CN103053610A - Glufosinate-aryloxyphenoxypropionic acid herbicide weeding composition - Google Patents

Glufosinate-aryloxyphenoxypropionic acid herbicide weeding composition Download PDF

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CN103053610A
CN103053610A CN2012105856476A CN201210585647A CN103053610A CN 103053610 A CN103053610 A CN 103053610A CN 2012105856476 A CN2012105856476 A CN 2012105856476A CN 201210585647 A CN201210585647 A CN 201210585647A CN 103053610 A CN103053610 A CN 103053610A
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ammonium phosphine
propionic acid
aryloxy group
careless ammonium
acid class
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陈佛祥
刘鹏
颜石雷
张志伟
冷忠国
王礼文
朱刚
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Guangdong Zhongxun Agri Science Corp
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Guangdong Zhongxun Agri Science Corp
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Abstract

The invention discloses a glufosinate-aryloxyphenoxypropionic acid herbicide weeding composition. The glufosinate-aryloxyphenoxypropionic acid herbicide weeding composition comprises glufosinate and an aryloxyphenoxypropionic acid herbicide as active ingredients, and the balance pesticide assistants. A weight ratio of glufosinate to the aryloxyphenoxypropionic acid herbicide in the glufosinate-aryloxyphenoxypropionic acid herbicide weeding composition is in a range of (50: 1) to (1: 1). The glufosinate-aryloxyphenoxypropionic acid herbicide weeding composition comprises 10 to 80wt% of glufosinate and the aryloxyphenoxypropionic acid herbicide. The glufosinate-aryloxyphenoxypropionic acid herbicide weeding composition can be used for preventing and removing weeds in bare places, orchards and field ridges, has effects superior to effects of a single aryloxyphenoxypropionic acid herbicide or glufosinate, reduces a use amount of a pesticide, reduces the adverse influence produced by a pesticide on the ecological environment, and effectively solves the problem of weed resistance to pesticides.

Description

The Herbicidal combinations of grass ammonium phosphine and aryloxy group phenoxy propionic acid class weed killer herbicide
Technical field
The present invention relates to a kind of Herbicidal combinations, is take careless ammonium phosphine and aryloxy group phenoxy propionic acid compounds as active ingredient, is used for preventing and kill off uncultivated area, orchard, farmland weed.
Background technology
The chemical method weeding is one of Main Means of the upper control of agricultural weeds.In recent years, because careless ammonium phosphine large tracts of land is used separately, caused a lot of weeds to develop immunity to drugs.Simultaneously, grass when weeds occur is complicated mutually, not only annual and perennial weed is mixed gives birth to, draft, liana and shrub have concurrently, and weeds emerge uneven, seed, the staggered generation of low age, advanced age weeds, so when the weed killer herbicide kind is used separately, all can show in a certain respect defective and limitation.
Grass ammonium phosphine, chemical formula:
Figure 2012105856476100002DEST_PATH_IMAGE001
Chemical name: (RS)-2-amino-4-(hydroxymethyl oxygen see base) butyric acid ammonium, English name: glufosinate-ammonium, other Chineses: careless fourth phosphine, phosphine oxamate.The effect characteristics: belonging to the acid herbicides of seeing, is glutamine synthetase inhibitor, has the non-selective contact weedicide of part systemic action.In the short time, disorder is sunk in the ammonium metabolism in the plant corpus after the dispenser, and the cytotoxic agent ammonium ion is accumulated in plant corpus, and meanwhile, photosynthesis is reached the weeding purpose by severe inhibition.
Aryloxyphenoxypropanoates class weed killer herbicide is fluorine-containing, heterocycle, the optical activity weed killer herbicide that a class is prevented and kill off grassy weed, and principal item has:
Diclofop-methyl, chemical name: 2[4 (2', 4'-dichlorophenoxy) phenoxy group] methyl propionate.
Efficient fluazifop, chemical name: (R)-the 2-{4-[(5-trifluoromethyl)-2-base-pyridine radicals] the oxygen base } butyl propionate.
Haloxyfop-r-methyl, chemical name: 2-[4-(5-trifluoromethyl-3-chloro-pyridine-2-oxygen base) phenoxy group] methyl propionate.
Quizalotop-ethyl, chemical name: (R)-and 2-[4-(6-chloroquinoxalin-2-yloxy) phenoxy group] ethyl propionate.
Fenoxaprop, chemical name: (R)-and 2-[4-(6-chloro-1,3-benzoxazole-2-base oxygen) phenoxy group] ethyl propionate.
Evil oxalic acid, chemical name: 2-isopropylidene amino-oxygen ethyl (R)-2-[4-(6-chloroquinoxalin-2-yloxy) phenoxy group] propionic ester.
Cyhalofop-butyl, chemical name: (R)-2-[4 (4-cyano group-2-fluorophenoxy) phenoxy group]-butyl propionate
Clodinafop-propargyl, chemical name: R-2-[4-(5-chloro-3-fluoro-2-oxygen yl pyridines)-phenoxy group]-propiolic acid.
Being mixed of different pesticide species is the common methods of the agriculture disease pest and weed of control.By the formulation of pesticide screening, filter out rational prescription, but the actual control efficiency of Effective Raise reduces dosage, reduces cost, delays the drug-fast generation of disease pest and weed, be the important means that agricultural synthesis is administered.The inventor conducts in-depth research the prescription screening of careless ammonium phosphine and aryloxy group phenoxy propionic acid class weed killer herbicide, find that careless ammonium phosphine and aryloxy group phenoxy propionic acid class weed killer herbicide are mixed and in certain mixed ratio scope weeds are had obvious summation action, after further study, finished the present invention.
Being mixed and using of grass ammonium phosphine and aryloxy group phenoxy propionic acid class weed killer herbicide there is no report at present.
Summary of the invention
Technical problem to be solved: the object of the invention is to solve the deficiency that above-mentioned weed killer herbicide is actual in using, a kind of efficient, low-cost, Herbicidal combinations of being conducive to the weeds comprehensive regulation is provided.
Another object of the present invention provides and this Herbicidal combinations is applied to prevent and kill off the weeds such as uncultivated area, orchard, ridge
Technical scheme: for achieving the above object, the invention provides a kind of Herbicidal combinations take careless ammonium phosphine and aryloxy group phenoxy propionic acid class weed killer herbicide as active ingredient, described aryloxy group phenoxy propionic acid class weed killer herbicide is a kind of of diclofop-methyl, efficient fluazifop, haloxyfop-r-methyl, Quizalotop-ethyl, fenoxaprop, propaquizafop, cyhalofop-butyl, quinoline standing grain sugar ester, clodinafop-propargyl.Grass ammonium phosphine and the ratio of weight and number of aryloxy group phenoxy propionic acid class weed killer herbicide in composition are 50:1~1:1, and careless ammonium phosphine and aryloxy group phenoxy propionic acid class weed killer herbicide weight summation percentage by weight in composition are 10%~80%.
Described Herbicidal combinations is prepared into a kind of of aqueous emulsion, suspending agent, wetting powder, water dispersible granules by pesticide production technology.The production technology of various application forms all belongs to existing known technology, does not repeat them here.
The Herbicidal combinations of careless ammonium phosphine provided by the invention and aryloxy group phenoxy propionic acid class can be applicable to prevent and kill off uncultivated area, orchard, farmland weed.
The Herbicidal combinations of careless ammonium phosphine provided by the invention and aryloxy group phenoxy propionic acid class adopts the method for directed spraying to use usually, also can adopt as required upper other operation techniques used of agricultural.
Herbicidal combinations provided by the invention has following beneficial effect.
1, the Herbicidal combinations of careless ammonium phosphine provided by the invention and aryloxy group phenoxy propionic acid class, in certain ratio range, show obvious summation action, the control efficiency of composition is significantly improved than single dose, reduced the using dosage of agricultural chemicals, reduced the medication number of times, reduce drug cost, reduced the adverse effect of agricultural chemicals to ecotope.
2, the Herbicidal combinations of careless ammonium phosphine provided by the invention and aryloxy group phenoxy propionic acid class, the combination of two kinds of active ingredients, not only can remedy careless ammonium phosphine single dose to the deficiency of the drug-resistant type weeds weak effects such as eleusine indica, Bermuda grass, and the weed killer herbicide that can remedy aryloxy group phenoxy propionic acid class can only be prevented and kill off broad leaved weed, sedge weed and the defective substantially invalid to other weeds classes.
3, the Herbicidal combinations of careless ammonium phosphine provided by the invention and aryloxy group phenoxy propionic acid class, two kinds of active ingredient mechanism of action are different, can overcome the shortcoming that long-term single use easily produces resistance, prolong the service life of medicament, to the comprehensive regulation important in inhibiting of Weed Resistance.
4, the Herbicidal combinations of careless ammonium phosphine provided by the invention and aryloxy group phenoxy propionic acid class, use cost is low, and is easy to use, time saving and energy saving, and it applies huge economic benefit and social benefit.
Embodiment
The present invention describes by following specific embodiment, but the invention is not restricted to following specific embodiment.Each component percentage composition is weight percentage among the embodiment.
Embodiment one:Grass ammonium phosphine is Yu fenoxaprop is mixed that the eleusine indica synergy is measured.
1, reagent agent: 96.5% Glufosinate-ammonium; The former medicine of 96% fenoxaprop.
2, for the examination material: eleusine indica (goosegrass) is that research and development centre of Guangdong Zhongxun Agricultural Technology Co., Ltd. weed seed warehouse is preserved.
3, medicament preparation: careless ammonium phosphine solution: accurately take by weighing the 0.276g96.5% Glufosinate-ammonium, dissolve with 0.2mlDMF, add the clear water 80ML that contains the 0.1%Tween80 emulsifier, stir, be mixed with careless ammonium phosphine 525g a.i./ha mother liquor, again with the clear water that contains the 0.1%Tween80 emulsifier be diluted to 420,270g a.i./ha concentration is for subsequent use.
Fenoxaprop solution: accurately take by weighing the former medicine of 0.0032g96% fenoxaprop, dissolve with 0.2ml DMF, add the clear water 80ML that contains the 0.1%Tween80 emulsifier, stir, be mixed with fenoxaprop 60 g a.i./ha mother liquors, again with the clear water that contains the 0.1%Tween80 emulsifier be diluted to 30,18g a.i./ha concentration is for subsequent use.
Contrast solution: 0.2mLDMF adds the water that 80mL contains the 0.1%Tween80 emulsifier.
4, test method: adopt potted plant cauline leaf facture (NY/T 1155.4-2006): at the in-built quantitative soil of the polypots of high 6cm, diameter 9cm, will be for the sowing of examination target weed seed 15-20 grain in polypots, be placed on cultivation in the greenhouse after covering the thick fine earth of 0.5-1cm, treat that weeds grow to the 2-4 leaf phase and carry out cauline leaf spraying processing, every alms bowl spraying liquid 1mL, every processing repeats for 4 times, and establishes the contrast that is treated to that does not contain medicament.The examination material places in the greenhouse in and cultivates after processing, the growing state of routine observation target weeds, and be injured symptom and growth inhibition situation of range estimation target behind the 20d, and claim acrial part fresh weight or strain fresh weight, with the toxicity action of target fresh weight inhibiting rate evaluation medicament to the target weeds.
5, data survey and statistical analysis.
5.1 investigation method:
Range estimation target be injured symptom and growth inhibition situation are processed behind the 20d in test, and claim to calculate fresh weight inhibiting rate (%) by the acrial part fresh weight.
Figure 628918DEST_PATH_IMAGE002
5.2 synergy evaluation method
Estimate weed killer herbicide mode of application (NY/T 1155.7-2006) with the Gowing method, formula is as follows:
Figure 700386DEST_PATH_IMAGE003
In the formula: X is careless ammonium phosphine consumption fresh weight preventive effect to eleusine indica when being P; Y when the fenoxaprop consumption is Q to the fresh weight preventive effect of barnyard grass; E 0When being P for careless ammonium phosphine consumption the fresh weight preventive effect+fenoxaprop consumptions of eleusine indica being Q to the fresh weight preventive effect of eleusine indica; E is the actual preventive effect of Mixed Pharmacy.
Evaluation criterion: E-E 0>10% is summation action; E-E 0<-10% is antagonism; E-E 0Value is addition between theoretical value ± 10%.
6, careless ammonium phosphine makes up the toxicity test result that eleusine indica is suppressed with fenoxaprop is mixed.Grass ammonium phosphine is with fenoxaprop and the herbicidal effect measurement result that makes up eleusine indica that is mixed thereof see Table 1.As seen careless ammonium phosphine is Yu fenoxaprop shows summation action to eleusine indica, its E-E with the combination that is mixed of 270+18,270+30,720+60,420+18,420+30,420+60,525+18,525+30,525+60 respectively 0Value is respectively 5.76,4.21,3.29,8.25,6.42,4.10,5.29,3.46,3.21.Combination is feasible to grass ammonium phosphine Yu fenoxaprop is mixed.
Table 1, the careless ammonium phosphine toxicity test that combination suppresses eleusine indica Yu fenoxaprop is mixed is table as a result.
Figure 11281DEST_PATH_IMAGE004
Embodiment two: the Herbicidal combinations preparation method of careless ammonium phosphine and aryloxy group phenoxy propionic acid class.
Preparation method embodiment 1: 15% careless ammonium phosphine efficient fluazifop aqueous emulsion:
Grass ammonium phosphine 13%,
Efficient fluazifop 2%,
1-METHYLPYRROLIDONE (solvent) 10%,
Naphthalene (bleeding agent) 2%,
Calcium dodecyl benzene sulfonate (emulsifier) 6%,
The newborn 600# phosphate of farming (emulsifier) 5%,
Organosilicon (defoamer) 3%,
Xanthans (stabilizing agent) 0.5%,
Water complements to 100%.
With above-mentioned material in proportion method evenly mix, dissolving makes oil phase; Careless ammonium phosphine and water mixing are made water; Under high-speed stirred, oil phase and water are mixed, make 15% careless ammonium phosphine efficient fluazifop aqueous emulsion.
Preparation method embodiment 2:20% careless ammonium Lin fenoxaprop suspending agent:
Grass ammonium phosphine ammonium salt 18.5%,
Fenoxaprop 1.5%,
The newborn 1601#(emulsifier of farming) 10%,
Soya-bean oil (organic solvent) 5%,
Triphenyl vinyl phenol polyoxyethylene poly-oxygen propylene aether (wetting agent) 5%,
Alkylphenol polyoxyethylene formaldehyde condensation products sulphate (dispersant) 4%,
Bentonite (thickener) 3%,
Xanthans (stabilizing agent) 0.3%,
Organosilicon (defoamer) 0.3%,
APG (surfactant) 5%,
Deionized water (medium) is supplemented to 100%.
Above-mentioned material is pulverized in proportion in advance, added in the sand mill and grind, allotment makes 20% careless ammonium Lin fenoxaprop suspending agent after high shear mixing.
Preparation method embodiment 3: 30% careless ammonium phosphine Quizalotop-ethyl wetting powder:
Grass ammonium phosphine 27%,
Quizalotop-ethyl 3%,
Neopelex (wetting agent) 5%,
Sodium lignin sulfonate (dispersant) 8%,
Talcum powder (filler) 3%,
White carbon (filler) 4%,
Attapulgite (filler) is supplemented to 100%.
Above-mentioned material entered in the blender after the coarse crushing in proportion mix, behind air-flow crushing, namely make again the different Quizalotop-ethyl wetting powder of 30% careless ammonium phosphine.
Preparation method embodiment 4:40% careless ammonium phosphine effective haloxyfop water dispersive granule:
Grass ammonium phosphine 36%,
Haloxyfop-r-methyl 4%,
Sodium Laurylsulfate (wetting agent) 5%,
Polycarboxylate (dispersant) 6%,
Sodium chloride (disintegrant) 2%,
Polyethylene glycol (binding agent) 3%,
Soluble starch (stabilizing agent) 3%,
Bentonite (filler) is supplemented to 100%.
In proportion method pulverizing of above-mentioned material, granulation, drying, screening are made 40% careless ammonium phosphine effective haloxyfop water dispersive granule.
Embodiment three:The Herbicidal combinations of grass ammonium phosphine and aryloxy group phenoxy propionic acid class is prevented and kill off the citrus orchard weeds.
Reagent agent and dispenser dosage:
(1) 15% careless ammonium phosphine efficient fluazifop aqueous emulsion (13% careless ammonium phosphine: 2% efficient fluazifop), effective ingredient consumption 800a.i.g/ha.
(2) 20% careless ammonium Lin fenoxaprop suspending agents (18.5% careless ammonium phosphine: 1.5% fenoxaprop), effective ingredient consumption 800a.i.g/ha.
(3) 30% careless ammonium phosphine Quizalotop-ethyl wetting powders (27% careless ammonium phosphine: 3% Quizalotop-ethyl wetting powder), effective ingredient consumption 800a.i.g/ha.
(4) 40% careless ammonium phosphine effective haloxyfop water dispersive granules (36% careless ammonium phosphine: 4% haloxyfop-r-methyl), effective ingredient consumption 800a.i.g/ha.
(5) 20% careless ammonium phosphine aquas, effective ingredient consumption 1050a.i.g/ha.
(6) 10.8% fenoxaprop aqueous emulsions, effective ingredient consumption 80a.i.g/ha.
Spraying time: the weeds 2-7 leaf phase, be watered directed spraying.
Result of the test: see Table 2.As can be seen from the test results, after the dispenser 15 days, the preventive effect that the Herbicidal combinations of careless ammonium phosphine of the present invention and aryloxy group phenoxy propionic acid class weed killer herbicide is prevented and kill off the citrus orchard weeds reaches more than 97.66%, the weed killer herbicide that preventive effect obviously is better than careless ammonium phosphine and aryloxy group phenoxy propionic acid class uses separately, reduced the using dosage of agricultural chemicals, reduce the adverse effect of agricultural chemicals to ecotope, effectively administered the herbicide resistance problem.
Unless table 2, anti-citrus orchard weeds result of the test.
Figure 2012105856476100002DEST_PATH_IMAGE005

Claims (6)

1. the Herbicidal combinations of a careless ammonium phosphine and aryloxy group phenoxy propionic acid class weed killer herbicide is characterized in that, active ingredient is careless ammonium phosphine and aryloxy group phenoxy propionic acid class weed killer herbicide, and surplus is insecticides adjuvant.
2. the Herbicidal combinations of careless ammonium phosphine according to claim 1 and aryloxy group phenoxy propionic acid class weed killer herbicide, it is characterized in that, described aryloxy group phenoxy propionic acid class weed killer herbicide is a kind of of diclofop-methyl, efficient fluazifop, haloxyfop-r-methyl, Quizalotop-ethyl, fenoxaprop, propaquizafop, cyhalofop-butyl, quinoline standing grain sugar ester, clodinafop-propargyl.
3. the Herbicidal combinations of careless ammonium phosphine according to claim 1 and aryloxy group phenoxy propionic acid class weed killer herbicide is characterized in that, careless ammonium phosphine and the ratio of weight and number of aryloxy group phenoxy propionic acid class weed killer herbicide in composition are 50:1~1:1.
4. the Herbicidal combinations of careless ammonium phosphine according to claim 1 and aryloxy group phenoxy propionic acid class weed killer herbicide is characterized in that, careless ammonium phosphine and aryloxy group phenoxy propionic acid class weed killer herbicide weight summation percentage by weight in composition are 10%~80%.
According to claim 1 careless ammonium phosphine and the Herbicidal combinations of aryloxy group phenoxy propionic acid class weed killer herbicide, it is characterized in that, described Herbicidal combinations becomes a kind of of aqueous emulsion, suspending agent, wetting powder, water dispersible granules when reality is used.
6. the Herbicidal combinations of careless ammonium phosphine according to claim 1 and aryloxy group phenoxy propionic acid class weed killer herbicide is characterized in that, is used for preventing and kill off uncultivated area, orchard, farmland weed.
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CN103688994A (en) * 2013-12-31 2014-04-02 利尔化学股份有限公司 Weeding composition with glufosinate and efficient haloxyfop-methyl, and preparation method of weeding composition
CN105557748A (en) * 2015-12-30 2016-05-11 北京明德立达农业科技有限公司 Weedicide composition and application thereof
CN107136124A (en) * 2017-05-17 2017-09-08 广西品位生物科技有限公司 A kind of biological weed killer
CN107467059A (en) * 2016-06-07 2017-12-15 湖北润增绿色植保有限公司 A kind of herbicidal composition and preparation and its application
WO2018078478A1 (en) * 2016-10-25 2018-05-03 Upl Limited Stable herbicidal compositions
CN108576047A (en) * 2018-08-08 2018-09-28 许昌市建安区昌盛日化实业有限公司 A kind of ternary weeding composition and herbicidal composition of Glufosinate-ammoniumpesticideng
CN109042720A (en) * 2018-07-25 2018-12-21 安徽华星化工有限公司 A kind of glufosinate-ammonium, Quizalotop-ethyl, Oxyfluorfen herbicidal composition
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WO2019030087A1 (en) * 2017-08-09 2019-02-14 Basf Se Herbicidal mixtures comprising l-glufosinate or its salt and at least one lipid biosynthesis inhibitor
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WO2019030090A1 (en) * 2017-08-09 2019-02-14 Basf Se Herbicidal mixtures comprising l-glufosinate and their use in rice cultures
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WO2019030091A3 (en) * 2017-08-09 2019-05-02 Basf Se Herbicidal mixtures comprising l-glufosinate and their use in cotton cultures
CN114617132A (en) * 2022-04-20 2022-06-14 浙江新安化工集团股份有限公司 Weeding composition, herbicide and preparation method

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CN103688994A (en) * 2013-12-31 2014-04-02 利尔化学股份有限公司 Weeding composition with glufosinate and efficient haloxyfop-methyl, and preparation method of weeding composition
CN105557748B (en) * 2015-12-30 2018-06-05 北京明德立达农业科技有限公司 A kind of herbicidal composition and application thereof
CN105557748A (en) * 2015-12-30 2016-05-11 北京明德立达农业科技有限公司 Weedicide composition and application thereof
CN107467059A (en) * 2016-06-07 2017-12-15 湖北润增绿色植保有限公司 A kind of herbicidal composition and preparation and its application
US11259525B2 (en) 2016-10-25 2022-03-01 Upl Limited Stable herbicidal compositions
WO2018078478A1 (en) * 2016-10-25 2018-05-03 Upl Limited Stable herbicidal compositions
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CN109862789B (en) * 2016-10-25 2022-04-29 Upl 有限公司 Stable herbicidal compositions
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CN109862789A (en) * 2016-10-25 2019-06-07 Upl 有限公司 Stable Herbicidal combinations
CN107136124A (en) * 2017-05-17 2017-09-08 广西品位生物科技有限公司 A kind of biological weed killer
WO2019030091A3 (en) * 2017-08-09 2019-05-02 Basf Se Herbicidal mixtures comprising l-glufosinate and their use in cotton cultures
EP3440939A1 (en) * 2017-08-09 2019-02-13 Basf Se Herbicidal mixtures comprising l-glufosinate
WO2019030095A3 (en) * 2017-08-09 2019-03-21 Basf Se Herbicidal mixtures comprising l-glufosinate and their use in corn cultures
WO2019030086A3 (en) * 2017-08-09 2019-03-21 Basf Se Herbicidal mixtures comprising l-glufosinate and their use in canola cultures
WO2019030090A1 (en) * 2017-08-09 2019-02-14 Basf Se Herbicidal mixtures comprising l-glufosinate and their use in rice cultures
WO2019030088A1 (en) * 2017-08-09 2019-02-14 Basf Se Herbicidal mixtures comprising l-glufosinate and their use in cereal cultures
WO2019030087A1 (en) * 2017-08-09 2019-02-14 Basf Se Herbicidal mixtures comprising l-glufosinate or its salt and at least one lipid biosynthesis inhibitor
WO2019030097A3 (en) * 2017-08-09 2019-03-21 Basf Se Herbicidal mixtures comprising l-glufosinate and their use in soybean cultures
US11666053B2 (en) 2017-08-09 2023-06-06 Basf Se Herbicidal mixtures comprising L-glufosinate and their use in cotton cultures
US11589591B2 (en) 2017-08-09 2023-02-28 Basf Se Herbicidal mixtures comprising L-glufosinate and their use in corn cultures
US11363818B2 (en) 2017-08-09 2022-06-21 Basf Se Herbicidal mixtures comprising L-glufosinate and their use in soybean cultures
CN109042720A (en) * 2018-07-25 2018-12-21 安徽华星化工有限公司 A kind of glufosinate-ammonium, Quizalotop-ethyl, Oxyfluorfen herbicidal composition
CN108576047A (en) * 2018-08-08 2018-09-28 许昌市建安区昌盛日化实业有限公司 A kind of ternary weeding composition and herbicidal composition of Glufosinate-ammoniumpesticideng
CN114617132A (en) * 2022-04-20 2022-06-14 浙江新安化工集团股份有限公司 Weeding composition, herbicide and preparation method

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Application publication date: 20130424