JPH01287003A - Herbicidal method and compound - Google Patents

Abstract

PURPOSE: To well control a wide range of various weeds, especially broad leaf weeds, in the habitat of grain crops after their germination by applying both bifenox and benazolin to the habitat. CONSTITUTION: This concentrated type or tank mix type herbicide compound comprising (A) bifenox of the formula, (B) one or more kinds of herbicidally active ingredients selected from benazolin, its salt and its ester, and one or more kinds of diluents or carriers which are not plant poisons is applied to the habitat of grain crops after their germination in an A:B weight ratio of 60:1 to 1:1. The ingredient A is applied in an amount of 0.25-3.0kg, preferably 0.5-1.5kg, especially 0.5-0.75kg, per ha of the habitat, and the ingredient B is applied in an amount of 0.05-0.25kg. The herbicide compound can well control the weeds, especially Stellaria media, Galium aparine and Viola spp. weeds.

Description

[Detailed description of the invention]

The present invention relates to a method for controlling weeds in cereal crops and to herbicidal formulations useful inter alia in said method. In order to control a wide variety of weeds in crops such as cereal crops, it is often necessary to use not only one but several herbicides. Despite the use of such mixed species, weeds still resist herbicide treatments and damage winter and spring crops such as wheat, barley, oats and rye. It has now been discovered by the present invention that a special combination of herbicides not only achieves extensive weed control but is also unexpectedly effective against weeds, especially broad-leaved weeds, in cereal crops. . That is, the present invention provides a method for controlling weeds, particularly broad-leaved weeds, in a cereal crop growing area, which method comprises controlling bifenox having the following formula I and the following after germination of the crop in the growing area. The method consists of applying one or more herbicidal active ingredients selected from the following active ingredients: [1) benazolin or its salts or esters. In an embodiment outside the scope of the present invention, in washing with water, the following ingredients are additionally added: (2) a benzoic acid herbicide, dicamba
amba) or 2,3,6-TBA or their salts or estenope (3) Phenoxy acid herbicides such as dichlorprop or 2,4-DB
or salts or esters thereof, (4) dinitrophenol herbicides, i.e. DNOC, dinot
erb) or dinoseb or their salts or esters, (5) benzonitrile herbicides ioxynil or bromoxyn i 1 or their salts or esters, and (6) 3,6-DCP. It is also possible to apply one or more herbicidal active ingredients selected from or their salts or esters. The method of the present invention is characterized by the use of the above-mentioned active ingredient (1), but embodiments (2) to (2) which are outside the scope of the present invention include
It will be appreciated that one or more of the six active ingredients may also be used and that further herbicidally active compounds may also be used together with the active ingredients (1) to (6). . If the herbicidal active ingredient is acidic or phenolic, salts or esters may be used, provided that they are not phytotoxic to the crop, i.e. substantially less phytotoxic than the free acid or phenol. It is. The nature of these salts and esters are well known to the art of painting. The preparation of biphenox, methyl 5-(2,4-dichlorophenoxy)-2-nitropenzoate, is described in United Kingdom Patent No. 1232368 and its use as a herbicide is also described in the literature (Proc. N, ε). , Weed Sci, Conf, 1973.
27.31). Similarly, dicamba, which is a benzoic acid herbicide,
Jushi Rest Mango UJ is disclosed in US Pat. No. 3,013,054;'! :,A”1,also2゜3.6-,-~T
BΔ so 132, 3, 6-1・tsuk i:'li
i'ff benzoic acid is US Pat. No. 284114 'γ08
・5bi31) 811f32 Kidney notification 1 detailed document 1: Disclosed. 7]. No) "Silic acid-based remover" 11 agents are well-known compound group "-C" and are quite common in 71JI IIJI:
It was widely used9).
-, -(2,4jikuoo)ffノ”!”shi) Pro 1:'
Onic acid ship name Q'J5, also known as (1': 1.,,,
- Te2, 4.8-r-)P (!-iv Name i
i'knowledge'F＞41. . B, 4-I) B is the name -ζ-A1? ”
),. 11 N (1(
, : (Chemical name 2・-medil~4.toji,″′nido1
-'J], 4. UK Patent No. 425295-”
f> (!: I,,,,,,, ゛Protection 3\I'7.
．． -(:iro 3. dinoceb is 2 SeC-butyl,,
-4,5-G:,, t = 1 near, l engineering, /-le's ~・ship name is confirmed, Yoneda Patent No. 2 Hli'! 197A
- 1, dinofluorub as disclosed in the specification 32;
,,,,,,-te-butyl-4,6-di7",)
r17: For example, pod 1 patent No. 11266
No. 58 Specification ij, Disclosure 5'1, (,'' is a benzonitrile herbicide, Iokij 7゛,)) [11shi4 Human Tl1ll 4::C... 5
Jo Doben Zo “L Lil and 1' Dobu! 1 (
・"・shi", le 3 + ri~jibro 壬~・1 (-,
Do I'l xy-bency:, Trill is both 1) '1 box in the UK, for example! l "i '(""/ J +'j "'
Fi specification iyu) 1, °disclosure, ゛tatami 9. ζ, there. Beno” pudding is changed, - # structure and 1, 2 = 4) January -
r-, -2-,,-;, 18 toso;
National Patent No. 862226 Specification
-Jino 7j 711 vinyl] 7fJJ '7. ','f
A-3Yl, ゛, :i'1. ,, i;i US Wi
No. 331'1549, disclosed by Jill. Cereal crops are for example wheat, barley, oats or rye11. However, the method of the present invention has the greatest utility in wheat and barley, especially in wheat, winter barley, and winter barley. Crop susceptibility 2 - The severity of the weed control problem is determined by the application of activators,
・Decision 4″ru1, j, or 1. while general 11,
The application rate of 1-゛〕'-tsuk, ・mi is 0.25 per 17% acre = −3,0 kr<, preferably 0.5-・ per 1 hectare],, 5 0.5-□
-0,75]<H”'Q ;4'> W ,, in the end,
;1.1; and ° should be used together. (1) - (

I like the ingredients of [)) L, good jlf! ! Example 116-゛) 〒4 (vero o fif 2 or 1 drop--, derived from mail, applied amount of ingredient 1; t, free-]; (per acid per 11 or phenol) .Benzoic acid-based moth removal agent, i.e., dicano, ba or 2. 3. 6-
If TBA is used, the dosage should be 0.05 to 0.2 kg per hectare of bed, and the risk of benzoic acid herbicides such as Pi, J-, Nox and benzoic acid herbicides. is 60
: 1.~, 1:1, preferably 30:1~.4:1 8. When the benzoic acid herbicide is wet, the alkali metal salt, e.g., the sodium salt or potassium salt of the benzoic acid herbicide. , or in its military form such as C, -C8 al+ru, r sprue, etc. For phenoxy acid herbicides, use Zino 00bu Tlbu or 2
,4・-D B is used, and its preferred application speed i is 1/
＼It is 0.1 to 3.5 kg per kutar! 1. 'Fenox vs. 7': Chongsha, an r-noxy acid herbicide, has 30
: ] to 1:15, especially 8:1 to 1:6. In a particularly preferred embodiment, Bifuenox is 0°5 per 1.
~0.75 kg, phenoxy acid herbicides are applied at a rate of 1.5.-3.0 kg per 1'% kutar. 7(
゛,)・TOC0・nMi Thread remover IIA salt example Aba1”□
``Lukari metal i?4.Special 1.
=- Suitable to be used in the form of um salt! ? J5ro,
An example of the Niester type of 2so'-nokidic acid system removal ^i + J is 1.-) 3 carbon atoms side in the sub-nod group,
“P, Bago 21 Ru 2, Isobu 11 Building and Bujiru Yusder - r゛possible 4゜゜゜l:”:1 Trof D Nord type detective A (! There is D
N.O.C. When dinonorub or dinoceb is used, these application rates are preferably <0.
5=. 5.0 kg and more preferred), 2. In the case of Nijinone' Lubu or Ginoceb, 1.. 0.5 to 2.0 kg per 1 kuku. Against Ji,!, Do l] Bu, L-nor type moth remover 1 year 1 1; 1 6: 1 = · · · 1: '20 is preferable, 3:1 - = ·
1:6 is even better. Examples of suitable forms of dinitrophenol herbicides may be salts with organic bases or organic bases, particularly salts such as salts and salts. But that's fine. ■ As an example of sprue, C is an organic acid such as a carboxylic acid. 0.05~0.
Preferably it is applied at a rate of 5 kg, more preferably from 0.1 to 0.35 kg per hectare. The weight ratio of bifenox to benzonitrile herbicide is preferably 60:1 to 1:2, more preferably 15:1 to 2:1. In a special embodiment, both ioxynil and bromoxynil are used in combination with bifuenox, in which case the preferred application rates and weight ratios are as above, based on the total weight of both ioxynil and bromoxynil. Preferred salt forms of ioxinil and bromoxynil are the alkali metal salts, such as the sodium and potassium salts. Suitable esters include ioxynyl octanoate and bromoxynyl octanoate. When using benazoline, it is applied at a weight ratio of 0.05 to 0.25 kg per 1 λ ctal. The weight ratio of bifuenox to benazoline is preferably 60:
The ratio is 1 to 1:1, more preferably 15:1 to 5:2. Suitable salt forms of benazoline include the alkali metal salts, particularly the sodium and potassium salt forms. Preferred esters are those containing 1 to 4 carbon atoms in the ester group, especially the ethyl ester. 3. When using 6-DCP, preferably 0.025 to 0.15 kg of this per hectare. More preferably 0.05 to 0.1 k per hectare
Apply at the rate of g. Bifuenocus vs. 3. 5-DPC
A preferred weight ratio is 30:1 to 3:1, and a more preferred ratio is 15:1 to 5:1. 3. Examples of salt forms of 5-DPC are the alkali metal salts, such as the sodium and potassium salts, and the amine or ammonium salts, such as the monoethanolamine salt. Examples of esters given are those containing 1 to 8 carbon atoms in the ester group. The method of the present invention can be applied to cereal crops at the one leaf stage.
It is preferable to carry out the process at an intermediate point between the stage and the formation of the second node. When Bifuenox is used in combination with benzoic acid herbicides, the weed species Stellariamed
ia), Polygonum 5pp
), Spergula alpensis (Spergula a
rvensis), Tripleurospermum maritim
Particularly good control has been observed for the following species: um), Viola species (Viola 5pp) and Veronica species (Veronica 5pp). When Bifuenox is used in combination with phenoxy acid herbicides, weed species Gallium abarin (Galiumapar)
Particularly good control has been observed for Stellaria mejia and Veronica species. When Bifuenox was used in combination with dinitrophenol herbicides, the weed species Galeopsis tetrahito (Gal)
eopsis tetrahit), Fumaria officinalis
), Polygonum compolvulus
Particularly good control has been observed for gallium abarin (G. convolvulus) and gallium abarin. When Bifuenox is used in combination with benzonitrile herbicides, the weed species Matricaria sp.
p), Polygonum sp. and Gallium abarin have been observed to achieve particularly good control. Particularly good control has been observed to be achieved against Stellaria media, Gallium abarin and Viola species when Bifuenox is used in combination with Benazoline. Particularly good control achieved against the weed species Veronica sp. and Matricaria sp. has been observed when Bifuenox is used in combination with 3.6-DCP. Examples of additional herbicidally active compounds that can be used in combination with Bifuenox and the active ingredients (1) to (6) above include MCPA, MCPB and mecopr.
op), all of which are well-known herbicides, described in the literature and listed in the Pesticide Menu (“P
e5ticide Manual", fifth
ition, 1ssued by the Br1t
ish Crop Protection Council
l) is displayed. Bifuenox and the above herbicidal active ingredients (1) to (6) and optionally additional herbicidal active compounds can be applied to the crop growing area at the same time or at different times. In the latter case 1.
1'f110. Length of time between periods of use (,), shortest example: 1 day or less than 7 days) ('2 is better!
El... stomach. However, it is far more preferable to apply the compound to be applied simultaneously as a tn formulation. stomach. Manufacture, storage and transportation The production of herbicide formulations, usually in concentrated form, for the purpose of
``,',,-,,;1 (as necessary to obtain an application rate of 14!3'1) t diluted with water over -4''; In November, - the formulation to be applied has an active herbicide component (tosi number) of 0, ()[).
・Contains 3.0% (33% concentration) (33% concentration, the desired formulation is generally 1% = 9()%, preferably 1% is 5-815%) % of the herbicidal active ingredient in a non-vegetable carrier, the carrier may be a type of excipient or an excipient, and the concentrated formulation forms part of the present invention. There are two things, i.e., in the method of the present invention, there are two exclusive
A concentrated herbicidal formulation that can be specially used is provided. This formulation is bis 1-. Nox and (1) As an embodiment of the present invention, (1) agglomeration of benazoline or i is an embodiment other than the present invention.
(2) %', except for the zoic acid series, namely dicamba or 2.3.6-TBA or their salts. (3) Pheno-decacic acid herbicides, i.e., Ginol R1 Lup 1:1 or 2.4-013 琥: Haiyu Y4 is also L.
I" Sprue, (4) Dinitroph J-Nol herbicide immediately!
DNOC, dinoterb or dinoceb or (= their salts are I, sprue, (5) benzonitrile thread remover, i. Chowa, Ra no Shio Moil, Rihari, Thrall, and (6)
7J, 6-1→C1' or A, one or more active ingredients selected from 1 or sprue as a non-phytotoxin carrier) Or it contains -f-11 or more combinations. This formulation has an odor. L Nox vs each active ingredient (1
) =, = (6) weight company uses the method of the present invention and 1y1 series (
2f In the preamble, there is a preferred line 1゛S, which is 7 and . Concentrated formulations according to the invention are usually in the form of wettable powders, emulsifiable concentrates or aqueous suspensions. and the moistened and fried powder formulation for use in the method of the present invention.
Good'#1. It's a good thing 4. ,, for cereal crops, the plant CJ and the properties of 4 grains 9: (-1, more than concentrates that can be emulsified (It is better than concentrates that can be emulsified, excluding powders that can be moistened) Minute and 1st @
,"',S(is the inert carrier and jβ′1′
J′j(′7) 1 containing an intimate mixture with a 4-surface active agent, the inert carrier may be e.g.
tapulgite clays), montmorillonite clay, diatomaceous earth, kaolin, mica, kuruku and refined silicon i! ! Selected from i2 salt. Effective surfactants include sulfonic acid, naphthalene sulfonate, condensed naphthalene sulfonate, alkyl succinate, alkino!・benze]/sulfonates, alkyl sulfonate and non-imene surfactants such as FZ
13 Emulsifiable concentrates are obtained from herbicidal active ingredients and surfactants dissolved in suitable solvents or suitable solvents. Become. Suitable surfactants may be selected, for example, from those mentioned above in connection with the wettable powders. Suitable solvents include alkyl@substituted benzenes, 0-chlorotoluene, heavy aromatic naphthalenes, glycolueders, and cyclic getones. Aqueous suspensions and aqueous solutions are water or (additional to appropriate solvents) <
Contains a suspended or dissolved herbicidal active ingredient and a desired surfactant, thickening agent, antifreeze agent or preservative. Suitable surfactants are associated with the wettable powder (7) and are selected from those listed above. Preservatives include a wide range of substances, such as various basibene antibacterial agents. agent,
Phenol, 0-1-11:I1/sol,)J,
-゛, mercury nitrate, mercury nitrate, alde 1;, de. Another formulation method is to mix two or more herbicidal active ingredients with water in a spray tank immediately before use. to form a herbicide formulation. Therefore, water acts as a non-phytotoxin carrier. (tank m1xes)'', but
, which form another aspect of the invention. In this tank mix, the weight ratio of Bifuunox herbicidal active ingredients (1) to (6) is preferably the above-mentioned weight ratio suitable for the method of the present invention. “Tankomics type” in the claims of this specification
The term tank m1x) J refers to the method of packaging the multiple components forming the formulation of the present invention. That is, the plurality of components are stored in separate containers, and when used, they are added together into a tank for preparing agricultural propellants, and then the required amount of water is added to dilute in the tank. It is a type of compound. The following examples are illustrative of concentrated herbicide formulations according to the invention. When the herbicide component is an acid or a phenol derivative, the amount of the component is based on acid equivalents or phenol equivalents. Among these examples, Examples 3.12 and 24 are examples of the present invention, and the others are reference examples. Examples 1-9 Wettable powders were prepared using the following raw ingredients. Weight% (1) Bifuenox 50 Ioxynyl 5 Disodium salt of condensed naphthalene sulfonic acid Ethoxylated alkylphenol 4 Heat-resolved silica 5 Montmorillonite Added until the total amount was 100 (2) Bifuenox 42 Bromoxynil 6 Sodium lauryl sulfate 5 Sodium lignin sulfonate 3 Precipitation Method silica 8 Kaolin Add until the total amount becomes 100 (3) Biphenox 48 Benazoline (ethyl ester) 4 Ethoxylated nonylphenol 4 Sulfite method leachate powder 4 (Sulfite lye
powder) pyrogenic silica
5 Attapal guide Add until the total amount is 100 (4)
Bifuenox 403, 6-
DCP (monoethanolamine salt) 4-sodium lauryl sulfate 4-sodium lignin sulfonate 3 Precipitated silica 8
Add kaolin until the total amount reaches 100 (5)
Bifuenox 202.4-D
B (Potassium salt) 30 Ethoxylated alkyl phenol 2 Sulfite method leachate powder 4 Pyrolysis method silica
5 Attapal guide Add until the total amount is 100 (6) Bifuenox 20
Dichlorprob (potassium salt) 40 Sodium dialkyl sulfo 3 Succinate lignosulfonate 2 Microcrystalline silica 7 (micronised 5
ilica) Diatomaceous earth Add until the total amount is 100 (7) Bifuenox
45 Ioxynyl 2.5 Bromoxynil Trisodium lauryl sulfide Disodium lignin sulfonate
3 Precipitation method silica 5 Montmorillonite Add until the total amount reaches 100 (8) Pifuenox 402
, 3.6-TO8 (sodium salt) 5-sodium lauryl sulfate 3-sodium lignin sulfonate 3-precipitation silica
4 Add kaolin until the total amount reaches 100 (
9) Biphenox 40 Dicamba (sodium salt) 4 Ethoxylated alkylphenol 4 Lignosulfonate
2Pyrolytic silica 3Sodium aluminosilicate・)・Total amount 100 (!-Norome 1. Addition) Carefully mix the herbicidal active ingredients on each side in a conventional mixing device with 2 special excipients 5 3. Add the mixture to a fluid energy mill (formerly known as d energy mill).
1) to a size range of 1 to 10 microns. Examples 10 to 21 An emulsifiable concentrate 1.1d product having the following components was prepared. Weight % αO biphenox 25 Ioxynyl (Octatsuyu・-1・) 3 Calcium dodecylbenzene 4 Sulfonate alkylphenoxy polyoxy 2 Ethylene ethanol cyclohexanone 35 Xylene
Add until the total amount is 100 A1) Biphenox 20 pro-xynyl (octanonyto) 4 dodecylbenzenesulfonic acid
3rmine salt polyoxytamine tylene triglyceride 3 cyclohexanone 30 orthochlorotoluene Addition and beating until the total amount becomes 100 Bifuenox 20 Bepzolin (Nibrunisal) 2 Calcium dodecylbenzene 2 Sulfonate ethoxylated alkylphenol 4 Isophorone
35 Total amount of aromatic naphtha] Added until reaching 00 αω Bifuenox 6D N
OC20 Calcium dodecylbenzene 3 Sulfonate Ethoxylated alkylphenol 3 Cyclono\xanone 25 Aromatic naphtha Added until total amount 100 00 Bifuenox 20 Dinoterb 10 Alkylaryl sulfonate 2 Alkyl phenoxypolyoxy 4 Ethylene ethanol isophorone 30 Orthochlorotoluene Total amount 100 αω Added until
Addition until total amount of 20% aromatic naphtha is 100% Bifuenox 203
, 6-11CP 4 Calcium dodecylbenzene 4 Sulfonate ethoxylated alkylphenol 4 Isophorone
Added until the total amount of 30% aromatic naphtha reached 100% Biff J Nox 152
．． 4-DB (isopropyl ester) 30 alkylaryl sulfone) 4-bolyoxyethylene triglyceride 2-cyclohexanone
２５ Bifuenox 20 Ioxynyl (octanoate) 1.5 Bromoxynyl (octanoate) 2 Calcium dodecylbenzene 3 Sulfonate alkylphenoxy polyoxy 4 Ethylene ethanol isophorone 30 Orthochlorotoluene Add until the total amount reaches 100 ■ Bifuenox 252, 3.
6-TBA (ester) 3 Calcium dodecylbenzene 3 Sulfonate ethoxylated alkylphenol 3 Isophorone
30 Orthochlorotoluene Add until the total amount reaches 100 (21) Biphenox 20 Dicamba 2 Alkylaryl sulfonate 4 Alkylphenoxypolyoxy 2 Ethylene ethanol Cyclohexanone 25 Xylene
The added herbicidal active ingredient was added to a suitable solvent (single or plural) under stirring until the total amount reached 100%, and optionally heated to easily dissolve the ingredient. Next, surfactant was added. After dissolution, the solution was filtered to remove insoluble impurities. Examples 22-24 Aqueous suspensions were prepared from the following components. Weight/Volume% (22) Biphenox 40 Ioxynyl (sodium salt) 4 Ethoxylated nonylphenol 3 Hydroxymethyl cellulose 2 Silicon antiform 0.1 Water
Add until total volume reaches 100 (23) Biphenox 35 Bromoxynil (potassium salt > 3.5 Ethotosylated nonylphenol 2
．． 5 Hydroxymethyl cellulose 1.7 Silicon antiform 0.1 Water
Add until the total volume is 100 (24) Bifuenox
48 Benazoline (potassium salt)
8 Sodium Lauryl Sal 3 Phate Acpal Guide 1.5 Silicone Antiform 0.15 Water Mix the added herbicide component with a surfactant and a foam suppressant until the total volume is 100, then stir vigorously in water to make a crude product. An aqueous suspension was formed. Next, this was wetted and crushed to reduce the particle size of the herbicidal active ingredient to 0.5 to 20 microns. An aqueous suspension of a thickening agent or suspending agent (hydrate) was added to this wet mashed product. Example 25 below is an example of a test method for determining the effectiveness of the methods and formulations of the invention. Example 25 (Test Method) An appropriate amount of a formulation product (e.g., one of the concentrated formulation products of Examples 1-24) is placed in a microspray.
The dispersion was completed by adding to the water in a -5 player) and stirring. Adjust sprayer to 40psi (
The jet was designed to inject a volume equal to 200β/hectare under a pressure of approximately 2,72 atm (approximately 2.8 kg/cm”).
standard nozzle (Allman No.,
0) was equipped on the sprayer. The product of the present invention was applied after both the crop and the weeds had germinated, but the application period was changed to when the crop was in the three-leaf stage (31eaf).
stage) to early stem elongation at various times. The timing of application to weeds can also be varied at various times when the growth of the weeds is from the cotyledon stage to the seedling stage.

Claims (11)

[Claims] (1) One or more herbicidal active ingredients selected from bifenox and benazolin or their salts or esters having the following formula I: ▲There are mathematical formulas, chemical formulas, tables, etc.▼ are applied to cereal crops. A method for controlling weeds in a cereal crop growing area, the method comprising applying the weed to the cereal crop growing area after germination. (2) The method according to claim (1), characterized in that Bifuenox is applied at a rate of 0.25 to 3.0 kg per hectare of cereal crop growing area. (3) Bifuenox 0.5 to 1.5 per hectare
The method according to claim (2), characterized in that it is applied at a rate of 1.0 kg. (4) Bifuenox 0.5-0.7 per hectare
The method according to claim (3), wherein the method is applied at a rate of 5 kg. (5) Benazoline 0.05-0.2 per hectare
The method according to any one of claims (1) to (4), characterized in that it is applied at a rate of 5 kg. (6) Concentrated or tankomic type weed control characterized by combining one or more of bifuenox and benazoline or its salts or esters with one or more non-phytotoxic diluents or carriers. formulations for use. (7) Weight ratio of bifuenox to benazoline is 60:1 or more
Herbicidal formulation according to claim 6, characterized in that the ratio is 1:1. (8) The herbicidal formulation is a concentrated formulation and has a concentration of 15 to 85%.
% of herbicidal active ingredient. (9) The herbicidal formulation according to claim (8), characterized in that the herbicidal formulation is an emulsifiable concentrate, an aqueous suspension or a wetting powder formulation. (10) A herbicidal formulation according to claim (6) as described in any of Examples 3, 12 and 24 and substantially as hereinbefore described. (11) One or more herbicidal active ingredients selected from bifuenox and benazoline or their salts or esters are used in a method for controlling weeds in cereal crop growing areas, which involves applying the herbicidal active ingredients to the cereal crop growing areas after the cereal crops have germinated. A herbicidal formulation according to any one of claims (6) to (10).