CN111644168A - Method for preparing atomic-scale catalyst by slowly raising temperature to greatly improve yield of hydrogen peroxide - Google Patents

Method for preparing atomic-scale catalyst by slowly raising temperature to greatly improve yield of hydrogen peroxide Download PDF

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CN111644168A
CN111644168A CN202010313678.0A CN202010313678A CN111644168A CN 111644168 A CN111644168 A CN 111644168A CN 202010313678 A CN202010313678 A CN 202010313678A CN 111644168 A CN111644168 A CN 111644168A
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hydrogen peroxide
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黄凯
雷鸣
张茹
樊雨婷
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Beijing University of Posts and Telecommunications
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    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/74—Iron group metals
    • B01J23/75—Cobalt
    • 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
    • B01J23/06—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of zinc, cadmium or mercury
    • 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
    • B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J23/32—Manganese, technetium or rhenium
    • B01J23/34—Manganese
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/72—Copper
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/74—Iron group metals
    • B01J23/745—Iron
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/74—Iron group metals
    • B01J23/755—Nickel
    • B—PERFORMING OPERATIONS; TRANSPORTING
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Abstract

The invention relates to a method for preparing an atomic-scale catalyst by slowly raising the temperature so as to greatly improve the yield of hydrogen peroxide, and belongs to the field of material science, engineering technology and chemistry. The raw materials of the catalyst prepared by the invention are phthalocyanine metal and carbon nano materials, and the related metals comprise non-noble metal elements such as Fe, Co, Ni, Mn, Cu, Zn and the like. Firstly, preparing a mixed solution A containing phthalocyanine metal and a precursor carbon fluoride nanotube in a certain load proportion, carrying out ultrasonic treatment and stirring at normal temperature to enable the mixed solution A to fully react and be uniformly loaded, removing a dispersing solvent after the loading is finished, putting a prepared intermediate product B into a tube furnace, and heating for several hours under the condition of inert gas to obtain a product C. The method has the advantages of simple operation, high efficiency, wide application range and the like. Compared with the traditional method for preparing the hydrogen peroxide, the method has the advantages of easy operation, high yield, safety, reliability and the like.

Description

Method for preparing atomic-scale catalyst by slowly raising temperature to greatly improve yield of hydrogen peroxide
Technical Field
The invention relates to a method for preparing an atomic-scale catalyst by slowly raising the temperature so as to greatly improve the yield of hydrogen peroxide, and belongs to the field of material science, engineering technology and chemistry.
Background
Hydrogen peroxide is not only a versatile and environmentally friendly chemical oxidant widely used in water treatment, pulp bleaching and chemical synthesis, but also a potential energy storage substance. Today, the large demand for hydrogen peroxide makes this chemical one of the world's important products. However, the industrial production of hydrogen peroxide was mainly based on the Riedl-Pfleideerpro (Ridel-Perdermoprol) process developed by the last 70 years, involving the sequential hydrogenation and oxidation of anthraquinones. The inherent complexity and high energy consumption of this process has prompted researchers to explore alternative processes for hydrogen peroxide production. Against this background, the development of a process for the preparation of O in alkaline medium2Partial reduction to H2O2Would be an attractive strategy, however, we are still lacking an electrocatalyst that shows high activity and selectivity, is practical and cost-effective in the production of hydrogen peroxide. Considering that the temperature is taken as an important parameter influencing the kinetics and thermodynamics of a chemical reaction, the method adopts a widely-applied catalyst preparation method and a slow heating method, controls the temperature to be increased under a gas environment, changes the bonding mode among substance elements, activates the catalytic sites of metals, and enables metal atoms to be combined with NFC to form efficient active centers at a proper thermal activation temperature to obtain the catalyst with strong ORR performance. The catalyst is in two-electron and four-electron2In the reduction way, the catalyst has stronger HOO adsorption capacity, achieves higher catalytic activity of hydrogen peroxide, and greatly improves the yield of hydrogen peroxide in electrochemical catalysis.
Disclosure of Invention
1. Objects of the invention
The invention aims to obtain a method for greatly improving the yield of hydrogen peroxide. The ORR performance of the metal catalyst and the extremely high hydrogen peroxide selectivity can be improved by a slow heating method.
2. The invention of the technology
The key points of the invention are as follows:
(1) the method comprises the steps of preparing a reactant solution A with the mass-volume concentration of 2-4mg/ml by using phthalocyanine metal, an inorganic material and a solvent, wherein metal salt elements are Fe, Co, Ni, Mn, Cu and Zn, the inorganic material is a fluorinated carbon nanotube, and the solvent is absolute ethyl alcohol.
(2) And (3) carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. After the reactant is completely dried, the obtained reactant is put in a vacuum tube furnace for calcination, nitrogen or argon is generally used as protective gas, the annealing temperature is 500-800 ℃, the annealing time is 9-14h, the heat preservation time is 1h, the heating rate is 1 ℃/min
The catalyst prepared by slowly raising the temperature improves the yield of hydrogen peroxide, and has the advantages that: the method has wide application range, can synthesize various metal catalysts such as Fe, Co, Ni, Mn, Cu, Zn and the like, has stable chemical properties, easily obtained raw materials and simple synthesis process, and can be used for large-scale production.
Drawings
FIG. 1 is a scanning transmission electron microscope image of nanotubes loaded with cobalt phthalocyanine according to the method of the present invention. FIG. 2 is a graph of hydrogen peroxide production versus electron transfer number for cobalt doped catalysts;
Detailed Description
The following describes embodiments of the method of the invention:
example 1
Preparation of 3% -800 ℃ -Co-NFC catalyst
Firstly, fully mixing cobalt phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the cobalt phthalocyanine to a precursor is 3%, preparing a mixed solution A of 2mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 2
Preparation of 3% -800 ℃ -Fe-NFC catalyst
Firstly, fully mixing iron phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the iron phthalocyanine to the precursor is 3%, preparing a mixed solution A of 2mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 3
Preparation of 3% -800 ℃ -Cu-NFC catalyst
Firstly, copper phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol are fully mixed, the loading ratio of the copper phthalocyanine to a precursor is 3%, a mixed solution A of 2mg/ml is prepared, the solution is subjected to ultrasonic treatment until no particles exist, stirring is carried out for 12 hours, suction filtration is carried out, and a reactant is obtained on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 4
Preparation of 3% -800 ℃ -Ni-NFC catalyst
Firstly, fully mixing nickel phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the nickel phthalocyanine to a precursor is 3%, preparing a mixed solution A of 2mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 5
Preparation of 3% -800 ℃ -Zn-NFC catalyst
Firstly, fully mixing zinc phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the zinc phthalocyanine to a precursor is 3%, preparing a mixed solution A of 2mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 6
Preparation of 3% -800-Mn-NFC catalyst
Firstly, fully mixing manganese phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the manganese phthalocyanine to a precursor is 3%, preparing a mixed solution A of 2mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 7
Preparation of 5% -800 ℃ -Co-NFC catalyst
Firstly, fully mixing cobalt phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the cobalt phthalocyanine to a precursor is 5%, preparing a mixed solution A of 3mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 8
Preparation of 5% -800 ℃ -Fe-NFC catalyst
Firstly, fully mixing iron phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the iron phthalocyanine to the precursor is 5%, preparing a mixed solution A of 3mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 9
Preparation of 5% -800 ℃ -Cu-NFC catalyst
Firstly, copper phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol are fully mixed, the loading ratio of the copper phthalocyanine to the precursor is 5%, a mixed solution A of 3mg/ml is prepared, the solution is subjected to ultrasonic treatment until no particles exist, stirring is carried out for 12 hours, suction filtration is carried out, and a reactant is obtained on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 10
Preparation of 5% -800 ℃ -Zn-NFC catalyst
Firstly, fully mixing zinc phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the zinc phthalocyanine to a precursor is 5%, preparing a mixed solution A of 3mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 11
Preparation of 5% -800 ℃ -Ni-NFC catalyst
Firstly, fully mixing nickel phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the nickel phthalocyanine to a precursor is 5%, preparing a mixed solution A of 3mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 12
Preparation of 5% -800-Mn-NFC catalyst
Firstly, fully mixing manganese phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading capacity of the manganese phthalocyanine and a carrier is 5%, preparing a mixed solution A of 3mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 13
Preparation of 3% -500 ℃ -Co-NFC catalyst
Firstly, fully mixing cobalt phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the cobalt phthalocyanine to a precursor is 3%, preparing a mixed solution A of 2mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 14
Preparation of 3% -500 ℃ -Fe-NFC catalyst
Firstly, fully mixing iron phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the iron phthalocyanine to the precursor is 3%, preparing a mixed solution A of 2mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 15
Preparation of 3% -500 ℃ -Cu-NFC catalyst
Firstly, copper phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol are fully mixed, the loading ratio of the copper phthalocyanine to a precursor is 3%, a mixed solution A of 2mg/ml is prepared, the solution is subjected to ultrasonic treatment until no particles exist, stirring is carried out for 12 hours, suction filtration is carried out, and a reactant is obtained on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 16
Preparation of 3% -500 ℃ -Zn-NFC catalyst
Firstly, fully mixing zinc phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the zinc phthalocyanine to a precursor is 3%, preparing a mixed solution A of 2mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 17
Preparation of 3% -500-Ni-NFC catalyst
Firstly, fully mixing nickel phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the nickel phthalocyanine to a precursor is 3%, preparing a mixed solution A of 2mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.
Example 18
Preparation of 3% -500-Mn-NFC catalyst
Firstly, fully mixing manganese phthalocyanine, carbon fluoride nanotubes and absolute ethyl alcohol, wherein the loading ratio of the manganese phthalocyanine to a precursor is 3%, preparing a mixed solution A of 2mg/ml, carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper. And after the reactants are completely dried, putting the obtained reactants into a vacuum tube furnace for calcination, generally using nitrogen or argon as protective gas, annealing at 800 ℃, keeping the temperature for 1h, heating at the rate of 1 ℃/min, and cooling to room temperature after heating is finished to obtain the final product.

Claims (1)

1. A method for preparing an atomic-scale catalyst by slowly raising the temperature so as to greatly improve the yield of hydrogen peroxide is characterized by comprising the following steps:
(1) preparing a reactant solution A of 2-4mg/ml by using phthalocyanine metal, a carbon nano material and a solvent, wherein the phthalocyanine metal elements are Fe, Co, Ni, Mn, Cu and Zn, the carbon nano material is a fluorinated carbon nano tube, and the solvent is absolute ethyl alcohol.
(2) And (3) carrying out ultrasonic treatment on the solution until no particles exist, stirring for 12 hours, carrying out suction filtration, and obtaining a reactant on qualitative filter paper.
(3) After the reactants are completely dried, the obtained reactants are put in a vacuum tube furnace for annealing, nitrogen or argon is generally used as protective gas, the annealing temperature is 500-800 ℃, the annealing time is 9-14h, the heat preservation time is 1h, the heating rate is 1 ℃/min, and the reactants are naturally cooled to the room temperature after the heating is finished.
(4) Taking out the reactant, and the obtained catalyst can be applied to O2The reduction reaction of (2) improves the yield of the hydrogen peroxide.
CN202010313678.0A 2020-04-20 2020-04-20 Method for preparing atomic-scale catalyst by slowly raising temperature to greatly improve yield of hydrogen peroxide Pending CN111644168A (en)

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CN116024601A (en) * 2022-12-28 2023-04-28 大连理工大学 Carbon nano tube-based porous hollow fiber electrode for electrocatalytic reduction reaction and application
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Publication number Priority date Publication date Assignee Title
CN112619683A (en) * 2021-01-12 2021-04-09 南开大学 g-C co-modified by iron phthalocyanine and tungsten oxide3N4Catalyst and preparation method thereof
CN116024601A (en) * 2022-12-28 2023-04-28 大连理工大学 Carbon nano tube-based porous hollow fiber electrode for electrocatalytic reduction reaction and application
CN116237077A (en) * 2023-03-20 2023-06-09 周口师范学院 Method for synthesizing metal single-atom catalyst by using metal phthalocyanine compound
CN116237077B (en) * 2023-03-20 2023-10-17 周口师范学院 Method for synthesizing metal single-atom catalyst by using metal phthalocyanine compound

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Application publication date: 20200911