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US3696110A - Certain hyoscyaminium compounds - Google Patents

Certain hyoscyaminium compounds Download PDF

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US3696110A
US3696110A US82813A US3696110DA US3696110A US 3696110 A US3696110 A US 3696110A US 82813 A US82813 A US 82813A US 3696110D A US3696110D A US 3696110DA US 3696110 A US3696110 A US 3696110A
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Prior art keywords
hyoscyaminium
bromide
compounds
gastric
quaternary ammonium
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US82813A
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Satoru Tanaka
Kazunori Hasimoto
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GISAI KK
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GISAI KK
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D451/00Heterocyclic compounds containing 8-azabicyclo [3.2.1] octane, 9-azabicyclo [3.3.1] nonane, or 3-oxa-9-azatricyclo [3.3.1.0<2,4>] nonane ring systems, e.g. tropane or granatane alkaloids, scopolamine; Cyclic acetals thereof
    • C07D451/02Heterocyclic compounds containing 8-azabicyclo [3.2.1] octane, 9-azabicyclo [3.3.1] nonane, or 3-oxa-9-azatricyclo [3.3.1.0<2,4>] nonane ring systems, e.g. tropane or granatane alkaloids, scopolamine; Cyclic acetals thereof containing not further condensed 8-azabicyclo [3.2.1] octane or 3-oxa-9-azatricyclo [3.3.1.0<2,4>] nonane ring systems, e.g. tropane; Cyclic acetals thereof
    • C07D451/04Heterocyclic compounds containing 8-azabicyclo [3.2.1] octane, 9-azabicyclo [3.3.1] nonane, or 3-oxa-9-azatricyclo [3.3.1.0<2,4>] nonane ring systems, e.g. tropane or granatane alkaloids, scopolamine; Cyclic acetals thereof containing not further condensed 8-azabicyclo [3.2.1] octane or 3-oxa-9-azatricyclo [3.3.1.0<2,4>] nonane ring systems, e.g. tropane; Cyclic acetals thereof with hetero atoms directly attached in position 3 of the 8-azabicyclo [3.2.1] octane or in position 7 of the 3-oxa-9-azatricyclo [3.3.1.0<2,4>] nonane ring system
    • C07D451/06Oxygen atoms
    • C07D451/10Oxygen atoms acylated by aliphatic or araliphatic carboxylic acids, e.g. atropine, scopolamine
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B42BOOKBINDING; ALBUMS; FILES; SPECIAL PRINTED MATTER
    • B42DBOOKS; BOOK COVERS; LOOSE LEAVES; PRINTED MATTER CHARACTERISED BY IDENTIFICATION OR SECURITY FEATURES; PRINTED MATTER OF SPECIAL FORMAT OR STYLE NOT OTHERWISE PROVIDED FOR; DEVICES FOR USE THEREWITH AND NOT OTHERWISE PROVIDED FOR; MOVABLE-STRIP WRITING OR READING APPARATUS
    • B42D17/00Hanging or securing devices for books, newspapers or the like

Definitions

  • the new quaternary ammonium salts according to the present invention exhibit a strong parasympathetic blocking activity with low toxicity. They therefore are advantageously utilizable for chemotherapeutical treatment of patients suffering from diseases such as, for example, gastric cramp, gastric ulcer, duodenal ulcer and the like.
  • Aqueous solutions of these salts are stable and are administrated to patients through venous and subcutaneous injections as well as oral administration.
  • This invention relates to a process for synthesizing new quaternary salts of atropine or its optical isomer called hyoscyamine base and represented by the formula wherein R is lower alkyl or alkenyl group and X is 3. Anti-acetylcholine effect against the contraction halogen atom.
  • Atropine and its optical isomer called hyoscyamine base are the essential components of the main alkaloids contained in belladonna and scopolia. These compounds exhibit a strong parasympathetic blocking activity and they therefore are utilized for the purpose of therapeutical treatment of diseases such as gastric cramp, gastric ulcer, duodenal ulcer and the like. Unfortunately it was found that they show undesirable side effects such as dryness of mouth, retention of urine, disturbance of heart rhythm and an injurious effect on central nervous system.
  • Typical solvents which have been found preferable to carry out the above reaction include lower alcohol, acetone, ether and the like.
  • the reaction takes place readily at room temperature. In order to prevent from racemisation of the reacting materials, it is advisable to carry out the reaction at low temperature.
  • reaction mixture had a turbid appearance followed by separation of white crystals.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)
  • Nitrogen Condensed Heterocyclic Rings (AREA)

Abstract

A class of new quaternary ammonium salts derived from atropine or its optical isomer called hyoscyamine base with p-alkoxy or alkenoxy-substituted benzyl halide. The new quaternary ammonium salts according to the present invention exhibit a strong parasympathetic blocking activity with low toxicity. They therefore are advantageously utilizable for chemotherapeutical treatment of patients suffering from diseases such as, for example, gastric cramp, gastric ulcer, duodenal ulcer and the like. Aqueous solutions of these salts are stable and are administrated to patients through venous and subcutaneous injections as well as oral administration.

Description

United States Patent 1 3,696,110
Tanaka et al. 1 Oct. 3, 1972 [54] CERTAIN HYOSCYAMINIUM [56] References Cited CO UNDS OTHER PUBLICATIONS [72] inventors: Satoru Tanaka; Kazunorl Ilulnmto, smithuisl chem Abstracts. VOL 66, Item both Of Tokyo, Japan [73] Assignee: Gisal Kabushiki Kalsha, Tokyo, The Merck index, Seventh Edition, Page 547, 1960 Japan The Merck index, Eighth Edition, Page 558, i968 [22] Filed: Oct. 21, 1970 Pd E r Man L. R0
[ PP 32,813 Attorney-Wenderoth, Lind & Ponack Related U.S. Application Data Continuation of Ser. No. 858,110, Sept. 15, I969, abandoned.
Foreign Application Priority Data ABSTRACT A class of new quaternary ammonium salts derived from atropine or its optical isomer called hyoscyamine base with p-alkoxy or alkenoxy-substituted benzyl halide. The new quaternary ammonium salts according to the present invention exhibit a strong parasympathetic blocking activity with low toxicity. They therefore are advantageously utilizable for chemotherapeutical treatment of patients suffering from diseases such as, for example, gastric cramp, gastric ulcer, duodenal ulcer and the like. Aqueous solutions of these salts are stable and are administrated to patients through venous and subcutaneous injections as well as oral administration.
5 Cldms, No Drawings CERTAIN I-IYOSCYAMINIUM COMPOUNDS This is a continuation of U.S. application, Ser. No. 858,] filed Sept. 15, I969, now abandoned.
This invention relates to a process for synthesizing new quaternary salts of atropine or its optical isomer called hyoscyamine base and represented by the formula wherein R is lower alkyl or alkenyl group and X is 3. Anti-acetylcholine effect against the contraction halogen atom.
Atropine and its optical isomer called hyoscyamine base are the essential components of the main alkaloids contained in belladonna and scopolia. These compounds exhibit a strong parasympathetic blocking activity and they therefore are utilized for the purpose of therapeutical treatment of diseases such as gastric cramp, gastric ulcer, duodenal ulcer and the like. Unfortunately it was found that they show undesirable side effects such as dryness of mouth, retention of urine, disturbance of heart rhythm and an injurious effect on central nervous system.
It was found as the result of several researches which had recently been conducted that the aforementioned drawbacks especially the undesired side effect on central nervous system caused by these researches which had recently been conducted that the afore-mentioned drawbacks especially the undesired side effect on central nervous system caused by these compounds can considerably be reduced, although their aimed original parasympathetic blocking activity is also somewhat reduced, when these compounds are administrated in a form of their conventional quaternary salts. The quaternary salts of atropine such as atropine methyl bromide and butyl scopolaminium bromide in commercial name Buscopan, for example, are now available in market.
It cannot, however, be pronounced that difficulty of the side effect on central nervous system presented by these quaternary salts was satisfactorily eliminated.
It has now been found according to our extensive researches in this field that the aforementioned drawbacks or difficulty can satisfactorily be removed by providing the new quaternary salts of atropine or hyoscyamine base with p-alkoxy or p-alkenoxy-substituted benzyl halide.
The followings are comparative data with respect to the pharmacological effects and toxicities (as acute toxicity LD of p-butoxybenzyl hyoscyaminium bromide as one of the typical quaternary salts according to the present invention and the hitherto known butyl scopolaminium bromide.
I Experiment on Isolated Stomac of Rat According to Magnus Method 1. Direct Effect:
a. With 1 X 10- g/ml of p-butoxybenzyl hyoscyaminium bromide, 74.7 percent control and with l X 10" g/ml of the compound, 42.5 percent control of spontaneous motility were respectively observed.
b. With 1 X 10" g/ml of butyl scopolaminium bromide, no appreciable control was observed.
2. Blocking Effect on the Contraction caused by l X l0 g/ml of Barium Chloride:
caused by l X l0" g/ml of acetylcholine:
a. With 1 X 10" g/ml of p-butoxybenzyl ,hyoscyaminium bromide, 72.5 percent control of the contraction were observed.
b. With l X l0" g/ml of butyl scopolaminium bromide, only 15 .0 percent control of the contraction were observed.
ll. Experiment on the Isolated Small lntestin of Mouse According to Magnus' Method 1. Blocking Effect on the Contraction caused by 5 x 10" glml of Barium Chloride:
a. With 1 X [0" g/ml of p-butoxybenzyl hyoscyaminium bromide, 40.0 percent control of contraction, and with l X l0" g/ml of butyl scopolaminium bromide, only 27.1 percent control of the contraction were respectively observed.
2. Anti-acetylcholine Effect on the Contraction caused by l X l0 g/ml of Acetylcholine:
a. With 1 X 10" g/ml of butyl scopolaminium bromide, 22.6 percent control of the contraction were observed.
lII. Acute Toxicity on Male Mouse Weighing ca 20 Grams intravenous injection (LD 12.0 mg/kg (1 l.0-l 3.1
s/ s) Subcutaneous injection (LD 660 mg/kg wherein Rznd X have the same meanings as previously defined.
Typical solvents which have been found preferable to carry out the above reaction include lower alcohol, acetone, ether and the like. The reaction takes place readily at room temperature. In order to prevent from racemisation of the reacting materials, it is advisable to carry out the reaction at low temperature.
Since p-alkoxy or alkenoxy benzyl halide is generally unstable in some extent and is liable to be contaminated with resinous matters thus formed, it is desirable to use it soon after purification by distillation.
In practice, however, no appreciable lowering in yield of the contemplated quaternary salts was observed even though the reaction was conducted with crude substance.
Because no report or reports are found in the literatures so far as our knowledge is concerned with respect to the particular p-alkoxy or alkenoxy benzyl hyoscyaminium halides according to the present invention, the compounds are regarded as new substances.
They are tolerably water-soluble. The aqueous solutions thus obtained are relatively stable to heat. ln
aqueous solutions, the compounds have no tendency to cause racemisation. The fact offers one of the serious advantages in the production of pharmaceutical preparations.
The following examples illustrate the invention.
EXAMPLE 1 Preparation of p-Methoxybenzyl Hyoscyaminium Bromide To 40 milliliters of ice-cooled ethanol solution containing 6 grams of hyoscyamine base were added drop by drop with stirring under ice-cooling l milliliters of an ethanol solution containing grams of p-methoxybenzyl bromide. After stirring for two hours, separation of white crystals appeared. The stirring was continued for additional 5 hours at room temperature. The crystals separated out were then recovered by filtration. The crude crystals were dissolved in 40 milliliters of methanol and 200 milliliters of ethyl ether were then added to the solution. There was recovered 7.5 grams of the white needles having the melting point at 1 90- 200 C.
Upon elementary analysis, the product gave the following results:
For C,,H,,NO Br; molecular weight 490.45;
C H N Calculated (12): 61.22 6.58 2.86 Found (Q1): 6|.27 6.33 3.02
Rotatory polarization of the product was l in" -5(0 0.5 in water) EXAMPLE 2 Preparation of p-Ethoxybenzyl Hyoscyaminium Bromide To 50 milliliters of an acetone solution containing 8.4 grams of hyoscyamine base were added drop by drop 10 millimeters of an acetone solution containing 7.4 grams of p-ethoxybenzyl bromide while ice-cooling. After stirring for a while, white crystals separated out. The reaction mixture was stirred at room temperature for additional 5 hours. The crystalline substance was recovered by filtration, which was then recrystallized from isopropanol. 10.4 Grams of the purified product were obtained in a form of white needles which had the melting point of 164- 166 C.
Analysis of the product gave the following results:
For C H, N0,Br; molecular weight: 504.47; H N
C Calculated (5): 61.89 6.80 2.78 Found ('5): 61.62 7 l7 2.84
EXAMPLE 3 For C, H N0 Br; molecular weight: 516.48;
H N Calculated (as 62.78 6.64 2.11 Found (I): 62.30 6.73 2.73
EXAMPLE 4 Preparation of p-Butoxybenzyl Hyoscyaminium Bromide To milliliters of an isopropanol solution containing 11.8 grams of hyoscyamine base were added drop by drop with stirring l0 milliliters of an isopropanol solution containing 1 1 grams of p-n-butoxybenzyl bromide.
After a while, the reaction mixture had a turbid appearance followed by separation of white crystals.
After stirring for 5 hours at room temperature, the crystals were recovered by filtration, which were then recrystallized from milliliters of isopropanol. There was obtained 15.8 grams of white needles having the melting point of l 58-160 C.
Analysis of the product gave the following properties:
For C H NOJIr; molecular weight: 532.50;
H N Calculated 63.10 7.20 2.63 Found 63.34 7.31 2.69 Rotatory polarization:
lul --21 .7 (c 0.5 in water) What is claimed is: l. Atropinium and hyoscyaminium quaternary salts represented by the formula:
s oQcm-racm 9-0-0 04 ri-cmoa

Claims (4)

  1. 2. A compound according to claim 1, which is, p-methoxybenzyl hyoscyaminium bromide.
  2. 3. A compound according to claim 1, which is, p-ethoxybenzyl hyoscyaminium bromide.
  3. 4. A compound according to claim 1, which is, allyloxybenzyl hyoscyaminium bromide.
  4. 5. A compound according to claim 1, which is, p-butoxybenzyl hyoscyaminium bromide.
US82813A 1969-02-18 1970-10-21 Certain hyoscyaminium compounds Expired - Lifetime US3696110A (en)

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Application Number Priority Date Filing Date Title
JP1153169 1969-02-18

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US (1) US3696110A (en)
CH (1) CH510030A (en)
DE (1) DE1950378C2 (en)
FR (1) FR2034553B1 (en)
GB (1) GB1235957A (en)
NL (1) NL142674B (en)
SE (1) SE351848B (en)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0002051A1 (en) * 1977-11-16 1979-05-30 Eisai Co., Ltd. Use of butoxybenzylhyoscyamine bromide in pharmaceutical compositions against deafness and tinnitus
US20050226920A1 (en) * 2004-04-13 2005-10-13 Kirk Voelker Method of decreasing nicotine withdrawal symptoms during smoking cessation.

Family Cites Families (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1062704B (en) * 1956-08-07 1959-08-06 Licencia Talalmanyokat Process for the production of quaternary atropines
DE1163845B (en) * 1960-10-18 1964-02-27 Egyesult G>ogyszer es Tapszer g>ar Budipest λ ertr Dr C W I otter hos und Dr Ing FI W Lotterhos Pat Anwalte Frankfurt"^ Process for the preparation of p-alkylbenzyl-tropinium derivatives.
AT246339B (en) * 1960-10-18 1966-04-12 Egyt Gyogyszervegyeszeti Gyar Process for the preparation of new p-alkylbenzyltropinium derivatives
DE1165037B (en) * 1961-11-21 1964-03-12 Dr. Schwarz Arzneimittelfabrik G.m.b.H., Monheim (RhId.) Process for the preparation of esters of quaternary atropinium salts.
FR1539224A (en) * 1966-09-02 1968-09-13 Boehringer Sohn Ingelheim Process for making tropic acid derivatives

Non-Patent Citations (3)

* Cited by examiner, † Cited by third party
Title
Smithuis, Chem. Abstracts, Vol. 66, Item No. 79,545 a, 1967 *
The Merck Index, Eighth Edition, Page 558, 1968 *
The Merck Index, Seventh Edition, Page 547, 1960 *

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0002051A1 (en) * 1977-11-16 1979-05-30 Eisai Co., Ltd. Use of butoxybenzylhyoscyamine bromide in pharmaceutical compositions against deafness and tinnitus
FR2409263A1 (en) * 1977-11-16 1979-06-15 Eisai Co Ltd MEDICINAL PRODUCT BASED ON BUTOXYBENZYLHYOSCYAMINE BROMIDE FOR USE IN THE TREATMENT OF DEAFDESS AND EAR TINNING
US20050226920A1 (en) * 2004-04-13 2005-10-13 Kirk Voelker Method of decreasing nicotine withdrawal symptoms during smoking cessation.

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DE1950378A1 (en) 1970-08-27
FR2034553B1 (en) 1974-02-01
NL7001733A (en) 1970-08-20
SE351848B (en) 1972-12-11
CH510030A (en) 1971-07-15
FR2034553A1 (en) 1970-12-11
NL142674B (en) 1974-07-15
GB1235957A (en) 1971-06-16
DE1950378C2 (en) 1985-10-03

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