Combination of Encapsulated Phenothrin and Emulsified Prallethrin

Abstract

Disclosed is a combination of encapsulated, in particular micro-encapsulated phenothrin and emulsified prallethrin in water, preferably in a ratio of 10:1. This combination has excellent suitability for use as an insecticide. The suitable concentration is about 0.1% by mass of phenothrin and 0.01% by mass of prallethrin. The insecticide is used at a concentration of 20 ml/m.sup.2 to 60 ml/m.sup.2 on non-porous surfaces or in a concentration of 40 ml/m.sup.2 to 120 ml/m.sup.2 on porous surfaces. Despite the low amounts of active ingredients, the insecticide shows a rapid knockdown effect and a prolonged depot effect.

Claims

1. A combination of encapsulated phenothrin and emulsified prallethrin in water.

2. The combination according to claim 1, wherein the mass ratio of phenothrin to prallethrin is between 5:1 and 20:1.

3. The combination according to claim 1, wherein the phenothrin is microencapsulated.

4. The combination according to claim 3, wherein the specific particle size of phenothrin is between 1.8 μm and 3.3 μm.

5. The combination according to claim 1, wherein it is co-formulated with a UV stabilizer.

6. The combination according to claim 1, wherein the concentration of phenothrin is 9-11% by mass and the concentration of prallethrin is 0.9-1.1% by mass.

7. The combination according to claim 1, wherein the concentration of phenothrin is 0.09-0.11% by mass and the concentration of prallethrin is 0.009-0.011% by mass.

8. An insecticide comprising the combination according to claim 7.

9. A method or using the insecticide according to claim 8 comprising applying the insecticide at a concentration of 20 ml/m.sup.2 to 60 ml/m.sup.2 on non-porous surfaces.

10. A method of using of the insecticide according to claim 8 comprising applying the insecticide at a concentration of 40 ml/m.sup.2 to 120 ml/m.sup.2 on porous surfaces.

11. The combination according to claim 1, wherein the mass ratio of phenothrin to prallethrin is approximately 10:1.

12. An insecticide comprising the combination according to claim 1.

13. The insecticide according to claim 12 wherein it has a concentration of 20 ml/m.sup.2 to 60 ml/m.sup.2.

14. The insecticide according to claim 8 wherein it has a concentration of 20 ml/m.sup.2 to 60 ml/m.sup.2.

Description

EXAMPLE 1

Preparation of Capsule Suspension (CS)

[0066] For 5 kg of the end product 1670 g CS are required. All figures are % by weight.

TABLE-US-00004 TABLE 4 Oil phase % weight Water Phase % weight 1R-trans Phenothrin 31.932 Synperonic PE/F 127 1.5 TMXDI 0.450 BrijO20 0.056 ONGRONAT 2100 3.000 Zephrym PD3315 3.0 Cymel 1170 0.300 Water 44.912 Radia 7117 14.400 Cycat 4040 0.45

[0067] Maintain the water phase and the oil phase at 40° C. in a 2 litre jacketed reactor before the emulsion process.

[0068] In a jacketed reactor of 2 litre capacity, equipped with a cawless agitator and a high shear agitator, add the water phase at 40° C. With the cawless agitator on at 1600 rpm, the oil phase is added very fast (˜1 minute) to the water phase, starting the emulsion polymerization process.

[0069] After all the oil phase is emulsified completely, the high shear agitator is on at 4600 rpm. The emulsion polymerization is finished after 4 minutes.

[0070] Transfer the capsule suspension to the other jacketed reactor at 60° C., equipped only with an anchor agitator at 36 rpm.

[0071] The capsule suspension is maintained at 60° C. under the agitation for 3 hours until the capsules are cured and stable formed.

Preparation of the Emulsion in Water (EVV)

[0072] For 5 kg of the end product 3330 g EW are required. All figures are % by weight.

TABLE-US-00005 TABLE 5 Propylenglycol 7.5 Zephrym PD3315 3.0 Xanthan Gum 0.6 Break Thru AF5503 0.0225 Proxel GXL 0.15 Water 87.1175 Prallethrin TG 1.61

[0073] In a jacketed reactor of 5 litre capacity, equipped with a high shear agitator, add all the components of the EW formulation, except Xanthan Gum and prallethrin.

[0074] Mix the initial components using the high shear agitator at 1200 rpm and heat up the solution at 40° C.

[0075] After the temperature reaches 40° C., add Xanthan Gum at 4600 rpm until the complete transparent gelification.

[0076] Add prallethrin technical heated at 40° C. under the agitation at 4600 rpm for 4 minutes obtaining a homogenous stable emulsion in water (EW).

Preparation of the Final Suspension of Capsules Mixed with the EW to Form a ZW Formulation

[0077] In a jacketed reactor of 6 Liter capacity, mix 1670 g of capsule suspension with 3330 g of the EW using an anchor agitator at 36 rpm for at least 4 hours until the suspension is equilibrated and stable.

[0078] Measure the particle size of ZW formulation using a laser diffraction equipment and the stability of the dispersion of the capsules in a hard water of 342 ppm at the ratio of use 1:99.

EXAMPLE 2

Preparation of Capsule Suspension (CS)

[0079] For 5 kg of the end product 1670 g CS are required. All figures are % by weight.

TABLE-US-00006 TABLE 6 Oil phase % weight Water Phase % weight 1R-trans Phenothrin 31.932 Synperonic PE/F 127 2.25 TMXDI 0.450 BrijO20 0.056 ONGRONAT 2100 3.150 Zephrym PD3315 3.00 Cymel 1170 0.300 Water 44.912 Radia 7117 13.500 Cycat 4040 0.45

[0080] The manufacturing steps are the same as in example 1.

Preparation of the Emulsion in Water (EVV)

[0081] For 5 kg of the end product 3330 g EW are required. All figures are % by weight.

TABLE-US-00007 TABLE 7 Propylenglycol 12 Zephrym PD3315 3.52 Xanthan Gum 0.6 Break Thru AF5503 0.0225 Proxel GXL 0.15 Water 82.0975 Prallethrin TG 1.61

[0082] The manufacturing steps for the water emulsion and for the final suspension are the same as in example 1.

EXAMPLE 3

Preparation of Capsule Suspension (CS)

[0083] For 5 kg of the end product 1670 g CS are required. All figures are % by weight.

TABLE-US-00008 TABLE 8 Oil phase % weight Water Phase % weight 1R-trans Phenothrin 31.932 Synperonic PE/F 127 2.52 TMXDI 0.900 BrijO20 0.056 ONGRONAT 2100 4.200 Zephrym PD3315 3.0 Cymel 1170 0.75 Water 41.102 Radia 7117 15.00 Cycat 4040 0.54

[0084] The manufacturing steps are the same as in example 1.

Preparation of the Emulsion in Water (EVV)

[0085] For 5 kg of the end product 3330 g EW are required. All figures are % by weight.

TABLE-US-00009 TABLE 9 Propylenglycol 11.25 Zephrym PD3315 3.00 Xanthan Gum 0.525 Break Thru AF5503 0.0225 Proxel GXL 0.15 Water 83.442 Prallethrin TG 1.61

[0086] The manufacturing steps for the water emulsion and for the final suspension are the same as in example 1.

EXAMPLE 4

Preparation of Capsule Suspension (CS)

[0087] For 5 kg of the end product 1670 g CS are required. All figures are % by weight

TABLE-US-00010 TABLE 10 Oil phase % weight Water Phase % weight 1R-trans Phenothrin 31.932 Synperonic PE/F 127 2.76 TMXDI 1.20 BrijO20 0.056 ONGRONAT 2100 4.50 Zephrym PD3315 3.0 Cymel 1170 0.90 Water 36.902 Radia 7117 18.00 Cycat 4040 0.75

[0088] The manufacturing steps are the same as in example 1.

Preparation of the Emulsion in Water (EVV)

[0089] For 5 kg of the end product 3330 g EW are required. All figures are % by weight.

TABLE-US-00011 TABLE 11 Propylenglycol 13.5 Zephrym PD3315 3.52 Xanthan Gum 0.45 Break Thru AF5503 0.0225 Proxel GXL 0.15 Water 80.7475 Prallethrin TG 1.61

[0090] The manufacturing steps for the water emulsion and for the final suspension are the same as in example 1.

EXAMPLE 5

Preparation of Capsule Suspension (CS)

[0091] For 5 kg of the end product 1670 g CS are required. All figures are % by weight.

TABLE-US-00012 TABLE 12 Oil phase % weight Water Phase % weight 1R-trans Phenothrin 31.932 Synperonic PE/F 127 2.52 TMXDI 0.30 BrijO20 0.056 ONGRONAT 2100 2.40 Zephrym PD3315 3.000 Cymel 1170 0.54 Water 34.502 Radia 7117 24.00 Cycat 4040 0.75

[0092] The manufacturing steps are the same as in example 1.

Preparation of the Emulsion in Water (EW)

[0093] For 5 kg of the end product 3330 g EW are required. All figures are % by weight.

TABLE-US-00013 TABLE 13 Propylenglycol 15.00 Zephrym PD3315 2.70 Xanthan Gum 0.45 Break Thru AF5503 0.0225 Proxel GXL 0.15 Water 80.0675 Prallethrin TG 1.61

[0094] The manufacturing steps for the water emulsion and for the final suspension are the same as in example 1.

Critical Parameters for Microcapsule Selection

[0095] The selection of microcapsule for the stability and efficacy trials was based on the targeted properties defined for the end product.

[0096] The most critical property is the release rate of the microcapsules which is mainly controlled by:

[0097] 1. Microcapsule size in μm

[0098] 2. Degree of crosslinking (ratio wall-forming versus crosslinker)

[0099] 3. Wall thickness (ratio polymer versus encapsulated oil phase);

[0100] 4. Mobility of the oil phase as function of percent solvent.1.

[0101] Considering all the four listed properties, for each example prepared, the following data can be established:

TABLE-US-00014 TABLE 14 1 2 3 4 5 Particle size medium/ medium/ low/ low/ medium/high high high medium medium Degree of high high medium medium low crosslinking Wall thickness low low high high low Mobility of oil medium medium medium medium/ high phase high

[0102] Medium/high particle size implies low number of particles per unit volume;

[0103] low/medium particle size implies high number of particles per unit volume.

[0104] High degree of crosslinking implies slow release with a long residual efficacy;

[0105] medium degree of crosslinking implies fast release with a medium residual efficacy;

[0106] low degree of crosslinking implies fast release with a low residual efficacy.

[0107] High wall thickness implies medium diffusion;

[0108] low wall thickness implies high diffusion.

[0109] Therefore, one can conclude that in examples 1 and 2, number of particles per unit volume is low, therefore there is insufficient surface for delivery of the active ingredient which leads to a low efficacy; thus, this example is not acceptable for further testing.

[0110] In example 3, the number of particles per unit volume is high, which enables a surface of high(er) delivery of the active ingredient, leading to a higher efficacy. In addition, the particle size distribution is narrow, which allows a better dispersion stability. The degree of crosslinking gives a medium release profile with a high % of wall forming, enabling a medium diffusion that provides a residual efficacy. This example was the one chosen for further testing.

[0111] Example 4 is same as example 3, but it shows a less narrow particle size distribution and a higher mobility; this formulation would be also acceptable, but it is not ideal as this is the case for example 3.

[0112] In example 5, the number of particles per unit volume is medium to high. There is a medium surface available for the delivery of the active ingredient, with a low residual efficacy due to a very fast release profile. Thus, this example is not acceptable for further testing.

[0113] At the end, example 3 was chosen for further testing (e.g., efficacy, toxicity studies).

Efficacy Studies Data (No Choice Test)—the End Product

[0114] The concentrate was diluted in a ratio of 1:99 to be applied as the ready to use formulation.

[0115] For the assessment of the residual efficacy of this end product in terms of knockdown and mortality, age adult insects of mixed sex have been used.

[0116] After the well shaking of the product prior to application, 100 ml/m.sup.2 have been applied on carpet, concrete, and wood whereas 50 ml/m.sup.2 were applied onto ceramic surfaces. The surfaces were stored under ambient conditions prior the use. The total surface treated was 1 m.sup.2 to adhere as closely as possible to practical conditions. An untreated control (no product applied) was prepared in the same fashion for comparative purposes.

[0117] This was a “no-choice” test, whereby the insects were forced to stay on the treated surface. The persistence was measured by performing the same efficacy test after 4 and 8 weeks of the storage of the panels. Insects were checked for two purposes: [0118] knockdown effect [0119] lethal effect.

[0120] A complementary trial was performed by spraying directly the end product onto the target insects, whereby the immediate knockdown effect and mortality after 24 h were measured. In both cases the result was 100%.

[0121] On the spray treated surfaces, a 100% knockdown effect was observed [0122] on day 0 after 15 min [0123] after four weeks after 45 min [0124] after eight weeks after 60 min

[0125] The killing rate was observed on four different surfaces (concrete, wood, carpet, ceramic tiles) for the following insects:

[0126] Musca domestica (house fly)

[0127] Aedes aegypti (yellow fever mosquito)

[0128] Culex pipiens (house mosquito)

[0129] Anopheles gambiae (tropical mosquito)

[0130] Blattella germanica (German cockroach)

[0131] Periplaneta americana (American cockroach)

[0132] Lasius niger (common black ant)

[0133] Ixodes ricinus (castor bean tick, a hard-bodied tick)

[0134] Ctenocephalides felis (cat flea)

[0135] Lepisma saccharina (silverfish)

[0136] Cimex lectularius (bedbug)

[0137] Tineola bisselliella (clothing moth)

[0138] Dermatophagoides pteronyssinus (house dust mites)

[0139] Tegenaria domestica (house spider)

[0140] Pediculus humanus (head louse)

[0141] On day 0 as well as after eight weeks the mortality was 100%.

[0142] Therefore, it was shown that after spray treatment at a dose of 50 ml/m.sup.2 on non-porous surfaces and 100 ml/m.sup.2 on porous surfaces there is [0143] a very good insecticide effectiveness with a fast knockdown and a complete mortality; [0144] a residual efficacy lasting at least eight weeks after treatment on various materials such as ceramic tiles, carpets, wood and concrete.

Efficacy Studies Data (Simulated Use Trial)—the End Product—8 Weeks

[0145] Additional tests were conducted to mimic the realistic conditions to which the insects are exposed, and can move.

[0146] The test was conducted in four 15 m.sup.3 (6 m.sup.2 floor) test chambers with four replicates in compliance with the standard BSI 4172 Part 1&2 concerning the hand-held pressurized insecticide testing (1993). The test chambers were maintained at the temperature of 26° C.±1° C. and a relative humidity of 70%±5% during the period of testing.

[0147] The test chamber materials were washable and non-porous material on the wall/ceiling and on the floor, respectively epoxy-painted steel, and ceramic tiles.

[0148] To stimulate what happens in premises, some polystyrene blocks and cardboards were set into the test chamber to be harborages and a water and food source with: [0149] Water source (six 25 cm long water vials with a cotton wick) [0150] Food source (four locations on the floor, under harborages, two Petri dishes with pet-food biscuit.

[0151] The insects were able to reach water and food sources without being in contact with the insecticide. They had many places to hide. Only the half of the area was treated thus the target organisms had the choice not to be in contact with the end product.

[0152] For each mode of treatment and repetition, batches were used as follows: 25 of each species, except for house spiders which were difficult to find and for whom only 5 were used per replicate including the corresponding untreated controls.

[0153] The control batches were intended to check the quality of the batches used for the tests and unintentional effects introduced by handling and experimental conditions.

[0154] The insects were released two hours after treatment to let enough time for the period to dry out.

[0155] The application was done using a professional sprayer GLORIA 81 with an anti-drop nozzle. The liquid was vigorously shaken between each treatment.

[0156] The application dose was 50 ml/m.sup.2 and the treated area was half of the test chamber, i.e. 3 m.sup.2; then the quantity of product applied in each replicate was 150 ml of product per 3 m.sup.2 area.

[0157] The pathway to the food and water sources was not treated.

[0158] Tests were performed for the following insects:

[0159] Musca domestica (house fly)

[0160] Aedes aegypti (yellow fever mosquito)

[0161] Culex pipiens (house mosquito)

[0162] Anopheles gambiae (tropical mosquito)

[0163] Blattella germanica (German cockroach)

[0164] Periplaneta americana (American cockroach)

[0165] Lasius niger (common black ant)

[0166] Solenopsis invicta (fire ant)

[0167] Reticulitermes santonensis (eastern subterranean termite)

[0168] Lepisma saccharine (silver fish)

[0169] Cimex lectularius (bedbug)

[0170] Tegenaria domestica (house spider)

[0171] On day 0 as well as after eight weeks the killing rate was 100%.

[0172] In the conditions of this simulated use trial, the end product applied at a rate of 50 ml/m.sup.2 has proven a complete control in less than one week with a complete mortality at 100%. The residual efficacy has remained constant over a period of eight weeks after treatment.

Efficacy Studies Data (Simulated Use Trial) for 12 and 16 Weeks—the End Product

[0173] Additional studies were conducted for evaluation of the efficacy and residual life of the end product which was applied to control various insect pests.

[0174] The trial was done in the laboratory in a test chamber with materials simulating the real conditions of use (cardboard=harborages+food/water source) and only the half of the area was treated by the product, thus the target organisms had the choice not to be in contact with the product.

[0175] The efficacy was quantified by a percentage of population's reduction after treatment and after 8 and 12 weeks.

[0176] Doses tested were 50 ml/m.sup.2 for non-porous surfaces (ceramic tiles) and 100 ml/m.sup.2 on porous surfaces (fiber-cement).

[0177] The chosen species for testing were Musca domestica (house fly) and Blattella germanica (German cockroach).

[0178] The product has proven a very good control in both target insect pest organisms with a complete kill (100%) until 12 weeks exposure time.

[0179] Testing for additional 4 weeks has shown a continuous efficacy in Musca domestica but only to a low extent in Blattella germanica:

TABLE-US-00015 TABLE 15 8 weeks 12 weeks 16 weeks Musca domestica 100% 100% 100% Blattella germanica 100% 100%  17%

Toxicity Studies—the End Product

[0180] An acute oral toxicity test was conducted with rats to determine the potential for the end product to produce toxicity from a single dose via the oral route. Under the conditions of the study, the acute oral LD.sub.50 of the end product is greater than 5000 mg/kg of body weight in female rats. All animals survived, gained body weight, and appeared active and healthy during the study. Based on the results, the end product meets the requirements for GHS Toxicity Category 5, i.e. no symbols and no specific label elements are required.

[0181] An acute inhalation toxicity test was conducted with rats to determine the potential for the end product to produce toxicity from a single exposure via the inhalation (nose-only exposure) route. Under the condition of the study, LC.sub.50 of the test substance is greater than 5.03 mg/l in male and female rats. Based on the results, the end product meets the requirement for GHS Toxicity Category 5.

[0182] All animals survived exposure and gained body weight during the study. Following exposure, all rats exhibited irregular respiration. However, all animals recovered by day 2 and appeared active and healthy for the remained of the 14-day observation period. No gross abnormalities were noted for any of the animals when necropsied at the conclusion of the 14-day observation period.

[0183] The acute dermal toxicity was not tested as the lethal dose in rats for the concentrate has already revealed a value above 5000 mg/kg.

Toxicity Studies—the Concentrate

[0184] Similar studies for the concentrate (10% phenothrin and 1% prallethrin) have revealed that the LD.sub.50-value is above 5000 mg/kg body weight with the oral toxicity test as well as with the dermal acute toxicity test. This meets the requirements for GHS Toxicity Category 5, i.e. no symbols and no specific label elements are required.

[0185] In the study for an acute oral toxicity, all animals were observed for mortality, signs of gross toxicity, and behavioral changes at least once daily for 13 or 14 days. All animals have survived, gained body weight, and appeared active and healthy. There were neither signs of gross toxicity nor adverse pharmacologic effects or abnormal behavior.

[0186] In the study for an acute dermal toxicity, all animals were observed for mortality, signs of gross toxicity, and behavioral changes at least once daily for 14 days. All animals have survived the exposure and gained body weight. No gross abnormalities were noted for any of the animals when necropsied at the conclusion of the 14-day observation period.

[0187] In the study for acute inhalation toxicity, the values meet the requirements for GHS Toxicity Category 4. All animals have survived exposure to the test atmosphere. Following exposure, eight rats were hypoactive and in addition, all animals exhibited irregular respiration, an abnormal gait, and tremors (H332). However, all animals recovered by day 4 and appeared active and healthy for the remained of the 14-day observation period. Although several animals lost or failed to gain body weight by day 1, all animals gained body weight over the 14-day observation period. The observed body weight losses were not considered to be of toxicological importance. No gross abnormalities were noted for any of the animals when necropsied at the conclusion of the 14-day observation period.

Storage Stability—the End Product and the Concentrate

[0188] Physical and chemical properties have been conducted in accordance with the OECD principles of good laboratory practice and the GLP principles of the Chemicals Act of Austria, 1996. The study has been conducted in 0.375 l polyethylene terephthalate (PET) spray bottles as final packaging material. Typical parameters as physical state, color, odor, active ingredients content, density, pH, wet sieve residue, persistent foam, particle size, pourability, dispersion stability as well as corrosion properties were determined. Four samples were analysed: [0189] freshly prepared product [0190] product after 4 freeze/thaw cycles for 18 hours at −10±2° C. and 6 hours at 20±2° C. [0191] product after 7 days at 0±2° C. [0192] product after 14 days at 54±2° C.

[0193] The end product as well as the concentrate were stable with these samples and accelerated aging.

Evaluation of Anaerobic Biodegradation—the End Product

[0194] The anaerobic biodegradability of the end product in accordance to OECD 310:2014 was evaluated. Samples have been kept at the temperature of 20±2° C. for the whole period of the test (28 days).

[0195] Since the amount of TIC at the end of the test period was less than 10%, it is established that abiotic degradation has not occurred. In accordance to OECD 310:2014, the end product should be considered not biodegradable in aerobic conditions.

Dose Finding Test Data in Non-Porous Surfaces

[0196] The purpose of this study was to assess several doses of the end product on non-porous surfaces against

[0197] Musca domestica (common house fly)

[0198] Blattella germanica (german cockroach) and

[0199] Tegenaria domestica (house spider).

[0200] The trial was done by exposing the insects on porous surfaces impregnated with different dosages at 12 ml/m.sup.2, 25 ml/m.sup.2 and 35 ml/m.sup.2. In addition, a control was done, in which the surface was treated with water.

[0201] Some ceramic tiles of 15 cm×15 cm were treated with the product and the insects were exposed one hour on it. The experimenter recorded the mortality at regular time intervals.

[0202] The testing has revealed the following results:

[0203] On the tiles treated with water the mortality was lower than 5%, validating the trial.

[0204] On the tiles treated with 12 ml/m.sup.2 the following percentages of insects were killed:

TABLE-US-00016 TABLE 16 time 1 h 2 h 3 h 4 h 5 h 6 h 7 h 8 h 24 h 48 h 72 h Musca 0 0 0 0 0 1 1 5 49 93 100 domestica Blattella 0 0 0 0 0 0 1 1 9 44 44 germanica Tegenaria 0 0 0 0 0 0 0 0 15 55 55 domestica

[0205] It can be seen that this dosage is insufficient, because after 24 h not all insects were killed.

[0206] On the tiles treated with 25 ml/m.sup.2, the following percentages were observed:

TABLE-US-00017 TABLE 17 time 1 h 2 h 3 h 4 h 5 h 6 h 7 h 8 h 24 h 48 h 72 h Musca 0 0 0 2 5 8 13 19 100 100 100 domestica Blattella 0 0 0 2 4 13 13 16 100 100 100 germanica Tegenaria 0 0 5 5 10 19 19 20 100 100 100 domestica

[0207] This dosage is sufficient: after 24 hours, all insects are killed.

[0208] On the tiles treated with 35 ml/m.sup.2 the following percentages were observed:

TABLE-US-00018 TABLE 18 time 1 h 2 h 3 h 4 h 5 h 6 h 7 h 8 h 24 h 48 h 72 h Musca 0 1 9 17 37 55 100 100 100 100 100 domestica Blattella 0 0 3 6 11 19 24 30 100 100 100 germanica Tegenaria 0 5 10 15 20 20 25 45 100 100 100 domestica

[0209] By this dosage increase the efficacy was improved: the house fly was completely killed after 7 hours, and also for both other insects the dosage increase resulted in an improvement.

Dose Finding Test Data in Porous Surfaces

[0210] The purpose of this study was to assess several doses of the end product on porous surfaces against

[0211] Musca domestica (common house fly)

[0212] Blattella germanica (German cockroach).

[0213] The trial was done by exposing the insects on concrete impregnated with different dosages at 25 ml/m.sup.2, 35 ml/m.sup.2 and 50 ml/m.sup.2. In addition, a control was done, in which concrete was treated with water.

[0214] The experimenter recorded the mortality at regular time intervals.

[0215] The testing has revealed the following results:

[0216] On the concrete treated with water, the mortality was below 5%, validating the trial.

[0217] On the tiles treated with 25 ml/m.sup.2 the following percentages were observed:

TABLE-US-00019 TABLE 19 time 1 h 2 h 3 h 4 h 5 h 6 h 7 h 8 h 24 h 48 h 96 h Musca 0 0 0 0 0 0 0 0 100 100 100 domestica Blattella 0 0 0 0 0 0 0 0 19 36 77 germanica

[0218] It can be seen that this dosage is insufficient, because after 24 h not all insects were killed.

[0219] On the tiles treated with 35 ml/m.sup.2, the following percentages were observed:

TABLE-US-00020 TABLE 20 time 1 h 2 h 3 h 4 h 5 h 6 h 7 h 8 h 24 h 48 h 96 h Musca 0 0 0 2 9 11 16 23 100 100 100 domestica Blattella 0 0 0 0 0 0 0 0 30 52 93 germanica

[0220] In this case, more insects are killed after 24 hours, but not all. This dosage is therefore also insufficient.

[0221] On the tiles treated with 50 ml/m.sup.2, the following percentages were observed:

TABLE-US-00021 TABLE 21 time 1 h 2 h 3 h 4 h 5 h 6 h 7 h 8 h 24 h 48 h 96 h Musca 0 0 3 11 16 22 28 47 100 100 100 domestica Blattella 0 0 0 0 5 8 12 17 100 100 100 germanica

[0222] Here, the dosage is sufficient: after 24 hours, all insects are killed.