and other pollutants which poison fuel cell electrode materials.
In one embodiment, the Pt monatomic BaTiO prepared according to the invention3The piezoelectric porous ceramic material hydrogen production system is applied to running automobiles, converts vibration energy in the running process of the automobiles into electric energy, and then produces hydrogen through piezoelectric catalytic reaction to serve as automobile fuel, so that self-powered hydrogen production is realized.
In one embodiment, the Pt-BaTiO prepared by the invention3Piezoelectric porous ceramic materialThe hydrogen production system is applied to a production workshop with large noise, and converts sound waves generated during workshop production into electric energy to realize self-powered hydrogen production.
Compared with the prior art, the invention has the advantages that:
(1) the invention provides Pt-BaTiO3The porous ceramic material has low Pt content and high catalytic activity, and reduces the use of noble metals, thereby greatly reducing the production cost.
(2) The invention provides Pt-BaTiO3The porous ceramic has a function of collecting sound waves, water waves, wind waves, ultrasonic waves and mechanical vibration energy.
(3) The invention provides Pt-BaTiO3The porous ceramic can provide vehicle-mounted high-purity hydrogen for the hydrogen fuel cell, and does not contain gases such as carbon monoxide, hydrogen sulfide, phosphine, chloride ions and the like which poison the fuel cell.
Detailed Description
In view of the deficiencies in the prior art, the inventors of the present invention have made extensive studies and extensive practices to provide technical solutions of the present invention. The technical solution, its implementation and principles, etc. will be further explained as follows.
The technical solution of the present invention is further explained below with reference to several examples.
The medicines used in the examples of the application are all commercially available.
Example 1
(1) Preparation of BaTiO3And (3) particle: reacting barium chloride, titanium chloride and ammonia water to generate BaTiO3Particles;
(2) and (3) granulation: adding the BaTiO prepared in the step (1)3Respectively adding 0.5 wt% of starch and a certain amount of polyvinyl alcohol solution into the granules, and ball-milling and granulating;
(3) preparing a greenware: BaTiO prepared in the step (2)3Adding the granules into a mold with the diameter of 20mm multiplied by 20mm, and pressing the granules into a greenware by a film pressing machine under the pressure of 10 MPa;
(4) pore-forming and degumming: heating the greenware to 3500 ℃, and keeping the temperature for 1 h; continuously heating to 500 ℃ for degumming treatment;
(5) molding: after degumming, processing for 2h at the temperature of 1150 ℃, and cooling to obtain BaTiO3A porous ceramic;
(6) and (3) polarization treatment: mixing BaTiO3Polarizing the porous ceramic plate for 20min under the voltage of 3KV/mm, and standing for 24h to obtain BaTiO3An energy harvesting porous ceramic;
(7)Pt-BaTiO3preparing porous ceramic with energy collection and catalysis functions: mixing BaTiO3The piezoelectric porous ceramic is placed in 0.1mol/LH2PtCl6Carrying out ultrasonic treatment in the solution to obtain the Pt monoatomic BaTiO3The piezoelectric energy collection is porous ceramic with catalytic function.
The hydrogen production reaction is as follows:
the method comprises the following steps: providing 100mL of NH at a concentration of 0.05mol/L3BH3Putting the solution into a reactor, and adding the self-energized Pt-BaTiO into the solution3Covering the piezoelectric porous ceramic with a quartz glass plate and sealing the reactor;
step two: connecting the hydrogen production system and the low-temperature constant-temperature tank in the first step, sealing, controlling the temperature of the low-temperature constant-temperature tank to be 1 ℃, then pumping the system to be vacuum, and controlling the temperature of the system to be 25 ℃ through the low-temperature constant-temperature tank after the system reaches a vacuum state;
step three: and (3) placing the reactor in a 28KHz ultrasonic cleaner, turning on the ultrasonic, adjusting the hydrogen production system to a system circulation state, performing an experiment, and detecting the hydrogen yield of each hour by a gas chromatograph every other hour.
Example 2
(1) Preparation of BaTiO3And (3) particle: reacting barium chloride, titanium sulfate and sodium hydroxide to generate BaTiO3Particles;
(2) and (3) granulation: adding the BaTiO prepared in the step (1)3Adding 1.0 wt% of starch and a certain amount of polyvinyl alcohol solution into the granules respectively, and ball-milling and granulating;
(3) preparing a greenware: BaTiO prepared in the step (2)3Adding the granules into a mold with the diameter of 20mm multiplied by 20mm, and pressing the granules into a greenware by a film pressing machine under the pressure of 15 MPa;
(4) pore-forming and degumming: heating the greenware to 400 ℃, and keeping the temperature for 2 hours; continuously heating to 550 ℃ for degumming treatment;
(5) molding: treating for 0.5h at 1150 ℃ after degumming, and cooling to obtain BaTiO3A porous ceramic;
(6) and (3) polarization treatment: mixing BaTiO3Polarizing the porous ceramic plate for 30min under the voltage of 4KV/mm, and standing for 24h to obtain BaTiO3Piezoelectric porous ceramics;
(7)Pt-BaTiO3preparing porous ceramic with energy collection and catalysis functions: mixing BaTiO3The piezoelectric porous ceramic is placed in 0.2mol/LH2PtCl6Carrying out ultrasonic treatment in the solution to obtain the Pt monoatomic BaTiO3The piezoelectric energy collection is porous ceramic with catalytic function.
The hydrogen production reaction is as follows:
the method comprises the following steps: providing 100mL of NH at a concentration of 0.05mol/L3BH3Putting the solution into a reactor, adding the self-energized piezoelectric porous ceramic into the solution, covering a quartz glass plate, and sealing the reactor;
step two: connecting the hydrogen production system and the low-temperature constant-temperature tank in the first step, sealing, controlling the temperature of the low-temperature constant-temperature tank to be 1 ℃, then pumping the system to be vacuum, and controlling the temperature of the system to be 25 ℃ through the low-temperature constant-temperature tank after the system reaches a vacuum state;
step three: and (3) placing the reactor in a 28KHz ultrasonic cleaner, turning on the ultrasonic, adjusting the hydrogen production system to a system circulation state, performing an experiment, and detecting the hydrogen yield of each hour by a gas chromatograph every other hour.
Example 3
(1) Preparation of BaTiO3And (3) particle: barium nitrate, titanium nitrate and potassium hydroxide are reacted to generate BaTiO3Particles;
(2) and (3) granulation: adding the BaTiO prepared in the step (1)3Adding 2.0 wt% of starch and a certain amount of polyvinyl alcohol solution into the granules respectively, and ball-milling and granulating;
(3) preparing a greenware: BaTiO prepared in the step (2)3Adding the granules into a mold with the diameter of 20mm multiplied by 20mm, and pressing the granules into a greenware by a film pressing machine under the pressure of 20 MPa;
(4) pore-forming and degumming: heating the greenware to 450 ℃, and keeping the temperature for 1 h; continuously heating to carry out degumming treatment at the temperature of 550 ℃;
(5) molding: after degumming, processing for 1.0h at the temperature of 1200 ℃, and cooling to obtain BaTiO3A porous ceramic;
(6) and (3) polarization treatment: mixing BaTiO3Polarizing the porous ceramic plate for 40min under the voltage of 5KV/mm, and standing for 24h to obtain BaTiO3Piezoelectric porous ceramics;
(7)Pt-BaTiO3preparing porous ceramic with energy collection and catalysis functions: mixing BaTiO3The piezoelectric porous ceramic is placed in 0.5mol/LH2PtCl6Carrying out ultrasonic treatment in the solution to obtain the Pt monoatomic BaTiO3The piezoelectric energy collection is porous ceramic with catalytic function.
The hydrogen production reaction is as follows:
the method comprises the following steps: providing 100mL of NH at a concentration of 0.05mol/L3BH3Putting the solution into a reactor, adding the self-energized piezoelectric porous ceramic into the solution, covering a quartz glass plate, and sealing the reactor;
step two: connecting the hydrogen production system and the low-temperature constant-temperature tank in the first step, sealing, controlling the temperature of the low-temperature constant-temperature tank to be 1 ℃, then pumping the system to be vacuum, and controlling the temperature of the system to be 25 ℃ through the low-temperature constant-temperature tank after the system reaches a vacuum state;
step three: and (3) placing the reactor in a 28KHz ultrasonic cleaner, turning on the ultrasonic, adjusting the hydrogen production system to a system circulation state, performing an experiment, and detecting the hydrogen yield of each hour by a gas chromatograph every other hour.
Example 4
(1) Preparation of BaTiO3And (3) particle: reacting barium chloride, titanium chloride and ammonia water to generate BaTiO3Particles;
(2) and (3) granulation: adding the BaTiO prepared in the step (1)35.0 wt% of starch and a certain amount of polyvinyl alcohol are respectively added into the granulesBall milling and granulating the solution;
(3) preparing a greenware: BaTiO prepared in the step (2)3Adding the granules into a mold with the diameter of 20mm multiplied by 20mm, and pressing the granules into a greenware by a film pressing machine under the pressure of 30 MPa;
(4) pore-forming and degumming: heating the greenware to 450 ℃, and keeping the temperature for 2 hours; continuously heating to 600 ℃ for degumming treatment;
(5) molding: treating at 1350 deg.C for 0.5h after degumming, and cooling to obtain BaTiO3A porous ceramic;
(6) and (3) polarization treatment: mixing BaTiO3Polarizing the porous ceramic plate for 60min under the voltage of 3KV/mm, and standing for 24h to obtain BaTiO3Piezoelectric porous ceramics;
(7)Pt-BaTiO3preparing porous ceramic with energy collection and catalysis functions: mixing BaTiO3The piezoelectric porous ceramic is placed in 0.5mol/LH2PtCl6Carrying out ultrasonic treatment in the solution to obtain the Pt monoatomic BaTiO3The piezoelectric energy collection is porous ceramic with catalytic function.
The hydrogen production reaction is as follows:
the method comprises the following steps: providing 100mL of NH at a concentration of 0.05mol/L3BH3Putting the solution into a reactor, adding the self-energized piezoelectric porous ceramic into the solution, covering a quartz glass plate, and sealing the reactor;
step two: connecting the hydrogen production system and the low-temperature constant-temperature tank in the first step, sealing, controlling the temperature of the low-temperature constant-temperature tank to be 1 ℃, then pumping the system to be vacuum, and controlling the temperature of the system to be 25 ℃ through the low-temperature constant-temperature tank after the system reaches a vacuum state;
step three: and (3) placing the reactor in a 28KHz ultrasonic cleaner, turning on the ultrasonic, adjusting the hydrogen production system to a system circulation state, performing an experiment, and detecting the hydrogen yield of each hour by a gas chromatograph every other hour.
Example 5
(1) Preparation of BaTiO3And (3) particle: reacting barium chloride, titanium chloride and ammonia water to generate BaTiO3Particles;
(2) granulating: adding the BaTiO prepared in the step (1)3Respectively adding 8.0 wt% of starch and a certain amount of polyvinyl alcohol solution into the granules, and ball-milling and granulating;
(3) preparing a greenware: BaTiO prepared in the step (2)3Adding the granules into a mold with the diameter of 20mmX20mm, and pressing the granules into a greenware by a film pressing machine under the pressure of 25 MPa;
(4) pore-forming and degumming: heating the greenware to 450 ℃, and keeping the temperature for 2 hours; continuously heating to 550 ℃ for degumming treatment;
(5) molding: treating for 1h at 1150 ℃ after degumming, and cooling to obtain BaTiO3A porous ceramic;
(6) and (3) polarization treatment: mixing BaTiO3Polarizing the porous ceramic plate for 30min under the voltage of 3KV/mm, and standing for 24h to obtain BaTiO3Piezoelectric porous ceramics;
(7)Pt-BaTiO3preparing porous ceramic with energy collection and catalysis functions: mixing BaTiO3The piezoelectric porous ceramic is placed in 1.0mol/LH2PtCl6Carrying out ultrasonic treatment in the solution to obtain the Pt monoatomic BaTiO3The piezoelectric energy collection is porous ceramic with catalytic function.
The hydrogen production reaction is as follows:
the method comprises the following steps: providing 100mL of NH at a concentration of 0.05mol/L3BH3Putting the solution into a reactor, adding the self-energized piezoelectric porous ceramic into the solution, covering a quartz glass plate, and sealing the reactor;
step two: connecting the hydrogen production system and the low-temperature constant-temperature tank in the first step, sealing, controlling the temperature of the low-temperature constant-temperature tank to be 1 ℃, then pumping the system to be vacuum, and controlling the temperature of the system to be 25 ℃ through the low-temperature constant-temperature tank after the system reaches a vacuum state;
step three: and (3) placing the reactor in a 28KHz ultrasonic cleaner, turning on the ultrasonic, adjusting the hydrogen production system to a system circulation state, performing an experiment, and detecting the hydrogen yield of each hour by a gas chromatograph every other hour.
Example 6
The Pt monoatomic BaTi prepared in example 1 to example 5 was usedO3The hydrogen prepared from the piezoelectric porous ceramics is dried and then placed in a hydrogen purity analyzer to detect the gases which do not contain carbon monoxide, hydrogen sulfide, phosphine, chloride ions and the like and poison the fuel cell, and the prepared hydrogen is high-purity hydrogen.
It should be understood that the above-mentioned embodiments are merely illustrative of the technical concepts and features of the present invention, which are intended to enable those skilled in the art to understand the contents of the present invention and implement the present invention, and therefore, the protection scope of the present invention is not limited thereby. All equivalent changes and modifications made according to the spirit of the present invention should be covered within the protection scope of the present invention.
Claims (9)
1. Pt-BaTiO with energy collection and catalysis functions3Porous ceramic, characterized in that it comprises BaTiO3The piezoelectric ceramic comprises a piezoelectric porous ceramic matrix and Pt monoatomic atoms uniformly dispersed on the surface and pore channels of the piezoelectric porous ceramic;
wherein the mass fraction of the Pt monoatomic atoms is 0.01 wt% -0.1 wt%;
the BaTiO3The aperture of the piezoelectric porous ceramic matrix is 0.01 mm-0.1 mm.
2. The Pt-BaTiO of claim 1 with energy harvesting catalysis3The preparation method of the porous ceramic comprises the following steps:
(1) preparation of BaTiO3And (3) particle: reacting barium salt and titanium salt with alkali to generate BaTiO3Particles;
(2) and (3) granulation: adding the BaTiO prepared in the step (1)3Respectively adding 0.5-8 wt% of starch and a certain amount of polyvinyl alcohol solution into the granules, and ball-milling and granulating;
(3) preparing a greenware: BaTiO prepared in the step (2)3Adding the granules into a mould with a certain size, and pressing into a greenware by a film pressing machine under the pressure of 10-30 MPa;
(4) pore-forming and degumming: heating the ceramic blank to 350-450 ℃, and keeping the temperature for 1-2 h; continuously heating for degumming treatment;
(5) molding: after degumming, the mixture is treated at the temperature of 900-1150 DEG CTidying for 0.5h to 2h, and cooling to obtain BaTiO3A porous ceramic;
(6) and (3) polarization treatment: mixing BaTiO3Polarizing the porous ceramic plate for 20-60min at the voltage of 3-5 KV/mm, and standing for 24h to obtain BaTiO3Piezoelectric porous ceramics;
(7) Pt-BaTiO with energy collection and catalysis functions3Preparing porous ceramics: mixing BaTiO3The piezoelectric porous ceramic is arranged in H2PtCl6Carrying out ultrasonic treatment in the solution to obtain the Pt-BaTiO with the energy collecting and catalyzing function3The porous ceramic of (1).
3. The Pt-BaTiO with energy-harvesting catalyst function of claim 23The method for producing a porous ceramic according to (1), wherein the barium salt is at least one selected from the group consisting of barium chloride, barium nitrate and barium oxide;
preferably, the titanium salt is selected from at least one of titanium sulfate and titanium chloride;
preferably, the base is selected from at least one of sodium hydroxide, potassium hydroxide and ammonia.
4. The Pt-BaTiO with energy-harvesting catalyst function of claim 23The method for preparing the porous ceramic is characterized in that the mass concentration of the polyvinyl alcohol (PVA) solution is 5.0 wt% -8.0 wt%.
5. The Pt-BaTiO with energy-harvesting catalyst function of claim 33The preparation method of the porous ceramic is characterized in that the degumming temperature is 500-600 ℃.
6. The Pt-BaTiO of claim 2 with energy harvesting catalytic function3The preparation method of the porous ceramic is characterized in that the ultrasonic treatment time is 30-80 min, and the ultrasonic treatment frequency is 20-60 KHz.
7. Catalytic work with energy harvesting as claimed in claim 1Pt-BaTiO capable of being used as catalyst3Or Pt-BaTiO prepared as described in any of claims 2 to 6 having an energy harvesting catalytic function3The porous ceramic is applied to self-powered hydrogen production.
8. Use according to claim 7, wherein the mechanical energy is from vibrational energy, sonic energy or ultrasonic energy.
9. Use according to claim 7, wherein the Pt-BaTiO with catalytic function for energy harvesting is used3The porous ceramic is applied to vehicle-mounted self-powered hydrogen production.
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