CN1433301A - New formula for hindering plant ethylene reaction, its preparation method and its use method - Google Patents

Abstract

A tablet for inhibiting the ethylene response in plants is disclosed, which comprises a blocking agent having an inhibitory activity on the binding site of ethylene in plants, and a foaming ingredient, in admixture with one or more acceptable excipients. The invention also discloses a method for preparing the tablet and a method for inhibiting the ethylene reaction of plants.

Description

New formulations for blocking ethylene response in plants, methods for their preparation and methods of use

field of invention

The present invention relates to a novel tablet formulation for the regulation of plant physiology, in particular for blocking the ethylene response, comprising blocking agents mixed with effervescent ingredients, and one or more acceptable excipients, and methods of making such formulations and methods of inhibiting various ethylene reactions by administering the formulations of the present invention.

Background technique

Phytohormones play an important role in plant growth responses. Ethylene is a growth hormone that has many important effects on plant growth, development, and aging. The most important effects of ethylene include processes related to fruit ripening, flower decay and leaf abscission. The commercial value of fresh produce is often reduced by excess ethylene gas, which accelerates fruit ripening, flower decay and premature leaf abscission.

Due to the problems induced by ethylene, a great deal of research has focused on methods of preventing or reducing its effects on plants. One of the most effective ways to mitigate the effects of ethylene is to use the principle of blocking the receptors in plants that receive ethylene signals. One of the best known compounds for this purpose is silver thiosulfate ("STS"). STS provides an irreversible blockage of ethylene binding sites in plant cells, thereby preventing or reducing the deleterious effects of ethylene on plants. Although STS is very effective, it poses a serious waste disposal problem because silver is a heavy metal that is toxic to most living organisms.

Plant Growth Reg. 9, 1587-164, 1990 by Sisler et al. revealed cyclopentadiene as a potent blocker of plant ethylene binding sites. US Patent No. 5,100,462 also discloses a potent diazocyclopentadiene. However, cyclopentadiene and diazocyclopentadiene are unstable and have a strong odor.

US Patent No. 5,518,988 discloses the use of gaseous cyclopropene and its derivatives, such as methylcyclopropene, as an ethylene binding site blocking agent. Methylcyclopropene is effective at very low doses in the parts per billion range, making it as safe to use on fruits and vegetables as it is on flowers. Methylcyclopropene is prone to oxidation and other reactions, so it is very unstable. In the most recent US Patent No. 6,017,849, methylcyclopropene is gas-encapsulated in a carrier. Carriers such as α-cyclodextrin can be used to stabilize the reactivity and instability of cyclopropene gas, thereby providing a convenient and safe method of storing, transporting, applying or delivering this gas to plants.

Commercial methylcyclopropene powder products typically contain 0.43% methylcyclopropene gas content. This gas is released when the powder is mixed with water or buffer. A final methylcyclopropene concentration of 900 ppb can be achieved at an application rate of 0.5 grams of powder per cubic meter in an enclosed space. Exposure to this concentration for at least 4 hours as a post-harvest treatment will significantly extend the shelf life of flowers, fruits and vegetables.

Powder products are far more convenient to use than gaseous products, but they are still disadvantageous to users. It still has the disadvantages of using powder in this field, such as: it is very prone to premature moisture and measurement errors. In addition, it is usually recommended to mix large quantities of powder by hand, such as: when fumigation of large spaces requires using more than 10 grams per batch. In the confined space, due to the workers entering and exiting the confined space during the mixing process, the amount of methylcyclopropene may be reduced than originally expected, thereby reducing the beneficial effect of methylcyclopropene.

The present invention provides an effervescent tablet formulation that alleviates the disadvantages associated with mixing powder forms.

Summary of the invention

Therefore, the object of the present invention is to provide a foaming tablet for inhibiting plant ethylene response, which comprises a medicament for blocking plant ethylene binding sites, a foaming component and one or more acceptable carriers and/or Excipients are mixed.

Another object of the present invention is to provide a process for the preparation of the novel tablet of the present invention.

A further object of the present invention is to provide a method for inhibiting ethylene response in plants.

Detailed Description of the Invention

The present invention provides a novel tablet formulation comprising an agent for blocking ethylene binding sites in plants and an effervescent component, mixed with one or more acceptable carriers and/or excipients.

According to the present invention, agents that block ethylene binding sites in plants include all compounds conventionally used to inhibit ethylene responses in plants such as, but not limited to, cyclopropene, 1-methyl-cyclopropene, 3,3-dimethylcyclopropane, ethylene Methylcyclopropane, diazocyclohexadiene, trans-cyclooctene, cis-cyclooctene, and 2,5-protobornadiene. Related prior art, such as U.S. Patent Nos. 3,879,188, 5,100,462, 5,518,988, and 6,017,849, and Plant Growth Reg. 9 by Sisler et al., 157-164, 1990 are fully incorporated herein by reference in the manual. A preferred agent for blocking ethylene binding sites in plants is 1-methylcyclopropene.

According to the present invention, the term "plant" includes, in addition to woody plants, field crops, potted plants, cut flowers, harvested fruits, vegetables and ornamental plants.

Plants treated with tablets according to the invention which inhibit the ethylene response must be treated in a non-phytotoxic amount. This phytotoxic amount varies not only with the plant, but also with the cultivated plant variety.

According to the present invention, many ethylene reactions can be prevented as disclosed in US Patent Nos. 5,518,988 and 3,879,188. Ethylene reactions can be initiated by exogenous or endogenous ethylene sources. Ethylene responses include, for example, ripening and/or senescence of flowers, fruits, and vegetables; abscission of leaves, flowers, and fruit; ripening and/or shortening of lifespan in ornamentals such as potted plants, cut flowers, shrubs, and dormant seedlings; inhibition of some plant Such as the growth of peas; and stimulate the growth of some plants such as rice.

Plants acceptable for treatment to inhibit senescence according to the present invention include green leafy vegetables such as lettuce (e.g., Lactuea sativa), spinach (Spinaca oleracea) and cabbage (Brassica oleracea); various root crops such as potato (Solanum tuberosum) , carrot (Daucus); bulbs, such as onion (Allium sp.); spice plants, such as basil (Ocimum basilicum), oregano (Origanum vulgare) and dill (Anethumgraveolens); and soybean (Glycine max), Lima Beans (Phaseolus limensis), peas (Lathyrus sp.), corn (Zea mays), broccoli (Brassica oleraceaitalica), cauliflower (Bfassica oleracea botrytis) and stone cypress (Asparagus officinalis).

Fruits which may be treated according to the invention to inhibit their ripening include tomato (Lycopersicon esculentum), apple (Malus domes tica), banana (Musasapientum), pear (Pyrus communis), papaya (Carica papya), mango (Mangifera indica), Peach (Prunus persica), Apricot (Prunusarmeniaca), Nectarine (Prunus persica nectarina), Orange (Citrus sp.), Lemon (Citrus limonia), Lime (Citrus aurantifolia), Grapefruit (Citrusparadisi), Orange (Citrus nobilis deliciosa), kiwi (Actinidia. Chinenus), melons such as Roman cantaloupensis (C. cantalupensis) and muskmelon (C. melo), pineapple (Aranae comosus), persimmon (Diospyros sp.), and raspberry (e.g., Fragaria or Rubus ursinus), blueberries (Vaccinium sp.), green beans (Phaseolus vulgaris), members of the melon genus such as cucumbers (C. sativus) and avocados (Persea Americana).

According to the present invention, ornamentals that may be treated to inhibit senescence and/or prolong flowering and appearance (eg, delayed wilting) include potted ornamentals and cut flowers. Acceptable potted ornamental plants and cut flowers treated by the method of the present invention include Rhododendron spp., Macrophylla hydrangea, Hibiscus rosasanensis, Antirrhinum sp., Euphorbia pulcherima , cactus (e.g., Cactaceae schlumbergera truncata), begonia (Begonia sp.), rose (Rosa sp.), tulip (Tulipa sp.), daffodil (Narcissus sp.), morning glory (Petunia hybrida), carnation (Dianthus caryophyllus), lily (eg Lilium sp.), gladiolus (Gladiolus sp.), lily narcissus (Alstroemaria brasiliensis), anemone (eg Anemone bland), columbine (Aquilegia sp.), genus (eg chimney) , Aster carolinianus (such as Aster carolinianus), Jiuzhong (Bougainvillea sp.), Camellia (Camellia sp.), Campanula (Campanula sp.), Celosia (Celosia sp.), Cypress (Chamaecyparis sp.), Chrysanthemum ( Chrysanthemum sp.), clematis (Clematis sp.), primrose (Cyclamen sp.), freesia (e.g., Freesia refracta), and orchids of the family Orchidaceae.

According to the present invention, plants that can be treated to inhibit the removal of leaves, flowers and fruits include cotton (Gossypium spp.), apple, pear, cherry (Prunus avium), walnut (Carvaillinoensis), grape (Vitis vinifera), olive ( For example, dormant seedlings of Olea europaea), coffee (Cofffea arabica), bean (Phaseolus vulgaris) and weeping fig (Ficus benjamina) and many fruit trees including apples, ornamental plants, shrubs and tree seedlings.

In addition, according to the present invention, shrubs that can be treated to inhibit leaf loss include Ligustrum sp., Photina sp., Ilex sp., ferns of the family Water keelaceae, Schefflera sp. sp.), evergreen (Aglaonema sp.), cotoneaster (Cotoneaster sp.), barberry (Berberris sp.), red bayberry (Myrica sp.), arboria (Abelia sp.), acacia (Acacia sp.) , and pineapple (Bromeliades) of the family Bromeliaceae.

According to the present invention, the foaming component is used to control the rate of decomposition of the plant ethylene binding site blocking agent in aqueous solution. Any reaction mixture that can induce foaming efficacy can be used in the present invention. Preferred embodiments of the foaming composition of the present invention include mildly basic compounds and mildly acidic compounds that are solid at normal temperatures. A mildly basic compound reacts with a mildly acidic compound in a solvent to produce carbon dioxide gas.

According to the present invention, the ratio of mildly basic compound to mildly acidic compound is from about 9:1 to about 1:1. The ratio is preferably about 4:1.

Preferred examples of mild basic compounds are NaHCO ₃ , KHCO ₃ , CaCO ₃ , Na ₂ CO ₃ , K ₂ CO ₃ , NaKCO ₃ and sodium glycine carbonate, with NaHCO ₃ being more preferred.

Preferred specific examples of mildly acidic compounds are tartaric acid, citric acid, fumaric acid, salicylic acid, oxalic acid, succinic acid, maleic acid, malic acid, glycolic acid, ornithic acid and gluconic acid, and Malic acid is even better.

According to the present invention, dosages for blocking ethylene binding sites in plants are from about 0.01% to about 0.5%. Preferably, this amount is from about 0.05% to about 0.24%.

All carriers and excipients known in the formulation of tablets are suitable for use in the present invention. Preferred specific examples of carriers and excipients include, but are not limited to, glyceryl/polyethylene glycol behenate.

The main advantage of the dosage form of the present invention is that it provides an effective and truly beneficial dosage form for non-technical customers, florists and wholesalers. The effervescent tablet reduces the disadvantages of the mixing process associated with the powder form.

The invention further provides a process for preparing the tablet of the invention. All customary methods can be used by those skilled in the art for the preparation of tablet formulations for the preparation of tablets according to the invention.

In accordance with the present invention, the conventional method of preparing the patented tablets involves mixing the ingredients, feeding the mixed powder into a die, and compressing the die into a dosage form at a pressure of about 5 to about 8 kg/cm2.

The tablet of the present invention can be made into a suitable dosage form for easy administration. For good protection during storage and transportation, the tablet of the present invention can be packaged in plastic blister packs at a low relative humidity of eg less than 30%, or can be packaged in aluminum foil.

Another specific embodiment of the present invention is a method for inhibiting plant ethylene response. This method involves contacting the effervescent tablet of the present invention with a solvent. Agents that block ethylene binding sites in plants are released from the tablet into the air by foaming and then come into contact with the plants.

The foaming action of the present invention facilitates the rupture of the tablet in aqueous solution, thereby facilitating the release of the blocking agent into the treated environment. In addition, the convective force of the bubbling gas in the aqueous solution provides the mixing effect required for uniform dissolution and release of the blocking agent into the environment.

According to the present invention, solvents used herein include, but are not limited to, water and dilute alkaline solutions.

Without further elaboration, one skilled in the art can, using the above disclosure and the following examples, utilize the present invention to its fullest extent. The following examples are provided only to illustrate how a person skilled in the art can implement the claimed method and do not limit the remaining disclosure in any way.

Example 1

tablet preparation

The following general procedure can be used to prepare tablets. Generally, these steps are performed in a controlled environment at low relative humidity, eg, less than 30%, and a temperature of 25°C. All ingredients are evenly mixed. The powder mixture is then compressed at a pressure of about 8 kg/cm ² using a tablet press equipped with dies of the specified size and shape. The tablets are then inspected and stored at low relative humidity followed by packaging in plastic blister packs or aluminum foil.

Example 2

comparative test

A. Non-foaming methylcyclopropene tablets

Get 10 grams of 1-methylcyclopropene powder ( ^AnsiP® , Litong Enterprise Co., Ltd., Taipei, Taiwan, the Republic of China) ( ^AnsiP® from Lytone Enterprise, Inc.Taipei, Taiwan, ROC) and prepare tablets according to the method of the above-mentioned example agent. Each tablet contains 0.5 to 1 gram of 1-methylcyclopropene powder. A small amount of lubricant is required to prevent the tablet from sticking to the die. Two forms of tablets were manufactured for this trial. One also contains a bulking agent, the other does not. The finished tablet is dropped into water or a dilute alkaline solution to test its solubility. Tablet cracking and dissolution was observed to be very slow, even for tablets containing bulking agents. After 4 hours, they were still not fully dispersed or dissolved. Therefore, tablet forms made from 1-methylcyclopropene powder are not satisfactory without the use of effervescent agents.

B. Effervescent 1-methylcyclopropene tablet

The 1-methylcyclopropene powder was prepared into a foam tablet, which contained 40% by weight of NaHCO ₃ , 10% malic acid and 50% of the 1-methylcyclopropene powder produced by the above method. Each tablet weighs from 0.5 to 2 grams, depending on the size of the mold used. When this effervescent tablet is dropped into water, it fizzes immediately and completely dissolves in water within 60 minutes.

Example 3

Dispensing of tablets

Tablet of the present invention can be allocated according to the following:

Formula A

Ingredients per tablet

1-methylcyclopropene powder 500mg

(contains 0.1 to 0.5% 1-methylcyclopropene,

The rest are inert carriers)

_NaHCO3 400 mg

Malic acid 100mg

Glyceryl/Polyethylene Glycol Behenate 50 mg

Claims (15)

1. A foaming tablet, which comprises a medicament for blocking ethylene binding sites in plants and foaming components, mixed with one or more acceptable carriers and/or excipients. 2. The tablet as claimed in claim 1, wherein the medicament of blocking plant ethylene reaction is selected from: cyclopropene, 1-methylcyclopropene, 3,3-dimethylcyclopropene, methylene cyclopropene Propane, diazocyclopentadiene, trans-cyclooctene, cis-cyclooctene and 2,5-protobornadiene and their derivatives, and mixtures thereof. 3. The tablet according to claim 2, wherein the agent for blocking ethylene binding sites in plants is 1-methylcyclopropene. 4. The tablet as claimed in claim 1, wherein said effervescent component comprises a mildly basic compound and a mildly acidic compound which are solid at normal temperature. 5. The tablet as claimed in claim 4, wherein said mild alkaline compound is selected from the group consisting of: NaHCO ₃ , KHCO ₃ , CaCO ₃ , Na ₂ CO ₃ , K ₂ CO ₃ , NaKCO ₃ and sodium glycine carbonate , and mixtures thereof. 6. The tablet of claim 4, wherein said mild acidic compound is selected from the group consisting of: tartaric acid, citric acid, fumaric acid, salicylic acid, oxalic acid, succinic acid, malic acid, maleic acid , glycolic acid, ornithic acid, gluconic acid and mixtures thereof. 7. The tablet as claimed in claim 1, wherein the dosage of said drug for blocking ethylene binding site in plants is 0.01% to 0.5%. 8. The tablet as claimed in claim 7, wherein the amount of the drug for blocking ethylene binding sites in plants is 0.05% to 0.24%. 9. The tablet of claim 4, wherein the ratio of the mildly basic compound to the mildly acidic compound is 9:1 to 1:1. 10. The tablet of claim 9, wherein the ratio of mildly basic compound to mildly acidic compound is 4:1. 11. The tablet according to any one of claims 1 to 3, wherein the agent for blocking ethylene binding sites in plants is released in a gaseous state. 12. A method of preparing a tablet as claimed in claim 1, which comprises mixing an agent for blocking ethylene binding sites in plants, a foaming component and one or more acceptable carriers and/or excipients. 13. A method for inhibiting plant ethylene response, comprising contacting the foamed tablet as claimed in claim 1 with a solvent, and then through foaming, the tablet releases the medicament for blocking the plant ethylene binding site. 14. The method of claim 13, wherein said solvent is selected from water and dilute alkaline solutions. 15. The method of claim 14, wherein the solvent is water.