Carbon-coated nickel-aluminum nanocomposite, preparation method therefor and application thereof

Patent metadata

Field	Value
Publication number	US-12467622-B2
Application number	US-202017755112-A
Country	US
Kind code	B2
Filing date	Oct 20, 2020
Priority date	Oct 21, 2019
Publication date	Nov 11, 2025
Grant date	Nov 11, 2025

Abstract

A nanocomposite has a core-shell structure with an outer shell and an inner core. The outer shell is a graphitized carbon film, and the inner core contains nickel oxide and alumina, with a nickel oxide content of 59%-80%, an alumina content of 19%-40%, and a carbon content of not more than 1%, based on the total weight of the nanocomposite. The process for catalytic combustion of volatile organic compounds may utilize the nanocomposite as a catalyst.

First claim

The invention claimed is:

1 . A carbon-coated nickel-aluminum nanocomposite, comprising a core-shell structure with an outer shell and an inner core, wherein the outer shell is a graphitized carbon film, wherein the inner core consists substantially of nickel oxide and alumina, wherein the carbon-coated nickel-aluminum nanocomposite has a nickel oxide content of 59%-80%, an alumina content of 19%-40%, and a carbon content of not more than 1%, and an elemental nickel content in an amount of not more than 1%, based on a total weight of the carbon-coated nickel-aluminum nanocomposite, and wherein the graphitized carbon film is substantially composed of graphitized carbon.

2 . The carbon-coated nickel-aluminum nanocomposite according to claim 1 , wherein the nickel oxide content is 69%-79%, the alumina content is 20%-30%, and the carbon content is 0.3%-1%.

3 . The carbon-coated nickel-aluminum nanocomposite according to claim 1 , a weight ratio of a carbon element content determined by X-ray photoelectron spectroscopy to a carbon element content determined by elemental analysis is not less than 10.

4 . The carbon-coated nickel-aluminum nanocomposite according to claim 1 , having a Raman spectrum with a ratio of an intensity of a G peak located near 1580 cm −1 to an intensity of a D peak located near 1320 cm −1 of greater than 2.

5 . The carbon-coated nickel-aluminum nanocomposite according to claim 1 , wherein the core-shell structure has a particle size of 2 nm to 100 nm.

6 . The carbon-coated nickel-aluminum nanocomposite according to claim 1 , wherein the inner core further comprises an alkali metal oxide in an amount of not more than 5% by weight, relative to the total weight of the carbon-coated nickel-aluminum nanocomposite.

7 . The carbon-coated nickel-aluminum nanocomposite according to claim 1 , wherein the nanocomposite comprises elemental nickel in an amount of not more than 0.1% based on the total weight of the carbon-coated nickel-aluminum nanocomposite.

8 . A process for preparing the carbon-coated nickel-aluminum nanocomposite according to claim 1 , comprising the steps of:
preparing a nickel-aluminum precursor; carrying out a heating treatment on the nickel-aluminum precursor, and carrying out a vapor deposition by using an alkane as a carbon source gas; and carrying out oxygen treatment on a product obtained after the vapor deposition, to provide the carbon-coated nickel-aluminum nanocomposite.

9 . The process according to claim 8 , wherein the oxygen treatment comprises introducing a standard gas into the product obtained after the vapor deposition and heating, wherein the standard gas contains 10-40 vol % of oxygen and a balance gas.

10 . The process according to claim 8 , wherein the oxygen treatment is carried at a temperature of 200° C. to 500° C. for 0.5 h to 10 h.

11 . The process according to claim 8 , wherein the nickel-aluminum precursor is prepared by coprecipitation and/or hydrothermal crystallization.

12 . The process according to claim 8 , wherein the nickel-aluminum precursor is prepared using a method comprising:
simultaneously dropwise adding an alkaline solution and an aqueous solution containing trivalent aluminum salt and divalent nickel salt into water for precipitation treatment, so that the trivalent aluminum salt and the divalent nickel salt generate a coprecipitate; and aging the coprecipitate.

13 . The process according to claim 12 , wherein the trivalent aluminum salt comprises aluminum nitrate and/or aluminum chloride, the divalent nickel salt comprises nickel nitrate and/or nickel chloride, and the molar ratio of aluminum in the trivalent aluminum salt to nickel in the divalent nickel salt is 1:(2-4);
the alkaline solution is an aqueous solution containing sodium hydroxide and sodium carbonate, with a concentration of sodium hydroxide 0.2-4 mol/L, and a concentration of sodium carbonate of 0.1-2 mol/L in the alkaline solution; and the molar ratio of sodium hydroxide to the total moles of aluminum and nickel in the trivalent aluminum salt and the divalent nickel salt is (2-4):1, and the molar ratio of sodium carbonate to the total moles of aluminum and nickel in the trivalent aluminum salt and the divalent nickel salt is (0.5-2):1.

14 . The process according to claim 12 , wherein the precipitation treatment is carried out at a temperature of 40° C. to less than 100° C., and the aging treatment is carried out at a temperature of 40° C. to less than 100° C. for 2 to 48 hours.

15 . The process according to claim 8 , further comprising contacting the heat-treated nickel-aluminum precursor with hydrogen to perform reduction treatment, at a temperature of 500-900° C., for 120-480 min, with a hydrogen flow rate of 30-50 ml/(min·g nickel-aluminum precursor).

16 . The process according to claim 8 , further comprising mixing the nickel-aluminum precursor and a salt solution of an alkali metal for coprecipitation reaction, and then carrying out a heat treatment on a resulting precipitate, wherein the molar ratio of the alkali metal to nickel is not more than 0.2.

17 . The process according to claim 8 , wherein the heat treatment comprises raising the temperature of the nickel-aluminum precursor to 500-900° C. in the presence of a protective gas, wherein the protective gas is nitrogen and/or argon, with a flow rate of the protective gas of 10-500 ml/(min·g nickel-aluminum precursor), and a temperature-rising rate of 1-5° C./min;
the vapor deposition is carried out at a temperature of 750-900° C., for 5-240 min; and
the carbon source gas is methane or ethane, which is used at a flow rate of 10 to 500 ml/(min·g nickel-aluminum precursor).

18 . A method for decomposition of nitrous oxide, comprising: contacting the carbon-coated nickel-aluminum nanocomposite according to claim 1 with nitrous oxide to generate nitrogen and oxygen.

19 . A process of catalytically oxidizing volatile organic compounds, comprising: using the carbon-coated nickel-aluminum nanocomposite according to claim 1 as a catalyst for catalyzing the oxidation of volatile organic compounds.

20 . The process according to claim 19 , wherein the oxidation reaction comprises catalytic combustion of a mixed gas containing volatile organic compounds and a standard gas containing oxygen by contacting the mixed gas with the catalyst.

21 . The process according to claim 20 , wherein the mixed gas comprises 0.1-2 vol % of the volatile organic compounds, and 5-20 vol % of oxygen.

22 . The process according to claim 19 , wherein the volatile organic compound is one or more selected from the group consisting of hydrocarbons having 1 to 4 carbon atoms.

23 . The process according to claim 19 , wherein the oxidation reaction is carried out at a space velocity of 1000-5000 ml reaction gas/(hour-g catalyst).

24 . The process according to claim 19 , wherein the oxidation reaction is carried out at a temperature of 300° C. to 450° C.

Assignees

• China Petroleum & Chem Corp
• Sinopec Res Inst Petroleum

Inventors

• Rong Junfeng
• Yu Peng
• Xie Jingxin
• Wu Genghuang
• Zong Mingsheng
• Lin Weiguo
• Ji Hongbo

Classifications

• B01J2235/30

  Scanning electron microscopy; Transmission electron microscopy · CPC title

• B01J35/45

  Nanoparticles · CPC title

• B01J2235/15

  X-ray diffraction · CPC title

• B01J35/70

  characterised by their crystalline properties, e.g. semi-crystalline (catalysts comprising carbon B01J21/18; molecular sieves B01J29/00) · CPC title

• B22F1/16

  Metallic particles coated with a non-metal (coated with lubricating or binding agents or with organic material B22F1/10) · CPC title