The invention relates to a method for the preparation of bis(fluorosulfonyl)-imide, the method starts from bis(chlorosulfonyl)-imide or its respective derivatives, which is reacted with HF in the presence of chlorosulfonyl isocyanate, and uses a certain extraction step for extraction of bis(fluorosulfonyl)-imide from an aqueous solution; the invention is also useful for the preparation of certain salts of bis(fluorosulfonyl)-imide and its derivatives.

BACKGROUND OF THE INVENTION

In the following text, the following meanings are used, if not otherwise stated:

ACN acetonitrile;

C1SI bis(chlorosulfonyl)-imide, that is compound of formula (2);

chlorosulfonyl isocyanate, that is compound of formula (3);

CSOS, CSA chlorosulfonic acid;

DCB dichlorobenzene, if not otherwise stated it is 1 ,2-dichlorobenzene;

DCE dichloroethane, if not otherwise stated it is 1 ,2-dichloroethane;

DCM dichloromethane;

DFAC1 difluoro acetic acid chloride;

DFAF difluoro acetic acid fluoride;

halide stands for fluoride, chloride, bromide or iodide, preferably fluoride, chloride or bromide, more preferably fluoride or chloride, even more preferably chloride;

halogen F, CI, Br or I, preferably F, CI or Br, more preferably F or CI.

HFSI bis(f uorosulfonyl)-imide, that is compound of formula (1);

LiFSI Lithium bis(fluorosulfonyl)-imide, that is compound of formula (5);

OO

Th

F F

(5)

©

Mp melting point;

MTBE methyl-tert butyl ether ;

TEA triethylamine;

THF tetrahydrofuran;

MeTHF 2-methyl tetrahydrofuran;

VN valeronitrile;

wt%, % by weight percent by weight.

For the purpose of this invention, distillation and evaporation means essentially the same, that is a vaporizing of a volatile compound; this is done preferably to remove said volatile compound from a mixture. The difference between distillation and evaporation lies primarily in the type of devices used for said vaporizing. Therefore the two terms distillation and evaporation are used interchangeably herein, if not stated otherwise.

Salts of bis(fluorosulfonyl)-imide, as for example LiFSI, are used for the production of electrolytes in electrochemical devices, examples are lithium ion batteries. HFSI is an intermediate used for the production salts of bis(fluorosulfonyl)-imide.

US 2013/0331609 Al discloses a method for producing a metal salt of fluorosulfonyl imide in two steps, in a first step di(chlorosulfonyl)imide is reacted with the flourinating agent NH4F providing the ammonium di(fluorosulfonyl)imide, in a second step the ammonium

di(fluorosulfonyl)imide is converted with LiOH to lithium di(flurosulfonyl)imide. The first step is done in the presence of a solvent, in the example acetonitrile is used and the reaction was performed under reflux conditions at 80 to 84°C for 4 hours.

WO 2009/123328 Al discloses a method for preparation of metal salts of symmetrical and asymmetrical fluorosulfonylimide in a solvent by a reaction of a respective symmetrical or asymmetrical chlorosulfonylimide with a fluoride compound containing at least one element selected from the group consisting of elements of Group 11 to Group 15 and Period 4 to Period 6 (excluding arsenic and antimony), these metal salts are then converted in a second step to salts of various amines and symmetrical and asymmetrical fluorosulfonylimide in a cation exchange reaction.

US 2015/0246812 Al discloses a method for the preparation of symmetrical and

asymmetrical f ourosulfonylimides from symmetrical and asymmetrical chlorosulfonylimides, wherein the reaction is done in an organic solvent.

WO 2015/012897 Al discloses a method for producing FSI from CISI using HF, wherein the HCl that is produced by the reaction is selectively removed during the reaction to produce HFSI in at least 80% yield. The reaction takes place at ambient (e.g. atmospheric) pressure. Reaction times are much longer than 3 hours. Both requirements, the rather long reaction times and the requirement for separating HCl from the reaction mixture during the reaction, require a special continuous stirred-tank reactor ("CSTR") set-up with a device for the required separation of HCl during the reaction when carrying out the reaction in a continuous way. To do the reaction in a simple continuously working tube shaped reactor creates problems.

Also disclosed is the exchange of Br and I instead of CI against F, that is the conversion of hydrogen bis(halosulfonyl)imide (HXSI) with hydrogen fluoride for producing hydrogen bis(fluorosulfonyl)imide (HFSI), where each X is independently a nonfluoro-halide, such as CI, Br, or I.

WO 2015/004220 Al discloses a method for the preparation of imidodisulfuryl compounds in a continuous reaction at elevated temperatures.

US 7,919,629 B2 discloses in Example 10 the reaction of distilled CISI, which was obtained by distillation under vacuum, with HF and reports i.a. 55% yield for the example with 2 h at 130°C. Reproduction of this example 10 in Comparative Example (i) and determination of the CSI content revealed a residual content of 0.3 wt-% of CSI in the starting material CISI which was obtained by said distillation under vacuum. Example 8 according to present invention shows a considerable higher yield of 82%.

Rolf Appel et al, Chemische Berichte, 1962, 95, 1753-1755, discloses on page 1755 the preparation of CISI from CSI and CSOS. The final product is obtained from distillation of the crude product under vacuum. According to Comparative Example (i) a residual content of 0.3 wt-% can be assumed in the CISI after distillation under vacuum.

EP 0 055 899 A2 discloses in example 1 the preparation of CISI from CSI and CSOS. The final product is obtained from distillation of the crude product under vacuum, and this distilled product is then used for further reactions. According to Comparative Example (i) a residual content of 0.3 wt-% can be assumed in the CISI after distillation under vacuum.

EP 2 662 332 A discloses in example 4 a method for preparation of ammonium

di(fluorosulfonyl)imide by reacting di(chlorosulfonyl)imide with NH4F in ethyl acetate.

EP 2 660 196 A discloses a method for preparation of ammonium di(fluorosulfonyl)imide by reacting di(chlorosulfonyl)imide and NH4F (HF)P. According to [0030] the reaction is done in an organic solvent, that is preferably dewatered prior to use, or it is done in the absence of a solvent. Example 1 uses acetonitrile as solvent.

EP 2 674 395 A discloses in [102] a process for producing the ammonium salt of

di(fluorosulfonyl)-imide, wherein anhydrous hydrogen fluoride in acetonitrile is reacted with ammonium di(chlorosulfonyl)imide. Addition of ethylacetat and water follows, the organic phase was separated and the water phase was extracted 3 times with ethyl acetate. The organic phases obtained in the extraction operations were combined, and the combined organic phase was washed with water, and ammonium di(fluorosulfonyl)-imide was isolated from the organic phase. The ammonium di(fluorosulfonyl)-imide stays in the organic phase all the time.

EP 2 505 551 A1 discloses in Experimental Example 1 a fluorination reaction between di(chlorosulfonyl) imide and ZnF2. The reaction is done in butyl acetate. The reaction solution is added after the reaction to ammonia water. Two phases are formed, the water phase is removed, the desired fluorosulfonylimide is in the organic layer in form of the ammonium salt of di(chlorosulfonyl) imide.

EP 2 578 533 Al discloses in Experimental Example 1-1 a fluorination reaction between di(chlorosulfonyl) imide and ZnF2. The reaction is done in butyl acetate. The reaction solution is added after the reaction to ammonia water. Two phases are formed, the water phase is removed, the desired fluorosulfonylimide is in the organic layer in form of the ammonium salt of di(chlorosulfonyl) imide.

There was a need for a method for preparation of salts of bis(fluorosulfonyl)-imide starting from C1SI that does not require mandatorily a solvent in the fluorination reaction, that does not require mandatorily metal salts in the fluorination reaction, and that has few steps, that produces salts of bis(fluorosulfonyl)-imide in high yields and where the fluorination reaction both batch wise and in a continuous manner in a continuous reactor, and also in a continuous tube shape reactor. The method should allow for the fluorination with HF, and should not require the use of sources of F in other forms than HF, such as NH4F or ZnF2.

The method should allow for purification of HFSI that can be easily incorporated into the method for preparation of HFSI, which allows for example removal of water soluble impurities.

Furthermore the method should allow for the preparation and purification of HFSI without mandatorily requiring the formation of a salt of HFSI such as an ammonium salt.

Furthermore the method should allow for subsequent preparation of salts of HFSI, such as

LiFSI. The method should allow the preparation of said salts in high yields. It should allow to be done both batch wise and in a continuous manner in a continuous reactor, and also in a continuous tube shape reactor.

The method should not require the separation of HC1 during the fluorination reaction for enhancement of the yield, as it is disclosed in WO 2015/012897 Al and should allow to carry out the fluorination reaction in relatively short reaction times.

It was found that it is possible to purify HFSI from water and not from an organic solvent, and to extract HFSI from water with an organic solvent, without mandatorily requiring the use of ammonia or the formation of the ammonium salt of HFSI.

This purification can be used for the preparation of HFSI and in the preparation of salts of HFSI.

The method of present invention for purification or preparation of HFSI and for preparation of salts of bis(fluorosulfonyl)-imide can start from C1SI and can proceed via HFSI as

intermediate, it does not require a solvent in the fluorination reaction, it does not require metal salts in the fluorination reaction, it uses F in form of HF, it has few steps, it produces HFSI in the fluorination reaction in high yields in spite of the poor solubility and miscibility of HF in C1SI and vice versa, and the fluorination reaction can be done both batch wise or in a continuous manner and also in a continuous tube shape reactor, and the method is

distinguished by short reaction times especially in the fluorination reaction.

The method does not require the separation of HC1 during the fluorination reaction, which is formed by the fluorination reaction, and still provides the intermediate HFSI in good yields. This was unexpected in view of the disclosure of WO 2015/012897 Al . Furthermore it was unexpected that the use of C1SI containing CSI in the reaction with HF provides for significantly higher yield than the use of C1SI which was obtained by distillation as disclosed in US 7,919,629 B2. This is exemplified herein with Comparative Example (i) versus

Example 8.

None of the prior art discloses the use of C1SI for the preparation of HFSI, where this C1SI contains deliberately CSI, instead the various preparation examples in the prior art always end with a distillation of the C1SI, which is clearly meant for purification of C1SI for further use, and the residual content of CSI after such a distillation was determined to be only 0.3 wt-%. There is also no motivation or hint in the prior art to carry out the preparation of HFSI in the presence of CSI, and there is no hint in the prior art that the presence of CSI might increase the yield of HFSI. Especially for the use of LiFSI in batteries, the purity of LiFSI is a critical issue and various patent applications take this requirement into consideration by claiming LiFSI in high purities. Also for this reason the skilled person would not consider starting with a C1SI which is not purified, for example by distillation, and that would therefore contain major amounts of impurities, these impurities leading to by products in the reactions to HFSI and in the reactions to the salts of HFSI. These by products would need to be separated in order to attain the high purity profile of LiFSI that is required in batteries.

The fluorination reaction can be done with relatively short reaction times compared to the disclosure in the prior art, which allows to do the fluorination reaction not only batch wise, but also in continuous manner, also in a continuous tube shape reactor.

SUMMARY OF THE INVENTION

Subject of the invention is a method for preparation of compound of formula (I)

the method comprises a step STEP1, a step STEPMIX and a step STEPEXTR;

STEP1 comprises a reaction REAC 1-1;

in REAC 1-1 a compound of formula (II) is reacted with HF

at a temperature TEMP 1-1, TEMP 1-1 is at least 80°C;

wherein at the beginning of REACl-1 compound of formula (III) is present in the reaction mixture;

the amount of compound of formula (III), that is present in the reaction mixture at the

beginning of REACl-1, is at least 0.5%, the % are % by weight and are based on the weight of the reaction mixture at the beginning of REACl-1 excluding from said weight of the reaction mixture the weight of the HF;

X is identical with XI or with X2;

XI and X2 are identical or different and independently from each other selected from the group consisting of F, CI, Br, I, RESF, and tolyl;

with the proviso that at least one of the residues XI and X2 is CI, Br, or I;

RESF is fluorinated Ci_9 alkyl, which is unsubstituted or substituted by a substituent OCF3;

in STEPMIX compound of formula (I) is mixed with water by a mixing MIX, MIX provides a mixture MIXWAT, MIXWAT is the mixture of compound of formula (I) with water,

in STEPEXTR compound of formula (I) is extracted from MIXWAT by an extraction EXTR, EXTR is the extraction of compound of formula (I) from MIXWAT with an organic solvent SOLVORG, SOLVORG is an organic solvent that forms a biphasic system with water;

EXTR provides compound of formula (I) in form of a solution SOLCOMP 1 , SOLCOMP 1 is the solution of compound of formula (I) in SOLVORG.

DETAILED DESCRIPTION OF THE INVENTION

"Fluorinated alkyl" means, that at least one H is exchanged for F.

The reaction product of REACl-1 is compound of formula (I).

Preferably,

RESF is fluorinated Ci_6 alkyl, which is unsubstituted or substituted by a substituent OCF3;

more preferably,

RESF is fluorinated Ci_4 alkyl, which is unsubstituted or substituted by a substituent OCF3;

even more preferably,

RESF is fluorinated Ci_2 alkyl, which is unsubstituted or substituted by a substituent OCF3.

Especially, any RESF herein is a perfluoroalkyl.

Specific embodiments of RESF are for example CF3, CHF2, CH2F, C2F5, C2HF4, C2H2F3, C2H3F2, C2H4F, C3F7, C3HF6, C3H2Fs, C3H4F3, C3H6F, C4F9, C4H2F7, C4H4F5, C4HsF,

C5F11, the C 5 the H 10 F, the C 3 F 5 ( OCF ) 3 , the C 2 F 4 ( OCF ) 3 , the C 2 the H 2 F 2 ( OCF ) 3 , the CF 2 ( OCF ) 3 , the C 6 Fi 3 , the C 6 Hi 2 F, C7F15,
preferably CF3, CHF2, CH2F, fluoroethyl, difluoroethyl, 2,2,2-trifluoroethyl, pentafluoroethyl, 3,3,3-trifluoropropyl, a perfluoro-n-propyl, fluoropropyl, perfluoroisopropyl, fluorobutyl, 3,3,4,4,4-pentafluorobutyl, perfluoro-n-butyl, perfluoroisobutyl, perfluoro-t-butyl, perfluoro-sec-butyl, fluoropentyl, perfluoropentyl, perfluoroisopentyl, perfluoro-t-pentyl, fluorohexyl, perfluoro-n-hexyl and perfluoroisohexyl;

more preferably, trif uoromethyl, pentafluoroethyl and perfluoro-n-propyl;

even more preferably, trifluoromethyl and pentafluoroethyl.

Preferably,

XI and X2 are identical or different and independently from each other selected from the group consisting of F, CI, Br, I, RESF, RESF being preferably Ci_6 perfluoroalkyl, and tolyl;

more preferably,

XI and X2 are identical or different and independently from each other selected from the group consisting of F, CI, Br, RESF, RESF being preferably Ci_6 perfluoroalkyl, and tolyl;

even more preferably,

XI and X2 are identical or different and independently from each other selected from the group consisting of F, CI, and RESF, RESF being preferably Ci_4 perfluoroalkyl;

especially,

XI and X2 are identical or different and independently from each other selected from the group consisting of CI, and RESF, RESF being preferably Ci_2 perfluoroalkyl; more especially,

XI and X2 are identical or different and independently from each CI or CF3.

Preferably,

X is selected from the group consisting of F, CI, Br, I, RESF, and tolyl.

More preferably,

X is selected from the group consisting of F, CI, Br, I, RESF, RESF being preferably Ci_6 perfluoroalkyl, and tolyl.

Even more preferably,

X is selected from the group consisting of F, CI, Br, RESF, RESF being preferably Ci_6 perfluoroalkyl, and tolyl.

Especially,

X is selected from the group consisting of F, CI, and RESF, RESF being preferably Ci_4 perfluoroalkyl.

More especially,

X is selected from the group consisting of CI, and RESF, RESF being preferably Ci_2

perfluoroalkyl.

Even more especially,

X is Cl or CF3.

Specific embodiments of compound of formula (I) are compound of formula (1) and

compound of formula (1-CF3).

Specific embodiments of compound of formula (II) are compound of formula (2) and

compound of formula (2-CF3).

Specific embodiment of compound of formula (III) is compound of formula (3).

Compound of formula (III) can also react during REACl-1, and if this happens then

compound of formula (III) is not necessarily present in REACl-1 from the beginning to the end. So the terminology "at the beginning of REACl-1 compound of formula (III) is present in the reaction mixture" comprises also the case that REACl-1 is started in the presence of compound of formula (III), or that compound of formula (III) is present in the reaction mixture at the beginning of REACl-1, and it comprises also the case where

compound of formula (III) is present in REACl-1 or during REACl-1, and it comprises also the case that the amount of compound of formula (III) decreases during REACl-1. Preferably, the amount of compound of formula (III), that is present in the reaction mixture at the beginning of REACl-1, is at least 0.5%, more preferably at least 0.75%, even more preferably at least 1%, especially at least 2%, more especially at least 3%, even more especially at least 4%, the % are % by weight and are based on the weight of the reaction mixture at the beginning of REACl-1 excluding from said weight of the reaction mixture the weight of the HF.

Preferably, not more than 50%, more preferably not more than 25%, even more preferably not more than 15%, especially not more than 12.5%, more especially not more than 10%, of compound of formula (III) is present in the reaction mixture at the beginning of

REACl-1, the % are % by weight and are based on the weight of the reaction mixture at the beginning of REACl-1 excluding from said weight of the reaction mixture the weight of the HF.

Any of the lower limits can be combined with any of the upper limits of the amount of

compound of formula (III) that is present at the beginning of REACl-1.

Preferably, REACl-1 is done in a continuous way.

STEP1 can comprise a purification PUR1, in PUR1 compound of formula (I) is purified by extraction, distillation, evaporation, membrane assisted separation, or a combination thereof;

preferably by distillation or evaporation.

PUR1 is done after REACl-1.

Membrane assisted separation is preferably membrane assisted pervaporation or vapor

permeation, or membrane assisted filtration.

Preferably, distillation or evaporation is done by using a film evaporator, wiped film

evaporator, falling film evaporation, rectification, flash distillation, short path distillation, or a combination thereof;

more preferably distillation or evaporation is done by using a falling film evaporation,

rectification, wiped film evaporator, or a combination thereof;

even more preferably, distillation or evaporation is done by using a falling film evaporation combined with a rectification or wiped film evaporator.

Preferably, PUR1 is done continuously.

Further subject of the invention is a method for purification of compound of formula (I), wherein the method comprises the step STEPMIX and the step STEPEXTR.

Preferably, MIXWAT has a content of from 0.5 to 50%, more preferably of from 0.5 to 35%, even more preferably of from 0.5 to 20%, especially of from 1 to 10%, more especially of from 2 to 8%, of compound of formula (I), the % are % by weight and are based on the combined amount of water and compound of formula (I), preferably based on the weight of MIXWAT.

Therefore compound of formula (I) and water are mixed in such a ratio so as to obtain said content of compound of formula (I) in water.

MIX can be done by charging water to compound of formula (I) or by charging compound of formula (I) to water.

MIX can be done batchwise or in a continuous way, preferably MIX is done continuously. Preferably, MIX is done preferably by using a mixer, preferably a static mixer. Such mixers are known to the skilled person.

Preferably, MIX is done in the absence of an organic solvent.

Preferably, MIX is done in the absence of a solvent other than water.

Preferably, MIX is done in the absence of an organic base containing nitrogen.

Preferably, MIX is done in the absence of a salt of an organic base containing nitro;

Preferably, MIX is done in the absence of an organic base.

Preferably, MIX is done in the absence of a salt of an organic base.

Preferably, MIX is done in the absence of a base.

Preferably, MIX is done in the absence of a salt of a base.

Preferably, MIX is done at a temperature of from -5 to 50°C, more preferably of from 0 to 40°C.

Preferably, MIX is done at ambient pressure. It is possible to do MIX at elevated pressure, preferably at a pressure of from ambient pressure to 10 bar, more preferably of from ambient pressure to 5 bar, even more preferably of from ambient pressure to 2.5 bar.

Preferably, the mixing time TIMEMIX of MIX is from 1 min to 2 h, more preferably from 2 min to 1.5 h, even more preferably 5 min to 1 h, especially from 5 min to 30 min. In another preferred embodiment, TIMEMIX is from 5 min to 10 h.

Preferably, SOLVORG is selected from the group consisting of carbonate-based solvent, aliphatic ether-based solvent, ester-based solvent, amide -based solvent, nitro-based solvent, sulfur-based solvent, nitrile-based solvent, keton based solvent, and mixtures thereof.

Preferably, SOLVORG is selected from the group consisting

We Claims.

1. Method for preparation of compound of formula (I)

the method comprises a step STEP1, a step STEPMIX and a step STEPEXTR;

STEP1 comprises a reaction REAC 1-1;

in REAC 1-1 a compound of formula (II) is reacted with HF

at a temperature TEMP 1-1, TEMP 1-1 is at least 80°C;

wherein at the beginning of REACl-1 compound of formula (III) is present in the reaction mixture;

the amount of compound of formula (III), that is present in the reaction mixture at the

beginning of REACl-1, is at least 0.5%, the % are % by weight and are based on the weight of the reaction mixture at the beginning of REACl-1 excluding from said weight of the reaction mixture the weight of the HF;

X is identical with XI or with X2;

XI and X2 are identical or different and independently from each other selected from the group consisting of F, CI, Br, I, RESF, and tolyl;

with the proviso that at least one of the residues XI and X2 is CI, Br, or I;

RESF is fluorinated Ci_g alkyl, which is unsubstituted or substituted by a substituent OCF3;

in STEPMIX compound of formula (I) is mixed with water by a mixing MIX, MIX provides a mixture MIXWAT, MIXWAT is the mixture of compound of formula (I) with water,

in STEPEXTR compound of formula (I) is extracted from MIXWAT by an extraction EXTR, EXTR is the extraction of compound of formula (I) from MIXWAT with an organic solvent SOLVORG, SOLVORG is an organic solvent that forms a biphasic system with water;

EXTR provides compound of formula (I) in form of a solution SOLCOMPl, SOLCOMPl is the solution of compound of formula (I) in SOLVORG.

2. Method for preparation of a compound of formula (V);

nl- M

nl is 1, 2 or 3;

M is selected from the group consisting of alkaline metal, alkaline earth metal and Al;

the method comprises STEP1 and a step STEP2;

with STEP1 as in claim 1;

in STEP2 the H of compound of formula (I) is exchanged against M.

3. Method according to claim 2, wherein

M is selected from the group consisting of Na, K, Li, Mg, and Al.

4. Method according to claim 2 or 3, wherein

the method comprises STEPMIX and STEPEXTR;

wherein STEPMIX and STEPEXTR are as defined in claim 1.

5. Method for preparation of a compound of formula (I -AMI);

[H-AMI] ©

compound AMI is selected from the group consisting of N(R100)(R200)R300 and

N(R400)R500;

RlOO, R200, R300 are identical or different and are selected from the group consisting of H, Ci_6 alkyl and halogenated Ci_6 alkyl; or

RlOO and R200 form together with the N a saturated 5, 6, 7 or 8 membered heterocyclic ring RINGA;

R400 and R500 form together with the N an unsaturated 5, 6, 7 or 8 membered heterocyclic ring RINGB;

RINGA and RINGB can have 1 or 2 additional endocyclic heteroatoms selected from the group consisting of N, O and S;

RINGA and RINGB are unsubstituted or substituted by 1 , 2 or 3 identical or different

substituents selected from the group consisting of Ci_6 alkyl, halogenated Ci_6 alkyl, Ci_6 alkoxy and halogen;

the method comprises STEP1 and a step STEP2-1;

in STEP2-1 the H of compound of formula (I) is exchanged against H-AMI;

with STEP1 as defined in claim 1.

6. Method according to claim 5, wherein

the method comprises STEPMIX and STEPEXTR;

wherein STEPMIX and STEPEXTR are as defined in claim 1.

7. Method for preparation of a compound of formula (V); wherein

the method comprises STEPl, STEP2-1 and a step STEP2-2;

in STEP2-2 the H-AMI of compound of formula (I- AMI) is exchanged against M;

with STEPl as defined in claim 1 and STEP2-1 as defined in claim 5.

8. Method according to claim 7, wherein

the method comprises STEPMIX and STEPEXTR;

wherein STEPMIX and STEPEXTR are as defined in claim 1.

9. Method according to one or more of claims 1 to 8, wherein

STEPl comprises a purification PUR1, in PUR1 compound of formula (I) is purified by extraction, distillation, evaporation, membrane assisted separation, or a combination thereof.

10. Method according to one or more of claims 1 to 9, wherein

in a step STEPDISSOL-Sl compound of formula (I) as obtained from STEPl, is dissolved in SOLVORG to provide a solution SOLCOMP1-S1, SOLCOMP-S1 is a solution of compound of formula (I) in SOLVORG;

with STEPl and SOLVORG as defined in claim 1.

11. Method for preparation of compound of formula (I);

the method comprises STEPl and STEPDISSOL-Sl;

with STEPl as defined in claim 1 and STEPDISSOL-Sl as defined in claim 10.

12. Method according to one or more of claims 1 to 11, wherein

TEMPl-1 is at least 90°C.

13. Method according to one or more of claims 1 to 12, wherein

at least one of the residues XI and X2 is CI or Br.

14. Method according to one or more of claims 1 to 13, wherein

compound of formula (II) is used for REACl-1 in form of a mixture MIX-II-III;

MIX-II-III is a mixture of compound of formula (II) with compound of formula (III).

15. Method according to one or more of claims 1 to 14, wherein

compound of formula (II) is prepared in a step STEPO;

STEPO comprises a reaction REACO-1;

REACO-1 is a reaction of compound of formula (III) with compound of formula (IV);

X2 is defined herein, also with all its embodiments;

n+ + + + + 2+ 2+ 2+ 2+

R is selected from the group consisting of H , Li , Na , K , Mg , Ca , Zn , Cu ,

AT 3+, Ti3+, Fe2+, Fe3+, B3+

, [N(R20)(R21)(R22)R23]+, and [P(R20)(R21)(R22)R23]+;

R20, R21, R22 and R23 are identical or different and independently from each other selected from the group consisting of H, Ci_s alkyl, C5-6 cycloalkyl, phenyl, benzyl, vinyl and allyl;