CN110575830A - platinum-containing catalyst and preparation method and application thereof - Google Patents

platinum-containing catalyst and preparation method and application thereof Download PDF

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CN110575830A
CN110575830A CN201910863252.XA CN201910863252A CN110575830A CN 110575830 A CN110575830 A CN 110575830A CN 201910863252 A CN201910863252 A CN 201910863252A CN 110575830 A CN110575830 A CN 110575830A
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catalyst
platinum
separated
mass
abundance
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肖松涛
欧阳应根
叶国安
王玲钰
刘协春
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China Institute of Atomic of Energy
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China Institute of Atomic of Energy
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Abstract

the invention belongs to the technical field of catalysts, and relates to a platinum-containing catalyst, and a preparation method and application thereof. The catalyst comprises a catalytic active substance, wherein the catalytic active substance comprises metal platinum or a compound thereof, the platinum element in the metal platinum or the compound thereof is composed of non-radioactive isotopes of which the composition and/or the abundance is changed from natural abundance, and the abundance of at least one non-radioactive isotope is changed from 1/20 to 20 percent on the basis of the natural abundance. The catalyst, the preparation method and the application thereof can ensure that the obtained platinum-containing catalyst has better catalytic performance.

Description

Platinum-containing catalyst and preparation method and application thereof
Technical Field
The invention belongs to the technical field of catalysts, and relates to a platinum-containing catalyst, and a preparation method and application thereof.
Background
Catalyst materials and catalytic technology are one of the fundamental and critical materials and technologies for the development of the chemical industry today. In modern industry, the production value produced by catalytic technology accounts for about 30% of the total value of national economy.
Noble metalThe Pt outer electron arrangement is 5d86s2And the second outer layer has 8 d electrons, and the track is not filled. And because the energy level contains unpaired electrons, Pt can show stronger ferromagnetism or paramagnetism in physical properties; in the chemical adsorption process, these d electrons of Pt can pair with p electrons or s electrons in the adsorbate, and chemical adsorption occurs to generate an intermediate product, thereby activating the adsorbed molecules.
In modern industry, platinum catalysts are mainly used in inorganic chemical industry, petroleum refining, organic chemical industry, C1 chemical industry, fine chemical industry, purification and treatment of automobile exhaust and industrial gas, and the fields of fuel cells, sensors and the like, so that the platinum catalysts have very important positions in the aspects of industrial catalysis, environmental protection and green energy technology and show wide application prospects.
However, pure Pt as a catalyst has 3 major disadvantages, namely low utilization, low poisoning resistance, and high price. In response to these disadvantages, much research worldwide has been devoted to the development of highly active platinum catalysts and the reduction of the amount of platinum catalyst used in order to improve the catalytic activity, selectivity, and life span of the Pt catalyst.
With respect to Pt catalysts, the main current research directions are:
1. Unitary Pt-based catalyst
The research direction of the unitary Pt-based catalyst focuses on finding a catalyst carrier with excellent performance and changing the size and surface state of Pt particles. For example, Zhu and the like adopt functionalized multi-wall carbon nanotubes dispersed in polyaniline as a carrier to synthesize a catalyst with good Pt/MWCNT/PAN dispersibility. Research results show that compared with a catalyst taking pure polyaniline as a carrier, the catalyst has higher catalytic activity. For example, Wu and the like are used for preparing a nano carbon material with a shell-core structure, carbon black particles are used as a core for loading, a graphite layer doped with carbon black is used as a shell, and the catalyst has high catalytic activity. For another example, Zhang and the like prepare the nanoflower with novel appearance through a template-free electrodeposition method, and the nanoflower has porous appearance and can provide larger active centers.
2. Binary Pt-based catalyst
The alloy type catalyst prepared by adding the second metal which is easy to adsorb oxygen-containing substances into the pure Pt catalyst can improve the poisoning resistance of the catalyst, thereby greatly improving the performance of the catalyst. The Pt-based binary catalysts which are researched more and have better catalytic effect at present comprise PtRu, PtPd, PtSn, PtAu, PtNi, PtCo and metal oxide (Pt + MO)xAnd wherein M ═ Ti, W, Zr, Ce, Ta), and the like.
3. Multi-element Pt-based catalyst
Researchers have attempted to improve Pt-based alloys by adding third and even fourth metals to increase their catalytic activity. For example, Park et al have studied the electronic and chemical effects of Pt/Ni, Pt/Ru/Ni nanocatalysts in the oxidation process of methanol. As another example, Jeon et al synthesized a PtCoCr three-way catalyst, and the experimental results showed that Pt30Co30Cr40The catalyst has good electro-oxidation property, stability and catalytic effect on methanol, and is an excellent methanol electro-oxidation catalyst.
In summary, although scientists have performed several works in the field of noble metal Pt catalysis, the different methods are superior and inferior. And the industrial application of these Pt catalytic materials still faces many challenges, such as large-scale controllable synthesis method, catalytic material stability, precise regulation of metal loading, catalyst poisoning resistance, how to better combine the advanced preparation method of metal materials with carbon loading materials, and the like. Therefore, new ideas for noble metal Pt catalysis are under way.
Disclosure of Invention
The primary object of the present invention is to provide a platinum-containing catalyst that can have better catalytic performance.
To achieve this object, in a basic embodiment, the present invention provides a platinum-containing catalyst comprising a catalytically active species comprising metallic platinum or a compound thereof, wherein the platinum element in the metallic platinum or the compound thereof is composed of a non-radioactive isotope whose composition and/or abundance is changed from natural, wherein the abundance (mass percentage content) of at least one non-radioactive isotope is changed by 1/20 or more and not less than 20% based on the natural abundance (natural abundance of platinum element isotope: Pt-190 is 0.01%, Pt-192 is 0.79%, Pt-194 is 32.9%, Pt-195 is 33.8%, Pt-196 is 25.3%, Pt-198 is 7.2%).
In a preferred embodiment, the present invention provides a platinum-containing catalyst wherein:
The catalytic active substance also comprises metallic ruthenium or a compound thereof, and the mass ratio of the metallic platinum or the compound thereof to the metallic ruthenium or the compound thereof is 1: 0.1-10;
The ruthenium element (natural abundance of ruthenium element isotope: 5.52% Ru-96%, 1.88% Ru-98%, 12.7% Ru-99%, 12.6% Ru-100%, 17% Ru-101%, 31.6% Ru-102%, 18.7% Ru-104) in the metal ruthenium or the compound thereof is composed of non-radioactive isotopes, and the composition and/or abundance of various isotopes are the same as or different from those of natural.
In a preferred embodiment, the present invention provides a platinum-containing catalyst wherein:
The catalytic active substance also comprises metallic copper or a compound thereof, and the mass ratio of the metallic platinum or the compound thereof to the metallic copper or the compound thereof is 1: 0.1-10;
The copper element (the natural abundance of the copper element isotope is 69.17 percent for Cu-63 and 30.83 percent for Cu-65) in the metal copper or the compound thereof consists of non-radioactive isotopes, and the composition and/or abundance of various isotopes are the same as or different from those of the natural isotopes.
In a preferred embodiment, the present invention provides a platinum-containing catalyst, wherein the catalyst further comprises a catalytic auxiliary substance, and the mass ratio of the catalytically active substance to the catalytic auxiliary substance is 1: 0.1-10.
In a more preferred embodiment, the present invention provides a platinum-containing catalyst, wherein the catalytic auxiliary material comprises a promoter selected from one or more of cobalt, gold, palladium, nickel, and rare earth elements.
In a more preferred embodiment, the present invention provides a platinum-containing catalyst, wherein the catalytic auxiliary material comprises a catalyst carrier selected from one or more of activated carbon, silicon carbide, alumina, graphene, silica and zeolite.
The second objective of the present invention is to provide a method for preparing the platinum-containing catalyst, so as to be able to better prepare the platinum-containing catalyst, and the prepared platinum-containing catalyst has better catalytic performance.
To achieve this object, in a basic embodiment, the present invention provides a method for preparing the platinum-containing catalyst described above, comprising the steps of:
(1) Preparation of catalytically active material: preparing the catalytic active substance or the compound thereof with changed isotope composition and/or abundance by using an isotope separation method, an isotope mixing method, a nuclear reaction method or an element artificial production method;
(2) Preparation of the catalyst: the catalysts are prepared using the respective catalytically active substances or compounds thereof.
Isotope separation methods can be mainly divided into chemical methods and physical methods, wherein the chemical methods include amalgam exchange methods, ion exchange chromatography, extraction methods and the like; physical methods include electromagnetic methods, molten salt electrolysis methods, electron transfer, molecular distillation, laser separation, and the like (see: Yangzhou, Zeng's title, stable isotope separation, atomic energy Press, first edition 1989, full book, especially page 23).
The isotope mixing method is to mix isotopes with different abundances to prepare isotopes with specified abundances, and mix the isotopes uniformly by a roller or the like.
The nuclear reaction method is a method of bombarding a nuclear nucleus with particles generated by a reactor or an accelerator, and mainly includes primary decay of (n, γ), (n, p), (n, d) (n,2n), (n, f), and target nuclides (see (U.S.) c.b. moore, eds. laser photochemical and isotope separation, atomic energy press, first edition 1988, full book, especially page 18) can be generated by combining the (n, p), (n, d), (n,2n) reaction and the secondary reaction (p, n), (p, d), (t, n), (t, 2 n).
The element artificial production method is to produce a new nuclide by nuclear fission or nuclear fusion (see (U.S.) Benedict (Benedict, M.) and the like, nuclear chemical engineering, atomic energy press, first edition 2011, full book, especially page 169).
a third object of the present invention is to provide the use of the platinum-containing catalyst described above to enable better catalytic performance.
To achieve this object, in a basic embodiment, the present invention provides the use of the above platinum-containing catalyst for catalyzing an electrocatalytic oxygen reduction reaction.
To achieve this, in a basic embodiment, the present invention provides the use of the platinum-containing catalyst described above for catalyzing the oxidation reaction of a battery.
To achieve this object, in a basic embodiment, the present invention provides the use of the platinum-containing catalyst described above for catalyzing an electrolytic water hydrogen evolution reaction.
the invention has the beneficial effect that the platinum-containing catalyst has better catalytic performance by utilizing the platinum-containing catalyst and the preparation method and the application thereof.
Detailed Description
The following examples further illustrate specific embodiments of the present invention.
Example 1: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-98. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-194 is 1.5%, the abundance ratio of Pt-195 is 98% and the abundance ratio of Pt-196 is 0.5% through ICP-MS detection.
Adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method (weighing salt of a catalytic active substance, dissolving the salt in deionized water, adding carrier conductive graphite, dipping for 1h, keeping the temperature at 40 ℃ for 2h, drying at 80 ℃ to obtain a catalyst precursor, adding a small amount of urea solution into the prepared catalyst precursor, carrying out hydrothermal treatment at 130 ℃ for 6h, then filtering, washing to be neutral, drying at 120 ℃ overnight, roasting at 550 ℃ for 4h to obtain the required catalyst, and the same applies to the hydrothermal method).
Example 2: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-190-20. And collecting the separated platinum at a discharge port, wherein the abundance ratio of Pt-190 is 20%, the abundance ratio of Pt-194 is 50% and the abundance ratio of Pt-198 is 30% through ICP-MS detection.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
Example 3: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-190-. The separated platinum is collected at a discharge port, and the abundance ratio of Pt-190 is 100 percent through ICP-MS detection.
Adding conductive graphite with the mass 4 times that of the separated platinum as a carbon source to prepare the Pt/C catalyst with the Pt mass fraction of 20%, wherein the preparation method comprises the following steps:
preparation of metal Pt into H2PtCl6Solution is prepared into 1mol/L H2PtCl6. Adding conductive graphite, stirring uniformly, adopting NaOH as a precipitator, adjusting the pH value to 7.5, obtaining a black precipitate through centrifugal washing, and calcining the black precipitate at 500 ℃ under the condition of hydrogen to obtain the catalyst.
example 4: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-192-100. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-192 is 100 percent through ICP-MS detection.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
Example 5: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-194-100. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-194 is 100 percent through ICP-MS detection.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
Example 6: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-100. The separated platinum was collected at the outlet and the abundance of Pt-195 was 100% by ICP-MS.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
Example 7: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-196-100. The separated platinum was collected at the outlet and the abundance of Pt-196 was 100% by ICP-MS.
adding conductive graphite with the mass 4 times that of the separated platinum as a carbon source to prepare the Pt/C catalyst with the Pt mass fraction of 20%, wherein the preparation method comprises the following steps:
Preparation of metal Pt into H2PtCl6Solution is prepared into 1mol/L H2PtCl6. Adding conductive graphite, stirring uniformly, adopting NaOH as a precipitator,Adjusting the pH value to 7.5, obtaining a black precipitate substance by centrifugal washing, and calcining the substance at 500 ℃ under the condition of hydrogen to obtain the catalyst.
Example 8: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-198-100. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-198 is 100 percent through ICP-MS detection.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
Example 9: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-192-20. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-192 is 20 percent, the abundance ratio of Pt-194 is 50 percent and the abundance ratio of Pt-196 is 30 percent through ICP-MS detection.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
example 10: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-194-20. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-194 is 20%, the abundance ratio of Pt-195 is 50% and the abundance ratio of Pt-196 is 30% through ICP-MS detection.
Adding conductive graphite with the mass 4 times that of the separated platinum as a carbon source to prepare the Pt/C catalyst with the Pt mass fraction of 20%, wherein the preparation method comprises the following steps:
Preparation of metal Pt into H2PtCl6Solution is prepared into 1mol/L H2PtCl6. Adding conductive graphite, stirring uniformly, adopting NaOH as a precipitator, adjusting the pH value to 7.5, obtaining a black precipitate through centrifugal washing, and calcining the black precipitate at 500 ℃ under the condition of hydrogen to obtain the catalyst.
Example 11: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-194-31. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-194 is 31 percent, the abundance ratio of Pt-192 is 19 percent and the abundance ratio of Pt-195 is 50 percent through ICP-MS detection.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
Example 12: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-194-35. And collecting the separated platinum at a discharge port, wherein the abundance ratio of Pt-194 is 35%, the abundance ratio of Pt-192 is 30% and the abundance ratio of Pt-196 is 35% through ICP-MS detection.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
Example 13: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-20. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-195 is 20 percent, the abundance ratio of Pt-192 is 20 percent and the abundance ratio of Pt-194 is 60 percent through ICP-MS detection.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
Example 14: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-31. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-195, Pt-192 and Pt-194 is 31%, 30% and 39% respectively through ICP-MS detection.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
Example 15: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-35.5. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-195 is 35.5%, the abundance ratio of Pt-192 is 20% and the abundance ratio of Pt-194 is 44.5% through ICP-MS detection.
Adding conductive graphite with the mass 4 times that of the separated platinum as a carbon source to prepare the Pt/C catalyst with the Pt mass fraction of 20%, wherein the preparation method comprises the following steps:
Preparation of metal Pt into H2PtCl6Solution is prepared into 1mol/L H2PtCl6. Adding conductive graphite, stirring uniformly, adopting NaOH as a precipitator, adjusting the pH value to 7.5, obtaining a black precipitate through centrifugal washing, and calcining the black precipitate at 500 ℃ under the condition of hydrogen to obtain the catalyst.
Example 16: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-196-20. And collecting the separated platinum at a discharge port, wherein the abundance ratio of Pt-196 is 20%, the abundance ratio of Pt-192 is 10%, the abundance ratio of Pt-194 is 20% and the abundance ratio of Pt-195 is 50% through ICP-MS detection.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
Example 17: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-196-23. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-196 is 23%, the abundance ratio of Pt-195 is 37% and the abundance ratio of Pt-198 is 40% through ICP-MS detection.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
Example 18: preparation examples
the method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-196-27.5. The separated platinum was collected at the outlet and found by ICP-MS to have an abundance of Pt-196 of 27.5%, an abundance of Pt-195 of 50% and an abundance of Pt-198 of 22.5%.
And adding conductive graphite with the mass being 4 times that of the separated platinum as a carbon source, and preparing the Pt/C catalyst with the mass fraction of Pt being 20% by a hydrothermal method.
Example 19: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-198-20. The separated platinum is collected at the discharge hole, and the abundance ratio of Pt-198, Pt-195 and Pt-196 is 20%, 50% and 30% respectively, which are detected by ICP-MS.
Adding conductive graphite with the mass 4 times that of the separated platinum as a carbon source to prepare the Pt/C catalyst with the Pt mass fraction of 20%, wherein the preparation method comprises the following steps:
Preparation of metal Pt into H2PtCl6solution is prepared into 1mol/L H2PtCl6. Adding conductive graphite, stirring uniformly, adopting NaOH as a precipitator, adjusting the pH value to 7.5, obtaining a black precipitate through centrifugal washing, and calcining the black precipitate at 500 ℃ under the condition of hydrogen to obtain the catalyst.
Example 20: comparative preparation example
Conductive graphite with the mass 4 times that of the natural metal platinum powder is added to serve as a carbon source, and the Pt/C catalyst with the mass fraction of Pt being 20% is prepared through a hydrothermal method.
Example 21: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-98. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-194 is 1.5%, the abundance ratio of Pt-195 is 98% and the abundance ratio of Pt-196 is 0.5% through ICP-MS detection.
Adding 0.1 mass time of natural metal ruthenium and 4.4 mass times of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/C catalyst with the mass fraction of Pt and Ru being 20% by a hydrothermal method.
example 22: comparative preparation example
Adding 0.1 mass time of natural metal ruthenium and 4.4 mass times of conductive graphite into natural metal platinum powder as carbon sources, and preparing the Pt/Ru/C catalyst with the mass fraction of Pt and Ru being 20% by a hydrothermal method.
Example 23: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-190-20. And collecting the separated platinum at a discharge port, wherein the abundance ratio of Pt-190 is 20%, the abundance ratio of Pt-194 is 50% and the abundance ratio of Pt-198 is 30% through ICP-MS detection.
adding 1 time mass of natural metal ruthenium and 8 times mass of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/C catalyst with the mass fraction of Pt and Ru being 20% by a hydrothermal method.
Example 24: comparative preparation example
Adding 1 time mass of natural metal ruthenium and 8 times mass of conductive graphite into natural metal platinum powder as carbon sources, and preparing the Pt/Ru/C catalyst with the mass fraction of Pt and Ru being 20% by a hydrothermal method.
example 25: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-190-. The separated platinum is collected at a discharge port, and the abundance ratio of Pt-190 is 100 percent through ICP-MS detection.
Adding 10 times of mass of natural metal ruthenium and 44 times of mass of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/C catalyst with the mass fraction of Pt and Ru being 20% by a hydrothermal method.
Example 26: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-192-100. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-192 is 100 percent through ICP-MS detection.
Adding 0.1 times of mass of natural metal copper and 4.4 times of mass of conductive graphite into the separated platinum as a carbon source to prepare a Pt/Cu/C catalyst with the mass fraction of Pt and Cu being 20%, wherein the preparation method comprises the following steps:
Preparation of metal Pt into H2PtCl6Solution is prepared into 1mol/L H2PtCl6(ii) a Preparation of metallic Cu into CuCl2Preparing solution into 1mol/L CuCl2. Adding conductive graphite, stirring uniformly, adopting NaOH as a precipitator, adjusting the pH value to 7.5, obtaining a black precipitate through centrifugal washing, and calcining the black precipitate at 500 ℃ under the condition of hydrogen to obtain the catalyst.
Example 27: comparative preparation example
Adding 0.1 mass time of natural metal copper and 4.4 mass times of conductive graphite into natural metal platinum powder as carbon sources, and preparing the Pt/Cu/C catalyst with the mass fractions of Pt and Cu being 20% by a hydrothermal method.
example 28: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-194-100. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-194 is 100 percent through ICP-MS detection.
Adding 1 time mass of natural metal copper and 8 times mass of conductive graphite into the separated platinum as a carbon source, and preparing the Pt/Cu/C catalyst with the mass fractions of Pt and Cu being 20% by a hydrothermal method.
Example 29: comparative preparation example
Adding 1 time of natural metal copper and 8 times of conductive graphite as carbon sources into natural metal platinum powder, and preparing the Pt/Cu/C catalyst with the mass fraction of Pt and Cu being 20% by a hydrothermal method.
Example 30: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-100. The separated platinum was collected at the outlet and the abundance of Pt-195 was 100% by ICP-MS.
Adding 10 times of mass of natural metal copper and 44 times of mass of conductive graphite into the separated platinum as a carbon source, and preparing the Pt/Cu/C catalyst with the mass fractions of Pt and Cu being 20% by a hydrothermal method.
Example 31: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-196-100. The separated platinum was collected at the outlet and the abundance of Pt-196 was 100% by ICP-MS.
The method is characterized in that natural metal ruthenium is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science of China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameters are Ru-102-100. The separated ruthenium is collected at a discharge port, and the abundance ratio of the Ru-102 is 100 percent through ICP-MS detection.
Adding conductive graphite with the mass 8 times that of the platinum into the separated platinum and ruthenium with the same mass as the separated platinum and ruthenium to be used as a carbon source to prepare the Pt/Ru/C catalyst with the mass fraction of the Pt and the Ru being 20%, wherein the specific preparation method comprises the following steps:
Preparation of metal Pt into H2PtCl6Solution is prepared into 1mol/L H2PtCl6(ii) a Preparation of metallic Ru into RuCl3Preparing a solution into 1mol/L RuCl3. Adding conductive graphite, stirring uniformly, adopting NaOH as a precipitator, adjusting the pH value to 7.5, obtaining a black precipitate through centrifugal washing, and calcining the black precipitate at 500 ℃ under the condition of hydrogen to obtain the catalyst.
Example 32: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-198-100. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-198 is 100 percent through ICP-MS detection.
The method is characterized in that natural metal copper is separated by using an isotope separation method and using a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Cu-63-100. And collecting the separated copper at a discharge port, and detecting by ICP-MS, wherein the abundance ratio of Cu-63 is 100%.
And adding conductive graphite with the mass 8 times that of the platinum into the separated platinum and copper with the same mass as the separated platinum and copper to serve as a carbon source, and preparing the Pt/Cu/C catalyst with the mass fractions of Pt and Cu being 20% through a hydrothermal method.
Example 33: preparation examples
the method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-192-20. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-192 is 20 percent, the abundance ratio of Pt-194 is 50 percent and the abundance ratio of Pt-196 is 30 percent through ICP-MS detection.
Adding 0.1 mass time of natural metal ruthenium, 0.1 mass time of natural metal copper and 4.8 mass times of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/Cu/C catalyst with the mass fractions of Pt, Ru and Cu being 20% by a hydrothermal method.
Example 34: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-194-20. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-194 is 20%, the abundance ratio of Pt-195 is 50% and the abundance ratio of Pt-196 is 30% through ICP-MS detection.
Adding 0.1 mass time of natural metal ruthenium, 1 mass time of natural metal copper and 8.4 mass times of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/Cu/C catalyst with the mass fractions of Pt, Ru and Cu being 20% by a hydrothermal method.
Example 35: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-194-31. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-194 is 31 percent, the abundance ratio of Pt-192 is 19 percent and the abundance ratio of Pt-195 is 50 percent through ICP-MS detection.
And adding 0.1 mass time of natural metal ruthenium, 10 mass times of natural metal copper and 44.4 mass times of conductive graphite into the separated platinum as a carbon source, and preparing the Pt/Ru/Cu/C catalyst with the mass fractions of Pt, Ru and Cu being 20% by a hydrothermal method.
Example 36: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-194-35. And collecting the separated platinum at a discharge port, wherein the abundance ratio of Pt-194 is 35%, the abundance ratio of Pt-192 is 30% and the abundance ratio of Pt-196 is 35% through ICP-MS detection.
Adding 1 time mass of natural metal ruthenium, 1 time mass of natural metal copper and 12 times mass of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/Cu/C catalyst with the mass fractions of Pt, Ru and Cu being 20% by a hydrothermal method.
Example 37: comparative preparation example
Adding 1 time of natural metal ruthenium, 1 time of natural metal copper and 12 times of conductive graphite as carbon sources into natural metal platinum powder, and preparing the Pt/Cu/C catalyst with the mass fractions of Pt and Cu being 20% by a hydrothermal method.
Example 38: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-20. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-195 is 20 percent, the abundance ratio of Pt-192 is 20 percent and the abundance ratio of Pt-194 is 60 percent through ICP-MS detection.
Adding 1 time mass of natural metal ruthenium, 10 times mass of natural metal copper and 48 times mass of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/Cu/C catalyst with the mass fractions of Pt, Ru and Cu being 20% by a hydrothermal method.
Example 39: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-31. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-195, Pt-192 and Pt-194 is 31%, 30% and 39% respectively through ICP-MS detection.
Adding 10 times of mass of natural metal ruthenium, 1 time of mass of natural metal copper and 48 times of mass of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/Cu/C catalyst with the mass fractions of Pt, Ru and Cu being 20% by a hydrothermal method.
Example 40: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-35.5. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-195 is 35.5%, the abundance ratio of Pt-192 is 20% and the abundance ratio of Pt-194 is 44.5% through ICP-MS detection.
Adding 10 times of mass of natural metal ruthenium, 0.1 times of mass of natural metal copper and 44.4 times of mass of conductive graphite into the separated platinum to serve as a carbon source, and preparing the Pt/Ru/Cu/C catalyst with the mass fractions of Pt, Ru and Cu being 20%, wherein the specific preparation method is as follows:
Preparation of metal Pt into H2PtCl6Solution is prepared into 1mol/L H2PtCl6(ii) a Preparation of metallic Ru into RuCl3Preparing a solution into 1mol/L RuCl3(ii) a Preparation of metallic Cu into CuCl2Preparing solution into 1mol/L CuCl2. Adding conductive graphite, stirring, adjusting pH to 7.5 with NaOH as precipitant, centrifuging to obtain black precipitate, and washing the black precipitate at 500 deg.C under hydrogenCalcining to obtain the catalyst.
Example 41: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-196-20. And collecting the separated platinum at a discharge port, wherein the abundance ratio of Pt-196 is 20%, the abundance ratio of Pt-192 is 10%, the abundance ratio of Pt-194 is 20% and the abundance ratio of Pt-195 is 50% through ICP-MS detection.
The method is characterized in that natural metal copper is separated by using an isotope separation method and using a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Cu-63-100. And collecting the separated copper at a discharge port, and detecting by ICP-MS, wherein the abundance ratio of Cu-63 is 100%.
Adding 1 time of mass of separated copper, 1 time of mass of natural metal ruthenium and 12 times of mass of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/Cu/C catalyst with the mass fraction of Pt/Ru/Cu being 20% by a hydrothermal method.
example 42: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-196-23. The separated platinum is collected at the discharge port, and the abundance ratio of Pt-196 is 23%, the abundance ratio of Pt-195 is 37% and the abundance ratio of Pt-198 is 40% through ICP-MS detection.
The method is characterized in that natural metal ruthenium is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science of China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameters are Ru-102-100. The separated ruthenium is collected at a discharge port, and the abundance ratio of the Ru-102 is 100 percent through ICP-MS detection.
Adding 1 time of mass of the separated ruthenium, 1 time of mass of natural metal copper and 12 times of mass of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/Cu/C catalyst with the mass fraction of Pt/Ru/Cu being 20% by a hydrothermal method.
Example 43: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-196-27.5. The separated platinum was collected at the outlet and found by ICP-MS to have an abundance of Pt-196 of 27.5%, an abundance of Pt-195 of 50% and an abundance of Pt-198 of 22.5%.
The method is characterized in that natural metal ruthenium is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science of China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameters are Ru-102-100. The separated ruthenium is collected at a discharge port, and the abundance ratio of the Ru-102 is 100 percent through ICP-MS detection.
The method is characterized in that natural metal copper is separated by using an isotope separation method and using a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Cu-63-100. And collecting the separated copper at a discharge port, and detecting by ICP-MS, wherein the abundance ratio of Cu-63 is 100%.
Adding 1 time of mass of separated ruthenium, 1 time of mass of separated copper and 12 times of mass of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/Cu/C catalyst with the mass fraction of Pt/Ru/Cu being 20% by a hydrothermal method.
example 44: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-198-20. The separated platinum is collected at the discharge hole, and the abundance ratio of Pt-198, Pt-195 and Pt-196 is 20%, 50% and 30% respectively, which are detected by ICP-MS.
The method is characterized in that natural metal ruthenium is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science of China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameters are Ru-102-100. The separated ruthenium is collected at a discharge port, and the abundance ratio of the Ru-102 is 100 percent through ICP-MS detection.
The method is characterized in that natural metal copper is separated by using an isotope separation method and using a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Cu-63-100. And collecting the separated copper at a discharge port, and detecting by ICP-MS, wherein the abundance ratio of Cu-63 is 100%.
Adding 1 time of mass of separated ruthenium, 0.1 time of mass of separated copper and 8.4 times of mass of conductive graphite into the separated platinum to serve as a carbon source, and preparing the Pt/Ru/Cu/C catalyst with the mass fraction of Pt/Ru/Cu being 20%, wherein the specific preparation method comprises the following steps:
Preparation of metal Pt into H2PtCl6solution is prepared into 1mol/L H2PtCl6(ii) a Preparation of metallic Ru into RuCl3Preparing a solution into 1mol/L RuCl3(ii) a Preparation of metallic Cu into CuCl2Preparing solution into 1mol/L CuCl2. Adding conductive graphite, stirring uniformly, adopting NaOH as a precipitator, adjusting the pH value to 7.5, obtaining a black precipitate through centrifugal washing, and calcining the black precipitate under the condition of 500 ℃ hydrogen to obtain the catalyst.
Example 45: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-50. And collecting the separated platinum at a discharge port, wherein the abundance ratio of Pt-194 is 35%, the abundance ratio of Pt-195 is 50% and the abundance ratio of Pt-196 is 15% through ICP-MS detection.
The method is characterized in that natural metal ruthenium is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science of China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameters are Ru-102-100. The separated ruthenium is collected at a discharge port, and the abundance ratio of the Ru-102 is 100 percent through ICP-MS detection.
The method is characterized in that natural metal copper is separated by using an isotope separation method and using a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Cu-63-100. And collecting the separated copper at a discharge port, and detecting by ICP-MS, wherein the abundance ratio of Cu-63 is 100%.
adding 0.1 mass time of separated ruthenium, 10 mass times of separated copper and 44.4 mass times of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/Cu/C catalyst with the mass fraction of Pt/Ru/Cu being 20% by a hydrothermal method.
Example 46: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-196-95. And collecting the separated platinum at a discharge port, wherein the abundance ratio of Pt-194 is 1%, the abundance ratio of Pt-195 is 4% and the abundance ratio of Pt-196 is 95% through ICP-MS detection.
The method is characterized in that natural metal ruthenium is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science of China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameters are Ru-102-100. The separated ruthenium is collected at a discharge port, and the abundance ratio of the Ru-102 is 100 percent through ICP-MS detection.
The method is characterized in that natural metal copper is separated by using an isotope separation method and using a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Cu-63-100. And collecting the separated copper at a discharge port, and detecting by ICP-MS, wherein the abundance ratio of Cu-63 is 100%.
Adding 10 times of mass of separated ruthenium, 0.1 time of mass of separated copper and 44.4 times of mass of conductive graphite into the separated platinum as carbon sources, and preparing the Pt/Ru/Cu/C catalyst with the mass fraction of Pt/Ru/Cu being 20% by a hydrothermal method.
Example 47: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-98.5. And collecting the separated platinum at a discharge port, wherein the abundance ratio of Pt-194 is 1%, the abundance ratio of Pt-195 is 98.5% and the abundance ratio of Pt-196 is 0.5% through ICP-MS detection.
The method is characterized in that natural metal ruthenium is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science of China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameters are Ru-102-100. The separated ruthenium is collected at a discharge port, and the abundance ratio of the Ru-102 is 100 percent through ICP-MS detection.
The method is characterized in that natural metal copper is separated by using an isotope separation method and using a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Cu-63-100. And collecting the separated copper at a discharge port, and detecting by ICP-MS, wherein the abundance ratio of Cu-63 is 100%.
Adding 0.1 times of mass of separated ruthenium, 1 time of mass of separated copper and 8.4 times of mass of conductive graphite into the separated platinum as a carbon source to prepare the Pt/Ru/Cu/C catalyst with the mass fraction of Pt/Ru/Cu being 20%, wherein the preparation method comprises the following steps:
Preparation of metal Pt into H2PtCl6Solution is prepared into 1mol/L H2PtCl6(ii) a Preparation of metallic Ru into RuCl3Preparing a solution into 1mol/L RuCl3(ii) a Preparation of metallic Cu into CuCl2Preparing solution into 1mol/L CuCl2. Adding conductive graphite, stirring uniformly, adopting NaOH as a precipitator, adjusting the pH value to 7.5, obtaining a black precipitate through centrifugal washing, and calcining the black precipitate at 500 ℃ under the condition of hydrogen to obtain the catalyst.
Example 48: preparation examples
The method is characterized in that natural metal platinum powder is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Pt-195-98.5. And collecting the separated platinum at a discharge port, wherein the abundance ratio of Pt-194 is 1%, the abundance ratio of Pt-195 is 98.5% and the abundance ratio of Pt-196 is 0.5% through ICP-MS detection.
The method is characterized in that natural metal ruthenium is separated by a CAE-1 type magnetic separation device of nuclear institute of atomic energy science of China, based on the principle of an isotope separation method, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameters are Ru-102-100. The separated ruthenium is collected at a discharge port, and the abundance ratio of the Ru-102 is 100 percent through ICP-MS detection.
The method is characterized in that natural metal copper is separated by using an isotope separation method and using a CAE-1 type magnetic separation device of nuclear institute of atomic energy science, and the specific operation conditions are as follows: the vaporization temperature is 2500 ℃, the magnetic field voltage is 1000V, and the magnetic separation parameter is Cu-63-100. And collecting the separated copper at a discharge port, and detecting by ICP-MS, wherein the abundance ratio of Cu-63 is 100%.
Adding 10 times of mass of separated ruthenium, 1 time of mass of separated copper and 48 times of mass of conductive graphite into the separated platinum as a carbon source to prepare the Pt/Ru/Cu/C catalyst with the mass fraction of Pt/Ru/Cu being 20%, wherein the preparation method comprises the following steps:
Preparation of metal Pt into H2PtCl6Solution is prepared into 1mol/L H2PtCl6(ii) a Preparation of metallic Ru into RuCl3Preparing a solution into 1mol/L RuCl3(ii) a Preparation of metallic Cu into CuCl2Preparing solution into 1mol/L CuCl2. Adding conductive graphite, stirring uniformly, adopting NaOH as a precipitator, adjusting the pH value to 7.5, obtaining a black precipitate through centrifugal washing, and calcining the black precipitate at 500 ℃ under the condition of hydrogen to obtain the catalyst.
Example 49: examples of catalytic reactions
The catalysts prepared in the previous examples are respectively used as oxygen reduction catalysts and respectively loaded on a glassy carbon electrode to prepare a working electrode (cathode) at 0.1M HClO4Using rotating discs in the electrolyteThe electrode was tested for electrocatalytic oxygen reduction reaction. The loading amount of the catalytic active substance on the glassy carbon electrode is 7.65 mu g cm-2The rotation speed is 1600 rpm. Oxygen is continuously introduced in the test process, and the scanning rate of the linear scanning voltammetry is 5mV-1. The test results are shown in table 1 below.
TABLE 1 electrocatalytic oxygen reduction test results
Example 50: examples of catalytic reactions
The catalysts prepared in the previous examples were respectively loaded on a glassy carbon electrode to prepare a working electrode (anode) at 0.5M H2SO4+1M CH3The electrocatalytic methanol oxidation test was performed in the OH electrolyte, respectively, and the test results are shown in table 2 below.
TABLE 2 results of electrocatalytic methanol oxidation test
Example 51: examples of catalytic reactions
The catalysts prepared in the previous examples are respectively loaded on a glassy carbon electrode to prepare a working electrode (cathode): 2mg of catalyst was dissolved in 1ml of ethanol and 20. mu.L of Nafion was addedBinder, in an amount of 0.02mg/cm2the load measuring amount of the catalyst is a certain volume of solution which is dripped on a glassy carbon electrode, and after natural airing, hydrogen evolution catalysis test is carried out; wherein the glassy carbon electrode is a working electrode, the graphite carbon rod is a counter electrode, the saturated calomel electrode is a reference electrode, and the temperature is 0.5M H at 25 DEG C2SO4Carrying out electrolytic water oxygen evolution reaction test in the electrolyte: ar was passed through 0.5M H before testing using CHI640 electrochemical workstation and a rotating disk electrode to reduce mass transfer effects2SO4Removing air in the electrolyte; firstly, scanning 100 circles in a voltage interval of-0.2 to-0.8V at a scanning speed of 50mv/s to stabilize the activity of the catalyst, and then acquiring an lsv curve in a voltage interval of-0.2 to-0.8V at a scanning speed of 2mv/s to obtain corresponding I-ESCEThe curve, IR correction, compensates the voltage loss caused by the liquid resistance and the external circuit resistance, and is converted into I-ERHEand obtaining corresponding overpotentials under different current densities according to the converted lsv curve and carrying out Tafel slope fitting.
The test results are shown in table 3 below.
TABLE 3 test results of hydrogen evolution catalytic reaction
It will be apparent to those skilled in the art that various changes and modifications may be made in the present invention without departing from the spirit and scope of the invention. Thus, if such modifications and variations of the present invention fall within the scope of the claims of the present invention and their equivalents, the present invention is intended to include such modifications and variations. The foregoing examples or embodiments are merely illustrative of the present invention, which may be embodied in other specific forms or in other specific forms without departing from the spirit or essential characteristics thereof. The described embodiments are, therefore, to be considered in all respects as illustrative and not restrictive. The scope of the invention should be indicated by the appended claims, and any changes that are equivalent to the intent and scope of the claims should be construed to be included therein.

Claims (10)

1. A platinum-containing catalyst characterized by: the catalyst comprises a catalytic active substance, wherein the catalytic active substance comprises metal platinum or a compound thereof, the platinum element in the metal platinum or the compound thereof is composed of non-radioactive isotopes of which the composition and/or the abundance is changed from natural abundance, and the abundance of at least one non-radioactive isotope is changed from 1/20 to 20 percent on the basis of the natural abundance.
2. The catalyst of claim 1, wherein:
The catalytic active substance also comprises metallic ruthenium or a compound thereof, and the mass ratio of the metallic platinum or the compound thereof to the metallic ruthenium or the compound thereof is 1: 0.1-10;
The ruthenium element in the metal ruthenium or the ruthenium element compound consists of non-radioactive isotopes, and the composition and/or abundance of various isotopes are the same as or different from those of the natural ruthenium.
3. the catalyst of claim 1, wherein:
The catalytic active substance also comprises metallic copper or a compound thereof, and the mass ratio of the metallic platinum or the compound thereof to the metallic copper or the compound thereof is 1: 0.1-10;
The copper element in the metallic copper or the compound thereof consists of nonradioactive isotopes, and the composition and/or abundance of various isotopes are the same as or different from those of the natural isotopes.
4. The catalyst of claim 1, wherein: the catalyst also comprises a catalytic auxiliary substance, and the mass ratio of the catalytic active substance to the catalytic auxiliary substance is 1: 0.1-10.
5. The catalyst of claim 4, wherein: the catalytic auxiliary substance comprises a cocatalyst which is selected from one or more of cobalt, gold, palladium, nickel and rare earth elements.
6. The catalyst of claim 4, wherein: the catalytic auxiliary substance comprises a catalyst carrier which is selected from one or more of active carbon, silicon carbide, aluminum oxide, graphene, silicon dioxide and zeolite.
7. Process for the preparation of a catalyst according to one of claims 1 to 6, comprising the following steps:
(1) Preparation of catalytically active material: preparing the catalytic active substance or the compound thereof with changed isotope composition and/or abundance by using an isotope separation method, an isotope mixing method, a nuclear reaction method or an element artificial production method;
(2) Preparation of the catalyst: the catalysts are prepared using the respective catalytically active substances or compounds thereof.
8. Use of a catalyst according to any one of claims 1 to 6 for catalysing an electrocatalytic oxygen reduction reaction.
9. Use of a catalyst according to any one of claims 1 to 6 for catalysing the oxidation reaction in a battery.
10. Use of a catalyst according to any one of claims 1 to 6 for catalysing the reaction of electrohydrolytically evolving hydrogen.
CN201910863252.XA 2019-09-12 2019-09-12 platinum-containing catalyst and preparation method and application thereof Pending CN110575830A (en)

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115142071A (en) * 2022-07-21 2022-10-04 中国人民解放军空军勤务学院 Flower-shaped catalyst, preparation method and application thereof
CN115676891A (en) * 2022-11-04 2023-02-03 华北电力大学 UO in electrochemical separation fixed radioactive wastewater 22+ And ReO 4- Method (2)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115142071A (en) * 2022-07-21 2022-10-04 中国人民解放军空军勤务学院 Flower-shaped catalyst, preparation method and application thereof
CN115676891A (en) * 2022-11-04 2023-02-03 华北电力大学 UO in electrochemical separation fixed radioactive wastewater 22+ And ReO 4- Method (2)
CN115676891B (en) * 2022-11-04 2024-03-12 华北电力大学 Electrochemical separation and fixation of UO in radioactive wastewater 22+ And ReO 4- Is a method of (2)

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