Preparation method of mesoporous hollow nitrogen-doped carbon-coated copper nano catalyst

Abstract

The invention belongs to the field of preparation of carbon-based composites, and particularly relates to a preparation method of a mesoporous hollow nitrogen-doped carbon-coated copper nano catalyst. The preparation method is characterized in that polypyrrole is adopted as a carbon source and a nitrogen source, copper sulfate is adopted as an active component precursor, and PS microspheres are adopted as a template; after multilayer sequential wrapping, the materials are subjected to high-temperature carbonization under the condition that a proper surfactant is adopted; and after activation, the mesoporous nitrogen-doped carbon-coated copper catalyst of which the appearance and size can be controlled is prepared. The prepared catalyst presents relatively high catalytic activity and relatively good stability during DMC reaction of methyl alcohol preparation and has a remarkable effect on preventing agglomeration and peeling of active components and improving reaction catalytic activity, experimental data is accurate and detailed, the cost is low, the raw materials are easy to obtain, a product is black powder, the diameter of powder particles is smaller than 400 nm, the purity of the product reaches 98.9%, the DMC space time yield in reaction can reach 1251 mg / g.h, and selectivity reaches 99.99%.

Description

technical field

[0001] The invention belongs to the field of carbon-based composite material preparation, in particular to a preparation method of a mesoporous hollow nitrogen-doped carbon-coated copper nano-catalyst, which can be used to catalyze the oxidative carbonylation of methanol to prepare dimethyl carbonate. Background technique

[0002] Dimethyl carbonate (DMC) is a downstream product of methanol and has a wide range of uses. Compared with various preparation methods, methanol oxidative carbonylation method has become a hot research topic in recent years because of its low production cost, high selectivity and low corrosion to equipment.

[0003] In the catalyst research for the oxidative carbonylation of methanol, we proposed a composite material of hollow carbon spheres coated with copper nanoparticles. specific microenvironment.

[0004] The hollow carbon sphere-coated copper nanocatalyst has high stability, and the copper nanoparticles are not prone to large-...

Examples

Embodiment Construction

[0019] The chemical materials used in the present invention are: deionized water, ammonia water, copper sulfate, cetyltrimethylammonium bromide (CTAB), polyvinylpyrrolidone (PVP), pyrrole, styrene, azobisisobutyronitrile (AIBN), potassium persulfate, hydrazine hydrate, high-purity nitrogen, and high-purity hydrogen, the preparation amounts are as follows: in grams, milliliters, centimeters 3 unit of measure

[0020] Deionized water: H 2 O Liquid 3000 ml±50 ml

[0021] Ammonia:NH 3 •H 2 O Liquid 6 ml±0.1 ml

[0022] Pyrrole: C 4 H 5 N Liquid 3 ml±0.1 ml

[0023] Styrene:C 8 H 8 Liquid 9 ml±0.1 ml

[0024] Hydrazine hydrate: H 6 N 2 O liquid 280 µl±0.1 µl

[0025] Azobisisobutyronitrile:C 8 H 12 N 4 Solid 1 g ± 0.001 g

[0026] Potassium Persulfate: K 2 S 2 O 8 Solid 1 g ± 0.001 g

[0027] Copper sulfate:CuSO 4 • 5H 2 O solid 2 g ± 0.001 g

[0028] Cetyltrimethylammonium bromide: C1 9 H 42 BrN solid 1 g ± 0.001 g

[0029] Polyvinylpyrrolidone: (C 6 H ...

technical field

[0001] The invention belongs to the field of carbon-based composite material preparation, in particular to a preparation method of a mesoporous hollow nitrogen-doped carbon-coated copper nano-catalyst, which can be used to catalyze the oxidative carbonylation of methanol to prepare dimethyl carbonate. Background technique

[0002] Dimethyl carbonate (DMC) is a downstream product of methanol and has a wide range of uses. Compared with various preparation methods, methanol oxidative carbonylation method has become a hot research topic in recent years because of its low production cost, high selectivity and low corrosion to equipment.

[0003] In the catalyst research for the oxidative carbonylation of methanol, we proposed a composite material of hollow carbon spheres coated with copper nanoparticles. specific microenvironment.

[0004] The hollow carbon sphere-coated copper nanocatalyst has high stability, and the copper nanoparticles are not prone to large-...

Examples

Embodiment Construction

[0019] The chemical materials used in the present invention are: deionized water, ammonia water, copper sulfate, cetyltrimethylammonium bromide (CTAB), polyvinylpyrrolidone (PVP), pyrrole, styrene, azobisisobutyronitrile (AIBN), potassium persulfate, hydrazine hydrate, high-purity nitrogen, and high-purity hydrogen, the preparation amounts are as follows: in grams, milliliters, centimeters 3 unit of measure

[0020] Deionized water: H 2 O Liquid 3000 ml±50 ml

[0021] Ammonia:NH 3 •H 2 O Liquid 6 ml±0.1 ml

[0022] Pyrrole: C 4 H 5 N Liquid 3 ml±0.1 ml

[0023] Styrene:C 8 H 8 Liquid 9 ml±0.1 ml

[0024] Hydrazine hydrate: H 6 N 2 O liquid 280 µl±0.1 µl

[0025] Azobisisobutyronitrile:C 8 H 12 N 4 Solid 1 g ± 0.001 g

[0026] Potassium Persulfate: K 2 S 2 O 8 Solid 1 g ± 0.001 g

[0027] Copper sulfate:CuSO 4 • 5H 2 O solid 2 g ± 0.001 g

[0028] Cetyltrimethylammonium bromide: C1 9 H 42 BrN solid 1 g ± 0.001 g

[0029] Polyvinylpyrrolidone: (C 6 H ...

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