Carbon-based magnesium-containing composite material and synthetic method therefor

Patent metadata

Field	Value
Publication number	US-10537878-B2
Application number	US-201615546821-A
Country	US
Kind code	B2
Filing date	Jan 27, 2016
Priority date	Jan 27, 2015
Publication date	Jan 21, 2020
Grant date	Jan 21, 2020

Abstract

A carbonaceous material, based on the total weight of the carbonaceous material, contains 1-99 wt % of a carbon element, 0.2-60 wt % of a magnesium element, 0.5-60 wt % of an oxygen element and 0.1-40 wt % of a chlorine element. The process for preparing the carbonaceous material include (1) Mixing a solid carbon source, a precursor and water to produce a mixture; wherein said precursor contains a magnesium source and a chlorine source; (2) Drying the resulting mixture obtained in Step (1) to produce a dried mixture; and (3) Calcining the dried mixture obtained in Step (2). The carbonaceous material can be used in catalytic oxidation of hydrocarbons.

First claim

The invention claimed is:

1. A carbonaceous material, comprising: based on a total weight of the carbonaceous material, 1-99 wt % of carbon, 0.2-60 wt % of magnesium, 0.5-60 wt % of oxygen, and 0.1-40 wt % of chlorine, wherein the carbonaceous material has an x-ray photoelectron (XPS) spectrum in which the binding energy characteristic peak of the 2p electron of magnesium is located at >50.3 eV.

2. The carbonaceous material according to claim 1 , comprising 10-90 wt % of carbon, 2-50 wt % of magnesium, 2-50 wt % of oxygen, and 1-30 wt % of chlorine.

3. The carbonaceous material according to claim 2 , comprising 20-80 wt % of carbon, 5-30 wt % of magnesium, 5-40 wt % of oxygen, and 2-20 wt % of chlorine.

4. The carbonaceous material according to claim 3 , comprising 25-41 wt % of carbon, 20-30 wt % of magnesium, 19-40 wt % of oxygen, and 4-20 wt % of chlorine.

5. The carbonaceous material according to claim 1 , wherein, in the XPS spectrum of the carbonaceous material, a ratio of the content of chlorine as determined with a peak(s) in the range of 197.7-198.1 eV to the content of chlorine as determined with a peak(s) in the range of 199.7-200.1 eV is 0.5-2; a ratio of the content of oxygen as determined with a peak(s) in the range of 533.1-533.5 eV to a content of the oxygen element as determined with a peak(s) in the range of 531.8-532.2 eV is 0.2-5.

6. The carbonaceous material according to claim 1 , wherein, as determined by an X-ray micro zone elemental analysis, a coefficient of variation for the content of magnesium obtained using XPS is 20% or lower.

7. The carbonaceous material according to claim 1 , wherein said carbonaceous material has a peroxy group content of ≤2×10 −6 mol/g.

8. The carbonaceous material according to claim 1 , wherein said carbonaceous material has a peroxy group content of ≤1×10 −6 mol/g.

9. The carbonaceous material according to claim 1 , wherein said carbonaceous material has a peroxy group content of ≤0.8×10 −6 mol/g.

10. The carbonaceous material according to claim 1 , wherein said carbonaceous material comprises at least one structural form selected from the group consisting of carbon nanotube, graphene, fullerene, nano-carbon particle, active carbon, thin-layer graphite, nano-carbon fiber, and nano-adamas.

11. A process for preparing a carbonaceous material of claim 1 , wherein said process includes the following steps:
(1) Mixing a solid carbon source, a precursor and water to produce a mixture; wherein the precursor contains a magnesium source and a chlorine source, said magnesium source and said chlorine source are present in a dissolved state in the resulting mixture; the carbon element in said solid carbon source, and the magnesium element and the chlorine element in said precursor are present in a weight ratio of 1:(0.002-2):(0.01-20);
(2) Drying the resulting mixture obtained in Step (1) to produce a dried mixture;
(3) Calcining the dried mixture obtained in Step (2).

12. The process of claim 11 , wherein the carbon element in said solid carbon source, and the magnesium element and the chlorine element in said precursor are present in a weight ratio of 1:(0.01-1):(0.1-10).

13. The process according to claim 11 , wherein the weight ratio of water to the solid carbon source is (0.1-200):1.

14. The process of claim 11 , wherein the calcination temperature is 200-500° C., and the calcination time is 0.5-48 hours.

15. The process of claim 14 , wherein the calcination temperature is 300-450° C.

16. The process of claim 11 , wherein the calcination is conducted in an oxygen-containing gas; and based on the total volume of the oxygen-containing gas, the oxygen-containing gas has an oxygen content of 2-25 vol %.

17. The process of claim 11 , wherein said solid carbon source comprises at least one of carbon nanotube, graphene, fullerene, nano-carbon particle, thin-layer graphite, active carbon, nano-carbon fiber and nano-adamas; said magnesium source includes at least one of magnesium nitrate, magnesium nitrite, magnesium oxalate, magnesium oxide, magnesium hydroxide, magnesium sulfate, magnesium sulfite, magnesium tartrate, magnesium sulfide, magnesium cyanide, magnesium thiosulfate, magnesium rhodanate, magnesium iodide, magnesium chloride, magnesium bromide, magnesium acetate and magnesium carbonate; said chlorine source includes at least one of chlorine gas, magnesium chloride, hydrogen chloride, hypochlorous acid, magnesium hypochlorite, chloric acid, magnesium chlorite, perchloric acid and magnesium perchlorite.

18. The process of claim 11 , wherein said precursor contains magnesium chloride and/or magnesium nitrate.

19. The carbonaceous material prepared with the process according to claim 11 .

20. A method for catalytic oxidation of hydrocarbons, comprising: oxidizing a hydrocarbon stream in the presence of the carbonaceous material of claim 1 .

21. The method according to claim 20 , wherein said hydrocarbon has a carbon atom number of 2-15, said hydrocarbon comprises at least one of an alkane, an alkene and an aromatic hydrocarbon containing alkyl group(s); said alkyl contains at least two carbon atoms.

22. The method according to claim 20 , wherein said hydrocarbon comprises at least one of butane, 1-butene, ethylbenzene, propane, ethane and pentane.

Assignees

• China Petroleum & Chem Corp
• Sinopec Res Inst Petroleum

Inventors

• Rong Junfeng
• Shi Chunfeng
• Xie Jingxin
• Yu Peng
• Zong Mingsheng
• Lin Weiguo

Classifications

• B01J21/18 Primary

  Carbon · CPC title

• B01J37/02

  Impregnation, coating or precipitation ({B01J37/0009 and B01J37/0018 take precedence } ; protection by coating B01J33/00) · CPC title

• C07C11/04

  Ethene · CPC title

• Y02P20/52

  using catalysts, e.g. selective catalysts · CPC title

• C07C5/324

  with metals · CPC title