Pretreatment process for conversion of cellulose to fuel ethanol

• US 5,916,780 A
• Filed: 06/09/1997
• Issued: 06/29/1999
• Est. Priority Date: 06/09/1997
• Status: Expired due to Term

• Current Assignee: Iogen Corporation
• Original Assignee: Iogen Corporation
• Inventors: Tolan, Jeffrey S., Foody, Brian, Bernstein, Jerome D.
• Primary Examiner(s): Lilling, Herbert J.
• Application Number:
  US08/871,347
• Time in Patent Office: 750 Days
• Field of Search: 435/161, 435/165, 435/163, 435/162, 435/99, 435/105, 435/209, 127/37, 162/9, 162/15, 162/21, 162/22, 162/68
• US Class Current: 435/99
• CPC Class Codes: C12P 7/10 substrate containing cellulosic material
• CPC Class Codes: Y02E 50/10 Biofuels, e.g. bio-diesel

Abstract

An improved pretreatment of cellulosic feedstocks, to enable economical ethanol production by enzyme treatment. The improved pretreatment comprises choosing either a feedstock with a ratio of arabinoxylan to total nonstarch polysaccharides (AX/NSP) of greater than about 0.39, or a selectively bred feedstock on the basis of an increased ratio of AX/NSP over a starting feedstock material, and reacting at conditions that disrupt the fiber structure and hydrolyze a portion of the cellulose and hemicellulose. This pretreatment produces a superior substrate for enzymatic hydrolysis, by enabling the production of more glucose with less cellulase enzyme than any known procedures. This pretreatment is uniquely suited to ethanol production. Preferred feedstocks with an AX/NSP level greater than about 0.39 include varieties of oat hulls and corn cobs.

Claims

1. An improved process for pretreating a lignocellulosic feedstock intended to be converted to fuel ethanol, consisting essentially of the following steps:

a. Choosing a feedstock comprised of at least hemicellulose and cellulose, and characterized by a ratio of arabinan plus xylan to total nonstarch polysaccharides (AX/NSP) that is greater than 0.39, wherein the feedstock consists of oat hulls or corn cobs; and

b. Reacting the chosen feedstock at conditions which disrupt its fiber structure and effect an hydrolysis of a portion of the hemicellulose and cellulose, in order to create a pretreated feedstock with increased accessibility to being digested, during a treatment with cellulase enzymes.

2. A process according to claim 1, wherein the reaction step is carried out by subjecting the chosen feedstock at an average temperature of 180°

C. to 270°

C., pH 0.5 to 2.5 for a period of 5 seconds to 60 minutes.

3. A process according to claim 2, wherein the reaction step is carried out by subjecting the chosen feedstock at an average temperature of 220°

C. to 270°

C., pH 0.5 to 2.5 for a period of 5 seconds to 120 seconds.

4. A process according to claim 1, wherein the reaction step is carried out in two stages, with the first stage at an average temperature below 180°

C. and the second stage at an average temperature above 180°

C.

5. A process according to claim 4, wherein the first stage of the reaction step is carried out at an average temperature of 60°

C. to 140°

C. for 0.25 to 24 hours at pH 0.5 to 2.5.

6. A process according to claim 5, wherein the first stage of the reaction step is carried out at an average temperature of 100°

C. to 130°

C. for 0.5 to 3 hours at pH 0.5 to 2.5.

7. A process according to claim 4, wherein the second stage of the reaction step is carried out by subjecting the chosen feedstock to an average temperature of 180°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 60 minutes.

8. A process according to claim 7, wherein the second stage of the reaction step is carried out by subjecting the chosen feedstock at an average temperature of 220°

C. to 270°

C., at pH 0.5 to 2.5 for a period of 5 seconds to 120 seconds.

9. A process according to claim 1, wherein the feedstock is slurried in water during the reaction step.

10. A process according to claim 1, wherein the feedstock is free of externally-added moisture during the reaction step.

11. A process according to claim 1, wherein the reaction step is carried out with a steam explosion or extrusion device.

12. An improved process for converting a lignocellulosic feedstock to ethanol, consisting essentially of the following steps:

a. Choosing a feedstock comprised of at least hemicellulose and cellulose, and characterized by a ratio of arabinan plus xylan to total nonstarch polysaccharides (AX/NSP) that is greater than about 0.39, wherein the feedstock consists of oat hulls or corn cobs; and

b. Reacting the chosen feedstock at conditions which disrupt its fiber structure and effect an hydrolysis of a portion of the hemicellulose and cellulose, in order to create a pretreated feedstock with increased accessibility to being digested, during a treatment with cellulase enzymes; and

c. Hydrolyzing the pretreated feedstock by using cellulase enzymes; and

d. Fermenting the resulting sugars to ethanol; and

e. Recovering the ethanol.

13. A process according to claim 12 wherein the reaction step is carried out by subjecting the chosen feedstock to an average temperature of 180°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 60 minutes, and the subsequent enzymatic hydrolysis of cellulose is carried out with 1.0 to 10.0 filter paper units (FPU) of cellulase enzyme per gram of cellulose.

14. A process according to claim 13 wherein the reaction step is carried out by subjecting the chosen feedstock to an average temperature of 220°

C. to 270°

C., at pH 0.5 to 2.5 for a period of 5 seconds to 120 seconds, and the subsequent enzymatic hydrolysis of cellulose is carried out with 1.0 to 10.0 filter paper units (FPU) of cellulase enzyme per gram of cellulose.

15. A process according to claim 12 wherein the reaction step is carried out in two stages, with the first stage at an average temperature of below 180°

C. and the second stage at an average temperature of above 180°

C.

16. A process according to claim 15 wherein the first stage of the reaction step is carried out at an average temperature of 60°

C. to 140°

C. for 0.25 to 24 hours at pH 0.5 to 2.5.

17. A process according to claim 16 wherein the first stage of the reaction step is carried out at an average temperature of 100°

C. to 130°

C. for 0.5 to 3 hours at pH 0.5 to 2.5.

18. A process according to claim 15 wherein the second stage of the reaction step is carried out by subjecting the chosen feedstock at an average temperature of 180°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 60 minutes, and the subsequent enzymatic hydrolysis of cellulose is carried out with 1.0 to 10.0 filter paper units (FPU) of cellulase enzyme per gram of cellulose.

19. A process according to claim 15 wherein the second stage of the reaction step is carried out by subjecting the chosen feedstock at an average temperature of 220°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 120 seconds, and the subsequent enzymatic hydrolysis of cellulose is carried out with 1.0 to 10.0 filter paper units (FPU) of cellulase enzyme per gram of cellulose.

20. A process according to claim 12, wherein the feedstock is slurried in water during the reaction step.

21. A process according to claim 12, wherein the feedstock is free of externally-added moisture during the reaction step.

22. A process according to claim 12, wherein the pretreatment step is carried out with a steam explosion or extrusion device.

23. A process according to claim 12, wherein the cellulose hydrolysis step and ethanol fermentation step are carried out simultaneously.

24. An improved process for converting a lignocellulosic feedstock to glucose, consisting essentially of the following steps:

a. Choosing a feedstock comprised of at least hemicellulose and cellulose, and characterized by a ratio of arabinan plus xylan to total nonstarch polysaccharides (AX/NSP) of greater than about 0.39, wherein the feedstock consists of corn cobs or oat hulls; and

b. Reacting the chosen feedstock at conditions which disrupt its fiber structure and effect an hydrolysis of a portion of the hemicellulose and cellulose, in order to create a pretreated feedstock with increased accessibility to being digested, during a treatment with cellulase enzymes; and

c. Hydrolyzing at least 40% of the cellulose in the pretreated feedstock to glucose by using cellulase enzymes.

25. A process according to claim 24 wherein the reaction step is carried out by subjecting the chosen feedstock to an average temperature of 180°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 60 minutes, and the subsequent enzymatic hydrolysis of cellulose is carried out with 1.0 to 10.0 filter paper units (FPU) of cellulase enzyme per gram of cellulose.

26. A process according to claim 24 wherein the reaction step is carried out by subjecting the chosen feedstock to an average temperature of 220°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 120 seconds, and the subsequent enzymatic hydrolysis of cellulose is carried out with 1.0 to 10.0 filter paper units (FPU) of cellulase enzyme per gram of cellulose.

27. A process according to claim 24 wherein the reaction step is carried out in two stages, with the first stage at an average temperature below 180°

C. and the second stage at an average temperature above 180°

C.

28. A process according to claim 27 wherein the first stage of the reaction step is carried out at an average temperature ot 60°

C. to 140°

C. for 0.25 to 24 hours at pH 0.5 to 2.5.

29. A process according to claim 27 wherein the first stage of the reaction step is carried out at an average temperature of 100°

C. to 130°

C. for 0.5 to 3 hours at pH 0.5 to 2.5.

30. A process according to claim 27 wherein the second stage of the reaction step is carried out by subjecting the chosen feedstock to an average temperature of 180°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 60 minutes, and the subsequent enzymatic hydrolysis of cellulose is carried out with 1.0 to 10.0 filter paper units (FPU) of cellulase enzyme per gram of cellulose.

31. A process according to claim 27 wherein the second stage of the reaction step is carried out by subjecting the chosen feedstock to an average temperature of 220°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 120 seconds, and the subsequent enzymatic hydrolysis of cellulose is carried out with 1.0 to 10.0 filter paper units (FPU) of cellulase enzyme per gram of cellulose.

32. A process according to claim 24, wherein the feedstock is slurried in water during the reaction step.

33. A process according to claim 24, wherein the feedstock is free of externally-added moisture during the reaction step.

34. A process according to claim 24, wherein the reaction step is carried out with a steam explosion or extrusion device.

35. An improved process for pretreating a lignocellulosic feedstock for conversion to fuel ethanol, consisting essentially of the following steps:

a. Choosing a selectively bred feedstock, comprised of at least hemicellulose and cellulose, on the basis of an increased ratio of arabinan plus xylan to total nonstarch polysaccharides (AX/NSP) over a starting material to a level greater than about 0.39; and

b. Reacting the selectively bred feedstock at an average temperature of 180°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 60 minutes to disrupt the fiber structure and effect an hydrolysis of a portion of the hemicellulose and cellulose, in order to create a pretreated feedstock with increased accessibility to being digested, during a treatment with cellulase enzymes.

36. A process according to claim 35 wherein the reaction step is carried out by subjecting the selectively bred feedstock to an average temperature of 220°

C. to 270°

C., at pH 0.5 to 2.5 for a period of 5 seconds to 120 seconds.

42. A process according to claim 35 wherein the pretreatment is carried out with a steam explosion or extrusion device during the reaction step.

37. An improved process for pretreating a lignocellulosic feedstock for conversion to fuel ethanol, consisting essentially of the following steps:

a. Choosing a selectively bred feedstock, comprised of at least hemicellulose and cellulose, on the basis of an increased ratio of arabinan plus xylan to total nonstarch polysaccharides (AX/NSP) over a starting feedstock material to a level that is greater than about 0.39; and

b. Reacting the selectively bred feedstock in two stages, with the first stage at an average temperature below 180 C. and the second stage at an average temperature above 180 C. to disrupt the fiber structure and effect an hydrolysis of a portion of the hemicellulose and cellulose, in order to create a pretreated feedstock with increased accessibility to being digested, during a treatment with cellulase enzymes.

38. A process according to claim 37 wherein the first stage of the reaction step is carried out at an average temperature of 60°

C. to 140°

C. for 0.25 to 24 hours at pH 0.5 to 2.5.

39. A process according to claim 38 wherein the first stage-of the reaction step is carried out at an average temperature of 100°

C. to 130°

C. for 0.5 to 3 hours at pH 0.5 to 2.5.

40. A process according to claim 37 wherein the second stage of the reaction step is carried out by subjecting the selectively bred feedstock to an average temperature of 180°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 60 minutes.

41. A process according to claim 40 wherein the second stage of the reaction step is carried out by subjecting the chosen feedstock at an average temperature of 220°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 120 seconds.

43. A process for converting a lignocellulosic feedstock to ethanol, the process consisting essentially of the following steps:

a. Choosing a selectively bred feedstock, comprised of at least hemicellulose and cellulose, on the basis of an increased ratio of arabinan plus xylan to total nonstarch polysaccharides (AX/NSP) over a starting feedstock material to a level that is greater than about 0.39; and

b. Reacting the selectively bred feedstock at an average temperature of 180°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 60 minutes to disrupt the fiber structure and effect an hydrolysis of a portion of the hemicellulose and cellulose, in order to create a pretreated feedstock with increased accessibility to being digested, during a treatment with cellulase enzymes; and

c. Hydrolyzing the pretreated feedstock to sugars by using cellulase enzymes at a dosage of 1.0 to 10.0 filter paper units (FPU) of cellulase enzyme per gram of cellulose; and

d. Fermenting the resulting sugars to ethanol; and

e. Recovering the ethanol.

44. A process according to claim 43 wherein the reaction step is carried out by subjecting the selectively bred feedstock to an average temperature of 220°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 120 seconds.

50. A process according to claim 43 wherein the reaction step is carried out with a steam explosion or extrusion device.

45. A process for converting a lignocellulosic feedstock to ethanol, the process consisting essentially of the following steps:

a. Choosing a selectively bred feedstock, comprised of at least hemicellulose and cellulose, on the basis of an increased ratio of arabinan plus xylan to total nonstarch polysaccharides (AX/NSP) over a starting feedstock material to a level that is greater than about 0.39; and

b. Reacting the chosen feedstock in two stages, with the first stage at an average temperature below 180°

C. and the second stage at an average temperature above 180 C. to disrupt the fiber structure and effect an hydrolysis of a portion of the hemicellulose and cellulose, in order to create a pretreated feedstock with increased accessibility to being digested, during a treatment with cellulase enzymes; and

c. Hydrolyzing the pretreated feedstock to sugars by using cellulase enzymes at a dosage of 1.0 to 10.0 filter paper units (FPU) of cellulase enzyme per gram of cellulose; and

d. Fermenting the resulting sugars to ethanol; and

e. Recovering the ethanol.

46. A process according to claim 45 wherein the first stage of the reaction step is carried out at an average temperature of 60°

C. to 140°

C. for 0.25 to 24 hours at pH 0.5 to 2.5.

47. A process according to claim 46 wherein the first stage of the reaction step is carried out at an average temperature of 110°

C. to 130°

C. for 0.5 to 3 hours at pH 0.5 to 2.5.

48. A process according to claim 45 wherein the second stage of the reaction step is carried out by subjecting the bred feedstock to an average temperature of 180°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 60 minutes.

49. A process according to claim 48 wherein the second stage of the reaction step is carried out by subjecting the selectively bred feedstock to an average temperature of 220°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 120 seconds.

51. A process for converting a lignocellulosic feedstock to glucose, consisting essentially of the following steps:

a. Choosing a selectively bred feedstock, comprised of at least hemicellulose and cellulose, on the basis of an increased ratio of arabinan plus xylan to total nonstarch polysaccharides (AX/NSP) over a starting feedstock material to a level that is greater than about 0.39; and

b. Reacting the selectively bred feedstock at an average temperature of 180°

C. to 270°

C., at a pH of 0.5 to 2.5, for a period of 5 seconds to 60 minutes to disrupt the fiber structure and effect an hydrolysis of a portion of the hemicellulose and cellulose, in order to create a pretreated feedstock with increased accessibility to being digested, during a treatment with cellulase enzymes; and

c. Hydrolyzing at least 40% of the cellulose in the pretreated feedstock to glucose by using cellulase enzymes at a dosage of 1.0 to 10.0 filter paper units (FPU) of cellulase enzyme per gram of cellulose.

52. A process according to claim 51 wherein the reaction step is carried out by subjecting the selectively bred feedstock to an average temperature of 220°

C. to 270°

C., at a pH of 0.5 to 2.5, for a period of 5 seconds to 120 seconds.

58. The process according to claim 51 wherein the reaction step is carried out with a steam explosion or extrusion device.

53. A process for converting a lignocellulosic feedstock to glucose, consisting essentially of the following steps:

a. Choosing a selectively bred feedstock, comprised of at least hemicellulose and cellulose, on the basis of an increased ratio of arabinan plus xylan to total nonstarch polysaccharides (AX/NSP) over a starting feedstock material to a level greater than about 0.39; and

b. Reacting the selectively bred feedstock in two stages, with the first stage at an average temperature below 180°

C. and the second stage at an average temperature above 180 C. to disrupt the fiber structure and effect an hydrolysis of a portion of the hemicellulose and cellulose, in order to create a pretreated feedstock with increased accessibility to being digested, during a treatment with cellulase enzymes; and

c. Hydrolyzing at least 40% of the cellulose in the pretreated feedstock to glucose by using cellulase enzymes at a dosage of 1.0 to 10.0 filter paper units (FPU) of cellulase enzyme per gram of cellulose.

54. A process according to claim 53 wherein the first stage of the reaction step is carried out at an average temperature of 60°

C. to 140°

C. for 0.25 to 24 hours at pH 0.5 to 2.5.

55. A process according to claim 54 wherein the first stage of the reaction step is carried out at an average temperature of 110°

C. to 130°

C. for 0.5 to 3 hours at pH 0.5 to 2.5.

56. A process according to claim 53 wherein the second stage of the reaction step is carried out by subjecting the selectively bred feedstock to an average temperature of 180°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 60 minutes.

57. A process according to claim 56 wherein the second stage-of the reaction step is carried out by subjecting the chosen feedstock to an average temperature of 220°

C. to 270°

C., at pH 0.5 to 2.5, for a period of 5 seconds to 120 seconds.