Нові досягнення в асиметричній функціоналізації N-(трет-бутилсульфініл)поліфтороалкілімінів

The review covers the latest achievements in the application of N-(tert-butylsulfinyl)polyfluoroalkyl imines in the asymmetric synthesis and summarizes stereochemical observations of their behavior in different types of reactions (reduction of the C=N bond, addition reactions with organometallic rea...

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Опубліковано в:Журнал органічної та фармацевтичної хімії
Дата:2025
Том:23
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Сторінки:3-22
ISSN:2518-1548
Автори та афіліації:
  • Alona S. Cherednichenko — Institute of Organic Chemistry of the National Academy of Sciences of Ukraine
  • Yuliya V. Rassukana — Institute of Organic Chemistry of the National Academy of Sciences of Ukraine
Автори: Cherednichenko, Alona S., Rassukana, Yuliya V.
Формат: Стаття
Мова:Англійська
Опубліковано: National University of Pharmacy 2025
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Journal of Organic and Pharmaceutical Chemistry
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author Cherednichenko, Alona S.
Rassukana, Yuliya V.
author_facet Cherednichenko, Alona S.
Rassukana, Yuliya V.
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author_sort Cherednichenko, Alona S.
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container_title Журнал органічної та фармацевтичної хімії
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description The review covers the latest achievements in the application of N-(tert-butylsulfinyl)polyfluoroalkyl imines in the asymmetric synthesis and summarizes stereochemical observations of their behavior in different types of reactions (reduction of the C=N bond, addition reactions with organometallic reagents, C-H acids, etc.). Fluorinated N-(tert-butylsulfinyl) imines are convenient substrates for obtaining enantiomerically enriched derivatives of polyfluoroalkyl amines, amino alcohols, amino acids, and heterocyclic systems. In recent decades, various approaches to their functionalization have been proposed. With this in mind, important aspects of their reactivity, regio- and stereochemistry have been systematized in this paper.
doi_str_mv 10.24959/ophcj.25.321224
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fulltext ISSN 2308-8303 (Print) / 2518-1548 (Online) 3 Review Article http://ophcj.nuph.edu.ua UDC 542.913+547-304.2+547.478.92 A. S. Cherednichenko, Yu. V. Rassukana Institute of Organic Chemistry of the National Academy of Sciences of Ukraine, 5 Academik Kukhar str., 02094 Kyiv, Ukraine Recent advances in the asymmetric functionalization of N-(tert-butylsulfinyl)polyfluoroalkyl imines Abstract The review covers the latest achievements in the application of N-(tert-butylsulfinyl)polyfluoroalkyl imines in the asymmetric synthesis and summarizes stereochemical observations of their behavior in different types of reactions (reduction of the C=N bond, addition reactions with organometallic reagents, C-H acids, etc.). Fluorinated N-(tert-butylsulfinyl) imines are conveni- ent substrates for obtaining enantiomerically enriched derivatives of polyfluoroalkyl amines, amino alcohols, amino acids, and heterocyclic systems. In recent decades, various approaches to their functionalization have been proposed. With this in mind, important aspects of their reactivity, regio- and stereochemistry have been systematized in this paper. Keywords: tert-butylsulfinyl; polyfluoroalkyl imines; asymmetric synthesis; aldimines; ketimines; stereoselectivity А. С. Чередніченко, Ю. В. Рассукана Інститут органічної хімії Національної академії наук України, вул. Академіка Кухаря, 5, м. Київ, 02094, Україна Нові досягнення в асиметричній функціоналізації N-(трет-бутилсульфініл)поліфтороалкілімінів Анотація Огляд охоплює найновіші здобутки в застосуванні N-(трет-бутилсульфініл)поліфтороалкілімінів в асиметричному синтезі, а також узагальнює стереохімічні закономірності їхньої поведінки в різних типах реакцій (відновлення C=N зв’язку, приєднання металоорганічних реагентів, С-Н кислот тощо). Фторовмісні N-(трет-бутилсульфініл)іміни є зручними субстратами для одержання на їх основі енантіомерно збагачених похідних поліфтороалкілімінів, аміноспиртів, амі- нокислот і азотовмісних гетероциклів. За останні десятиліття було запропоновано різноманітні підходи до їх функціо- налізації. З огляду на це важливі аспекти щодо їхньої реакційної здатності, регіо- і стереохімії систематизовано в цій роботі. Ключові слова: трет-бутилсульфініл; поліфтороалкіліміни; асиметричний синтез; альдиміни; кетиміни; стереоселективність Citation: Cherednichenko, A. S.; Rassukana, Yu. V. Recent advances in the asymmetric functionalization of N-(tert-butylsulfinyl)polyfluoroalkyl imines. Journal of Organic and Pharmaceutical Chemistry 2025, 23 (1), 3 – 22. https://doi.org/10.24959/ophcj.25.321224 Received: 26 January 2025; Revised: 28 March 2025; Accepted: 1 April 2025 Copyright© 2025, A. S. Cherednichenko, Yu. V. Rassukana. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0). Funding: The work was supported by the National Academy of Sciences of Ukraine (grant No. 0124U002052). Conflict of interests: The authors have no conflict of interests to declare. ■ Introduction Since Ellman’s group introduced chiral N-tert- butylsulfinyl amides into synthetic practice [1], the corresponding N-sulfinyl imines have also found a wide application in organic synthesis, providing access to a variety of optically active amines [2]. Among different N-sulfinyl imines, compounds with a polyfluoroalkyl substituent at the imine carbon atom deserve special attention. On the one hand, the introduction of a powerful electron-withdrawing polyfluoroalkyl group sig- nificantly increases the imine electrophilicity, promoting reactions with nucleophilic reagents. On the other hand, the presence of fluorine atoms can lead to significant changes in the physico- chemical and biological properties of molecules compared to their non-fluorinated analogs [3 – 9]. ISSN 2308-8303 (Print) / 2518-1548 (Online) 4 Журнал органічної та фармацевтичної хімії 2025, 23 (2) Thus, N-(tert-butylsulfinyl)polyfluoroalkylimines can be convenient precursors of enantiomerical- ly pure α-polyfluoroalkylamines, important chi- ral substrates for the preparation of different non- racemic fluorine-containing compounds. Great in- terest in this type of imines is confirmed by dozens of works in this area over the past decades, which were described, in particular, in reviews by prof. Soloshonok and co-authors in 2016 – 2018 [10, 11]. In the present review, we attempt to systema- tize and generalize the regularities of the asym- metric functionalization of N-(tert-butylsulfinyl) polyfluoroalkyl imines, including the experimen- tal data obtained in recent years, which will al- low for an effective prediction of the configura- tion of the newly created stereocenter and should stimulate the further development of this area of organic chemistry. ■ Results and discussion 1. Reduction of the azomethine bond of N-(tert-butylsulfinyl)polyfluoroalkyl imines A stereoselective reduction of non-fluorinated N-(tert-butylsulfinyl)ketimines with sodium and lithium borohydrides was first determined in the late 2000s in the works of Ellman et al. [12, 13]. However, the possibility of involving α-polyfluo- roalkyl imines in this reaction was demonstra- ted only a decade later on the example of α,β- unsaturated N-(tert-butylsulfinyl)ketimines 1 bear- ing a trifluoromethyl group (Scheme 1) [14]. The screening of the spectrum of sodium or li- thium borohydrides and aluminum hydrides (NaBH4, LiBH4, NaBH3CN, CatBH, LiAlH4, Red-Al, LiBHEt3, L-Selectride) showed that the highest diastereo- selectivity (90 – 99 %) could be achieved when us- ing DIBAL-H in THF and L-Selectride in a mix- ture of THF/HMPA (5:1) at –78°С. N-(tert-butylsulfinyl)imines of trifluoroaceto- ne and trifluoroacetophenones generated in situ were subjected to reduction, skipping the isola- tion step. According to this procedure, a series of imines of α-trifluoromethyl aryl and alkyl ke- tones were reduced with sodium borohydrides and L-Selectride with de up to 98 % (Scheme 2, Table 1) [15 – 17]. Most likely, metal hydrides (NaBH4, LiBH4, NaBH3CN, LiAlH4, DIBAL-H) and organoboron compounds (CatBH) coordinate with the oxygen atom of the sulfinyl group, forming a closed tran- sition state A, which results in (R,R)-diastereo- mers of sulfinamides 4. In turn, L-Selectride dis- plays a worse propensity for the coordination and attack over the imine C=N bond occurs through the open transition state B, leading to (S,R)-ste- reoisomer of sulfinamides 4 (Scheme 3) [15, 18]. The screening of reducing agents for chemo- and stereoselective reduction of the azomethine bond of N-tert-butylsulfinyl trifluoromethylimi- noesters 5 also revealed similar dependence of the stereochemical outcome of the process on the nature of the reductant (Scheme 4, Table 2). The best results in terms of both chemo- and ste- reoselectivity were achieved when 9-borabicyclo- nonane (9-BBN) was used as a reducing agent [19]. The hydrolysis of N-(sulfinyl)aminocarboxy- late 6 gave an optically pure stereoisomer of F3C N S O F3C N H S O F3C N H S O ( )-R 1 ( )-R,R 2( )-S,R 2 R RR R = C6H5, 4-MeO-C6H4, 4-Me-C6H4, 4-Cl-C6H4, 4-Br-C6H4, 2-MeO-C6H4, 3-Br-C6H4, 1-naphtyl, 2-furyl, C6H5C C, Cn 8H17, C6H5(CH2)3 DIBAL-HL-Selectride THF/HMPA, -78°C THF, -78°C de 90 98 %– de 92 99 %– 60 99 %– 81 99 %– Scheme 1. A stereoselective reduction of α,β-unsaturated N-(tert-butylsulfinyl)ketimines Table 1. The reduction of trifluoromethyl ketimines 3 R [H] Yield ( %) Product de ( %) Ar NaBH4 66 – 85 (S,S)-4 90 – 98 L-Selectride 60 – 84 (R,S)-4 92 – 98 Alk NaBH4 52 – 79 (S,S)-4 96 – 98 L-Selectride 22 – 84 (R,S)-4 92 – 98 9-anthrylа LiBH4 71 (S,S)-4 97 Note: a The intermediate imine was chromatographically isolated in the individual state before the reduction ISSN 2308-8303 (Print) / 2518-1548 (Online) 5 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) 3,3,3-trifluoroalanine 7 – a biologically promis- ing α-amino acid. The (R)-isomer of trifluoroala- nine 7 was obtained similarly from sulfinamide (R,R)-6, the product of imine 5 reduction in (R)- configuration. On the other hand, the reduction of imines 5 with a complex of borane with dimethyl sulfide proceeded with the involvement of the carboxy- late function, in addition to the C=N bond [19]. It enabled a stereospecific preparation of synthe- tically attractive trifluoromethyl aminoethanols with either protected 8 or free amino group 9 (Scheme 5). Thus, the ability to control chemo- and stereo- selectivity by selecting the appropriate reducing agent allows for the synthesis of both stereoisomers F3C N S O F3C N H S OR F3C N H S OR + R ( )-S 3 ( )-S,S 4 ( )-R,S 4 S O H2N CF3 R O + [H]Ti(O Pr)i 4 or Zr(O Bu)t 4 R = C6H5, 4-MeO-C6H4, 4-Me-C6H4, 4-Br-C6H4, C6H5(CH2)3, Cn 8H17 [15], 9-anthryl [16], Me [17] Scheme 2. The reduction of aryl- and alkyl trifluoromethyl ketimines R N F3C S O R NH F3C S O N S O M H R tBu CF3 N F3C R O tBu H M R NH F3C S O MBH4 L-Selectride ( )-R 3 ( , )-R R 4 ( , )-S R 4 TS A TS B Scheme 3. Possible mechanisms of the reduction of the C=N bond of N-tert-butylsulfinyl trifluoromethyl ketimines 1. HCl (conc), 90oC 2. propylene oxide NH2F3C CO2H ( )-S 85 %7( )-S 5 ( )-S,S 6 N F3C MeO2C S O 9-BBN NH F3C MeO2C S O THF, 0oC Scheme 4. A stereoselective reduction of the C=N bond of N-tert-butylsulfinyl trifluoromethyl iminopyruvates Table 2. Reaction conditions for the reduction of C=N bond of iminopyruvate (S)-5 № [H] Conditions (S,S)/(R,S)-6 1 NaBH4 THF, –78оС 1:1.1 2 NaBH(OCOCH3)3 THF, rt 1:2 3 LiBH4 THF, –78оС 1:2.4 4 CatBH THF, –78оС 2.4:1 5 9-BBN THF, 0оС >99:1a Note: a (R,S)-6 is absent according to 1H and 19F NMR data ISSN 2308-8303 (Print) / 2518-1548 (Online) 6 Журнал органічної та фармацевтичної хімії 2025, 23 (2) of various β-polyfluoroalkylamines, starting from one enantiomer of N-(tert-butylsulfinyl)polyfluo- roalkyl imines. 2. Reactions of N-(tert-butylsulfinyl)po- lyfluoroalkyl imines with organometallic compounds The addition of Li- and Mg-organic com- pounds to the azomethine bond of imines, includ- ing N-(tert-butylsulfinyl)imines, is a convenient method for forming a new C-C bond with the con- current generation of a new stereogenic carbon atom. The interaction of imine of fluoral (S)-10 (generated in situ) with phenylmagnesium bro- mide allowed one to obtain amines (S,S)-11 with diastereoselectivity of 70 % (Scheme 6). The se- lectivity increased with the addition of Lewis acids (AlMe3, AlEt3, BF3•Et2O, TiCl4, Mg(OTf)2), but it led to a general decrease in yields [20]. The addition of phenyl lithium (2.5 equiv., 2.5M solution in THF) to trifluoroacetaldimine (S)-10 resulted in the formation of α-trifluoromethyl ben- zylamine (S,S)-11 in the yield of 66 % and with a significantly improved diastereomeric ratio (98:2) compared to the reaction with phenyl magnesium bromide. Various aryl lithium reagents were suc- cessfully involved in the reaction with imine 10 under optimal conditions (THF, –78°C) (Scheme 6). Later, it was shown that N-(tert-butylsulfinyl) imine of fluoral 10 purified by vacuum distilla- tion demonstrated better yields (83 % compared to 64 %) in the reaction with PhLi [21]. The au- thors [20] attributed the stereochemical result obtained in both reactions to the formation of open transition state A in the course of the reactions (Scheme 6). Similarly to aldimines, α,β-unsaturated N-(sul- finyl)ketimines (R)-12 successfully reacted with aryl, alkyl, and alkynyl lithium reagents to pro- vide α-polyfluoroalkyl allylamines (S,R)-13 with good yields (48 – 99 %) and diastereoselectivities (70 – 98 %) (Scheme 7) [22]. The addition of (trimethylsilyl)ethynyl lithi- um to trifluoroacetaldimine (S)-10 occurred with sufficiently high diastereoselectivity (de 86 %), however, the yield of propargylamine (R,S)-14 was only 33 % [23]. At the same time, when N-(tert- butylsulfinyl)imine of fluoral (R)-10 interacted with lithium arylacetylides generated in the presence of LiHMDS, the diastereomeric ratio varied from 52:48 to 70:30 (Scheme 8) [24]. Significantly better results were obtained in the reaction of lithium acetylides (including those with a trimethylsilyl substituent) with α-trifluoro- methylketimines 3 in the presence of titanium tetraisopropylate (Scheme 9). The correspond- ing α-trifluoromethyl-α-propargylamines (R,S)-16 were obtained with yields from 56 to 97 % and the diastereoselectivity of 98 % [25]. The stereochemical result of the reaction of polyfluoroalkylaldimines 18 with propargyl HCl HCl HCl/Et2O ( )-S 9 ( )-R 9 NH2F3C HO NH2F3C HO rt, 1 h Me2S BH3 THF, -20 C o 90 % ( )-S 5 ( )-R 5 ( )-R,R 8 ( )-S,S 8 N F3C MeO2C S O N F3C MeO2C S O N H F3C S O HO N H F3C S O HO 95 % * Scheme 5. The complete reduction of N-tert-butylsulfinyl trifluoromethyl iminopyruvates F3C N S O F3C N H S ORH ( )-S 10 ( , )-S S 54 66 %11, – RLi, THF, -78 oC de 70 99 %– or Ph DCM, -78oC R = C6H5, 4-MeO-C6H4, 4-MeS-C6H4, 4-F-C6H4, 3,5- -F-Cdi 6H3, 2-Me-C6H4, pyridin-2-yl N F3C H MR TS A O tBu M = Li, Mg Scheme 6. The addition of propargyl magnesium bromide to N-(tert-butylsulfinyl)polyfluoroalkyl imines ISSN 2308-8303 (Print) / 2518-1548 (Online) 7 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) magnesium bromide was found to be crucially de- pendent on the nature of the solvent, variating from de 12 % (in DCM) to de 92 – 98 % (in THF). α-Propargylamines (S,S)-19 were used for further transformation into derivatives of terpene alka- loids 21 by the synthesis of enynes 20 and their sub- sequent cyclization by the Pauson-Khand reaction scheme [26]. Additionally, enynes 20 were intro- duced into the ruthenium-catalyzed metathesis yielding tetrahydropyridines 22 [27] (Scheme 10). Lithiated thiazoles turned out to be conveni- ent reagents for the nucleophilic addition to the azomethine bond of N-(sulfinyl)imine (S)-10. The optimal conditions (1.1 equiv. of LDA, THF, –78°С) were suitable for thiazoles annulated with an imidazole or 1,2,4-triazole ring and provided reaction products (R,S)-23 with the yields of 61 – 72 % and stereoselectivities reaching 99 % (Scheme 11) [28, 29]. N-Sulfinyl imine of fluoral (S)-10 also under- goes a zinc-initiated reaction with allyl and alkyl bromides to form the corresponding enantiome- rically enriched sulfinamides (S,S)-24 and (S,S)- 25 (Scheme 12) [21, 30]. The stereochemical re- sult of the reaction is consistent with the open transition state previously proposed, which is si- milar to reactions with organomagnesium and organolithium reagents. The interaction of α,β-unsaturated N-(tert- butylsulfinyl)ketimines (R)-26 with ethyl bromo- acetate in the presence of zinc occurred with a high regio- and chemoselectivity (Scheme 13) [31]. RF N S O RF N H S O ( )-R 12 ( , )-S R 48 99 %13, – Ph Ph R RLi Et2O, -40oC RF = CF3, CHF2, CClF2, C3F5, C5F11 R = C6H5, 4-F-C6H4, 4-Cl-C6H4, 4-Me-C6H4, 4-MeO-C6H4, 3-Me-C6H4, 2-Me-C6H4, naphtyl, PhC C, Bun de 70 98 %– Scheme 7. The addition of Li-organic reagents to α,β-unsaturated N-(sulfinyl)ketimines HN F3C S O Ar H N F3C S O de 4 40 %– H Ar LiHMDS, -78°C DCM Ar = C6H5, 4-Me-C6H4, 4-MeO-C6H4, 4-EtO-C6H4, 3-Me-C6H4, 4-Me-C6H4, 4- Bu-Ct 6H4, 4-( -pentyl)-Cn 6H4, 3-F-C6H4, 4-F-C6H4, 4-Cl-C6H4, 3-Br-C6H4, 4-Br-C6H4, 3-O2N-C6H4 ( )-R 10( , )-R R 15 31 87 %– HN F3C S O ( , )-R S 14 TMS H N F3C S O ( )-S 10 de 86 % 33 % AlMe3, toluene -78°C...rt H TMS Scheme 8. N-(tert-butylsulfinyl)imine of fluoral in the reactions with Li-acetylides R N F3C S O ( )-S 3 HN F3C S O ( , )-R S 16 Li R' R'R HCl NH2 F3C R'R ( )-R 17 56 97 %– 87 97 %– de 98 % R = C6H5, 4-MeO-C6H4, 4-Cl-C6H4, Cn 6H11; R' = Bu, Hex, cyclopropyl, TMS, Cn n 6H5, CF3 Ti(O Pr)i 4, -78oC Scheme 9. N-(tert-butylsulfinyl)trifluoromethyl ketimines in the reaction with Li-acetylides ISSN 2308-8303 (Print) / 2518-1548 (Online) 8 Журнал органічної та фармацевтичної хімії 2025, 23 (2) H N RF S O (S)-18 HN RF S O ( , )-S S 19 N RF ( )-S 20 R1 Bus N O R2 RF R1 R2 Bus H RF = CF3, CHF2, C2F5, C3F7, C4F9, CF2Cl; R1 2 = H, Me, C6H5 42 81 %– ( )-S 21 92 98 %de – 33 76 %– N Bus RF ( )-S 22 THF, -78oC 60 87 %– 86 92 %– MgBr Scheme 10. The addition of propargyl magnesium bromide to N-(tert-butylsulfinyl)imine of fluoral F3C N S OH ( )-S 10 ( , )-R S 23 + X N N S R' R X N N S R' R HN CF3 S OX = CH, N X = N: R = H; R' = Me, Ph, 4-Cl-C6H4, 4-Br-C6H4, 4-F-C6H4, 3-Cl-C6H4, 3-Br-C6H4, 3,4- -Cl-Cdi 6H3, 2-naphtyl X =CH: R' = Me; R = Ph, 4-Cl-C6H4, 4-Br-C6H4, 4-F-C6H4, 4-Me-C6H4, 4-MeO-C6H4, 3-Cl-C6H4, 3-Br-C6H4, 3-MeO-C6H4, 2-MeO-C6H4, 3,4- -Cl-Cdi 6H3, 2-naphtyl 40 78 %– de 96 99 %– LDA, THF, -78 oC Scheme 11. The reaction of N-(tert-butylsulfinyl)imine of fluoral with lithiated thiazoles F3C N S O N H S OCF3H ( )-S 10 ( , )-S S 24 Zn, DMF, 0°C 52 86 %– de 6 96 %– R2 R1Br R1 R2 N H S OCF3 ( , )-S S 25 DMF, 0°C Zn, TMSCl 65 % de 91% EtO O R1 = R2 =R1 = R2 = H, R2 = H: R1 = CO2Et, Me R1 = H: R2 = Ph, CO2Et, Me Br CO2Et Scheme 12. N-(tert-butylsulfinyl)imine of fluoral in the Zn-mediated reactions with allyl and alkyl bromides N RF S O R Zn, THF 40 60– oC, 3 h HN S O R RF EtO2C de 70 90 %– RF = CF3, CClF2, Cn 3F7, Cn 5F11 R = Ph, 4-F-C6H4, 4-Cl-C6H4, 4-Me-C6H4, 4-MeO-C6H4, 2-Me-C6H4, 3-Me-C6H4, 1-naphtyl, 2-thienyl, C6H5(CH2)3 ( )-R 26 ( )-R,R 27 26 76 %– Br CO2Et Scheme 13. N-(tert-butylsulfinyl)trifluoromethyl ketimines in the Zn-mediated reaction with ethyl bromoacetate ISSN 2308-8303 (Print) / 2518-1548 (Online) 9 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) 3. Reaction of N-(tert-butylsulfinyl)poly- fluoroalkyl imines with CH-acids The reaction of polyfluoroalkyl imines with esters of carboxylic acids is a convenient method for the synthesis of fluorine-containing com- pounds with a β-aminocarboxylic acid fragment. Thus, β-aminomalonates 28 were synthesized by the interaction of N-(tert-butylsulfinyl)imine of fluoral (S)-10 with a number of dialkylmalonates (Scheme 14). The highest stereoselectivities were observed in the presence of nBuLi or sterically hindered phosphazene bases (P2-Et). The products of the Mannich reaction with diethylmalonate were successfully transformed into optically pure β-trifluoromethyl-β-alanine enantiomers (R)- and (S)-29 [32, 33]. Esters of β-trifluoromethyl-β-amino acids can be obtained directly, without an additional decarboxylation step, by the reaction of imines with alkyl acetates in the presence of LDA. (S,S)- diastereomer 30 was formed stereospecifically (de>99 %). The removal of the sulfinyl group and the subsequent cyclization with a substituted thio- urea yielded tetrahydro-6-oxo-pyrimidine (S)-31, a potential β-secretase inhibitor currently studied as a medicine for the treatment of Alzheimer’s disease (Scheme 15) [34]. Derivatives of methylsulfonic and phospho- nic acids also undergo the reaction with N-(tert- butylsulfinyl)imines 10 in the presence of strong bases (Scheme 16) [35, 36]. N-tert-butylsulfinyl polyfluoroalkyl aldimi- nes 18 were successfully involved in the aza-Henry reaction with nitromethane under mild condi- tions. The study of various factors, such as the nature of the base, solvent, temperature and the F3C N S O N H S OCF3 H F3C NH2 + nBuLi (10 mol%) R2O2C R2O2C R1 CO2H R1 = H, Me, F; R2 95 % ( )-S 10 ( , )-R S 28 ( )-R 29 P2-Et (10 mol%) N H S OCF3 F3C NH2 R2O2C R2O2C R1 CO2H 96 % ( , )-S S 28 ( )-S 29 de 16 84 %– de 84 98 %– 80 99 %– 22 98 %– H H N P P NMe2 Me2N NMe2 EtN NMe2 NMe2 P2-Et R1CH(CO2R2)2 for R1=H Scheme 14. The reaction of N-(tert-butylsulfinyl)imine of fluoral with dialkylmalonates F3C N S OH + LDA N NO CF3 NHBoc de 80 99 %– R = H, Me, -(CH2)3-, -(CH2)4-, -(CH2)5-, -(CH2)2O(CH2)2-, -CH2CH=CHCH2- 2Ph, allyl, CH2C6H4Me, CH2C6H4OMe N H S OCF3 OAlk O AlkO OR R RR ( )-S 10 ( )-S,S 30 ( )-S 31 toluene, -78°C 44 99 %– Scheme 15. The reaction of N-(tert-butylsulfinyl)imine of fluoral with alkyl acetates F3C N S O N H S OCF3H 75 %de LiHMDS ( )-S 10 ( , )-R S 32 S O O Ph N H S OCF3 95 %de nBuLi, THF CH3P(O)(OR)2 P RO O RO ( , )-R S 33 PhSO2CH3 75 %53 76 %– Scheme 16. The reaction of N-(tert-butylsulfinyl)imine of fluoral with derivatives of sulfonic and phosphonic acids ISSN 2308-8303 (Print) / 2518-1548 (Online) 10 Журнал органічної та фармацевтичної хімії 2025, 23 (2) sequence of the reagent addition, showed that the best chemo- and stereoselectivity of the reaction with imine of fluoral were achieved when the re- action was carried out in DMSO in the presence of 0.1 equiv. of Hünig’s base (Scheme 17) [37]. The reaction of N-(tert-butylsulfinyl)imines of trifluoropyruvate 5 with nitromethane in the pre- sence of quinine allowed for obtaining enantiome- rically pure α-trifluoromethyl substituted α-amino- β-nitrocarboxylates 34 (Scheme 18) [19]. The study of the effect of the reaction condi- tions on the stereoselectivity of the process sho- wed that the nature and amount of the base had a crucial impact on the diastereomeric excess of the products. In particular, the transition from stronger (Hünig’s base) to weaker (quinine) bas- es led to a complete reversal of the stereochemi- cal outcome of the reaction explained by the oc- currence of two different mechanisms with open and closed transition states (Scheme 19). The addition of ketones to fluorinated N-(tert- butylsulfinyl)imines provides access to another class of optically active compounds – β-amino- ketones 35 – precursors of nitrogen-containing heterocycles, 1,3-diamines, γ-aminoalcohols, and other polyfunctional compounds. However, the yields and diastereomeric excess vary widely depending on the nature of the substituents in the aromatic ring of both imines and ketones (Scheme 20) [38]. Recent experimental data have shown that the nature of an organometallic base and a sol- vent has a significant influence on the result of the addition of ketones to the azomethine. The best results in terms of yields and stere- oselectivity in the reaction of trifluoromethyl ketimine (S)-3 with p-tolylethan-1-one and me- thyl acetate were achieved when using KHMDS (Scheme 21) [39]. However, it turned out that the addition of tert-butyl acetate and tert-butyl acetoacetate to N-(sulfinyl)-α-fluoromethylaryl imines (R)-38 led to the opposite stereochemical result, and in the case of the reaction with (R)-imine 38, the newly created stereocenter has (S)-configuration (Scheme 22) [40 – 42]. RF N S O RF N H S O O2N ( )-R 18 DIPEA DMSO, 15oC RF = CF3, C2F5, HC2F4, CF2Br CH3NO2 ( )-R,R 33 N RF H O tBu TS A CH2NO2 66 86 %– de >99 % Scheme 17. The addition of nitromethane to N-(tert-butylsulfinyl)polyfluoroalkyl aldimines ( )-S 5 ( )-S,S 34 N F3C MeO2C S O N H F3C S O O2N CH3NO2 quinine (0.1 equiv) MeO2C N H F3C S O O2N MeO2C ( )-R,S 34 de 90 % + Scheme 18. The addition of nitromethane to N-tert-butylsulfinyl trifluoromethyl iminoesters N CF3MeO2C O CH2NO2 tBu TS A S O H N CO2Me F3C tBu O2N N δ+ δ- TS B ( , )-S S 34 O2NCH2 ( , )-R S 34 Scheme 19. Possible transition states of the nitromethane addition to N-tert-butylsulfinyl imines of trifluoropyruvate ISSN 2308-8303 (Print) / 2518-1548 (Online) 11 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) The reaction of imine 10 with β-ketoacids in the presence of Lewis acids makes it possible to obtain a wide range of products 40 with alkyl, cycloalkyl, aryl, and hetaryl substituents at- tached to the oxo-group. The decarboxylation of the intermediate adduct A at the last step of the process was confirmed by a mass spectrometric study of the reaction mixture (Scheme 23) [43]. In 2019, the addition of a derivative of boro- nic acids – benzylboropinacolate – to the C=N bond of N-(tert-butylsulfinyl)imine of trifluoroacetophe- none (R)-41 (Scheme 24) was reported for the first time [44, 45]. Similarly to other classes of esters, anion was generated in the presence of a strong base (nBuLi) [46]. The reaction pro- ceeded with a good yield, but with a low stereo- selectivity (de 26 %), and unfortunately, the con- figuration of the major diastereomer was not de- termined. The interaction of imine (S)-10 with the lithi- um enolate of indanone apparently occurred as a nucleophilic attack in the open transition state (Scheme 25, TS A), which was consistent with previous observations for aldimines [47]. The reaction of aldimine 10 with indanone con- taining a thiocyanate group led to the formation of both the product of the conventional Man- nich nucleophilic addition 44 and the spirocyclic F3C N S O N H S OCF3R + R1 CH3 O LDA R1 O 10 86 %de – R = Ph, 4-MeO-C6H4, 4-Cl-C6H4 R1 = Ph, 4-MeO-C6H4, 4-Cl-C6H4, 4-Me-C6H4, 2-Me-C6H4 R O LiN R' S(O) -But R F3C TS A( )S -3 ( , )-S S 35 29 91 %– THF, -78oC Scheme 20. The reaction of N-tert-butylsulfinyl trifluoromethyl ketimines with ketones F3C N S O N H S OCF3R Tol Me O KHMDS, Et2O Tol O de 94 % R -78oC R = C6H4O(CH2)3CF3 N H S OCF3 Me OMe O KHMDS, THF MeO O R -78oC de 95 % R = 4-MeO-C6H4 ( )-S 3( , )-S S 36 ( , )-S S 37 Scheme 21. The reaction of N-tert-butylsulfinyl trifluoromethyl ketimines with p‑tolylethan-1-one and methyl acetate N S OAr N H S O R O de >95 % Ar R = O Bu, CHt 2CO2tBu; Ar = 2-F-C6H4, 2-F-4-Br-C6H3 LDA + Me R O TiCl(O Pr)i 3 ( )-R 38 ( , )-S R 39 F F Scheme 22. The reaction of N-tert-butylsulfinyl fluoromethyl ketimines with ketones and alkyl acetates F3C N S O N H S OCF3 H + OH O R O de 90 98 %– R O Ni(SO3CF3)2 (10 mol%) THF, rt, 24 h N H S OCF3 R O HO2C ( )-S 10 ( , )-R S 40 A 70 99 %– Scheme 23. The Lewis acids-mediated addition of β-ketoacids to N-tert-butylsulfinyl imine of fluoral ISSN 2308-8303 (Print) / 2518-1548 (Online) 12 Журнал органічної та фармацевтичної хімії 2025, 23 (2) aziridine 45, which was the result of nucleo- philic substitution of the thiocyanate group. The screening of various bases showed that the percentage of aziridine 45 increased with the in- crease in basicity of the inorganic salt. Replacing the solvent with a more polar DMF facilitating the intramolecular nucleophilic cyclization gave the cyclic product 45 with high chemoselectivity. It is also important that mild conditions for the removal of the sulfinyl group enabled the synthe- sis of the unprotected aziridine 47 without the destruction of the spirocyclic part of the molecu- le (Scheme 26) [48]. The possibility of using cyclic amides (indol- 2-ones) in the Mannich reaction with trifluoro- acetaldimine 10 was demonstrated in 2014. The nature of the base has a decisive influence on conversion rates and diastereomeric excess, and lithium bases (LDA, LiHMDS, nBuLi) pro- vide the best results (Scheme 27) [49]. Stabilized α,α-difluoroenolates obtained by the cleavage of the C-C bond of the corresponding α-fluorinated gem-diols reacted with imine (S)-10 under mild conditions with a high chemo- and ste- reoselectivity with the formation of optically acti- ve β-amino ketones (S,S)-49 (Scheme 28) [50, 51]. This method has been proven to be effective for the synthesis of optically pure quaternary α-fluoro-β-ketoamines containing a C-F stereoge- nic center (Scheme 29) [52]. The asymmetric addition of trifluoromethyl gem-diols to chiral imines (R)-18 also provided α-difluoroalkyl-β-aminosulfones (S,R)-51. A de- tailed screening of the reaction conditions showed F3C N S OPh + -78 C, THF o de 26 % Ph Bpin F3C N H S OPh Ph ( )-R 41 ( , )/( , )-R R S R 42 nBuLi 62 % Scheme 24. Boropinacolates as CH-acids in the addition reaction with N‑tert‑butylsulfinyl trifluoromethyl ketimines F3C N S O N H S OCF3 + LDA de 93 98 %– O R -78o O R N O tBu CF3H OLi H TS A H ( )-S 10 ( , , )-S S S 43 85 95 %– Scheme 25. The addition of ring-substituted indanones to N-tert-butylsulfinyl imine of fluoral HN S O CF3 NaOAc, THF de 82 % O O SCN NCS N S O O CF3 Na2CO3, DMF de 80 % ( )-R 10 ( )-S 10 NH2 CF3 O SCN 73 % H N O CF391 % (2 ,1` ,R S RS)-44 (2 ,2` ,S S SS)-45 (2 ,1` )-R S 46 (2 ,2` )-S S 47 H H 84 % 67 % Scheme 26. Different pathways of the N-(tert-butylsulfinyl)trifluoroacetaldimine reaction with 2-thiocyanoindanone ISSN 2308-8303 (Print) / 2518-1548 (Online) 13 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) that the optimal values of yields and diastereo- meric excess were achieved only when the reaction time was extended to 4 hours (Scheme 30) [53]. A similar method was applied to 3-fluoroindo- line-2-one derivatives, which also formed fluori- nated enolates under the action of a mixture of Hünig’s base and lithium bromide (Scheme 31) [54]. It is known that 2-alkylpyridines can be used as CH-acids in functionalizations with carbonyl com- pounds and imines under catalysis by Brønsted or Le- wis acids [55 – 57]. The use of optically active N-(tert- butylsulfinyl)polyfluoroalkyl imines (S)-18 allowed for the preparation of enantiomerically enriched functionalized pyridines (S,S)-53 (Scheme 32) [58]. F3C N S O + LDA de 38 88 %– N R2 -78oC, DCM O R1 N R2 O R1 CF3 N H S O R1 R2 2Me, Me, OMe, CF3 N OR Li CF3 N H S O TS A H ( )-S 10 ( , , )-S S S 48 79 98 %– Scheme 27. The addition of indol-2-ones to N-tert-butylsulfinyl imine of fluoral de 94 98 %–( )-S 10 R O HO CF3 OH Et3N, LiBr THF, 0°C - CF3CO2 R O F F R O CF3 N H S O FF FF F3C N S OH ( , )-S S 49 30 min 83 98 %– Scheme 28. N-(tert-butylsulfinyl)trifluoroacetaldimine in the detrifluoroacetylative Mannich reaction RF N S O de 84 96 %– RF = CF3, C2F5, C3F7, C4F9, CF2Cl, CF2Br X = -(CH2)n-, n = 1, 2, 3; -(CH2O)- Et3N, LiBr 2-MeTHF, -40oCR + X R X O F CF3 OH OH CF3 N H S OO F ( )-S 18 ( , , )-S S S 50 79 97 %– Scheme 29. The detrifluoroacetylative Mannich reaction in the synthesis of quaternary α‑fluoro-β-ketoamines de 72 99 %– RF = CF3, CF2H, C2F5, C3F7, C4F9, CF2Cl Et3N, LiBr -78oC, 4 h R R S O O FF CF3 OH OH CF3 N H S O S FF O O RF N S O + ( )-R 18 ( , )-S R 51 37 86 %– Scheme 30. The detrifluoroacetylative Mannich reaction in the synthesis of α‑difluoroalkyl-β-aminosulfones ISSN 2308-8303 (Print) / 2518-1548 (Online) 14 Журнал органічної та фармацевтичної хімії 2025, 23 (2) N-(tert-Butylsulfinyl)imine of fluoral 10 suc- cessfully reacted with enolates of glycine esters in the presence of organic (Et3N, DMAP, DBU, LiHMDS, tBuOLi) and inorganic (K2CO3 and Cs2CO3, NaOH) bases. The best yields (49 – 87 %) and diastereoselectivity (84 – 98 %) were achieved when using 0.1 equiv. of Cs2CO3 in THF at room temperature (Scheme 33, path a) [59]. Another approach to compound 54 involves obtaining Schiff bases in situ by the interaction between lithium 2,2-diphenylglycine carboxylate and aldehydes (Scheme 33, path b). In the next step, interme- diate A reacts with trifluoroacetaldimine 10 under the catalysis by p- or m-nitrobenzoic acid with the formation of the corresponding diamines [60]. β-Trifluoromethyl-α,β-diamino acid (S,S)-56 was synthesized by the reaction of N-(sulfinyl) imine of fluoral (S)-10 with the nickel complex of Schiff bases and the subsequent destruction of the resulting complex 55 by hydrochloric acid (Scheme 34) [61]. N-(tert-Butylsulfinyl)polyfluoroalkylaldimi- nes (S)-18 entered the Lewis acid catalyzed re- action with vinylogous carbonyl compounds – si- lylated dienolates, and the regiochemistry of the addition depended on the nature of the catalyst. Thus, when AgBF4 was used, the Mannich reac- tion in the α-position of the enolate occurred, giv- ing β-amino-β-fluoroalkyl-α-vinyl esters (R,S)-57. The stereochemical result of the process can be RF N S O de 84 96 %– RF = CF3, C2F5, C3F7, CF2Cl, CF2Br DIPEA, LiBr 2-MeTHF, -40oC N O R1 R2 F HO CF3 OH + N O R1 R2 F F3C N H S O ( )-S 18 ( , , )-S S S 52 79 97 %– Scheme 31. Fluoroindolinones in the detrifluoroacetylative Mannich reaction with N-tert-butylsulfinyl polyfluoroalkyl aldimines RF N S O N R1 R2 N R2 R1 N H RF S OTi(O Pr)i 4, BuLin THF, -42oC de 60 94 %– RF = CF3, CHF2 ( )-S 18 ( , )-S S 53 31 84 %– + Scheme 32. 2-Alkylpyridines as CH-acids in the addition reaction with N-tert-butylsulfinyl polyfluoroalkyl aldimines 89 98 %– CO2R N PhPh a R1 O CO2LiH2N PhPh R1 H N O Li Ph Ph O MeOH, rtb N CF3 HN S Ph Ph O ( )-S 10 49 87 %– ( , , )- 84 99 %S S S de54 – A ( )-S 10 CO2R, R1 R1 Scheme 33. N-tert-butylsulfinyl imine of fluoral in the synthesis of trifluoromethyl-substitured vicinal diamines N N Ph Ni OO O N + de 88 % ( )-S 10 N N Ph Ni OO O N CF3 H N H S O DBU MeCN, rt BuBu BuBu COOH NH2 NH2 F3C 1M HCl 86 % ( , , )-S S S 55 ( , )-S S 56 77 % Scheme 34. N-tert-butylsulfinyl imine of fluoral in the synthesis of β-trifluoromethyl-α,β-diamino acids ISSN 2308-8303 (Print) / 2518-1548 (Online) 15 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) related to the formation of chelated TS A, in which the metal atom is coordinated with two oxygen atoms (of enolate and sulfinyl groups) and a nitro- gen atom, and as a result, an “α-product” with the (R,S)-configuration is formed. In the case of the ca- talysis by TMSOTf, the γ-addition takes place, re- sulting in α,β-unsaturated aminoesters (S,S)-58. Assumably, the oxygen atom of the sulfinyl group coordinates with the sterically hindered trimethylsilyl cation forming an open TS B (Scheme 35) [62, 63]. 3-Alkenyl-2-oxoindoles reacted with polyfluo- roalkylaldimines (S)-18 under the catalysis by organometallic bases (LDA, KНMDS), thus giv- ing γ-addition products 59 in the (S,S)-configu- ration (Scheme 36) [64]. In contrast to reactions with silyldienolates and oxoindoles, the interaction of imines (S)-18 with α,α-dicyanoalkenes led to (R,S)-isomers of γ-products 60. This is explained by the formation of TS A, in which the metal atom of the enolate chelates with the nitrogen atom of the aldimine, leading to the Re-face addition (Scheme 37) [65]. The use of heterocyclic siloxides (furan and pyrrole derivatives) in the addition reactions to imines (S)-18 resulted in non-racemic γ-bute- nolides 62 and γ-butyrolactams 61 It was found that when the reaction was carried out in a low polar solvent (DCM) in the presence of TMSOTf, the process occurred regio- and stereoselectively (Scheme 38) [62, 66]. The reaction of aldimines (S)-18 with indo- les occurred chemo- and stereoselectively in the presence of BF3•Et2O (in DCM) or LDA (in THF) and led to compounds 63 bearing an indole nu- cleus and the pharmacophoric 2,2,2-trifluoro- 1-aminoethyl function (Scheme 39) [67 – 69]. OTMS OR + RF N S O RF NH S O O OR RF NH S O O OR AgBF4 TMSOTf DCM, -78oCDCM, -50oC �� � RF = CF3, CHF2, CF2Br; R = Et, But de 84 98 %– de 86 98 %– N O tBu RFH Nu TS A LA AgO N RF RO Si S O BF4 TS B ( )-S 18 ( , )-R S 57 ( , )-S S 58 89 94 %–62 85 %– � Scheme 35. Different pathways of the silylated dienolates addition to N‑tert‑butylsulfinyl polyfluoroalkyl aldimines + RF N S O KHMDS THF, -78oC de 68 96 %– N O R1 R3 N O R1 R3 R2 R2 NH S O RF Ti(O Pr)i 4 ( )-S 18 ( , )-S S 59RF = CF3, CHF2; R1 = Boc, Moc, Bn, Me R2 = H, Me, OMe, Cl R3 = Me, Ph, 4-MeO-C6H4 4-Cl-C6H4 55 92 %– , Scheme 36. The vinylogous Mannich reaction of 3-alkenyl-2-oxoindoles with N‑tert‑butylsulfinyl polyfluoroalkyl aldimines ISSN 2308-8303 (Print) / 2518-1548 (Online) 16 Журнал органічної та фармацевтичної хімії 2025, 23 (2) The aza-Corey-Chaykovsky reaction is a con- venient method for the construction of an aziri- dine ring, which is an important moiety in syn- thetic chemistry. Thus, cyclization of a series of trifluoromethyl ketimines 3 with dimethylsul- foxonium methylide occurred successfully with both alkyl and aryl ketimines, and with a high stereoselectivity led to (R,S)-2-trifluoromethyl- aziridines 64 [70]. The introduction of N-(tert- butylsulfinyl)imine of trifluoropyruvate into the aza-Corey-Chaykovsky reaction allowed to syn- thesize 2-trifluoromethyl-2-ethoxycarbonylazi- ridine (S,S)-65, an interesting substrate for the synthesis of α-aminocarboxylic acid derivatives (Scheme 40) [71]. 4. Other types of reactions using N-(tert- butylsulfinyl)polyfluoroalkyl imines The aza-Baylis-Hillman reaction is a conve- nient method for the preparation of α-methylene- β-amino acids. The introduction of N-(tert-butyl- sulfinyl)imine of fluoral (R)-10 in the reaction pro- vided high yields and diastereoselectivity (>90 %) even with 10 mol % of a catalyst (Scheme 41) [72]. It is worth noting that the stereochemical result, namely the (R)-configuration of the new stereocen- ter, differs from the reaction with non-fluorinated +RF N S O RF = CF3, CHF2, C2F5, C3F7, C4F9, CF2Cl, CF2Br R = Me, OMe, Br tBuOK CNNC CNNC N H RF S OR R de >99 % K N F3C H S O H CN CN TS A ( )-S 18 ( , )-R S 60 39 95 %– Scheme 37. α,α-Dicyanoalkenes in the vinylogous Mannich reaction with N‑tert‑butylsulfinyl polyfluoroalkyl aldimines RF = CF3, CHF2, C2F5, C3F7, C4F9, CF2Cl, CF2Br45 80 %– de 30 96 %– RF N S O OR OTMS TMSOTf DCM, -78°C O O R RF HN S O N OTBS Boc TMSOTf DCM, -78°CN O RF HN S O Boc R = H: , 70 92 %67 95 % de– – R = Me: , > 99 %47 89 % de– ( )-S 18 ( , , )-S S S 62( , , )-S S S 61 Scheme 38. Siloxy-derivatives of furan and pyrrole in the addition reaction with N‑tert‑butylsulfinyl polyfluoroalkyl aldimines RF N S OH + BF3*Et2O, DCM or LDA, THF HN CF3 S O N R R1 R1 N R R1 R1 2 2Ph R1 = H, 2-Me, 4-CN, 4-MeO, 5-CN, 5-MeO, 5-Me, 5-CO2H, 5-CO2 2 6-Cl, RF = CF3 , 54 98 %36 96 % de– – RF = CF2P(O)(OEt)2 , >96 %49 81 % de– ( )-S 18 ( , )-S S 63 , Scheme 39. The reaction of N‑tert‑butylsulfinyl polyfluoroalkyl aldimines with functionalized indoles ISSN 2308-8303 (Print) / 2518-1548 (Online) 17 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) analogs [73, 74], which supports the conclusion that the process proceeds as an attack in the open TS A as in most reactions with polyfluoroalkyl aldimines. Several enantiomerically enriched α-(trifluoro- methyl)tryptamines were synthesized by the “ene” reaction with imine (R)-10. The reaction pro- ceeded with a high stereoselectivity regardless of the substituents in the indole ring and led to the predominant formation of the (R,R)-stereoi- somer 67 (Scheme 42) [75]. Lithiated ethyl and butyl vinyl ethers success- fully reacted with polyfluoroalkyl aldimines (S)-18 giving optically enriched amines 68 with a high diastereoselectivity (Scheme 43). The configura- tion of the product was assumed to be (S,S) based on previous observations for these types of in- teractions [76]. The addition of hydrophosphoryl compounds to optically pure N-(tert-butylsulfinyl)imines of fluoral or trifluoromethyl ketones leads to deri- vatives of polyfluoroalkyl-substituted α-amino- phosphonic acids. Thus, the reaction of diethyl phos- phite and imine (S)-10 occurred in the presence of potassium carbonate to give products 69 with good yields (65 %) and stereoselectivity (de 76 %). Replacing hydrophosphoryl compounds with their synthetic equivalents, trimethylsilyldialkylphos- phites generated in situ allowed to significantly improve diastereoselectivity (68 – 88 %), while the diastereomeric ratio increased in the series R = Me < Et ≈ Pr < i-Pr (Scheme 44) [77]. Trifluoromethylketimines (R)-70 also enter the reaction with phosphites under catalysis by Ti(OiPr)4 [78]. The reaction is effective for both CF3 N S O R -45oC, DMF R = CH2(CH2)9CH3, Ph, 4-MeOC6H4, 4-ClC6H4, 4-CF3C6H4, C C-1-(5-MeO)naphtyl, C C-1-(3,4-ClC6H3) de 72 99 %– S O CH2 TMSOI NaH, DMF, rt N F3C R S t-Bu O 0oC, toluene S O CH2 TMSOI NaH BuOKor t DMSO, rt N F3C CO2Et S t-Bu O R = CO2Et 24 % de >99 % ( )-S 3 ( , )-R S 64( , )-S S 65 45 93 %– Scheme 40. The aza-Corey-Chaykovsky reaction of N‑tert‑butylsulfinyl trifluoromethyl ketimines in the synthesis of 2-trifluoromethylaziridines + F3C N S O rt, neat de >90 % N CF3H TS A DABCO EWG CF3 NH S O EWG S O H N ORO ( )-R 10 ( , )-R R 66 EWG = CO2Me, CO2tBu, C(O)Me, CN 85 98 %– Scheme 41. The aza-Baylis-Hillman reaction of activated alkenes with N‑(tert‑butylsulfinyl)imine of fluoral + F3C N S O neat, 80oC de 66 76 %– N Boc N Boc HN S O CF3 R R ( )-R 10 ( , )-R R 67 R = 5-H, 5-Me, 5-OMe, 5-Cl, 5-F, 5-CF3, 6-CF3 47 71 %– Scheme 42. The uncatalyzed diastereoselective “ene” reaction of N‑(tert‑butylsulfinyl)trifluoroacetaldimine ISSN 2308-8303 (Print) / 2518-1548 (Online) 18 Журнал органічної та фармацевтичної хімії 2025, 23 (2) alkyl and aryl ketimines and leads to the for- mation of α-trifluoromethylaminophosphonates (S,R)-71 with a stereoselectivity from 87 to 99 %. Although, in contrast to the reaction with imine of fluoral, the use of K2CO3 in the reaction with polyfluoroalkyl ketimines did not lead to the de- sired product, its replacement with stronger in- organic bases, in particular rubidium and cesi- um carbonates, was proved to be more successful [79]. As a result, non-racemic adducts (S,R)-72 were obtained with yields from 56 to 88 % and a high diastereoselectivity (Scheme 45). By the addition of dimethylphosphine oxide to imines (R)-and (S)-18 in the presence of Ti(OiPr)4, enantiomerically pure α-amino-α-polyfluoroalkyl dimethylphosphine oxides 73 were synthesized in high yields and an excellent stereoselectivity. Upon deprotection, water-soluble optically pure amino-substituted dimethylphosphine oxides 74 were isolated in the form of hydrochloride salts (Scheme 46) [80]. Functionalized pyrrolones (S,S)-75 were ob- tained from the imine of trifluoropyruvate (S)-5 by the cyclocondensation with various push-pull + RF N S O tBuLi, THF 70 96 %de – 14 85 %– ( )-S 18 ( , )-S S 68 RF = CF3, CHF2 R = Et, Bu, -(CHn 2-CH2)- -78..0oC OR RF N H S O O R Scheme 43. The reaction of lithiated vinyl ethers with N‑tert‑butylsulfinyl polyfluoroalkyl aldimines F3C N S O N H S OCF3H 56 83 %– de 68 88 %– HP(O)(OEt)2 P RO O OR or Me3SiOP(OR)2 DCM, 0oC K2CO3, DCM, rt ( )-S 10 ( , )-S S 69 Scheme 44. N-(tert-butylsulfinyl)imines of fluoral in the asymmetric synthesis of α‑trifluoromethyl α-aminophosphonic acids RF N S OR HP(O)(OEt)2 Hex/Tol, -40oC Ti(O Pr)i 4 N H S ORF 48 90 %– de 87 99 %– P EtO O OEt RF = CF3, R = Ph, 4-Me-C6H4, 4-MeO-C6H4, 4-Cl-C6H4, Cn 6H13 DCM, rt N H S ORF 56 88 %– de 50 84 %– P R1O O OR1 M2CO3 M = Rb, Cs HP(O)(OR1)2 RF = CF3, CF2Cl, CF2H R1 = Me, Et, Ph ( )-R 70 ( , )-S R 71( , )-S R 72 R R Scheme 45. The addition of phosphites to N‑tert‑butylsulfinyl trifluoromethylketimines RF N S O >99 %de ( )-S 18 ( , )-S S 73 RF = CF3, CHF2, CF2Ph RF N H S OP Ti(O Pr)i 4 Et2O, 0oC P H O O 80 95 %– ( )-S 74 RF NH2 P OHCl dioxane HCl 75 89 %– >99 %de Scheme 46. The Ti-mediated addition of dimethyl phosphine oxide to N‑tert‑butylsulfinyl polyfluoroalkyl aldimines ISSN 2308-8303 (Print) / 2518-1548 (Online) 19 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) enamines, with diastereoselectivity dependent on the nature of substituents in the enamine mol- ecule (Scheme 47) [19]. A series of optically pure cyclic sulfoximines 78 was obtained by the interaction of ArSO2CF2- sulfinyl imines (S)-76 with trimethylsilylphenyl triflates 77, the cycloaddition occurred stereo- specifically to give diastereomer in (R,SS)-confi- guration, meaning that the configuration of the stereogenic sulfur atom was preserved [81, 82] (Scheme 48). ■ Conclusions The analysis of the asymmetric functionali- zation of the azomethine bond of N-(tert-butyl- sulfinyl)polyfluoroalkyl imines allows us to con- clude that the stereoresult of the reactions is determined both by the structure and geometry of the imine and by the reaction conditions (the nature of the solvent, the catalyst, and the tem- perature conditions of the process). The steric and electronic properties of polyfluoroalkyl sub- stituents affect the conformational state of imi- nes (the polyfluoroalkyl substituent is located in the trans position relative to the sulfinyl group), as well as the geometry of the transition state (polyfluoroalkyl substituents usually occupy the equatorial position). However, aldimines are more prone to form the open transition state in the addition reactions to the C=N bond, and the result of the process is therefore regulated by steric factors. While polyfluoroalkyl ketimines are more likely to form transition states with a closed geometry. In the latter case, the sulfinyl group usually participates in regulating the di- rection of the addition due to the ability of the oxygen atom to form coordination bonds. The review demonstrates that N-(tert-butyl- sulfinyl)polyfluoroalkyl imines are versatile sub- strates, which easily interact with different types of nucleophiles, providing access to a wide range of optically pure derivatives of polyfluoro- alkyl-substituted amines, amino alcohols and amino acids. ■ Acknowledgments The authors express their gratitude to the National Academy of Sciences for funding this work (grant No. 0124U002052) and to all the brave defenders of Ukraine. F3C N S O ( )-S 5 MeO2C N R O Me EWGNH CF3 ( , )-S S 75a c– S O Me NHR EWG H + Et2O THFor rt, 3-7 d a: EWG = CO2Et, R = H; : EWG = COb 2Me, R = Me; c: EWG = CN, R = H de 70 90 %– 75 80 %– Scheme 47. Push-pull enamines in the reaction with N‑tert‑butylsulfinyl trifluoromethyl iminopyruvates R CF2SO2Ar N S O tBu + Me3Si TfO R1 R2 S N R1 R2 ArO2SF2C R tBu O CsF, MeCN rt, 12 h Ar = Ph: R = Ph, 3-Me-C6H4, 4-Me-C6H4, 4-Cl-C6H4, 4-Br-C6H4, 3-MeO-C6H4, 4-MeO-C6H4, 4-CF3-C6H4, 6-Br-2-naphtyl, ( )-styryl, Pr; RE i 1, R2 = H, Me, MeO; R2+R3 = -(CH2)3-; R2 = Me, R3 = H Ar = 2-pyridyl: R = Ph, 3-Me-C6H4, 4-Me-C6H4, 3-MeO-C6H4, 4-MeO-C6H4, 4-CF3-C6H4, 4-F-C6H4, 4-Cl-C6H4, 4-Br-C6H4, 4-Ph-C6H4, naphtyl, ( )-styryl, Pr; RE i 1, R2 = H; R2 = Me, R3 = H; R2 = H, R3 = Me; R2+R3 = naphtyl de >99 %( )-S 76 ( , )-R S 78 36 90 %– 77 Scheme 48. The stereoselective [3+2] cycloaddition of N‑tert‑butylsulfinyl ketimines to arynes ISSN 2308-8303 (Print) / 2518-1548 (Online) 20 Журнал органічної та фармацевтичної хімії 2025, 23 (2) ■ References 1. Cogan, D. A.; Guangcheng, L.; Kyungjin, K.; Backes, B. J.; Ellman, J. A. Catalytic Asymmetric Oxidation of tert-Butyl Disulfide. 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spelling oai:ojs.journals.uran.ua:article-3212242026-08-22T19:54:27Z Recent advances in the asymmetric functionalization of N-(tert-butylsulfinyl)polyfluoroalkyl imines Нові досягнення в асиметричній функціоналізації N-(трет-бутилсульфініл)поліфтороалкілімінів Cherednichenko, Alona S. Rassukana, Yuliya V. трет-бутилсульфініл поліфтороалкіліміни асиметричний синтез альдиміни кетиміни стереоселективність tert-butylsulfinyl polyfluoroalkyl imines asymmetric synthesis aldimines ketimines stereoselectivity The review covers the latest achievements in the application of N-(tert-butylsulfinyl)polyfluoroalkyl imines in the asymmetric synthesis and summarizes stereochemical observations of their behavior in different types of reactions (reduction of the C=N bond, addition reactions with organometallic reagents, C-H acids, etc.). Fluorinated N-(tert-butylsulfinyl) imines are convenient substrates for obtaining enantiomerically enriched derivatives of polyfluoroalkyl amines, amino alcohols, amino acids, and heterocyclic systems. In recent decades, various approaches to their functionalization have been proposed. With this in mind, important aspects of their reactivity, regio- and stereochemistry have been systematized in this paper. Огляд охоплює найновіші здобутки в застосуванні N-(трет-бутилсульфініл)поліфтороалкілімінів в асиметричному синтезі, а також узагальнює стереохімічні закономірності їхньої поведінки в різних типах реакцій (відновлення C=N зв`язку, приєднання металоорганічних реагентів, С-Н кислот тощо). Фторовмісні N-(трет-бутилсульфініл)іміни є зручними субстратами для одержання на їх основі енантіомерно збагачених похідних поліфтороалкілімінів, аміноспиртів, амінокислот і азотовмісних гетероциклів. За останні десятиліття було запропоновано різноманітні підходи до їх функціоналізації. З огляду на це важливі аспекти щодо їхньої реакційної здатності, регіо- і стереохімії систематизовано в цій роботі. National University of Pharmacy 2025-04-11 Article Article application/pdf https://ophcj.nuph.edu.ua/article/view/321224 10.24959/ophcj.25.321224 Journal of Organic and Pharmaceutical Chemistry; Vol. 23 No. 2 (2025); 3-22 Журнал органической и фармацевтической химии; Том 23 № 2 (2025); 3-22 Журнал органічної та фармацевтичної хімії; Том 23 № 2 (2025); 3-22 2518-1548 2308-8303 en https://ophcj.nuph.edu.ua/article/view/321224/320261 Copyright (c) 2025 Alona S. Cherednichenko, Yuliya V. Rassukana http://creativecommons.org/licenses/by/4.0
spellingShingle трет-бутилсульфініл
поліфтороалкіліміни
асиметричний синтез
альдиміни
кетиміни
стереоселективність
Cherednichenko, Alona S.
Rassukana, Yuliya V.
Нові досягнення в асиметричній функціоналізації N-(трет-бутилсульфініл)поліфтороалкілімінів
title Нові досягнення в асиметричній функціоналізації N-(трет-бутилсульфініл)поліфтороалкілімінів
title_alt Recent advances in the asymmetric functionalization of N-(tert-butylsulfinyl)polyfluoroalkyl imines
title_full Нові досягнення в асиметричній функціоналізації N-(трет-бутилсульфініл)поліфтороалкілімінів
title_fullStr Нові досягнення в асиметричній функціоналізації N-(трет-бутилсульфініл)поліфтороалкілімінів
title_full_unstemmed Нові досягнення в асиметричній функціоналізації N-(трет-бутилсульфініл)поліфтороалкілімінів
title_short Нові досягнення в асиметричній функціоналізації N-(трет-бутилсульфініл)поліфтороалкілімінів
title_sort нові досягнення в асиметричній функціоналізації n-(трет-бутилсульфініл)поліфтороалкілімінів
topic трет-бутилсульфініл
поліфтороалкіліміни
асиметричний синтез
альдиміни
кетиміни
стереоселективність
topic_facet трет-бутилсульфініл
поліфтороалкіліміни
асиметричний синтез
альдиміни
кетиміни
стереоселективність
tert-butylsulfinyl
polyfluoroalkyl imines
asymmetric synthesis
aldimines
ketimines
stereoselectivity
url https://ophcj.nuph.edu.ua/article/view/321224
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