Metal/alpha-MoC1-X load-type single-atomic dispersion catalyst, synthesis method and applications

Patent metadata

Field	Value
Publication number	US-11141716-B2
Application number	US-201716311160-A
Country	US
Kind code	B2
Filing date	Jun 21, 2017
Priority date	Jun 23, 2016
Publication date	Oct 12, 2021
Grant date	Oct 12, 2021

Abstract

A metal/α-MoC1-x load-type single-atomic dispersion catalyst, a synthesis method therefor, and applications thereof. The catalyst uses α-MoC1-x as carrier, and has metal that has the mass fraction ranging from 1-100% and that is dispersed on carrier α-MoC1-x in the single atom form. The catalyst provided in the present application can be adapted to a wide alcohol/water proportion in hydrogen production based on aqueous-phase reforming of alcohols, outstanding hydrogen production performance can be obtained at a variety of proportions, and catalysis performance of the catalyst is much higher than that of metal loaded with an oxide carrier. Especially when the metal is Pt, catalysis performance of the catalyst provided in the present application in the hydrogen production based on aqueous-phase reforming of alcohols is much higher than that of a Pt/α-MoC1-x load-type catalyst on the α-MoC1-x carrier on which Pt is disposed on a layer form in the prior art. The hydrogen production performance of the catalyst provided in the present application can be higher than 20,000 h−1 at the temperature of 190° C.

First claim

The invention claimed is:

1. A catalyst comprising:
a metal and α-MoC 1-x ,
wherein the α-MoC 1-x is a support and the metal is an active component dispersed on the α-MoC 1-x support,
wherein 10-100% of the metal dispersed on the α-MoC 1-x support is in a single-atomic form,
wherein in the α-MoC 1-x support, x is 0-0.9, and
wherein the metal is at least one selected from the group consisting of platinum, ruthenium, palladium, nickel, copper, and cobalt.

2. The catalyst of claim 1 , wherein 90-100% of the metal dispersed on the α-MoC 1-x support is in a single-atomic form.

3. The catalyst of claim 1 , wherein the metal dispersed on the α-MoC 1-x support is 0.01-50% by mass, based on a total mass of the α-MoC 1-x support with the metal dispersed thereon.

4. The catalyst of claim 1 , wherein the metal dispersed on the α-MoC 1-x support is 0.01-10% by mass, based on a total mass of the α-MoC 1-x support with the metal dispersed thereon.

5. The catalyst of claim 1 , wherein the α-MoC 1-x support has a size of between 1-30 nm.

6. The catalyst of claim 1 , wherein the α-MoC 1-x support has a specific surface area of between 5-250 m 2 /g.

7. A method for preparing the catalyst of claim 1 , comprising:
1) synthesizing the α-MoC 1-x support;
2) dissolving a metal precursor salt to obtain a metal precursor salt solution, wherein the metal precursor salt is a precursor salt of the metal;
3) mixing the metal precursor salt solution in step 2) with the α-MoC 1-x support in step 1) to form a mixture;
4) drying the mixture to obtain a solid, wherein the metal of the metal precursor salt has a mass of between 0.01%-55% of a mass of the α-MoC 1-x support with the metal precursor salt mixed thereon;
5) lyophilizing the obtained solid in step 3) to obtain a catalyst precursor; and
6) carburizing the catalyst precursor in a carburization gas atmosphere containing both a carbon source and a hydrogen source to obtain the catalyst.

8. The method of claim 7 , wherein the metal precursor salt is a water-soluble salt.

9. The method of claim 8 , wherein the metal precursor salt is at least one selected from the group consisting of dipotassium tetrachloroplatinate, disodium tetrachloroplatinate, platinum bis(acetylacetonate), chloroplatinic acid, palladium chloride, palladium acetate, nickel chloride, copper chloride, cobalt chloride, nickel nitrate, copper nitrate, cobalt nitrate, nickel acetylacetonate, copper acetylacetonate, and cobalt acetylacetonate.

10. The method of claim 7 , wherein the metal precursor salt comprises the metal having a mass of between 0.01%-12% of a total mass of the α-MoC 1-x support with the metal precursor salt thereon.

11. The method of claim 7 , wherein:
the carbon source is at least one selected from the group consisting of alkane, olefin and alcohol;
the hydrogen source is hydrogen gas;
the volume ratio of the carbon source to the hydrogen source is of between 0.1:9 to 9:1;
the heating rate of temperature programming for carburization is 1-50° C./min; and
the carburization comprises a highest temperature step of between 490-900° C.

12. The method of claim 11 , wherein the carburization comprises a temperature step performed at between 200-300° C. for of between 0.1-50 hours and the highest temperature step is then performed of between 490-900° C. for of between 0.1-100 hours.

13. Use of the catalyst of claim 1 for the hydrogen production reaction of an alcohol aqueous phase reforming, comprising:
contacting the catalyst with an aqueous solution of an alcohol in a closed system at a reaction temperature to produce hydrogen.

14. The use of claim 13 , wherein the alcohol is selected from the group consisting of methanol, ethanol, glycerin and ethylene glycol.

15. The use of claim 13 , wherein the reaction temperature of the hydrogen production reaction of the alcohol aqueous phase reforming is of between 50-280° C.

16. The use of claim 13 , wherein the aqueous solution of the alcohol comprises the alcohol and water in a ratio of between 0.1:9 to 10:1.

Assignees

• Univ Beijing

Inventors

• Ma Ding
• Lin Lili
• Yao Siyu

Classifications

• B01J35/45

  Nanoparticles · CPC title

• B01J2235/00

  Indexing scheme associated with group B01J35/00, related to the analysis techniques used to determine the catalysts form or properties · CPC title

• B01J2235/15

  X-ray diffraction · CPC title

• B01J23/755

  Nickel · CPC title

• B01J23/42

  Platinum · CPC title