IP Library Granted Patent US 8,969,236
Granted Patent B2
US 8,969,236 · App. 13/286,987 · Granted Mar 3, 2015

Process and catalyst for production of mixed alcohols from synthesis gas

Inventors: Vijay K. Sethi (Laramie, WY); Yulong Zhang (Laramie, WY)
Assignee: University of Wyoming Research Corporation
B01J27/22B01J37/08B01J37/084B01J37/16B01J35/002B01J35/1009B01J35/1014C07C29/153
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Quick Facts
Patent No.
US 8,969,236
App. No.
13/286,987
Granted
Mar 3, 2015
Kind
B2
Abstract

A preferred embodiment of the process involves a generate a catalyst that comprises molybdenum carbide nickel material. Steps may involve heating a surface that comprises molybdenum oxide and a nickel salt while passing thereover a gaseous mixture that comprises a reductant and a carburizer. In certain embodiments, the reductant and the carburizer may both be carbon monoxide, or both be a saturated hydrocarbon. In others, the reductant may be carbon monoxide and the carburizer may be a saturated hydrocarbon.

Claims (56)

1. A process for producing a molybdenum carbide and nickel material comprising the steps of:

heating molybdenum oxide, nickel salt, a first quantity of carbon monoxide and a second quantity of carbon monoxide;

reducing said molybdenum oxide and said nickel salt with said first quantity of carbon monoxide;

carburizing said molybdenum oxide and said nickel salt with said second quantity of carbon monoxide; and

yielding said molybdenum carbide and nickel material.

2. A process for producing a molybdenum carbide and nickel material as described in claim 1 wherein said step of heating comprises the step of heating at a controlled heat rate.

3. A process for producing a molybdenum carbide and nickel material as described in claim 2 wherein said controlled heat rate comprises a programmed heat rate.

4. A process for producing a molybdenum carbide and nickel material as described in claim 1 wherein said steps of reducing and carburizing occur during said step of heating.

5. A process for producing a molybdenum carbide and nickel material as described in claim 1 wherein said step of reducing occurs before said step of carburizing.

6. A process for producing a molybdenum carbide and nickel material as described in claim 1 further comprising the step of establishing said molybdenum oxide and nickel salt in a reactor.

7. A process for producing a molybdenum carbide and nickel material as described in claim 6 wherein said reactor comprises a quartz reactor.

8. A process for producing a molybdenum carbide and nickel material as described in claim 7 wherein said step of carburizing said molybdenum oxide and said nickel salt with said second quantity of carbon monoxide occurs at a higher temperature than said step of reducing said molybdenum oxide and said nickel salt with said first quantity of carbon monoxide.

9. The molybdenum carbide and nickel material produced by the process of claim 1 .

10. A process for producing a molybdenum carbide and nickel material as described in claim 1 wherein said step of heating molybdenum oxide, nickel salt, a first quantity of carbon monoxide and a second quantity of carbon monoxide further comprises the step of also heating sodium.

11. A process for producing a molybdenum carbide and nickel material comprising the steps of:

establishing a surface that comprises MoO 3 and a nickel salt;

passing a gaseous reactant mixture over said surface;

applying heat; and

yielding said molybdenum carbide and nickel material,

wherein said gaseous reactant mixture comprises a first quantity of carbon monoxide as a reducing gas and a second quantity of carbon monoxide as a carburizing agent.

12. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said first quantity of carbon monoxide is passed over said surface before, and at a lower temperature than, said second quantity of carbon monoxide is passed over said surface.

13. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said step of applying heat comprises the step of increasing temperature so that said first quantity of carbon monoxide reduces and said second quantity of carbon monoxide, at a higher temperature that is said first quantity, carburizes.

14. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said step of applying heat comprises the step of applying heat with a heater established around a reactor.

15. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said nickel salt comprises NiO.

16. A process for producing a molybdenum carbide and nickel material as described in claim 15 wherein a sodium concentration in said NiO is less than 10 ppm by weight.

17. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said nickel salt comprises NiMoO 4 .

18. A process for producing a molybdenum carbide and nickel material as described in claim 17 wherein a sodium concentration in said NiMoO 4 is substantially 15,000 ppm by weight.

19. A process for producing a molybdenum carbide and nickel material as described in claim 17 wherein a sodium concentration in said NiMoO 4 is substantially 430 ppm by weight.

20. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said step of applying heat comprises the step of heating said gaseous reactant mixture while it passes over said surface.

21. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said molybdenum carbide and nickel material is a catalyst for a Fischer Tropsch process that yields alcohol.

22. A process for producing a molybdenum carbide and nickel material as described in claim 11 further comprising the step of agitating said surface.

23. A process for producing a molybdenum carbide and nickel material as described in claim 22 wherein said step of agitating said surface comprises the step of stirring materials of which said surface forms a part.

24. A process for producing a molybdenum carbide and nickel material as described in claim 22 wherein said step of agitating said surface comprises the step of rotating materials of which said surface forms a part.

25. A process for producing a molybdenum carbide and nickel material as described in claim 24 wherein said step of rotating materials comprises the step of rotating a reactor.

26. A process for producing a molybdenum carbide and nickel material as described in claim 25 wherein said step of rotating a reactor comprises the step of rotating a kiln.

27. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said step of establishing a surface comprises the step of establishing a surface that comprises molybdenum and nickel in a molybdenum to nickel molar ratio of from 3.0 to 0.5.

28. A process for producing a molybdenum carbide and nickel material as described in claim 27 wherein said step of establishing a surface comprises the step of establishing a surface that comprises molybdenum and nickel in a molybdenum to nickel molar ratio of from 2.0 to 1.0.

29. A process for producing a molybdenum carbide and nickel material as described in claim 28 wherein said step of establishing a surface comprises the step of establishing a surface that comprises molybdenum and nickel in a molybdenum to nickel molar ratio of from 1.75 to 1.25.

30. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said surface is a surface of a solid precursor and wherein said step of passing a gaseous reactant mixture over said surface comprises the step of passing a gaseous reactant mixture over said surface at from 5 to 40 SLM per mole of molybdenum of said solid precursor.

31. A process for producing a molybdenum carbide and nickel material as described in claim 30 wherein said step of passing a gaseous reactant mixture over said surface comprises the step of passing a gaseous reactant mixture over said surface at from 8 to 25 SLM per mole of molybdenum of said surface.

32. A process for producing a molybdenum carbide and nickel material as described in claim 31 wherein said step of passing a gaseous reactant mixture over said surface comprises the step of passing a gaseous reactant mixture over said surface at from 10 to 18 SLM per mole of molybdenum of said surface.

33. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said step of establishing a surface that comprises MoO 3 and a nickel salt comprises the step of establishing a surface that comprises MoO 3 and a nickel salt in a reactor.

34. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said step of applying heat comprises the step of applying heat to increase a temperature of said gaseous reactant mixture at a rate of from 0.05 to 5.0 degrees Celsius per minute.

35. A process for producing a molybdenum carbide and nickel material as described in claim 34 wherein said step of applying heat comprises the step of applying heat to increase a temperature of said gaseous reactant mixture at a rate of from 0.1 to 2.5 degrees Celsius per minute.

36. A process for producing a molybdenum carbide and nickel material as described in claim 35 wherein said step of applying heat comprises the step of applying heat to increase a temperature of said gaseous reactant mixture at a rate of from 0.25 to 1.0 degrees Celsius per minute.

37. A process for producing a molybdenum carbide and nickel material as described in claim 11 further comprising the step of passing a passivating gas over said surface.

38. A process for producing a molybdenum carbide and nickel material as described in claim 37 wherein said step of applying heat comprises the step of applying heat to increase a temperature of said gaseous reactant mixture substantially at 0.5 degrees Celsius per minute.

39. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said step of applying heat comprises the step of applying heat to increase temperature of said gaseous reactant mixture from a start temperature, wherein said start temperature is within a range of from 150 degrees Celsius to 290 degrees Celsius.

40. A process for producing a molybdenum carbide and nickel material as described in claim 39 wherein said start temperature is within a range of from 270 degrees Celsius to 280 degrees Celsius.

41. A process for producing a molybdenum carbide and nickel material as described in claim 40 wherein said start temperature is substantially 275 degrees Celsius.

42. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said step of applying heat comprises the step of applying heat to increase temperature of said gaseous reactant mixture to an end temperature, wherein said end temperature is within a range of from 600 degrees to 700 degrees Celsius.

43. A process for producing a molybdenum carbide and nickel material as described in claim 41 wherein said end temperature is within a range of from 650 degrees Celsius to 660 degrees Celsius.

44. A process for producing a molybdenum carbide and nickel material as described in claim 43 wherein said end temperature is substantially 655 degrees Celsius.

45. The molybdenum carbide and nickel material produced by the process of claim 11 .

46. A process for producing a molybdenum carbide and nickel material as described in claim 11 wherein said step of establishing a surface that comprises MoO 3 and a nickel salt comprises the step of establishing a surface that further comprises sodium.

47. A process for producing a molybdenum carbide and nickel material as described in claim 46 wherein said step of establishing a surface that further comprises sodium comprises the step of establishing a surface that further comprises Na 2 CO 3 .

Assignments (2)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Aug 26, 2022
From: THE UNIVERSITY OF WYOMING RESEARCH CORPORATION DBA WESTERN RESEARCH INSTITUTE
To: WESTERN RESEARCH INSTITUTE, INC.
Reel/Frame 060912/0373 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Nov 1, 2011
From: SETHI, VIJAY K.; ZHANG, YULONG
To: UNIVERSITY OF WYOMING RESEARCH CORPORATION D/B/A WESTERN RESEARCH INSTITUTE
Reel/Frame 027157/0461 →
Continuity (3)
Continuation In Part 12298733
Provisional Application 60796068 · Apr 27, 2006
Related Publication 20120302435A1 · Nov 29, 2012