DESC:IMPROVED STABLE INSECTICIDAL COMPOSITION WITH BUILT-IN ADJUVANT

FIELD OF THE INVENTION
The present invention relates to an improved, stable insecticidal composition having safe and non-toxic built-in adjuvant. Further, the present invention also provides a method for preparation and use thereof.

BACKGROUND OF THE INVENTION
Crop yield loss due to pest damage is a significant challenge faced by farmers globally, with estimates indicating that about 20% to 40% of global crop production is lost annually to pests. It is indispensable to mitigate these losses, effective formulations play an effective role in controlling pests, dangerous insects, and plant diseases that negatively affect agricultural productivity. The application of appropriate and efficient insecticidal formulation plays a critical role in reducing pest populations and ensuring optimal productions in agriculture fields.

Effective and stable insecticidal formulations should ensure proper distribution of the active ingredient to targeted pest or area. The efficacy of such formulations hinges on their ability to evenly disperse insecticides, thereby maximizing the utilization of amounts of active ingredient used. Moreover, there are environmental concerns, particularly due to the release of volatile organic compounds (VOCs) into the atmosphere, necessitate a re-evaluation of formulation components to mitigate pollution.

Several types of pesticide formulations are prevalent, with each having its advantages and disadvantages. Further, Water Dispersible Granules (WDG/WG) and Soluble Granules (SG) are widely used, however, WDG/WG have challenges such as high manufacturing costs, potential poor water dispersion, issues with tank mix compatibility, and environmental sensitivity. Furthermore, incorporation of bio-enhancing adjuvants into WG formulations can be challenging, with complex manufacturing process require high capital investment and longer production timelines. WG formulations necessitate higher melting points and are more susceptible to environmental factors such as moisture, which may affect the quality.

Conversely, SG are solid formulations that dissolve in water to form a true solution of the active ingredient. SG formulations helps to eliminate organic solvents that are often hazardous and contribute to health issues, such as eye irritation. SG formulations may be preferred due to ease of handling, minimal dust generation, and environmental friendliness. Further, SG formulations have uniformity, ease of measurement, and reduced environmental impact through the use of biologically derived fillers and minimal VOC emissions. SG formulations may deliver high concentrations of active ingredients, making them cost-effective formulation type. Despite the advantages of SG formulations, they often require and utilize excipients that are expensive, complex, and potentially hazardous, increasing productions costs and posing risks to human health and the environment. Further, the excipient used may adversely affect crops and beneficial organisms. Additionally, pesticide drift that is unintended air borne movement of pesticides spray droplets, poses risks to human health, wildlife, and the environment.

Therefore, there is need for an improved SG formulation having non-toxic adjuvants and excipients, with improved stability, and environmental safety of the insecticidal formulation. Further, the improved SG formulation should not maintain the benefits of traditional SG formulations, such as ease of use, uniformity, and effective delivery of active ingredients, while significantly reducing the environmental impact and health risks associated with conventional excipients.

Therefore, the present invention aims to overcome the aforementioned drawbacks by providing an improved insecticidal composition that is stable, safe, economical, and eco-friendly.

OBJECTIVES OF THE INVENTION
The primary objective of the invention is to provide an improved, stable insecticidal composition.

Another objective of the present invention is to provide a stable insecticidal composition comprising a compound of formula I:

Another objective of the present invention is to provide a method for preparing stable insecticidal composition.

Another objective of the present invention is to provide an insecticidal composition comprising a compound of formula I and at least one non-toxic built-in adjuvant.

Yet another objective of the present invention is to provide an improved and economical method for preparing a stable insecticidal composition.

Yet another objective of the present invention is to provide a stable insecticidal composition that increases the crop yield.

Yet another objective of the present invention is to provide a stable insecticidal composition that promotes plant health.

Another objective of the present invention is to provide a stable insecticidal composition with broad spectrum of control.

The present invention may achieve some or all of these and other objectives of the invention.

SUMMARY OF THE INVENTION

The following presents a simplified summary of the invention to provide a basic understanding of some aspects of the invention. This summary is not an extensive overview of the present invention. It is not intended to identify the key/critical elements of the invention or to delineate the scope of the invention. Its sole purpose is to present some concept of the invention in a simplified form as a prelude to a more detailed description of the invention presented later.

Accordingly, the present invention provides a stable insecticidal composition comprising at least one systemic insecticide.

In an aspect of the present invention, the stable insecticidal composition comprises of a compound of formula I:

wherein, X = CF3 and A = , and at least one non-toxic built-in adjuvant.

In an aspect, the present invention provides a stable insecticidal composition comprising:
a) a compound of formula I;

b) a built-in adjuvant;
c) a surface active agent; and
d) one or more agriculturally acceptable excipients.

In another aspect, the stable insecticidal composition comprises:
a) a compound of formula I in an amount in the range of 1 to 60% by weight;
b) a non-toxic built-in adjuvant in an amount in the range of 1 to 10% by weight;
c) a surface active agent in an amount in the range of 1 to 15% by weight; and
d) one or more agriculturally acceptable excipients.

In an aspect, the non-toxic built-in adjuvant may be selected from taurate compound, N-methyltaurine, Sodium N-methyltaurinate.

In further aspect, the non-toxic built-in adjuvant may be a taurate compound.

In another preferred aspect, the taurate compound is a compound of formula II.

In an aspect, the surface active agent may be selected from but not limited to anionic surfactant of naphthalene sulphonic acid condensate, sodium poly naphthalene formaldehyde sulfonate.
In yet another aspect, the surface active agent is Sodium dibutylnaphthalenesulphonate.

In another preferred aspect of the present invention, the stable insecticidal composition comprises of:
a) a compound of formula I;

b) a taurate compound of formula II;
c) a surface active agent; and
d) one or more agriculturally acceptable excipients.

In another aspect, the present invention provides a method for preparing stable insecticidal composition.

In another aspect of the present invention, the stable insecticidal composition controls various pests in field crops.

In another aspect, the stable insecticidal composition of the present invention comprises one or more agriculturally acceptable excipient selected from the group comprising of carrier(s), surfactant(s), binder(s), surface-active agent(s), disintegrating agent(s), dispersants or dispersing agent(s), wetting agent(s), pH modifier(s), biocide(s), preservative(s), anti-freezing agent(s), defoamer(s), solvents, water soluble polymer, and/or stabilizer(s) or a combination thereof. Additional components may also be included, e.g., protective colloids; adhesives; thickeners; stabilizers; etc. More generally, the active materials may be combined with any solid or liquid additive, which complies with usual formulation techniques.

In another embodiment of the present invention, the stable insecticidal composition may be formulated as Capsule suspension (CS), Dispersible concentrate (DC), Powder for dry seed treatment (DS), Emulsifiable concentrate (EC), Emulsifiable granule (EG), Emulsion water-in- oil (EO), Emulsifiable powder (EP), Emulsion for seed treatment (ES), Emulsion oil-in-water (EW), Flowable concentrate for seed treatment (FS), Granules (GR), Micro-emulsion (ME), Oil dispersion (OD), Oil miscible flowable concentrate (OF), Oil miscible liquid (OL), Oil dispersible powder (OP), Suspension concentrate (SC), Suspension concentrate for direct application (SD), Suspo-emulsion (SE), Water soluble granule (SG), Soluble concentrate (SL), Spreading oil (SO), Water soluble powder (SP), Water dispersible granules (WG), Wettable powder (WP), Water dispersible powder for slurry seed treatment (WS), a mixed formulation of CS and SC (ZC) or a mixed formulation of CS and SE (ZE), a mixed formulation of CS and EW (ZW).

In another aspect, the present invention provides a method for preparing a stable insecticidal composition comprising the steps of (a) charging active, non-toxic built-in adjuvant and other excipients into a pre-blender and homogenizing; (b) milling the mixture of step (a) for particle size reduction; (c) transferring the milled mass of step (b) into a post mixing vessel and mixing for 20 minutes; (d) adding water into the mass of step (c) under continuous mixing to form a dough for granulation; (e) initiating cylindrical granulation to obtain wet granules; and (f) drying wet granules of step (e) to obtain dry granules.

In another aspect, the present invention provides an improved insecticidal composition that is stable, environmentally safe and possesses enhanced efficacy for broad spectrum control of pests and diseases.

Other aspects, advantages, and salient features of the invention will become apparent to those skilled in the art from the following detailed description, which, details the invention in different embodiments.

DETAILED DESCRIPTION OF THE INVENTION
The definitions provided herein below for the terminologies used in the present disclosure are for illustrative purpose only and in no manner limit, the scope of the present invention disclosed in the present disclosure.

All technical and scientific phrases or terms used here have the same meanings as those that a person who is skilled in the field of study of the present invention would understand. Although other processes and materials similar to or equivalent, to those described herein may be used in the practice of the present invention, the preferred materials and process are described herein.

It is to be noted that, as used in the specification the singular forms “a”, “an” and “the” include plural referents unless the context clearly dictates otherwise. It should also be noted that the term “or” is generally employed in its sense including “and/or” unless the content clearly dictates otherwise.

The expression of various quantities in terms of “% w/w” or “%” means the percentage by weight, relative to the weight of the total solution or composition unless otherwise specified.

The term “active ingredient” (a.i.) or “active agent” or “actives” used herein refers to that component of the composition responsible for control and killing of pests/insects.

The use of terms “including,” “comprising,” or “having” and variations thereof herein; are meant to encompass the items listed thereafter and equivalents thereof as well as additional items. Further, the use of the expression “at least” or “at least one” suggests the use of one or more elements or ingredients or quantities, as the use may be in the embodiment of the disclosure to achieve one or more of the desired objects or results. Furthermore, the term “may” be used herein in a permissive sense (i.e. meaning having the potential to), rather than the mandatory sense, (i.e. meaning must).

The term “formulation” and “composition” as used herein convey the same meaning and may be used interchangeably.

The term “crop” shall include a multitude of desired crop plants or an individual crop plant. The term “control” means to inhibit the ability of pests to survive, grow, feed and/or reproduce, or to limit the pests? related damage or loss in crop plants. To “control” pests may or may not mean killing the insects although, it may mean killing the pests.

As used herein, the term “insecticide”, refers to any chemical substance used to destroy/kill, inhibit or otherwise adversely affect the insect pests.

The term “process” and “method” as used herein convey the same meaning and may be used interchangeably.

According to the present invention, "increased yield" of a plant, in particular, of an agricultural, silvicultural and/ or horticultural plant means that the yield of a product of the respective plant is increased by a measurable amount over the yield of the same product of the plant produced under the same conditions, but without the application of composition according to the present invention.

Increased yield may be characterized by improved properties such as increased plant weight, increased plant height, increased biomass such as higher overall fresh weight (FW), increased number of flowers per plant, higher grain yield, more tillers or side shoots (branches), larger leaves, increased shoot growth, increased leaf area index.

Another indicator for the condition of the plant is the “enhanced quality” of a plant and/or its products.

According to the present invention, enhanced quality means that certain plant characteristics, such as the content or composition of certain ingredients, are increased or improved by a measurable or noticeable amount over the same factor of the plant produced under the same conditions, but without the application of the composition of the present invention. Enhanced quality may be characterized, among others, by following improved properties of the plant or its product: increased nutrient content, increased protein content, increased content of fatty acids, increased metabolite content, increased carotenoid content, increased sugar content, increased amount of essential amino acids, improved nutrient composition, improved protein composition, the improved composition of fatty acids, improved metabolite composition, improved carotenoid composition, improved sugar composition, improved amino acids composition, improved or optimal fruit colour, improved leaf colour, higher storage capacity, higher process ability of the harvested products.

In an exemplary embodiment, the active insecticidal compound used in the present composition may comprise base or any salt form or ester form of the active which is known in the art.

An insecticidal composition, according to the present invention, comprises an effective amount of at least one insecticide and at least one non-toxic built-in adjuvant.

The term “plants” refers to all physical parts of a plant, including seeds, seedlings, saplings, roots, tubers, stems, stalks, foliage, and fruits. The term “locus” of a plant as used herein is intended to embrace the place on which the plants are growing, where the plant propagation materials of the plants are sown or where the plant propagation materials of the plants will be placed into the soil. The term “plant propagation materials” is understood to denote generative parts of a plant, such as seeds, vegetative materials such as cutting or tubers, roots, fruits, bulbs, rhizomes and parts of plants, germinated plants and young plants which are to be transplanted after germination or after emergence from the soil. These young plants may be protected before transplantation by total or partial treatment by immersion.

In accordance with an embodiment, the present invention provides a stable insecticidal composition comprising a compound of formula I:

wherein, X = CF3 and A = , and at least one non-toxic built-in adjuvant.

In another embodiment, the present invention composition comprises:
a) a compound of formula I;

b) a non-toxic built-in adjuvant;
c) a surface active agent; and
d) one or more agriculturally acceptable excipients.

In another embodiment, the stable insecticidal composition comprises:
a) a compound of formula I in an amount in the range of 1 to 60% by weight;
b) a non-toxic built-in adjuvant in an amount in the range of 1 to 10% by weight;
c) a surface active agent in an amount in the range of 1 to 15% by weight; and
d) one or more agriculturally acceptable excipients.

In another embodiment of the present invention, the non-toxic built-in adjuvant is a taurate compound.

In another embodiment of the present invention, the stable insecticidal composition comprises of:
a) a compound of formula I in an amount in the range of 1 to 60% by weight;
b) a taurate compound in an amount in the range of 1 to 10% by weight;
c) a surface active agent in an amount in the range of 1 to 15% by weight; and
d) one or more agriculturally acceptable excipients.

The stable insecticidal composition may comprise of non-toxic built-in adjuvant selected from taurate compound, N-methyltaurine, Sodium N-methyltaurinate or any combination thereof.

In a preferred embodiment of the present invention, the taurate compound is a compound of formula II;

The Taurate compound of Formula II protects the compound of Formula I from morphological changes during the formulation's shelf life. The compound of Formula II also acts as a dispersing and wetting agent, which makes it a super-spreading agent and enhances the spreading of active ingredients on the crop. Additionally, it contributes to the long-lasting adhesion of the active ingredient on the leaf surface, promoting improved plant health. Compound II ensures superior leaf surface coverage, leading to prolonged residual control. This extended residual control is due to the agent's ability to enhance the uniformity of the spray solution application across the leaf. The improved spreading properties result in more efficient distribution and retention of the active ingredients, ultimately increasing the treatment's overall efficacy and duration.

In an embodiment of the present invention, the surface active agent may be selected from anionic surfactant of naphthalene sulphonic acid condensate, sodium poly naphthalene formaldehyde sulfonate, sodium dibutylnaphthalenesulphonate or any combination thereof.

In yet another embodiment of the present invention, the surface active agent is sodium dibutylnaphthalenesulphonate.

In another preferred embodiment of the present invention, the stable insecticidal composition comprises of:
a) a compound of formula I;

b) a taurate compound of formula II;
c) a surface active agent; and
d) one or more agriculturally acceptable excipients.

In another embodiment of the present invention, the compound of formula I has IUPAC name N-(cyanomethyl)-4-(trifluoromethyl) pyridine-3-carboxamide.

In another embodiment of the present invention, the compound of formula II has IUPAC name sodium methyl oleoyl taurate.

In another exemplary embodiment, the stable insecticidal composition of the present invention may be formulated as Capsule suspension (CS), Dispersible concentrate (DC), Powder for dry seed treatment (DS), Emulsifiable concentrate (EC), Emulsifiable granule (EG), Emulsion water-in- oil (EO), Emulsifiable powder (EP), Emulsion for seed treatment (ES), Emulsion oil-in-water (EW), Flowable concentrate for seed treatment (FS), Granules (GR), Micro-emulsion (ME), Oil dispersion (OD), Oil miscible flowable concentrate (OF), Oil miscible liquid (OL), Oil dispersible powder (OP), Suspension concentrate (SC), Suspension concentrate for direct application (SD), Suspo-emulsion (SE), Water soluble granule (SG), Soluble concentrate (SL), Spreading oil (SO), Water soluble powder (SP), Water dispersible granules (WG), Wettable powder (WP), Water dispersible powder for slurry seed treatment (WS), a mixed formulation of CS and SC (ZC) or a mixed formulation of CS and SE (ZE), a mixed formulation of CS and EW (ZW).

In a preferred embodiment, the stable insecticidal composition of the present invention is formulated as a Soluble Granule (SG).

In another embodiment of the present invention, the insecticidal composition may comprise one or more agriculturally acceptable excipients selected from the group comprising of carrier(s), surfactant(s), binder(s), surface-active agent(s), disintegrating agent(s), dispersants or dispersing agent(s), adjuvants, non-toxic built-in adjuvants, wetting agent(s), pH modifier(s), thickener(s), biocide(s), preservative(s), anti-freezing agent(s), defoamer(s), solvents, water soluble polymer, and/or stabilizer(s) or a combination thereof.

Dispersing cum wetting agent may be selected from but not limited to residues (petroleum), catalytic reformer fractionator, sulfonated, polymers with formaldehyde, sodium salts, sulfonic acids, C14-16-alkane hydroxy and C14-16-alkene, sodium salts, Benzensulfonic acid, hydroxy-, polymer with formaldehyde, phenol and urea, sodium salt, Sodium dibutyl naphthalene sulphonate, olefin sulfonate, Sodium Poly Naphthalene Formaldehyde Sulfonate, and sodium methyl oleate taurate, or any combination thereof.

In one exemplary embodiment of the present invention, dispersing cum wetting agent is present in the range of 1-10% by weight of the total composition.

A surface active agent may be selected from the group consisting of salts of dodecylbenzene sulphonate, e.g. Ca-salts or amine salts, and sulphonates of other C11-C16 alkylbenzenes, sodium dibutylnaphthalenesulphonate, alkylether sulphates, alkylphenoletherphosphates and ester phosphates; non-ionic surfactants such as alkoxylated alcohols and alkylphenols, ethoxylated fatty acids, ethoxylated vegetable oils, e.g. ethoxylated castor oil, fatty acid esters, e.g. of sorbitol, and their ethoxylated derivatives, ethoxylated amines, and condensates of glycerol; and catanionic emulsifiers such as a cationic amine, optionally in combination with an alkylsulphonate or ether sulphonate or ether phosphate, alkoxylated alcohols; alkoxylated alkylphenols; ethoxylated fatty acids; ethoxylated vegetable oils; ethoxylated tristyrylphenol; fatty acid esters of sorbitol and ethoxylated derivatives thereof; ethoxylated amines and condensates of glycerol; sulfonated alkylbenzenes in the range C11-C16 and salts thereof; alkylether sulphates; alkyletherphosphates; alkylphenoletherphosphates; or combinations thereof; salts of phosphate esters of ethoxylated tristyrylphenol; salts of sulphated ethers of ethoxylated tristyrylphenol; or a catanionic system, wherein a cationic amine is present in combination with an alkylsulphonate, an alkylethersulphonate, an ether sulphate, or an ether phosphate such as an alkyletherphosphate, nonylphenol polyethoxy ethanols, castor oil polyglycol ethers, polyadducts of ethylene oxide and polypropylene, tributyl phenoxy polyethoxy ethanol, octyl phenoxy polyethoxy ethanol or combination thereof.

In a preferred embodiment of the present invention, surface active agent is sodium dibutylnaphthalenesulphonate, present in the range of 1 – 20% by weight of the total composition.

Anti-foam chemicals are frequently added during the manufacture stage or before filling into bottles to reduce the tendency to foam. Anti-foam agents are classified into two types, silicones and non-silicones.

Anti-foaming agent may be selected from the group consisting of Silicon Defoamer SAG 1572, polydimethylsiloxanes and other silicones derivative.

Antifoaming agents may be selected from the group comprising of silicon emulsion based anti-foam agents, siloxane polyalkyleneoxide, trisiloxane ethoxylates and mixtures thereof.

In another exemplary embodiment of the present invention, defoamers may be present in the range of 0.1 - 2.0% by weight of the total composition.

In an exemplary embodiment of the present invention, the carriers may be selected from the group comprising of lactose present in the “Quantum Satis” i.e., Q.S quantity.

In another embodiment, the present invention provides a method for preparation of stable insecticidal composition comprising the steps of (a) charging active, non-toxic built-in adjuvant and other excipients into a pre-blender and homogenizing; (b) milling the mixture of step (a) for particle size reduction; (c) transferring the milled mass of step (b) into a post mixing vessel and mixing for 20 minutes; (d) adding water into the mass of step (c) under continuous mixing to form a dough for granulation; (e) initiating cylindrical granulation to obtain wet granules; and (f) drying wet granules of step (e) to obtain dry granules.

In another embodiment of the present invention, the particle size in step (b) is below 50 microns.

In another embodiment of the present invention, the granules are dried in step (f) at a temperature in the range of 50 to 60°C.

EXAMPLES
Below are the various examples for preparing different formulations according to the present invention. However, the below examples are given solely for the purpose of illustration and are not to be construed as limitations of the present invention, as many variations thereof are possible without departing from the spirit and scope of the invention.

Example 1:

Table 1: Soluble Granule (SG) formulation of 50% Compound of formula I and 3% Compound of formula II
S. No. Ingredients Function Quantity In % W/W
1 Compound of formula I Active 50.00%
2 Silicon Defoamer SAG 1572 Anti-foaming agent 0.75%
3 Compound of formula II Dispersing cum wetting agent 3.00%
4 Sodium dibutylnaphthalenesulphonate Surface active agent 5.00%
5 Lactose mono hydrate Carrier QS

Preparation Process
Step I - Blending & Granulation:
(i) Charged all ingredients as specified above into pre-blender and mixed properly for 20 mins for homogeneous mixing;
(ii) Next, the mixture obtained was milled using an air jet mill to reduce particle size below 50 microns;
(iii) The milled mass was transferred into post mixing vessel and mixed for another 20 mins to ensure uniform consistency;
(iv) The water was added into the mass in next steps and mixed for 10 minutes to form a dough for granulation;
(v) Initiated the cylindrical granulation to obtain wet granules.
Step II – Drying of Granules
(vi) The wet granules were transferred into a dryer and dried at a temperature in the range of 50 – 60°C to obtain dry soluble granules,
(vii) Samples were drawn for analysis.

Table 2: Storage Stability Data
S. No. Test Parameters 0 day @ 25°C 14 days @ 25°C 14 days @ 54°C
1 Physical state Solid Solid Solid
2 Colour Beige Beige Beige
3 Odour Odourless Odourless Odourless
4 AI (active ingredient) 50.27 50.27 50.19
5 pH 1 % Aq. Solution 6.87 6.81 6.95
6 Solubility Cycle 15 Cycle 15 Cycle 18 Cycle
7 Moisture (%) 0.79 0.71 0.28
8 Wet Sieve (75µ) complies Complies complies
9 Foaming 70 ml 70 ml 75 ml
10 Degree of dissolution Maximum: 2 % after 5 minutes. 0.05% 0.11% 0.15%
11 Quality Qualified Qualified
Table 3: Shelf-life Stability Data
S. No. Test Parameters 1 Y
1 Physical state Solid
2 Colour Beige
3 Odour Odourless
4 AI (active ingredient) 50.14
5 pH 1 % Aq. Solution 6.57
6 Solubility Cycle 28 Cycle
7 Moisture (%) 0.75
8 Wet Sieve (75µ) Complies
9 Foaming 75 ml
10 Degree of dissolution
Maximum: 2 % after 5 minutes. 0.96% after 5 min.
11 Quality Qualified

The above composition exhibits excellent accelerated storage stability, showing positive results for all parameters after 14 days at 25°C and after 14 days at 54°C under accelerated heat storage conditions (AHS). Furthermore, the composition exhibits stability even after 1 year of storage under room temperature conditions, with no significant changes in its properties, demonstrating its reliability and long-term stability.

Example 2:

Table 4: Soluble Granule (SG) formulation of 50% Compound of formula I and 5% Compound of formula II
S. No. Ingredients Function Quantity In % W/W
1 Compound of formula I Active 50.00%
2 Silicon Defoamer SAG 1572 Anti-foaming agent 0.82%
3 Compound of formula II Dispersing cum wetting agent 5.00%
4 Sodium dibutylnaphthalenesulphonate Surface active agent 6.20%
5 Lactose mono hydrate Carrier QS

Process for preparation of the composition
Step I - Blending & Granulation:
(i) Charged all ingredients as specified above into pre-blender and mixed properly for 20 mins to homogenize;
(ii) Next, the mixture obtained was milled using an air jet mill to reduce particle size below 50 microns;
(iii) The milled mass was transferred into post mixing vessel and mixed for another 20 minutes to ensure uniform consistency;
(iv) The water was added into the mass in next steps and mixed for 10 minutes to form a dough for granulation;
(v) Initiated the cylindrical granulation to obtain wet granules;
Step II – Drying of Granules
(vi) The wet granules were transferred into a dryer and dried at a temperature in the range of 50 – 60°C to obtain dry soluble granules,
(vii) Samples were drawn for analysis.

Table 5: Storage Stability Data
S. No. Test Parameters 0 day @ 25°C 14 days @ 25°C 14 days @ 54°C
1 Physical state Solid Solid Solid
2 Colour Beige Beige Beige
3 Odour Odourless Odourless Odourless
4 AI (active ingredient) 50.26 50.26 50.18
5 pH 1 % Aq. Solution 6.86 6.83 6.94
6 Solubility Cycle 15 Cycle 15 Cycle 17 Cycle
7 Moisture (%) 0.78 0.72 0.27
8 Wet Sieve (75µ) complies Complies complies
9 Foaming 70 ml 70 ml 75 ml
10 Degree of dissolution Maximum: 2 % after 5 minutes. 0.06% 0.12% 0.16%
11 Quality Qualified Qualified

Table 6: Shelf-life Stability Data
S. No. Test Parameters 1 Y
1 Physical state Solid
2 Colour Beige
3 Odour Odourless
4 AI (active ingredient) 50.15
5 pH 1 % Aq. Solution 6.58
6 Solubility Cycle 28 Cycle
7 Moisture (%) 0.76
8 Wet Sieve (75µ) Complies
9 Foaming 75 ml
10 Degree of dissolution
Maximum: 2 % after 5 minutes. 0.96% after 5 min.
11 Quality Qualified

Example 3:

Table 7: Soluble Granule (SG) formulation of 50% Compound of formula I and 7% Compound of formula II
S. No. Ingredients Function Quantity In % W/W
1 Compound of formula I Active 50.00%
2 Silicon Defoamer SAG 1572 Anti-foaming agent 0.77%
3 Compound of formula II Dispersing cum wetting agent 7.00%
4 Sodium dibutylnaphthalenesulphonate Surface active agent 8.00%
5 Lactose mono hydrate Carrier QS

Process for preparation of the composition
Step I - Blending & Granulation:
(i) Charged all ingredients as specified above into pre-blender and mixed properly for 20 mins to homogenize;
(ii) Next, the mixture obtained was milled using an air jet mill to reduce particle size below 50 microns;
(iii) The milled mass was transferred into post mixing vessel and mixed for another 20 mins to ensure uniform consistency;
(iv) The water was added into the mass in next steps and mixed for 10 mins to form a dough for granulation;
(v) Initiated the cylindrical granulation to obtain wet granules;
Step II – Drying of Granules
(vi) The wet granules were transferred into a dryer and dried at a temperature in the range of 50 – 60°C to obtain dry soluble granules,
(vii) Samples were drawn for analysis.

Table 8: Storage Stability Data
S. No. Test Parameters 0 day @ 25°C 14 days @ 25°C 14 days @ 54°C
1 Physical state Solid Solid Solid
2 Colour Beige Beige Beige
3 Odour Odourless Odourless Odourless
4 AI (active ingredient) 50.29 50.29 50.18
5 pH 1 % Aq. Solution 6.88 6.82 6.96
6 Solubility Cycle 15 Cycle 15 Cycle 18 Cycle
7 Moisture (%) 0.78 0.73 0.27
8 Wet Sieve (75µ) Complies Complies Complies
9 Foaming 70 ml 70 ml 75 ml
10 Degree of dissolution Maximum: 2 % after 5 minutes. 0.05% 0.15% 0.15%
11 Quality Qualified Qualified

Table 9: Shelf-life Stability Data
S. No. Test Parameters 1 Y
1 Physical state Solid
2 Colour Beige
3 Odour Odourless
4 AI (active ingredient) 50.17
5 pH 1 % Aq. Solution 6.58
6 Solubility Cycle 28 Cycle
7 Moisture (%) 0.75
8 Wet Sieve (75µ) Complies
9 Foaming 75 ml
10 Degree of dissolution
Maximum: 2 % after 5 minutes. 0.96% after 5 min.
11 Quality Qualified

Example 4:
Table 10: Soluble Granule (SG) formulation of 25% Compound of formula I and 3% Compound of formula II
S. No. Ingredients Function Quantity In % W/W
1 Compound of formula I Active 25.00%
2 Silicon Defoamer SAG 1572 Anti-foaming agent 0.76%
3 Compound of formula II Dispersing cum wetting agent 3%
4 Sodium dibutylnaphthalenesulphonate Surface active agent 12.00%
5 Lactose mono hydrate Carrier QS

Process for preparation of the composition
Step I - Blending & Granulation:
(i) Charged all ingredients as specified above into pre-blender and mixed properly for 20 mins to homogenize;
(ii) Next, the mixture obtained was milled using an air jet mill to reduce particle size below 50 microns;
(iii) The milled mass was transferred into post mixing vessel and mixed for another 20 mins to ensure uniform consistency;
(iv) The water was added into the mass in next steps and mixed for 10 mins to form a dough for granulation;
(v) Initiated the cylindrical granulation to obtain wet granules;
Step II – Drying of Granules
(vi) The wet granules were transferred into a dryer and dried at a temperature in the range of 50 – 60°C to obtain dry soluble granules,
(vii) Samples were drawn for analysis.

Table 11: Storage Stability Data
S. No. Test Parameters 0 day @ 25°C 14 days @ 25°C 14 days @ 54°C
1 Physical state Solid Solid Solid
2 Colour Beige Beige Beige
3 Odour Odourless Odourless Odourless
4 AI (active ingredient) 25.27 25.28 25.19
5 pH 1 % Aq. Solution 6.85 6.84 6.93
6 Solubility Cycle 15 Cycle 15 Cycle 17 Cycle
7 Moisture (%) 0.78 0.72 0.27
8 Wet Sieve (75µ) complies Complies complies
9 Foaming 70 ml 70 ml 75 ml
10 Degree of dissolution Maximum: 2 % after 5 minutes. 0.07% 0.13% 0.17%
11 Quality Qualified Qualified

Table 12: Shelf-life Stability Data
S. No. Test Parameters 1 Y
1 Physical state Solid
2 Colour Beige
3 Odour Odourless
4 AI (active ingredient) 25.16
5 pH 1 % Aq. Solution 6.56
6 Solubility Cycle 28 Cycle
7 Moisture (%) 0.76
8 Wet Sieve (75µ) Complies
9 Foaming 75 ml
10 Degree of dissolution
Maximum: 2 % after 5 minutes. 0.96% after 5 min.
11 Quality Qualified

Example 5:

Table 13: Soluble Granule (SG) formulation of 25% Compound of formula I and 5% Compound of formula II
S. No. Ingredients Function Quantity In % W/W
1 Compound of formula I Active 25.00%
2 Silicon Defoamer SAG 1572 Anti-foaming agent 1.00%
3 Compound of formula II Dispersing cum wetting agent 5%
4 Sodium dibutylnaphthalenesulphonate Surface active agent 12.00%
5 Lactose mono hydrate Carrier QS

Process for preparation of the composition
Step I - Blending & Granulation:
(i) Charged all ingredients as specified above into pre-blender and mixed properly for 20 mins to homogenize;
(ii) Next, the mixture obtained was milled using an air jet mill to reduce particle size below 50 microns;
(iii) The milled mass was transferred into post mixing vessel and mixed for another 20 mins to ensure uniform consistency;
(iv) The water was added into the mass in next steps and mixed for 10 mins to form a dough for granulation;
(v) Initiated the cylindrical granulation to obtain wet granules;
Step II – Drying of Granules
(vi) The wet granules were transferred into a dryer and dried at a temperature in the range of 50 – 60°C to obtain dry soluble granules,
(vii) Samples were drawn for analysis.

Table 14: Storage Stability Data
S. No. Test Parameters 0 day @ 25°C 14 days @ 25°C 14 days @ 54°C
1 Physical state Solid Solid Solid
2 Colour Beige Beige Beige
3 Odour Odourless Odourless Odourless
4 AI (active ingredient) 25.28 25.25 25.16
5 pH 1 % Aq. Solution 6.87 6.85 6.91
6 Solubility Cycle 15 Cycle 15 Cycle 17 Cycle
7 Moisture (%) 0.78 0.72 0.27
8 Wet Sieve (75µ) complies Complies complies
9 Foaming 70 ml 70 ml 75 ml
10 Degree of dissolution Maximum: 2 % after 5 minutes. 0.06% 0.12% 0.16%
11 Quality Qualified Qualified

Table 15: Shelf-life Stability Data
S. No. Test Parameters 1 Y
1 Physical state Solid
2 Colour Beige
3 Odour Odourless
4 AI (active ingredient) 25.17
5 pH 1 % Aq. Solution 6.58
6 Solubility Cycle 28 Cycle
7 Moisture (%) 0.77
8 Wet Sieve (75µ) Complies
9 Foaming 75 ml
10 Degree of dissolution
Maximum: 2 % after 5 minutes. 0.96% after 5 min.
11 Quality Qualified

Example 6:

Table 16: Soluble Granule (SG) formulation of 25% Compound of formula I and 7% Compound of formula II
S. No. Ingredients Function Quantity In % W/W
1 Compound of formula I Active 25.00%
2 Silicon Defoamer SAG 1572 Anti-foaming agent 0.76%
3 Compound of formula II Dispersing cum wetting agent 7.00%
4 Sodium dibutylnaphthalenesulphonate Surface active agent 10.00%
5 Lactose mono hydrate Carrier QS

Process for preparation of the composition
Step I - Blending & Granulation:
(i) Charged all ingredients as specified above into pre-blender and mixed properly for 20 mins to homogenize;
(ii) Next, the mixture obtained was milled using an air jet mill to reduce particle size below 50 microns;
(iii) The milled mass was transferred into post mixing vessel and mixed for another 20 mins to ensure uniform consistency;
(iv) The water was added into the mass in next steps and mixed for 10 mins to form a dough for granulation;
(v) Initiated the cylindrical granulation to obtain wet granules;
Step II – Drying of Granules
(vi) The wet granules were transferred into a dryer and dried at a temperature in the range of 50 – 60°C to obtain dry soluble granules,
(vii) Samples were drawn for analysis.

Table 17: Storage Stability Data
S. No. Test Parameters 0 day @ 25°C 14 days @ 25°C 14 days @ 54°C
1 Physical state Solid Solid Solid
2 Colour Beige Beige Beige
3 Odour Odourless Odourless Odourless
4 AI (active ingredient) 25.26 25.27 25.18
5 pH 1 % Aq. Solution 6.85 6.85 6.92
6 Solubility Cycle 15 Cycle 15 Cycle 17 Cycle
7 Moisture (%) 0.79 0.73 0.28
8 Wet Sieve (75µ) complies Complies complies
9 Foaming 70 ml 70 ml 75 ml
10 Degree of dissolution Maximum: 2 % after 5 minutes. 0.08% 0.14% 0.18%
11 Quality Qualified Qualified

Table 18: Shelf-life Stability Data
S. No. Test Parameters 1 Y
1 Physical state Solid
2 Colour Beige
3 Odour Odourless
4 AI (active ingredient) 25.18
5 pH 1 % Aq. Solution 6.57
6 Solubility Cycle 28 Cycle
7 Moisture (%) 0.77
8 Wet Sieve (75µ) Complies
9 Foaming 75 ml
10 Degree of dissolution
Maximum: 2 % after 5 minutes. 0.96% after 5 min.
11 Quality Qualified

Example 7:

Table 19: Soluble Granule (SG) formulation of 60% Compound of formula I and 3% Compound of formula II
S. No. Ingredients Function Quantity In % W/W
1 Compound of formula I Active 60.00%
2 Silicon Defoamer SAG 1572 Anti-foaming agent 0.78%
3 Compound of formula II Dispersing cum wetting agent 3%
4 Sodium dibutylnaphthalenesulphonate Surface active agent 4.00%
5 Lactose mono hydrate Carrier QS

Process for preparation of the composition
Step I - Blending & Granulation:
(i) Charged all ingredients as specified above into pre-blender and mixed properly for 20 mins to homogenize;
(ii) Next, the mixture obtained was milled using an air jet mill to reduce particle size below 50 microns;
(iii) The milled mass was transferred into post mixing vessel and mixed for another 20 mins to ensure uniform consistency;
(iv) The water was added into the mass in next steps and mixed for 10 mins to form a dough for granulation;
(v) Initiated the cylindrical granulation to obtain wet granules;
Step II – Drying of Granules
(vi) The wet granules were transferred into a dryer and dried at a temperature in the range of 50 – 60°C to obtain dry soluble granules,
(vii) Samples were drawn for analysis.

Table 20: Storage Stability Data
S. No. Test Parameters 0 day @ 25°C 14 days @ 25°C 14 days @ 54°C
1 Physical state Solid Solid Solid
2 Colour Beige Beige Beige
3 Odour Odourless Odourless Odourless
4 AI (active ingredient) 60.09 60.12 60.16
5 pH 1 % Aq. Solution 6.85 6.85 6.89
6 Solubility Cycle 15 Cycle 15 Cycle 17 Cycle
7 Moisture (%) 0.77 0.73 0.28
8 Wet Sieve (75µ) complies Complies complies
9 Foaming 70 ml 70 ml 75 ml
10 Degree of dissolution Maximum: 2 % after 5 minutes. 0.07% 0.14% 0.18%
11 Quality Qualified Qualified

Table 21: Shelf-life Stability Data
S. No. Test Parameters 1 Y
1 Physical state Solid
2 Colour Beige
3 Odour Odourless
4 AI (active ingredient) 60.14
5 pH 1 % Aq. Solution 6.55
6 Solubility Cycle 28 Cycle
7 Moisture (%) 0.77
8 Wet Sieve (75µ) Complies
9 Foaming 75 ml
10 Degree of dissolution
Maximum: 2 % after 5 minutes. 0.96% after 5 min.
11 Quality Qualified

Example 8:

Table 22: Soluble Granule (SG) formulation of 60% Compound of formula I and 5% Compound of formula II
S. No. Ingredients Function Quantity In % W/W
1 Compound of formula I Active 60.00%
2 Silicon Defoamer SAG 1572 Anti-foaming agent 0.72%
3 Compound of formula II Dispersing cum wetting agent 5%
4 Sodium dibutylnaphthalenesulphonate Surface active agent 4.90%
5 Lactose mono hydrate Carrier QS

Process for preparation of the composition
Step I - Blending & Granulation:
(i) Charged all ingredients as specified above into pre-blender and mixed properly for 20 mins to homogenize;
(ii) Next, the mixture obtained was milled using an air jet mill to reduce particle size below 50 microns;
(iii) The milled mass was transferred into post mixing vessel and mixed for another 20 mins to ensure uniform consistency;
(iv) The water was added into the mass in next steps and mixed for 10 mins to form a dough for granulation;
(v) Initiated the cylindrical granulation to obtain wet granules;
Step II – Drying of Granules
(vi) The wet granules were transferred into a dryer and dried at a temperature in the range of 50 – 60°C to obtain dry soluble granules,
(vii) Samples were drawn for analysis.

Table 23: Storage Stability Data
S. No. Test Parameters 0 day @ 25°C 14 days @ 25°C 14 days @ 54°C
1 Physical state Solid Solid Solid
2 Colour Beige Beige Beige
3 Odour Odourless Odourless Odourless
4 AI (active ingredient) 60.27 60.28 60.18
5 pH 1 % Aq. Solution 6.87 6.86 6.92
6 Solubility Cycle 15 Cycle 15 Cycle 17 Cycle
7 Moisture (%) 0.76 0.73 0.28
8 Wet Sieve (75µ) complies Complies complies
9 Foaming 70 ml 70 ml 75 ml
10 Degree of dissolution Maximum: 2 % after 5 minutes. 0.07% 0.13% 0.17%
11 Quality Qualified Qualified

Table 24: Shelf-life Stability Data
S. No. Test Parameters 1 Y
1 Physical state Solid
2 Colour Beige
3 Odour Odourless
4 AI (active ingredient) 60.15
5 pH 1 % Aq. Solution 6.57
6 Solubility Cycle 28 Cycle
7 Moisture (%) 0.76
8 Wet Sieve (75µ) Complies
9 Foaming 75 ml
10 Degree of dissolution
Maximum: 2 % after 5 minutes. 0.96% after 5 min.
11 Quality Qualified

Example 9:

Table 25: Soluble Granule (SG) formulation of 60% Compound of formula I and 7% Compound of formula II
S. No. Ingredients Function Quantity In % W/W
1 Compound of formula I Active 60.00%
2 Silicon Defoamer SAG 1572 Anti-foaming agent 0.75%
3 Compound of formula II Dispersing cum wetting agent 7.00%
4 Sodium dibutylnaphthalenesulphonate Surface active agent 4.8%
5 Lactose mono hydrate Carrier QS

Process for preparation of the composition
Step I - Blending & Granulation:
(i) Charged all ingredients as specified above into pre-blender and mixed properly for 20 mins to homogenize;
(ii) Next, the mixture obtained was milled using an air jet mill to reduce particle size below 50 microns;
(iii) The milled mass was transferred into post mixing vessel and mixed for another 20 mins to ensure uniform consistency;
(iv) The water was added into the mass in next steps and mixed for 10 mins to form a dough for granulation;
(v) Initiated the cylindrical granulation to obtain wet granules;
Step II – Drying of Granules
(vi) The wet granules were transferred into a dryer and dried at a temperature in the range of 50 – 60°C to obtain dry soluble granules,
(vii) Samples were drawn for analysis.

Table 26: Storage Stability Data
S. No. Test Parameters 0 day @ 25°C 14 days @ 25°C 14 days @ 54°C
1 Physical state Solid Solid Solid
2 Colour Beige Beige Beige
3 Odour Odourless Odourless Odourless
4 AI (active ingredient) 60.27 60.25 60.16
5 pH 1 % Aq. Solution 6.84 6.85 6.93
6 Solubility Cycle 15 Cycle 15 Cycle 17 Cycle
7 Moisture (%) 0.78 0.74 0.27
8 Wet Sieve (75µ) complies Complies complies
9 Foaming 70 ml 70 ml 75 ml
10 Degree of dissolution Maximum: 2 % after 5 minutes. 0.09% 0.13% 0.17%
11 Quality Qualified Qualified

Table 27: Shelf-life Stability Data
S. No. Test Parameters 1 Y
1 Physical state Solid
2 Colour Beige
3 Odour Odourless
4 AI (active ingredient) 60.17
5 pH 1 % Aq. Solution 6.56
6 Solubility Cycle 28 Cycle
7 Moisture (%) 0.78
8 Wet Sieve (75µ) Complies
9 Foaming 75 ml
10 Degree of dissolution
Maximum: 2 % after 5 minutes. 0.96% after 5 min.
11 Quality Qualified

Example 10: Present invention composition without Compound of formula II

Table 28: Soluble Granule (SG) formulation of 50% Compound of formula I without Compound of formula II
S. No. Ingredients Function Quantity In % W/W
1 Compound of formula I Active 50.00%
2 Silicon Defoamer SAG 1572 Defoamer 0.75%
3 Blend of sodium salt of alkylbenzene sulfonic acid and sodium sulfate Dispersing cum wetting agent 2.00%
4 Fatty acids, C14-26, sodium salts Surface active agent 4.00%
5 Lactose mono hydrate Carrier QS

Process for preparation of the composition: Introduced active into a pre-blender, followed by the addition of a blend of sodium salt of alkylbenzene sulfonic acid and sodium sulfate, Fatty acids, C14-26, sodium salts, and carrier. The contents were mixed thoroughly for 20 mins to obtain a homogeneous blend. Next, the mixture was milled using an air jet mill to reduce particle size below 50 microns. The milled mass was transferred to a post-mixing vessel and mixed for an additional 20 minutes to ensure uniform consistency. The water was added to the mass and mixed for 10 minutes to form a cohesive dough for granulation. However, the granules did not form upon initiating the cylindrical granulation.
Table 29: Storage Stability Data
S. No. Test Parameters 0 day @ 25°C 14 days @ 25°C 14 days @ 54°C
1 Physical state Solid Solid Solid
2 Colour Grey Grey Grey
3 Odour Odourless Odourless Odourless
4 AI (active ingredient) 50.29 50.29 45.05
5 pH 1 % Aq. Solution 6.88 6.82 6.96
6 Solubility Cycle 30 Cycle 30 Cycle 50 Cycle
7 Moisture (%) 0.78 0.73 0.27
8 Wet Sieve (75µ) Failed Failed Failed
9 Foaming 70 ml 70 ml 75 ml
10 Degree of dissolution Maximum: 2 % after 5 minutes. Disqualified Disqualified Disqualified
11 Quality Disqualified Disqualified

Table 30: Shelf-life Stability Data
S. No. Test Parameters 1 Y
1 Physical state Hazy Liquid
2 Colour Grey
3 Odour Odourless
4 AI Failed in Parameter Shelf-life Study
5 pH 1 % Aq. Solution
6 Solubility Cycle
7 Moisture (%)
8 Wet Sieve (75µ)
9 Foaming
10 Degree of dissolution
Maximum: 2 % after 5 minutes.
11 Quality

As evident from the above tables, the composition without compound of formula II exhibited poor stability results. Additionally, the composition did not perform well in the parameter study after one year of shelf storage. In contrast, the composition of the present invention demonstrated optimal long-term stability.

Example 11: Evaluation of present invention composition for bio-efficacy against whitefly (Bemisia tabaci) & Aphids (Aphis gossypii) in Cotton.

TRIAL 1: Field Experimental Details
Season Kharif 2023
Location Narsampet, Warangal, Telangana
Crop Cotton
Age of Crop 70 Days
Temperature Range during Trial 29-40°C
Variety Rasi (Magic RCH 386 BG II)
Single plot size 25 m2
Date of Transplanting/Sowing 16/07/2023
Number of applications 01
Date of application 25/09/2023
Target Pest Whitefly & Aphids
Method of application Foliar

Table 31: Treatment Details
S. No. Treatments Active Ingredient (AI) (gm/ha) Dose (gm or ml/ha)
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 75gm + 10.5gm 150gm
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 75gm + 7.5gm 150gm
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 75gm + 4.5gm 150gm
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 75gm 150gm
IE5 Compound of formula I 50% WG (Comparative Composition) 75gm 150gm
IE6 Compound of formula I 25% DC
(Comparative Composition) 75gm 300ml
IE7 Control - -

Observation & Methodology:
1. The experiment was laid out in randomized block design, replicating thrice with a single plot area of 25 m2. The test sample as per the treatment schedule were applied at pest appearance by using 500 litres of water per hectare using a knapsack sprayer.
2. A pre count was taken prior to the spray application. Pests count was recorded from (Area of observation) randomly selected five plants per replication from three leaves per plant.
3. Post-spray application pest count was recorded on the 3rd, 7th, and 10th days after spray application.
4. Per cent reduction in Pest Population was calculated by using a formula given by Henderson and Tilton as mentioned below:

Corrected Per cent control = 100 × (1- (Ta × Cb) / (Tb × Ca))
Where, Ta = Number of insects after treatment
Tb = Number of insects before treatment
Ca = Number of insects in untreated check after treatment
Cb = Number of insects in untreated check before treatment.

Table 32: Effectiveness of present invention composition against Cotton Whitefly (Bemisia tabaci)
S. No. Treatments Dose gm or ml/ha Effectiveness of Present invention composition (50% SG) against Cotton Whitefly
Corrected Per cent control
Pre count (Avg. pest count per leaf) 3 DAA 7 DAA 10 DAA
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 150gm 10.33 75.61 90.07 87.91
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 150gm 10.13 73.95 88.19 86.65
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 150gm 11.53 77.63 87.15 86.46
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 150gm 10.07 67.81 79.06 78.29
IE5 Compound of formula I 50% WG (Comparative Composition) 150gm 10.13 66.84 78.63 77.92
IE6 Compound of formula I 25% DC
(Comparative Composition) 300ml 10.20 70.59 82.68 81.12
IE7 Control - 10.20 0.00 0.00 0.00

The effectiveness of the present invention composition was evaluated against Cotton whitefly (Bemisia tabaci) in cotton crops. The effectiveness was measured as the percentage reduction of whitefly over control at different intervals, i.e., 3, 7, and 10 days after application (DAA). Table 32 shows that the present invention composition Compound of formula I 50% + 7% Compound of formula II SG at a dose 150gm/ha resulted in the highest efficacy, achieving percent control of 90.07 % at 7 DAA, and 87.91% at 10 DAA.

Table 33: Effectiveness of present invention composition against Cotton Aphids (Aphis gossypii)
S. No. Treatments Dose gm or ml/ha Effectiveness of Present invention composition (Compound of Formula I 50% SG) against Cotton Aphids
Corrected Per cent control
Pre count (Avg. pest count per leaf) 3 DAA 7 DAA 10 DAA
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 150gm 17.07 86.58 92.51 93.61
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 150gm 17.40 84.34 91.69 92.31
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 150gm 17.27 81.71 90.66 91.67
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 150gm 17.20 78.40 84.49 85.30
IE5 Compound of formula I 50% WG (Comparative Composition) 150gm 17.40 78.29 84.35 85.19
IE6 Compound of formula I 25% DC
(Comparative Composition) 300ml 17.60 79.59 85.79 86.48
IE7 Control - 17.40 0.00 0.00 0.00

The effectiveness of the present invention composition was evaluated against Cotton Aphids (Aphis gossypii) in cotton crops. The effectiveness was measured as the percentage reduction of aphids over control at different intervals, i.e., 3, 7, and 10 days after application (DAA). Table 33 shows that the present invention composition Compound of formula I 50% + 7% Compound of formula II SG at dose 150gm/ha resulted in the highest efficacy, achieving percent control of 92.51 % at 7 DAA, and 93.61% at 10 DAA.

Example 12: Evaluation of present invention composition for bio-efficacy against Aphids (Aphis gossypii) & Jassids (Amrasca biguttula biguttula) in Okra crop

TRIAL 2: Field Experimental Details
Season Kharif 2023
Location Rasulpur, Prantij, Gujarat
Crop Okra
Age of Crop 45 Days
Temperature Range during Trial 27-38°C
Variety Namdhari NS862
Single plot size 25 m2
Date of Transplanting/Sowing 23/12/2023
Number of applications 01
Date of application 07/02/2024
Target Pest Aphids & Jassids
Method of application Foliar

Table 34: Effectiveness of present invention composition against Okra Jassids (Amrasca biguttula biguttula)
S. No. Treatments Dose gm or ml/ha Effectiveness of Present Invention Composition (Compound of Formula I 50% SG) against Okra Jassids
Corrected Per cent Control
Pre count (Avg. pest count per leaf) 3 DAA 7 DAA 10 DAA
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 150gm 5.67 79.95 84.41 80.77
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 150gm 5.80 78.70 83.16 79.76
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 150gm 5.53 75.89 80.67 77.27
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 150gm 5.87 70.53 75.43 72.85
IE5 Compound of formula I 50% WG (Comparative Composition) 150gm 5.93 70.02 74.92 72.45
IE6 Compound of formula I 25% DC
(Comparative Composition) 300ml 5.93 71.69 76.49 73.86
IE7 Control - 5.53 0.00 0.00 0.00

The effectiveness of the present invention composition was evaluated against Okra Jassids (Amrasca biguttula biguttula). The effectiveness was measured as the percentage reduction of jassids over control at different intervals, i.e., 3, 7, and 10 days after application (DAA). Table 34 shows that the present invention composition Compound of formula I 50% + 7% Compound of formula II SG at dose 150gm/ha resulted in the highest efficacy, achieving percent control of 84.41 % at 7 DAA and 80.77% at 10 DAA.

Table 35: Effectiveness of present invention composition against Okra Aphids (Aphis gossypii)
S. No. Treatments Dose gm or ml/ha Effectiveness of Present Invention Composition (Compound of Formula I 50% SG) against Okra Aphids
Corrected Per cent Control
Pre count (Avg. pest count per leaf) 3 DAA 7 DAA 10 DAA
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 150gm 10.20 82.06 89.64 95.73
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 150gm 11.00 79.49 87.87 92.08
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 150gm 11.80 76.23 87.27 91.23
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 150gm 11.00 70.62 79.78 81.67
IE5 Compound of formula I 50% WG (Comparative Composition) 150gm 11.20 70.60 79.64 81.51
IE6 Compound of formula I 25% DC
(Comparative Composition) 300ml 10.93 72.67 80.16 82.06
IE7 Control - 10.73 0.00 0.00 0.00

The effectiveness of the present invention composition was evaluated against Okra Aphids (Aphis gossypii). The effectiveness was measured as the percentage reduction of aphids over control at different intervals, i.e., 3, 7, and 10 days after application (DAA). Table 35 shows that the present invention composition Compound of formula I 50% + 7% Compound of formula II SG at dose 150gm/ha resulted in the highest efficacy, achieving percent control of achieving 88.55 % at 7 DAA, and 95.73% at 10 DAA.

Example 13: Evaluation of Phytotoxicity of present invention composition in Cotton crop
Visual observations were recorded 3, 7, and 10 days after the application (DAA) of the tested product. The parameters observed were leaf injury on tip/surface, stunting, necrosis, chlorosis, vein clearing, epinasty, hyponasty, and wilting based on the 0-10 scale given in the table below. A total of 20 plants per plot were observed.

Table 36: Phytotoxicity symptoms scoring and rating for leaf injury on tip/surface
?Leaf injury on tips /surface? Rating
0%? 0?
1-10%? 1?
11-20%? 2?
21-30%? 3?
31-40%? 4?
41-50%? 5?
51-60%? 6?
61-70%? 7?
71-80%? 8?
81-90%? 9?
91-100%? 10?

Table 37: Phytotoxic effect of various treatments on cotton crop after 3 DAA?at recommended dose
S. No.? Treatment details? Dose gm or ml/ha? 3 DAA?
L? S? N? C? V? E? H? W?
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 150gm 0 0 0 0 0 0 0 0
IE5 Compound of formula I 50% WG (Comparative Composition) 150gm 0 0 0 0 0 0 0 0
IE6 Compound of formula I 25% DC
(Comparative Composition) 300ml 0 0 0 0 0 0 0 0
IE7 Control - 0 0 0 0 0 0 0 0
*DAA – Days after application, L-Leaf injury on tips/surface, S-stunting, N-Necrosis, C-Chlorosis, V- Vein clearing, E-Epinasty, H-Hyponasty, W-wilting?

Table 38: Phytotoxic effect of various treatments on cotton crop after 7 DAA?at recommended dose
S. No.? Treatment details? Dose gm or ml/ha? 7 DAA?
L? S? N? C? V? E? H? W?
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 150gm 0 0 0 0 0 0 0 0
IE5 Compound of formula I 50% WG (Comparative Composition) 150gm 0 0 0 0 0 0 0 0
IE6 Compound of formula I 25% DC
(Comparative Composition) 300ml 0 0 0 0 0 0 0 0
IE7 Control - 0 0 0 0 0 0 0 0
*DAA – Days after application, L-Leaf injury on tips/surface, S-stunting, N-Necrosis, C-Chlorosis, V- Vein clearing, E-Epinasty, H-Hyponasty, W-wilting?

Table 39: Phytotoxic effect of various treatments on cotton crop after 10 DAA?at recommended dose
S. No.? Treatment details? Dose gm or ml/ha? 10 DAA?
L? S? N? C? V? E? H? W?
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 150gm 0 0 0 0 0 0 0 0
IE5 Compound of formula I 50% WG (Comparative Composition) 150gm 0 0 0 0 0 0 0 0
IE6 Compound of formula I 25% DC
(Comparative Composition) 300ml 0 0 0 0 0 0 0 0
IE7 Control - 0 0 0 0 0 0 0 0
*DAA – Days after application, L-Leaf injury on tips/surface, S-stunting, N-Necrosis, C-Chlorosis, V- Vein clearing, E-Epinasty, H-Hyponasty, W-wilting?

Table 40: Phytotoxic effect of various treatments on cotton crop after 3 DAA?at double dose
S. No.? Treatment details? Dose gm or ml/ha? 3 DAA?
L? S? N? C? V? E? H? W?
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 300gm 0 0 0 0 0 0 0 0
IE5 Compound of formula I 50% WG (Comparative Composition) 300gm 0 0 0 0 0 0 0 0
IE6 Compound of formula I 25% DC
(Comparative Composition) 600ml 0 0 0 0 0 0 0 0
IE7 Control - 0 0 0 0 0 0 0 0
*DAA – Days after application, L-Leaf injury on tips/surface, S-stunting, N-Necrosis, C-Chlorosis, V- Vein clearing, E-Epinasty, H-Hyponasty, W-wilting?

Table 41: Phytotoxic effect of various treatments on cotton crop after 7 DAA?at double dose
S. No.? Treatment details? Dose gm or ml/ha? 7 DAA?
L? S? N? C? V? E? H? W?
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 300gm 0 0 0 0 0 0 0 0
IE5 Compound of formula I 50% WG (Comparative Composition) 300gm 0 0 0 0 0 0 0 0
IE6 Compound of formula I 25% DC
(Comparative Composition) 600ml 0 0 0 0 0 0 0 0
IE7 Control - 0 0 0 0 0 0 0 0
*DAA – Days after application, L-Leaf injury on tips/surface, S-stunting, N-Necrosis, C-Chlorosis, V- Vein clearing, E-Epinasty, H-Hyponasty, W-wilting?

Table 42: Phytotoxic effect of various treatments on cotton crop after 10 DAA?at double dose
S. No.? Treatment details? Dose gm or ml/ha? 10 DAA?
L? S? N? C? V? E? H? W?
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 300gm 0 0 0 0 0 0 0 0
IE5 Compound of formula I 50% WG (Comparative Composition) 300gm 0 0 0 0 0 0 0 0
IE6 Compound of formula I 25% DC
(Comparative Composition) 600ml 0 0 0 0 0 0 0 0
IE7 Control - 0 0 0 0 0 0 0 0
*DAA – Days after application, L-Leaf injury on tips/surface, S-stunting, N-Necrosis, C-Chlorosis, V- Vein clearing, E-Epinasty, H-Hyponasty, W-wilting?

Tables 37 to 39 above evidence that the application of Compound of formula I and Compound of formula II in all doses showed no phytotoxicity symptoms like leaf injury on tips, leaf injury on the surface, wilting, vein clearing, necrosis, epinasty and hyponasty in cotton crop. Further, as evident from tables 40, 41 and 42, the application of Compound of formula I and Compound of formula II at even double doses shows no phytotoxicity. Thus, applying the present invention composition may be considered completely safe for crops.

Example 14: Evaluation of Phytotoxicity of present invention composition in Okra crop
Table 43: Phytotoxic effect of various treatments on okra crop after 3 DAA?at recommended dose
S. No.? Treatment details? Dose gm or ml/ha? 3 DAA?
L? S? N? C? V? E? H? W?
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 150gm 0 0 0 0 0 0 0 0
IE5 Compound of formula I 50% WG (Comparative Composition) 150gm 0 0 0 0 0 0 0 0
IE6 Compound of formula I 25% DC
(Comparative Composition) 300ml 0 0 0 0 0 0 0 0
IE7 Control - 0 0 0 0 0 0 0 0
*DAA – Days after application, L-Leaf injury on tips/surface, S-stunting, N-Necrosis, C-Chlorosis, V- Vein clearing, E-Epinasty, H-Hyponasty, W-wilting?

Table 44: Phytotoxic effect of various treatments on okra crop after 7 DAA?at recommended dose
S. No.? Treatment details? Dose gm or ml/ha? 7 DAA?
L? S? N? C? V? E? H? W?
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 150gm 0 0 0 0 0 0 0 0
IE5 Compound of formula I 50% WG (Comparative Composition) 150gm 0 0 0 0 0 0 0 0
IE6 Compound of formula I 25% DC
(Comparative Composition) 300ml 0 0 0 0 0 0 0 0
IE7 Control - 0 0 0 0 0 0 0 0
*DAA – Days after application, L-Leaf injury on tips/surface, S-stunting, N-Necrosis, C-Chlorosis, V- Vein clearing, E-Epinasty, H-Hyponasty, W-wilting?

Table 45: Phytotoxic effect of various treatments on okra crop after 10 DAA?at recommended dose
S. No.? Treatment details? Dose gm or ml/ha? 10 DAA?
L? S? N? C? V? E? H? W?
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 150gm 0 0 0 0 0 0 0 0
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 150gm 0 0 0 0 0 0 0 0
IE5 Compound of formula I 50% WG (Comparative Composition) 150gm 0 0 0 0 0 0 0 0
IE6 Compound of formula I 25% DC
(Comparative Composition) 300ml 0 0 0 0 0 0 0 0
IE7 Control - 0 0 0 0 0 0 0 0
*DAA – Days after application, L-Leaf injury on tips/surface, S-stunting, N-Necrosis, C-Chlorosis, V- Vein clearing, E-Epinasty, H-Hyponasty, W-wilting?

Table 46: Phytotoxic effect of various treatments on okra crop after 3 DAA?at double dose
S. No.? Treatment details? Dose gm or ml/ha? 3 DAA?
L? S? N? C? V? E? H? W?
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 300gm 0 0 0 0 0 0 0 0
IE5 Compound of formula I 50% WG (Comparative Composition) 300gm 0 0 0 0 0 0 0 0
IE6 Compound of formula I 25% DC
(Comparative Composition) 600ml 0 0 0 0 0 0 0 0
IE7 Control - 0 0 0 0 0 0 0 0
*DAA – Days after application, L-Leaf injury on tips/surface, S-stunting, N-Necrosis, C-Chlorosis, V- Vein clearing, E-Epinasty, H-Hyponasty, W-wilting?

Table 47: Phytotoxic effect of various treatments on okra crop after 7 DAA?at double dose
S. No.? Treatment details? Dose gm or ml/ha? 7 DAA?
L? S? N? C? V? E? H? W?
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 300gm 0 0 0 0 0 0 0 0
IE5 Compound of formula I 50% WG (Comparative Composition) 300gm 0 0 0 0 0 0 0 0
IE6 Compound of formula I 25% DC
(Comparative Composition) 600ml 0 0 0 0 0 0 0 0
IE7 Control - 0 0 0 0 0 0 0 0
*DAA – Days after application, L-Leaf injury on tips/surface, S-stunting, N-Necrosis, C-Chlorosis, V- Vein clearing, E-Epinasty, H-Hyponasty, W-wilting?

Table 48: Phytotoxic effect of various treatments on okra crop after 10 DAA?at double dose
S. No.? Treatment details? Dose gm or ml/ha? 10 DAA?
L? S? N? C? V? E? H? W?
IE1 Compound of formula I 50% + 7% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE2 Compound of formula I 50% + 5% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE3 Compound of formula I 50% + 3% Compound of formula II
(Present Invention Composition) 300gm 0 0 0 0 0 0 0 0
IE4 Compound of formula I 50% SG without Compound of formula II
(Comparative Composition) 300gm 0 0 0 0 0 0 0 0
IE5 Compound of formula I 50% WG (Comparative Composition) 300gm 0 0 0 0 0 0 0 0
IE6 Compound of formula I 25% DC
(Comparative Composition) 600ml 0 0 0 0 0 0 0 0
IE7 Control - 0 0 0 0 0 0 0 0
*DAA – Days after application, L-Leaf injury on tips/surface, S-stunting, N-Necrosis, C-Chlorosis, V- Vein clearing, E-Epinasty, H-Hyponasty, W-wilting?

Tables 43 to 45 above evidence that the application of Compound of formula I and Compound of formula II in all doses showed no phytotoxicity symptoms like leaf injury on tips, leaf injury on the surface, wilting, vein clearing, necrosis, epinasty and hyponasty in okra crop. Further, as evident from tables 46, 47 and 48, the application of Compound of formula I and Compound of formula II at even double doses shows no phytotoxicity. Thus, applying the present invention composition may be considered completely safe for crops.

From the foregoing it will be observed that numerous modifications and variations can be effectuated without departing from the true spirit and scope of the novel concepts of the present invention. It is to be understood that no limitations with respect to the specific embodiments illustrated is intended or should be inferred. It should be understood that all such modifications and improvements have been deleted herein for the sake of conciseness and readability but are properly within the scope of the following claims.
,CLAIMS:We Claim:

1. A stable insecticidal composition comprising:
a) a compound of formula I:

wherein , X = CF3 and A = ;
b) a non-toxic built-in adjuvant;
c) a surface active agent; and
d) one or more agriculturally acceptable excipients.

2. The stable insecticidal composition as claimed in claim 1 or 2, comprising:
a) the compound of formula I in an amount in the range of 1 to 60% by weight;
b) the non-toxic built-in adjuvant in an amount in the range of 1 to 10% by weight;
c) the surface active agent in an amount in the range of 1 to 15% by weight; and
d) one or more agriculturally acceptable excipients.

3. The stable insecticidal composition as claimed in claim 1, wherein the compound of formula I is:

4. The stable insecticidal composition as claimed in claim 1, wherein the non-toxic built-in adjuvant is a taurate compound.

5. The stable insecticidal composition as claimed in claim 4, wherein the taurate compound is a compound of formula II:

6. The stable insecticidal composition as claimed in claim 1, wherein the surface active agent is Sodium dibutylnaphthalenesulphonate.

7. The stable insecticidal composition as claimed in claim 1, wherein the agriculturally acceptable excipient is selected from the group comprising of carrier(s), surfactant(s), binder(s), surface-active agent(s), disintegrating agent(s), dispersants or dispersing agent(s), wetting agent(s), pH modifier(s), thickener(s), biocide(s), preservative(s), anti-freezing agent(s), defoamer(s), solvents, water soluble polymer, and/or stabilizer(s) or a combination thereof.

8. The stable insecticidal composition as claimed in claim 1, wherein the composition is formulated as a Soluble Granule (SG).

9. A method for preparing a stable insecticidal composition, comprising the steps of:
a) homogenizing active ingredient, non-toxic built-in adjuvant and other excipients in a pre-blender to form a pre-mixture;
b) milling the pre-mixture of step (a) for particle size reduction;
c) transferring the milled mass of step (b) into a post mixing vessel and mixing for 20 minutes;
d) adding water into the mass of step (c) under continuous mixing to form a dough for granulation;
e) initiating cylindrical granulation to obtain wet granules; and
f) drying wet granules of step (e) to obtain dry granules.

10. The method as claimed in claim 9, wherein the active is a compound of formula I,

I =

and is present in an amount in the range of 1 to 60% by weight.

11. The method as claimed in claim 9, wherein the non-toxic built-in adjuvant is a compound of formula II,
and is present in an amount in the range of 1 to 10% by weight.

12. The method as claimed in claim 9, wherein the particle size in step (b) is less than 50 microns.

13. The method as claimed in claim 9, wherein the granules are dried in step (f) at a temperature in the range of 50 to 60°C.