Fatty acid-acylated insulin analogs

Drug – bio-affecting and body treating compositions – Designated organic active ingredient containing – Peptide containing doai

Reexamination Certificate

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C514S012200, C530S300000, C530S303000, C530S324000, C424S185100

Reexamination Certificate

active

06444641

ABSTRACT:

FIELD OF THE INVENTION
This invention is in the field of clinical medicine and provides fatty acid-acylated insulin analogs with shifted isoelectric points useful for the treatment of diabetes and hyperglycemia.
BACKGROUND OF THE INVENTION
The availability of insulin replacement therapy has prevented the mortality and morbidity of acute complications in diabetes mellitus. However, chronic diabetic complications remain a major health problem due to persistent metabolic derangement, arising principally from poor control of blood glucose. Results emerging from the Diabetes Control and Complications Trial (DCCT) indicate that a decrease of 1% in HbAic (glycosylated hemoglobin) correlates with more than 35% improvement in the incidence of retinopathy [The DCCT Research Group,
New. Engl. J. Med
., 329, 977-986 (1993)].
In order to achieve normal glycemia, therapy must be designed to parallel as closely as possible the pattern of endogenous insulin secretion in normal individuals. The daily physiological demand for insulin fluctuates and can be separated into two phases: (a) the absorptive phase, which requires a pulse of insulin to dispose of the meal-related blood glucose surge, and (b) the post-absorptive phase, which requires a sustained amount of insulin to regulate hepatic glucose output for maintaining optimal fasting blood glucose. Accordingly, effective therapy involves the combined use of two types of exogenous insulin: a fast-acting meal-time insulin and a long-acting or intermediate-acting basal insulin.
The presently available long-acting or intermediate-acting basal insulins are suspensions which are not ideal in at least two respects. First, the degree of resuspension achieved by patients has been observed to be quite variable. This variable degree of resuspension increases the risk that the patient will withdraw and inject either too much insulin, or too little insulin. [Skyler, J. S.,
Medical Clinics of North America
, 72, 1337-1354 (1988)]. If too much insulin is injected, the patient faces an increased risk of hypoglycemia, and its attendant perils of fainting, convulsions, and coma. If too little insulin is injected, the patient's blood glucose level remains higher than desired, which increases the tendency to develop the degenerative vascular consequences of diabetes.
Second, many of these existing insulin formulations for long-acting or intermediate-acting basal glucose control are immunogenic. Beef insulin differs from human insulin at three positions, and long-term use of beef insulin (Ultralente) causes formation of neutralizing antibodies in some people with diabetes. Protamine is a fish protein which has been shown to cause antibody formation in some patients [Ellerhorst, J. A., et al.,
The American Journal of the Medical Sciences
, 299, 298-301 (1987)]. Thus, long-term use of beef Ultralente or insulin- NPH formulations carries an increased risk that the patient will become allergic to the insulin formulation, or that antibodies will alter the pharmacokinetics, especially of short-acting insulins. Such consequences may require the patient to stop using these insulin formulations.
Two alternative approaches have been pursued to minimize or avoid these problems. In the first approach, appropriate amino acid modifications are made to raise the isoelectric point of the insulin analog molecule to approximately that of the subcutaneous site. Such insulin analogs remain soluble in the vial because they are formulated at a pH well below their isoelectric points, namely, in the range of pH 3-5. After subcutaneous injection, quick adjustment to physiological pH causes these analogs to precipitate or crystallize. After that, their slow dissolution provides the desired delay in action. Certain insulin analogs are soluble at pH 3-5, yet have prolonged time-action compared with human insulin because they precipitate at higher physiological pH. See, for example, Markussen, J., et al.,
Protein Engineering
, 1, 215-223 (1987); Jorgensen, S., et al.,
British Medical Journal
, 299, 415-419 (1989); Markussen, J., U.S. Pat. No. 4,946,828, issued Aug. 7 , 1990; Zeuzem, S., et al.,
Diabetologia
, 33, 65-71 (1990); Vertesy, L., et al., U.S. Pat. No. 5,506,202, issued Apr. 9, 1996; Hofftnann, J., et al., U.S. Pat. No. 5,491,216, issued Feb. 13 1996; Dörschug, M., U.S. Pat. No. 5,656,722, issued Aug. 12, 1997; Chance, R.
E., et al., U.S. Provisional Application Serial. No. 60/055,828, filed Aug. 15, 1997. While the first approach has provided some interesting results, several problems remain in this area of insulin research.
A second general alternate approach to providing basal control of blood glucose has been to acylate insulin with fatty acids, and to rely on the binding of fatty acids by serum albumin to retain insulin activity in the circulation for extended periods of time [Walder, et al., WO 92/01476; Muranishi, et al., Japanese Patent Application 1-254,699; Hashimoto, M., et al.,
Pharmaceutical Research
, 6, 171-176 (1989); Baker, J. C., et al., U.S. Pat. No. 5,693,609, issued Dec. 2, 1997; Havelund, S., et al., WO95/07931, published Mar. 23, 1995; and Jonassen, I., et al., WO96/29342, published Sep. 26, 1996]. While providing some extension, the time-action of these acylated insulins and insulin analogs is not sufficiently long to provide an ideal basal control of blood glucose levels. In particular, they are required to be administered at least two times per day, whereas an ideal basal insulin would only require one administration per day. Furthermore, because certain of the acylated insulins suffer from low potency relative to insulin, significantly greater amounts of these acylated insulins are required to obtain adequate control of blood glucose levels.
SUMMARY OF THE INVENTION
The present invention provides a fatty acid-acylated insulin analog having an isoelectric point that is higher than the isoelectric point of insulin, comprising an insulin analog to which a fatty acyl chain is joined by an amide bond. None of the many publications mentioned above disclose acylated insulin analogs that have increased isoelectric points, and none has suggested their desirability. Acylation of insulin analogs that have increased isoelectric points, relative to insulin, is associated with excellent blood glucose control and provides basal insulin levels that are unexpectedly desirable therapeutically.
The invention further provides a soluble formulation comprising a fatty acid-acylated insulin analog of the present invention, together with one or more excipients selected from a preservative, a metal ion, an isotonicity agent, and a pharmaceutically-acceptable buffer. The invention also provides a method of treating hyperglycemia comprising administering to a patient in need thereof an effective dose of the fatty acid-acylated insulin analog of the present invention. The invention also provides a method of treating hyperglycemia comprising administering to a patient in need thereof an effective dose of the fatty acid-acylated insulin analog of the present invention.
The present invention includes a fatty acid-acylated insulin analog having an isoelectric point that is higher than the isoelectric point of insulin, comprising an insulin analog with a fatty acyl chain bonded to the insulin analog by an amide bond. The present invention also includes a fatty acid-acylated insulin analog having an isoelectric point that is higher than the isoelectric point of insulin, wherein the acylated insulin analog has at least one more net positive charge than insulin. The invention also includes a fatty acid-acylated insulin analog having an isoelectric point that is higher than the isoelectric point of insulin, wherein the acylated insulin analog has at least two more net positive charges than insulin.
The present invention encompasses a mono-acylated insulin analog having the formula below, comprising:
(a) a polypeptide of SEQ ID NO:1 properly crosslinked to a polypeptide of SEQ ID NO:2, or a pharmaceutically acceptable salt thereof, wherein t

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