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A kind of nitrogen-doped graphene copper-based bimetallic single-atom catalyst and preparation method and application thereof

A nitrogen-doped graphene and copper-based bimetallic technology, which is applied in chemical instruments and methods, preparation of organic compounds, physical/chemical process catalysts, etc., can solve problems such as multiple reaction steps, complex process flow, and development constraints. To achieve the effect of improving the amount of anchoring, high catalytic performance, fast mass and energy transfer

Active Publication Date: 2022-07-01
CHANGZHOU UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

At present, the industrial production method of phenol is mainly the cumene method, but the process is complicated, the reaction steps are many and its development is restricted by the parallel product acetone

Method used

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  • A kind of nitrogen-doped graphene copper-based bimetallic single-atom catalyst and preparation method and application thereof
  • A kind of nitrogen-doped graphene copper-based bimetallic single-atom catalyst and preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0035] (1) ultrasonically exfoliating graphite oxide to obtain graphene oxide (GO), mixing graphite oxide with water and dispersing uniformly to obtain a graphene oxide dispersion liquid, wherein the graphene oxide dispersion liquid concentration is 4 mg / mL;

[0036] (2) Add dicyandiamide (DCD) into (1), the mass ratio of DCD to pure GO is 3:1, the soluble salt of transition metal Cr is 0.1% of the total mass of DCD and GO, stir at room temperature for 10 h, and then freeze The Cr / DCD / GO precursor was obtained by drying.

[0037] (3) The precursor obtained in (2) was wrapped with copper mesh and placed in a quartz boat, and in a N2 atmosphere, at a heating rate of 5°C / min, treated at 600°C for 2h, at 800°C for 1h, cooled to room temperature, get black powder;

[0038] (4) The black powder obtained in (3) was added with 0.5M H 2 SO 4 The solution was completely immersed in the material, stirred at a constant temperature of 80°C for 10 hours, filtered and washed until neutral...

Embodiment 2

[0042] (1) ultrasonically exfoliating graphite oxide to obtain graphene oxide (GO), mixing graphite oxide with water and dispersing uniformly to obtain a graphene oxide dispersion liquid, wherein the graphene oxide dispersion liquid concentration is 4 mg / mL;

[0043] (2) Add dicyandiamide (DCD) into (1), the mass ratio of DCD to pure GO is 6:1, the soluble salt of transition metal Cr is 0.3% of the total mass of DCD and GO, stir at room temperature for 10 h, and then freeze The Cr / DCD / GO precursor was obtained by drying.

[0044] (3) The precursor obtained in (2) was wrapped with copper mesh and placed in a quartz boat, and in a N2 atmosphere, at a heating rate of 5°C / min, treated at 600°C for 2h, at 800°C for 1h, cooled to room temperature, get black powder;

[0045] (4) Add 0.5M H2SO4 solution to the black powder obtained in (3) until the material is completely submerged, stir at a constant temperature of 80°C for 10 hours, filter and wash to neutrality, and dry the solid i...

Embodiment 3

[0048] (1) ultrasonically exfoliating graphite oxide to obtain graphene oxide (GO), mixing graphite oxide with water and dispersing uniformly to obtain a graphene oxide dispersion liquid, wherein the graphene oxide dispersion liquid concentration is 4 mg / mL;

[0049] (2) Add dicyandiamide (DCD) into (1), the mass ratio of DCD to pure GO is 9:1, the soluble salt of transition metal Cr is 0.5% of the total mass of DCD and GO, stir at room temperature for 10 h, and then freeze The Cr / DCD / GO precursor was obtained by drying.

[0050] (3) The precursor obtained in (2) was wrapped with copper mesh and placed in a quartz boat, and in a N2 atmosphere, at a heating rate of 5°C / min, treated at 600°C for 2h, at 800°C for 1h, cooled to room temperature, get black powder;

[0051] (4) Add 0.5M H to the black powder obtained in (3) 2 SO 4 The solution was completely immersed in the material, stirred at a constant temperature of 80°C for 10 hours, filtered and washed until neutral, and th...

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Abstract

The invention discloses a nitrogen-doped graphene-copper-based bimetal single-atom catalyst, a preparation method and application thereof. The catalyst is composed of nitrogen-doped graphene-supported single-atom copper and transition metals, and the metal copper supports in the catalyst. is 0.5-6.0%, and the loading amount of transition metal M is 0.1-3.0%; wherein, the transition metal M includes chromium, iron, cobalt, nickel, manganese, vanadium and molybdenum. Nitrogen-doped graphene with a large specific surface area serves as a carrier, which is beneficial to the dispersion and immobilization of single-atom catalysts, and it also has a porous structure that enables fast mass and energy transfer, and its rich N atoms serve as anchoring centers , which is conducive to anchoring and dispersing single-atom Cu / M centers. During high-temperature treatment, a large number of N atoms will form coordination with metal Cu / M, thereby increasing the anchoring amount of single-atom Cu / M. Species are strongly anchored and confined to the derived nitrogen-doped graphene by N atoms, and no dissolution problem occurs.

Description

technical field [0001] The invention belongs to the technical field of heterogeneous catalysts, and in particular relates to a nitrogen-doped graphene copper-based bimetallic single-atom catalyst and a preparation method and application thereof. Background technique [0002] Phenol is an important organic chemical raw material, widely used in dyes, polymers, plastics, medicines, pesticides and other fields. The industrial production method of phenol is mainly the cumene method at present, but this technological process is complicated, and there are many reaction steps and its development is restricted by the parallel product acetone. [0003] In recent years, from the aspects of improving atom economy, energy saving and environmental protection, people have gradually shifted their attention to the preparation of phenol by directly catalyzing the hydroxylation of benzene. The process is simple, the reaction steps are short, and the pollution is small. An environmentally frie...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J27/24C07C37/60C07C39/04
CPCB01J27/24C07C37/60C07C39/04Y02P20/52
Inventor 陈海群何光裕赵宜涛陈群李乐朱俊武付永胜
Owner CHANGZHOU UNIV
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