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Controllable carbon-supported metal monatomic catalyst prepared based on cyclodextrin supramolecular chemistry and preparation method and application method of controllable carbon-supported metal monatomic catalyst

A technology of supramolecular chemistry and metal atoms, applied in the field of single-atom catalysis, can solve the problems of catalyst degradation system, unclear active components, low turnover frequency, etc., achieve cheap raw materials, simple and easy-to-operate preparation methods, and no metal loss Effect

Active Publication Date: 2021-06-01
PETROCHINA CO LTD +1
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0004] The present invention provides a controllable preparation of carbon-supported metal single-atom catalyst based on cyclodextrin supramolecular chemistry and its preparation method and application method, in order to solve the current problem of heavy oil In the slurry bed hydrogenation process, the oil-soluble molecular molybdenum catalyst has problems such as unclear active components, few active sites, low turnover frequency, rapid catalyst degradation and coke formation in the system, which limit industrial application.

Method used

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  • Controllable carbon-supported metal monatomic catalyst prepared based on cyclodextrin supramolecular chemistry and preparation method and application method of controllable carbon-supported metal monatomic catalyst
  • Controllable carbon-supported metal monatomic catalyst prepared based on cyclodextrin supramolecular chemistry and preparation method and application method of controllable carbon-supported metal monatomic catalyst
  • Controllable carbon-supported metal monatomic catalyst prepared based on cyclodextrin supramolecular chemistry and preparation method and application method of controllable carbon-supported metal monatomic catalyst

Examples

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Effect test

Embodiment 1

[0035] A carbon-supported metal single-atom catalyst based on cyclodextrin supramolecular chemistry controllable preparation, including heteroatom-doped cyclodextrin as a support and metal single atoms contained therein.

[0036] Among them, the metal atoms are Mo, Co, Ni, Fe, Pt, Ir, Au, Cu, Ru, Rh, Pd; the heteroatoms are one or more of O, S, N, and the carbon-supported metal single atom The load is between 1% and 20%.

[0037] The preparation method of carbon-supported metal single-atom catalyst in the present embodiment comprises the following steps:

[0038] (1) mixing metal salt compound, nitrogen source and deionized water to obtain a mixed aqueous solution;

[0039] (2) adding an appropriate amount of absolute ethanol to the mixed aqueous solution in step (1), and then adding cyclodextrin to obtain a mixed solution;

[0040] (3) mixing the sulfur source with deionized water, and adding it to the mixed solution configured in step (2) to obtain a reaction solution, and...

Embodiment 2

[0047] This example is based on the preparation of Example 1 based on cyclodextrin supramolecular chemical controllable preparation of carbon-supported metal single-atom catalysts for comparative experiments, as follows:

[0048] Weigh 20 mg of ammonium molybdate tetrahydrate and add it to the prepared 40 mL of deionized water, then add 690 mg of hydroxylamine chloride, ultrasonicate for five minutes until completely dissolved, then measure and add 40 mL of absolute ethanol, 130 mg of ring Dextrin, sonicated for ten minutes until completely dissolved, to obtain A solution.

[0049] Weigh 0.5 g of thiocyanuric acid and dissolve it in 40 mL of deionized water, and sonicate for ten minutes until it is completely dissolved to obtain solution B.

[0050] Add solution B to solution A dropwise under stirring, and stir for 12 h.

[0051] The mixed solution was placed in a dry oven at 70 °C for 24 h to form a solid precursor.

[0052] The precursor was taken out and calcined at 650°C...

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Abstract

The invention relates to the technical field of monatomic catalysis, in particular to a carbon-supported metal monatomic catalyst prepared based on cyclodextrin supramolecular chemistry in a controllable mode and a preparation method and application thereof.The carbon-supported metal monatomic catalyst comprises heteroatom-doped carbon serving as a carrier and metal monatomic anchored by the heteroatom-doped carbon, and the metal monatomic comprises Mo, Co, Ni, Fe, Pt, Ir, Au, Cu, Ru, Rh and Pd. According to the preparation method, cyclodextrin supermolecules are taken as a carbon source, a metal precursor is included in cavities of the cyclodextrin supermolecules by utilizing confinement and self-assembly effects of the cyclodextrin supermolecules, meanwhile, the cyclodextrin supermolecules and guest molecules containing heteroatoms are subjected to self-assembly, and the carbon-supported metal monatomic catalyst is prepared through high-temperature pyrolysis. The supramolecular self-assembly confinement pyrolysis method adopted by the invention is simple in preparation method, free of metal loss, free of pollution emission, green in synthesis and high in metal monatomic loading capacity.

Description

technical field [0001] The invention relates to the field of single-atom catalysis, mainly relates to the application of single-atom catalysts in the field of hydrogenation, in particular to a carbon-supported metal single-atom catalyst based on cyclodextrin supramolecular chemistry controllable preparation and its preparation method and application method. Background technique [0002] As the available crude oil becomes heavier and various residual oils are recycled, the lightening of heavy oil becomes more and more important. Slurry bed hydrogenation, as an emerging technology for lightening heavy oil, is very suitable for low-quality heavy oil with high sulfur, high metals, and high carbon residue. The bottlenecks that limit its industrial application are mainly activity, selectivity, and low price. The catalyst controllable preparation synthesis. The efficient utilization of precious metals has always been a difficult problem for major research teams. Studies have show...

Claims

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Application Information

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IPC IPC(8): B01J23/28B01J23/42B01J23/44B01J23/46B01J23/52B01J23/72B01J23/745B01J23/75B01J23/755B01J27/02B01J27/24B01J35/00B01J37/08C10G47/12C10G47/14
CPCB01J37/0009B01J23/28B01J23/75B01J23/745B01J23/755B01J23/42B01J23/468B01J23/52B01J23/72B01J23/462B01J23/464B01J23/44B01J27/24B01J27/02C10G47/14C10G47/12B01J35/391
Inventor 潘原孙广洵柳云骐刘士欢秦东琳汪云霞赵祎琳孙琪琪刘宾柴永明刘晨光
Owner PETROCHINA CO LTD
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