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Metal monoatomic catalyst loaded by flexible carbon-based carrier and preparation method and application of catalyst

A carbon-based carrier, metal-loaded technology, applied in the field of electrocatalysis, can solve the problems of limiting large-scale practical application, increasing electrode contact resistance, low mechanical strength, etc., and achieving uniform dispersion of single atoms, reduced contact resistance, and high mechanical strength. Effect

Active Publication Date: 2019-08-09
ZHONGBEI UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

At present, the preparation method of graphene-supported transition metal single-atom catalyst and its electrocatalytic reduction of CO have been reported in top journals at home and abroad. 2 However, most of the currently reported graphene-supported transition metal single-atom catalysts are powder materials, and they all need to be coated with a binder on a conductive substrate (such as carbon paper or glassy carbon electrode) to be used as an electrode for catalytic reactions. Not only It increases the electrode contact resistance, and there are problems such as difficult recycling and low mechanical strength, which limit its large-scale practical application

Method used

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  • Metal monoatomic catalyst loaded by flexible carbon-based carrier and preparation method and application of catalyst
  • Metal monoatomic catalyst loaded by flexible carbon-based carrier and preparation method and application of catalyst
  • Metal monoatomic catalyst loaded by flexible carbon-based carrier and preparation method and application of catalyst

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Experimental program
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Effect test

Embodiment 1

[0054] (1) Weigh 50 mg of graphene, 3 g of melamine and 0.5 g of porphyrin iron, and disperse them in 100 ml of anhydrous methanol, sonicate for 30 min, then stir at room temperature for 12 h to obtain a uniform mixture Slurry; (2) Choose flexible graphene film as the substrate, uniformly load the prepared homogeneous slurry on both surfaces of the graphene film by scraping method, and the loading thickness on both sides is 35 mm, and then place it Dry naturally at room temperature; (3) Place the dried composite membrane in step (2) in a high-purity argon atmosphere, and perform slow multi-step high-temperature pyrolysis treatment, and raise the temperature to 180 °C at a rate of 2 °C / min Hold for 2 hours, then raise the temperature to 360°C at a rate of 2°C / min and hold for 2 hours, then raise the temperature to 800°C at a rate of 2°C / min and hold for 2 hours, and finally cool down to room temperature at a rate of 2°C / min, the whole gas flow rate 10 ml / min; (4) Soak the heat-...

Embodiment 2

[0057] (1) Weigh 40 mg of graphene, 5 g of urea and 0.45 g of porphyrin zinc, and disperse the three in 300 ml of ultrapure water, ultrasonicate for 50 min, and then stir at room temperature for 12 h to obtain a uniform mixture Slurry; (2) Choose flexible carbon fiber cloth as the base, soak the carbon fiber cloth into the prepared homogeneous slurry by the soaking method, soak for 30 min, take it out and vacuum dry it in an oven at 70 °C for 2 h, and then place it Wet again, repeated 5 times, and dried in vacuum; (3) Place the dried composite film in step (2) in a high-purity argon atmosphere, and perform slow multi-step high-temperature pyrolysis treatment at a rate of 3 ℃ / min The temperature was raised to 200°C for 1.5 h, then raised to 380°C at a rate of 3°C / min and held for 2 h, then raised to 850°C at a rate of 3°C / min and held for 2 h, and finally lowered to At room temperature, the whole gas flow rate is 9 ml / min; (4) Soak the heat-treated carbon fiber composite cloth ...

Embodiment 3

[0059] (1) Weigh 45 mg of graphene, 4.5 g of dicyandiamide and 0.6 g of copper phthalocyanine, and disperse the three in 400 ml of anhydrous methanol, ultrasonicate for 60 min, and then stir at room temperature for 15 h to obtain a uniform (2) Choose flexible bamboo fiber cloth as the substrate, and load the prepared homogeneous slurry on the bamboo fiber cloth by spin coating method, the spin coating thickness is 30 mm, and the spin coating speed is 500 rpm, and then set Vacuum-dried in an oven at 90 °C for 10 h, repeated 3 times, and then vacuum-dried; (3) The composite film dried in step (2) was placed in a high-purity nitrogen atmosphere, and it was subjected to slow multi-step high-temperature pyrolysis treatment, The temperature was raised to 150°C at a rate of 5°C / min and kept for 1.5 h, then raised to 350°C at a rate of 5°C / min and held for 1.5 h, then raised to 780°C at a rate of 5°C / min and held for 2 h, and finally heated at 5°C / min down to room temperature, the wh...

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Abstract

The invention discloses a metal monoatomic catalyst loaded by a flexible carbon-based carrier and a preparation method and application of the catalyst, and belongs to the technical field of electrocatalysis. The catalyst is formed by coordinating and anchoring metal monoatoms and heteroatoms on graphene and loading the graphene on the flexible carbon-based carrier. The catalyst is prepared from, by weight, 0.001-4.0% of the metal monoatoms, 6-34.999% of the graphene, 50-80% of the carbon-based carrier and 5-20% of the heteroatoms. The preparation method of the metal monoatomic catalyst loadedby the flexible carbon-based carrier is simple, the content of the metal monoatoms is high, the metal monoatoms are dispersed uniformly and anchored on the carrier through coordination with the heteroatoms, and the physicochemical structure is stable. The catalyst is applied to electrocatalytic reduction of CO2 and has excellent CO selectivity, high CO Faraday efficiency and good recycling stability.

Description

technical field [0001] The invention relates to a metal single-atom catalyst supported by a flexible carbon-based carrier, a preparation method and application thereof, and belongs to the technical field of electrocatalysis. Background technique [0002] Since the Industrial Revolution, due to the massive consumption of coal and oil, atmospheric CO 2 content continued to increase, CO 2 The concentration has increased from about 280 ppm in the early 19th century to the current 385 ppm, and it is estimated that by 2100 CO 2 The concentration will reach nearly 600 ppm. CO 2 Increased levels lead to higher average global temperatures, which can lead to desertification and species extinction. Therefore, the search for efficient technology will CO 2 conversion into valuable fuels and chemicals, not only CO 2 Resource utilization can also reduce dependence on traditional fossil resources. Among them, the electrocatalytic reduction of CO 2 The technology uses electric energy...

Claims

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Application Information

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IPC IPC(8): B01J23/72B01J23/745B01J23/75B01J23/755B01J23/80C25B1/00C25B11/06
CPCB01J23/745B01J23/72B01J23/75B01J23/755B01J23/80C25B1/00C25B11/04
Inventor 张会念王俊中
Owner ZHONGBEI UNIV
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