Синтез піролів з нітроолефінів

The synthesis of pyrroles occupies a key place in synthetic organic chemistry due to the numerous biological properties of pyrrole derivatives, in particular antimicrobial, antibacterial, antifungal, antimalarial, anticancer activities, etc. Therefore, pyrroles serve as building blocks in the creati...

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Veröffentlicht in:Журнал органічної та фармацевтичної хімії
Datum:2025
Jahrgang:23
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Сторінки:48-58
ISSN:2518-1548
Автори та афіліації:
  • Andrii H. Hotynchan — Institute of Organic Chemistry of the National Academy of Sciences of Ukraine
  • Olena M. Kovtun — Dragomanov Ukrainian State University
  • Yuriy P. Kovtun — Institute of Organic Chemistry of the National Academy of Sciences of Ukraine
Hauptverfasser: Hotynchan, Andrii H., Kovtun, Olena M., Kovtun, Yuriy P.
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Sprache:Englisch
Veröffentlicht: National University of Pharmacy 2025
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Journal of Organic and Pharmaceutical Chemistry
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author Hotynchan, Andrii H.
Kovtun, Olena M.
Kovtun, Yuriy P.
author_facet Hotynchan, Andrii H.
Kovtun, Olena M.
Kovtun, Yuriy P.
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container_title Журнал органічної та фармацевтичної хімії
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description The synthesis of pyrroles occupies a key place in synthetic organic chemistry due to the numerous biological properties of pyrrole derivatives, in particular antimicrobial, antibacterial, antifungal, antimalarial, anticancer activities, etc. Therefore, pyrroles serve as building blocks in the creation of potential pharmaceuticals and also serve as the basis for the synthesis of boradipyrromethene dyes. One of the most well-known approaches to the synthesis of pyrroles is the reaction between nitroolefins, 1,3-dicarbonyl compounds, and amines, also known as the Grob-Camenisch reaction. This review is devoted to the historical chronology from the discovery of this transformation dating back to 1950s to the present, and covers the development of various modifications of the above reaction in the synthesis of pyrroles.
doi_str_mv 10.24959/ophcj.25.323775
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fulltext ISSN 2308-8303 (Print) / 2518-1548 (Online) 48 Review Article http://ophcj.nuph.edu.ua UDC 547.74:547.232 A. H. Hotynchan1, O. M. Kovtun2, Yu. P. Kovtun1 1 Institute of Organic Chemistry of the National Academy of Sciences of Ukraine, 5 Academik Kukhar str., 02094 Kyiv, Ukraine 2 Dragomanov Ukrainian State University, 9 Pyrohova str., 01601 Kyiv, Ukraine The Synthesis of Pyrroles from Nitroolefins Abstract The synthesis of pyrroles occupies a key place in synthetic organic chemistry due to the numerous biological properties of pyrrole derivatives, in particular antimicrobial, antibacterial, antifungal, antimalarial, anticancer activities, etc. Therefore, pyrroles serve as building blocks in the creation of potential pharmaceuticals and also serve as the basis for the synthesis of boradipyrromethene dyes. One of the most well-known approaches to the synthesis of pyrroles is the reaction between nitroolefins, 1,3-dicarbonyl compounds, and amines, also known as the Grob-Camenisch reaction. This review is devoted to the historical chronology from the discovery of this transformation dating back to 1950s to the present, and covers the development of various modifications of the above reaction in the synthesis of pyrroles. Keywords: pyrrole; Grob–Camenisch reaction; nitroolefines А. Г. Готинчан1, О. М. Ковтун2, Ю. П. Ковтун1 1 Інститут органічної хімії Національної академії наук України, вул. Академіка Кухаря, 5, м. Київ, 02094, Україна 2 Український державний університет імені Михайла Драгоманова, вул. Пирогова, 9, м. Київ, 01601, Україна Синтез піролів з нітроолефінів Анотація Синтез піролів займає ключове місце в синтетичній органічній хімії завдяки численним біологічним властивостям по- хідних піролу, зокрема антимікробній, антибактеріальній, протигрибковій, антималярійній, протираковій тощо. Саме тому піроли слугують будівельними блоками у створенні потенційних фармацевтичних препаратів, а також є основою для синтезу барвників бордипірометенового ряду. Одним із найвідоміших підходів до синтезу піролів є реакція між ні- троолефінами, 1,3-дикарбонільними сполуками та амінами, відома як реакція Гроба-Каменіша. Цей огляд висвітлює історичну хронологію від відкриття цього перетворення, датованого 1950-ми роками, до сьогодення та охоплює роз- робку різноманітних модифікацій вищезгаданої реакції в синтезі піролів. Ключові слова: пірол; реакція Гроба-Каменіша; нітроолефіни Citation: Hotynchan, A. H.; Kovtun, O. M.; Kovtun, Yu. P. The synthesis of pyrroles from nitroolefins. Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2), 48 – 58. https://doi.org/10.24959/ophcj.25.323775 Received: 26 February 2025; Revised: 4 June 2025; Accepted: 7 June 2025 Copyright© 2025, A. H. Hotynchan, O. M. Kovtun, Yu. P. Kovtun. This is an open access article under the CC BY license (http://creativecommons. org/licenses/by/4.0). Funding: The authors received no specific funding for this work. Conflict of interests: The authors have no conflict of interests to declare. ■ Introduction Heterocyclic compounds are very important in the field of organic chemistry as they are wide- ly spread in nature and commonly used as build- ing blocks in pharmacology. Among heterocycles, pyrrole is of great interest due to its presence in a variety of medicines, such as atorvastatin [1], tolmetin [2], ketorolac [3] etc., and its application in the dye synthesis, for example, BODIPY [4]. Therefore, the pyrrole core synthesis methods play a key role in contemporary organic chemistry. There are some well-known synthetic routes for the pyrrole synthesis. The first one is the Hantzsch reaction, including the transforma- tion between β-ketoesters, ammonia source, and ISSN 2308-8303 (Print) / 2518-1548 (Online) 49 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) haloketones [5]. Alternatively, the Knorr synthe- sis (the reaction between α-amino-ketones and 1,3-dicarbonyl compounds) [6] or the Paal-Knorr synthesis (the reaction between 1,4-diketones and different ammonia sources) [7] can be employed. Due to increased interest, other methods of the pyrrole synthesis were developed. One of them is based on the aza-Wittig reaction, involving the interaction between l-aza-l,3-bis(triphenylphos- phoranylidene)propane and 1,2-diketo-com- pounds [8], and another one includes the reac- tion between 3-formylchromones and amines under TMSCl-mediated conditions [9]. Nitroolefins are an efficient initial material for the synthesis of organic compounds. Their syn- thetic attractiveness refers to the simplicity of their preparation via the condensation between nitroalkanes and aldehydes, known as the Hen- ry reaction [10]. In β-nitrostyrene, the conjugation of the double bond with the nitro group enables it to participate in the Michael addition [11], a reaction that plays a crucial role in the syn- thesis of heterocycles. For example, nitroolefins are widely used in the synthesis of aziridines, pyrrolidines, oxazoles, indoles, etc. [12]. Taking the aforementioned information into account, the aim of this review is to discuss the historical development and progress in the pyr- role synthesis methods from nitroolefin deriva- tives. Discovery of the Grob-Camenisch reac- tion The first literary mention of the pyrroles syn- thesis from nitro compounds refers to the work of Grob and Kamenisch, dating back to 1953 [13]. Using 1-nitro-2-methylaminopropane and ace- toacetic ester, the authors synthesized ethyl 1,2,4-trimethyl-2-pyrrolecarboxylate with a yield of 31 %. They suggested the following mechanism (Scheme 1). In the solution, 1-nitro-2-methyl- aminopropane (1) exists in equilibrium with me- thylamine (2) and 1-nitropropene (3). After the addition of acetoacetic ester, the latter under- goes the condensation to form the corresponding enamine 4, which further reacts with 1-nitropro- pene, resulting in Michael’s product 5. This pro- duct 5 cyclizes into dihydropyrrole 6, eliminat- ing a molecule of nitrous acid, which, in turn, oxidizes intermediate 6, forming pyrrole 7. The further development of the reaction in- volving nitroolefins, 1,3-dicarbonyl compounds, and amines focused on identifying alternative synthetic approaches to increase pyrrole yields and expand the range of substrates that could be used. Currently, several variants of this reac- tion are known, including two-, three-, and four- component Grob-Camenisch-type reactions. A two-component Grob-Camenisch-type reaction The two-component Grob-Camenisch-type synthesis of pyrroles involves the reaction of β-enaminoesters or ketones with nitrostyrenes. First reported in 1981, this method utilized enamines 8, derived from acetoacetic ester and (E)-(2-nitroprop-1-en-1-yl)benzene (9) [14]. Reflux- ing the reaction mixture in ethanol for four to six hours allows the pyrroles 10 to be obtained with yields ranging from 16 % to 80 % (Scheme 2). The authors also found that using N-unsub- stituted enamine 11 in the reaction with nitro Me H N NO2 Me Me NH2 + Me NO2 Me O CO2Et Me NH2 Me NHMe CO2Et Me NO2 Me NO2 EtO2C NHMe - HNO2 N MeEtO2C HNO2 N MeEtO2C 1 2 3 4 5 67 MeMe Me MeMe 32 Scheme 1. The synthesis of pyrrole by Grob–Camenisch ISSN 2308-8303 (Print) / 2518-1548 (Online) 50 Журнал органічної та фармацевтичної хімії 2025, 23 (2) compound 9 by refluxing in ethanol for 14 hours could produce pyrrole 12 with a yield of 51 % (Scheme 3). Enaminoketones can also be used in a Grob- Camenisch-type reaction. However, harsher con- ditions are required, delivering the products with lower yields compared to standard substrates. Specifically, the reaction of enamine 13 with ni- trostyrene 10 in a melt at 150°C produces pyr- role 14 with a yield of only 26 % (Scheme 4) [14]. Further studies of the pyrrole synthesis from nitrostyrenes and β-enaminoesters or β-enami- noketones showed that enaminones 15 reacted with nitrostyrene or p-tolylnitrostyrene (16) un- der solvent-free conditions, yielding pyrroles in 70 – 90 % yield (Scheme 5) [15]. The mechanism proposed involves the Michael-type addition of β-enaminones to nitroolefins, forming interme- diate 17, which cyclizes to pyrroline 18 with the elimination of nitrous acid. The subsequent oxi- dation results in the production of the final pyr- role 19. The scope and diversity of pyrroles synthe- sized from β-enaminones or esters and nitroole- fins can be enhanced by using solvents or cata- lysts. For instance, the reaction of N-phenyl- substituted enamine 20 with substituted nitro- propene 21 in methanol at 120°C yields penta- substituted pyrroles 22 (Scheme 6) [16]. The authors observed that catalytic amounts of bases (e.g., sodium acetate or piperidine) and polar aprotic solvents (e.g., DMSO or acetonitrile) H N R Me H CO2Et N CO2Et MeMe Ph R + Ph Me NO2 8 9 10 R = Me ( ), cyclopropyl ( )80 % 16 % EtOH Scheme 2. The synthesis of pyrroles from methyl- and cyclopropyl-derived enaminoesters H2N Me H CO2Et N H CO2Et MeMe Ph + Ph Me NO2 11 9 12 EtOH 51 % Scheme 3. The synthesis of pyrrole from N-unsubstituted enaminoester O HN R N Ph Me O 13 14 R = OMe OMe + R Ph Me NO2 9 neat 150 Cº 26 % Scheme 4. The synthesis of pyrrole from enaminone based on dimedone + R O Me N Ar NO2 R O Me Ar NO2 N H R' - HNO2 N Me R' O R Ar 17 18 [Ox] R O Me HN R' Ar NO2 N Ar O R Me R' R = Me, OEt R' = Bn, Bu, -Hexn c Ar = Ph, Tolp- 15 16 19 R' neat 70 95 %– Scheme 5. The reaction mechanism of the pyrrole formation in the reaction between enamines and nitrostyrenes ISSN 2308-8303 (Print) / 2518-1548 (Online) 51 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) significantly decreased pyrrole yields. Electron- donating substituents on the aryl groups of ni- trostyrenes and β-enaminoesters substantially improve yields compared to electron-withdraw- ing ones. It is noteworthy that the use of [2-ni- troprop-1-en-1-yl]furan made it possible to syn- thesize pyrrole with a furyl group in position 3, yielding 79 % of the product. Additionally, the application of nitrostyrene as a reagent facilitates the production of α-CH pyrrole with good yields. Catalytic reactions provide an effective pre- parative method for synthesizing pyrroles from β-enaminoesters and nitroolefins. For instance, using iodine as a catalyst allows the formation of N-substituted pyrroles from nitrostyrene and β-enaminoesters derived from the acetoacetic ester. It is noteworthy that nitrostyrenes bearing electron-donating substituents result in pyrroles with significantly higher efficiency, whereas N-alkyl-substituted 3-aminobut-2-enoates lead to slightly lower yields due to competing side re- actions [17]. The Ph3PAuCl catalyst combined with AgO- Tf significantly enhances the pyrrole synthe- sis via a two-component reaction. Reactions of N-substituted enamines 23 obtained from ace- toacetic ester or acetylacetone with substituted nitrostyrenes 24 lead to pyrroles 25 with yields exceeding 80 % (Scheme 7) [18]. It is noteworthy that the nature of substituents in aryl groups has minimal impact on pyrrole yields, and N-alkyl- substituted enamines react without side reactions, also giving pyrroles in high yields. The PEG-400 catalyst demonstrated a high effectiveness for synthesizing isoxazole deriva- tives bearing a pyrrole moiety in position 4 [19]. The reaction of ethyl 3-((3-methyl-5-((E)-styryl)- isoxazol-4-yl)amino)but-2-enoate derivatives (26) with nitrostyrenes 27 gave the corresponding pyr- roles 28 with yields from 70 to 90 % (Scheme 8). A solid-phase method for the pyrrole synthe- sis was also developed [20]. Initially, Rink Amide resin (29) is acetoacetylated with diketene to form amide 30, which is subsequently converted to polymer-bound enaminone 31 upon the treatment with primary amines. Further reaction of polymer- bound 31 with nitroolefins in a DMF/EtOH sol- vent mixture at 60°C yielded pyrroles 32, which upon the treatment with trifluoroacetic acid pro- duced final amides 33. In this method, the pyr- role yield exceeds 80 % when using both alipha- tic and aromatic amines, as well as aliphatic ni- troolefins (Scheme 9). A three-component Grob-Camenisch-type reaction The three-component Grob-Camenisch syn- thesis of pyrroles involves the reaction of amines, 1,3-dicarbonyl compounds, and nitrostyrenes, R 2 R 1 NO2Me NHPh CO2Me MeOH, 120 ºC N CO2Me Me Ph R 2 R 3 2120 22 R 1 = H, Me R 2 = Ph, 4-Me-C6H4, 3-Me-C6H4, 4-OMe-C6H4, 4-Me-C6H4, 4-NMe2-C6H4, 4-F-C6H4, 2-furfuryl + 75 85 %– Scheme 6. The synthesis of N-substituted pyrroles 22 Me NH R 2 O O2N Ar R 1 Ph3PAuCl AgOTf NO2 Ar OR 2 NH Me R 1 N Ar OR 2 NH Me R 1 OH O N Ar O R 2 N Me R 1 OH HO - H2O - HNO N R 1 Me Ar O R 2 R 1 R 2 = Me, OEt 23 24 25 + 75 95 %– Scheme 7. The reaction mechanism of the pyrrole formation in the reaction between enamines and nitrostyrenes catalyzed with Ph3PAuCl ISSN 2308-8303 (Print) / 2518-1548 (Online) 52 Журнал органічної та фармацевтичної хімії 2025, 23 (2) which make it possible to prepare pyrroles with catalytic activity. For instance, research [21] de- monstrates that lactic acid serves as an effective medium for synthesizing tetrasubstituted pyr- roles from acetylacetone and substituted ani- lines, achieving yields of approximately 70 – 90 %. The study indicates that neither electron-with- drawing nor electron-donating substituents on the aniline significantly influence pyrrole yields. Iron-based catalysts, such as FeCl3, are wide- ly employed in the catalytic synthesis of pyrroles from nitroolefins and 1,3-dicarbonyl compounds. For instance, FeCl3 facilitates a three-component reaction, yielding pyrroles at 70 – 80 % using 1,3-dicarbonyl compounds like acetoacetic es- ter, acetylacetone, or ethylbenzyl acetate [22]. As a Lewis acid, FeCl3 promotes the formation of β-enaminoester 34, which undergoes the Mi- chael-type addition to nitrostyrene, followed by the cyclization of the resulting adduct 35 into pyrrole via the nitro group conversion to its aci- nitro form (Scheme 10). Interestingly, iron(III) chloride makes it pos- sible to synthesize pyrroles from nitrostyrene bearing ethynyl substituents in the ortho-position, obtaining the target products with a yield of about 50 % [23]. Additionally, the catalyst facili- tates the pyrrole synthesis from peptides with a free amino group [24]. An alternative to FeCl3 is the use of Fe3O4 na- noparticles, in particular Fe3O4@SiO2-CPTMS- guanidine-SO3H, which contain a terminal sulfo group [24]. This catalyst allows the synthesis of tetrasubstituted pyrroles from acetoacetic ester, acetylacetone, and para-chloro- or para-bromo- anilines with yields of approximately 90 % (Scheme 11). The sulfo group is supposed to ca- talyze the reaction similarly to FeCl3. Cerium(III) chloride serves as an alternative catalyst to FeCl3, effective in the microwave-as- sisted synthesis using nitromethane as a solvent [26]. This method allows the synthesis of tet- rasubstituted pyrroles from acetoacetic ester or acetylacetone, nitrostyrenes, and anilines, with yields of about 80 %. However, when para-chlo- ronitrostyrene is used, the yield decreases to about 50 %. An alternative to CeCl3 is cerium(IV) ammo- nium nitrate (CAN), which catalyzes the reac- tion of nitrostyrene 38, acetoacetic ester (36), N O HN Ar 1 Me Me O EtO Ar NO2 R PEG-400 (10 mol%) H2 N O Ar 1 Me N Me R Ar CO2Et 26 27 28 R 1 = H, Me, Ph + 70 90 %– O, reflux, 3–4 h Scheme 8. The synthesis of pyrroles 28 NH2 O O CH2Cl2 -15 C to rt, 2.5 hº N H O Me O rt, 48 h N H O Me HN R 1 DMF/EtOH (1:1) 60 C, 2hº R 3 H NO2 R 2 NMe R 2 R 3 R 1 N H O 20 % TFA/CH2Cl2, 30 min NMe R 2 R 3 R 1 H2N O 31 32 33 29 30 R 1 NH2 R 1 = 2-phenylethyl, pyperonyl, cyclopropyl, 2-furfuryl, thiophene-2-ethyl, R 2 = H, Me R 3 = H, Ph, -Cl-Cp 6H4, 4-OMe-C6H4, 3-OMe-C6H4, 4-bromothienyl, cyclohexyl 45 90 %– Scheme 9. The solid-phase synthesis of pyrroles from nitroolefins ISSN 2308-8303 (Print) / 2518-1548 (Online) 53 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) and benzylamine (37) at room temperature in me- thanol [27]. This method produces pyrroles with yields ranging from 50 to 75 % (Scheme 12). In addition to other metal-containing cata- lysts, Ph3PAuCl combined with AgOTf [28] and zirconyl dichloride complexes [29] makes it pos- sible to use acetoacetic ester and various β-dike- toamides as 1,3-dicarbonyl compounds, yielding pyrroles at approximately 70 %. Furthermore, diacetoxyiodobenzene serves as an effective non-metal catalyst for the pyrrole syn- thesis, producing pyrroles from acetoacetic ester and acetylacetone with yields of about 70 %, un- affected by substituents on nitrostyrene or ani- line [30, 31]. The combination of oxone and iodobenzene makes it possible to synthesize pyrroles from ni- trostyrenes, acetylacetone, or acetoacetic ester, and anilines, yielding 80 – 90 % of the desired product. Notably, neither electron-donating nor electron-withdrawing substituents on nitrosty- rene or aniline impact the pyrrole yield [31]. R 1 NO2 R 2 R 3 O O R 4 R 5 NH2 FeCl3 (5 mol%) N R 2R 3 R 5 R 1R 4 O FeCl3 - H2O R 3 NH O R 4 R 5 R 1 NO2 R 2 FeCl3 NH R 2 R 3 R 5 R 1 R 4 O N OH O - HNO - H2O 34 35 + + R 1 = Ph, 4-Me-C6H4, 4-Me-C6H4, 4-OMe-C6H4, 4-Cl-C6H4, Br-C6H4, 2-thiophenyl, 2-naphtyl R 2 = H, Me R 3 = Me, Ph R 4 = Me, OEt R 5 = 4-Me-C6H4, 4-Me-C6H4, 4-OMe-C6H4, 4-F-C6H4, 4-Cl-C6H4, Br-C6H4, 2-naphtyl 60 90 %– Scheme 10. The reaction mechanism of the three-component synthesis of pyrroles from nitroolefins catalyzed with FeCl3 O O R 2 Me R 1 NH2 HO3S NH Me O R 2 NO2 N O R 2 Me NH OH O HO3S N Me N HO OH R 2 O H - HNO - H2O N Me R 2 O 5 + R 1 R 3 R 1 R 3 R 3 R 1 R 3 R 1 R 1 = Ph, 4-Cl, 4-Br R 2 = Me, OEt R 3 = H, 4-Me, 4-Cl, 4-OMe 85 90 %– Scheme 11. The reaction mechanism of the three-component synthesis of pyrroles from nitroolefins catalyzed with Fe3O4@SiO2-CPTMS-guanidine-SO3H ISSN 2308-8303 (Print) / 2518-1548 (Online) 54 Журнал органічної та фармацевтичної хімії 2025, 23 (2) Ionic liquids, such as N-methyl-2-pyrrolido- nium methyl sulfonate, serve as effective catalysts for the three-component synthesis of pyrrole in- volving nitroolefins, amines, and 1,3-dicarbonyl compounds. Notably, the yields of pyrroles from substituted nitrostyrenes and anilines, ranging from 70 to 90 %, show no correlation with the sub- stituent effects. However, using aliphatic nitro- olefins and amines decreases yields to 30 % [32]. A four-component Grob-Camenisch-type reaction Another convenient option for the synthesis of pyrroles is a four-component reaction involv- ing aldehydes, nitroalkanes, 1,3-dicarbonyl com- pounds, and amines. Currently, only catalytic va- riants of this transformation have been developed using FeCl3 [32], palladium [34], and tungsten- based complexes [35], CuO nanoparticles [36], ionic liquids [37, 38], iodine [39], clay [40], NiCl2·6H2O [41], as well as organic acids – lactic and gluconic [42] (Scheme 13). The reaction mechanism includes the cata- lyzed formation of a β-enaminone from a nitro- olefin, followed by the Michael addition to form an intermediate. This intermediate undergoes eli- mination of a hyponitrous acid molecule, result- ing in the formation of pyrrole. The synthesis of N-unsubstituted α-CH pyrroles The synthesis of N-H α-CH pyrroles is of sig- nificant interest in the Grob cyclization, as these compounds serve as precursors for luminescent BODIPY borofluoride complexes and porphyrins. The earliest reported attempt to synthesize such Me O CO2Et Bn NH2 EtO2C Ph OAc NO2 CAN (15 mol%) MeOH, rt CAN Bn N H Me CO2Et CO2Et OAc Ph O2N - OAc, - H + SN2' N Me Bn O OEt NO2 Ph EtO2C H 5-exo-trig N OEt O O2N Ph H CO2Et Me Bn N EtO2C Ph CO2EtMe Bn - HNO2 36 37 38 + + + H + 65 % Scheme 12. The reaction mechanism of the three-component synthesis of pyrroles from nitroolefin 38 R 1 NH2 R 2 CHO R 3 O O R 4 R 5 NO2 N R 5R 3 R 1 R 2R 4 O Lewis acid R 3 NH O R 4 R 2 NO2 R 5 R 2 H NO R 4 R 2 N R 5 R 1 R 3 OHO N R 5 R 3 R 1 R 2 R 4 O H N OH OH - HNO - H2O + + + Lewis acid 40 85 %– R 1 = benzyl, cycloxehyl R 2 = Ph, 4-Me-C6H4, 4-OMe-C6H4, 4-F-C6H4, 4-Cl-C6H4, 4-Br-C6H4, 4-CN-C6H4, 4-NO2-C6H4, 2-thiophenyl, 2- furfuryl, 2-naphtyl R 3 =Ph, Me R 4 = OMe, OEt R 5 = H, Me Scheme 13. The reaction mechanism of the four-component synthesis of pyrroles from nitroolefins catalyzed by Lewis acids ISSN 2308-8303 (Print) / 2518-1548 (Online) 55 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) pyrroles was by Grob [13] where 1-nitropropan- 2-amine 39 and acetoacetic ester were used. However, instead of the expected N-H pyrrole, an N-substituted derivative 44 was obtained. This outcome was attributed to intermediate 41 possessing two nucleophilic centers: a carbon atom and a nitrogen one. Hence, two Michael additions occur, leading to intermediate 42, which under- goes further cyclization, thus yielding N-isopro- pyl derivative 44 instead of the expected N-H one (Scheme 14). In order to synthesize the corresponding N-H α-CH pyrrole, Grob first isolated interme- diate 45, which failed to transform into pyrrole 46 under different conditions (Scheme 15). The author attributed this to the conjugation of the nitrogen atom lone pair in intermediate 45 with the ethoxycarbonyl group reducing its nucleo- philicity. However, interestingly, upon the treat- ment of 45 with methylamine, pyrrole 48 could be isolated, assuming that the transamination occurred with the formation of 47, which then cyclized to 48. From this observation, it could be suspected that the presence of even weak elec- tron-donating groups favors the pyrrole synthe- sis by the Grob cyclization. In the subsequent study, Gómez-Sánchez [43] investigated the synthesis of N-H α-CH pyrro- les using nitro compounds, with a focus on the for- mation of anomalous Michael products from ni- trostyrene and acetylacetone. By employing non- catalytic amounts of sodium methoxide with ace- tylacetone and nitrostyrene 49, the authors obtain- ed anomalous Michael products 50 (Scheme 16). The latter product, upon the treatment with sa- turated methanolic ammonia solution at 0°C, gives rise to pyrrole 51 (Scheme 16). Based on this observation, the authors deve- loped a one-pot procedure of the pyrrole synthe- sis, including the treatment of nitrostyrene 49 with acetylacetone, acetoacetic ester, or methyl acetoacetate in methanol with a non-catalytic H2N Me NO2 + Me NO2 Me O CO2Et + Me NH2 CO2Et Me HN CO2Et Me NO2 N Me EtO2C Me N Me EtO2C Me 39 40 41 42 43 Me NO2 NH3 NH3 Me NO2 Me NO2 Me NO2 2-step addition -HNO2 HNO2 44, 55 % Scheme 14. The synthesis of pyrrole by Grob-Camenisch NH2Me EtO2C Me NO2 N H Me EtO2C Me 45 46 MeNH2 N H Me EtO2C Me NO2 47 N Me EtO2C Me 48, 31 % Me Me Scheme 15. Transformations of intermediate 45 ISSN 2308-8303 (Print) / 2518-1548 (Online) 56 Журнал органічної та фармацевтичної хімії 2025, 23 (2) amount of sodium methoxide at 0°C for 1 hour with further addition of an ammonia source, such as aniline, benzylamine or saturated methano- lic ammonia solution. This synthetic procedure allowed obtaining pyrroles 52 with yields of up to 80 % (Scheme 17). Two additional literature references describe similar methods for synthesizing N-H α-CH pyr- roles, involving the initial formation of the Mi- chael addition product between nitrostyrenes 53 and acetoacetic ester, followed by the treatment with ammonia (Scheme 18). Using this approach, pyrroles 54 were obtained, though in low yields, from 25 to 30 % [44, 45]. ■ Conclusions The Grob-Camenisch synthesis of pyrroles is highly valued for its straightforward methods and procedures, as evidenced by numerous pub- lications. The main advantage of this reaction is the possibility of obtaining tetra- and three-sub- stituted pyrrole derivatives. This reaction also allows the synthesis of pyrroles in multi-gram amounts. It is noteworthy that for this method, it is possible to use catalysts of different types (Lewis and Brønsted acids, nanoparticles, etc.), which broadens the synthetic possibilities of the pyrrole synthesis. ■ References 1. Novozhilov, Y. V.; Dorogov, M. V.; Blumina, M. V.; Smirnov, A. V.; Krasavin, M. An Improved Kilogram-Scale Preparation of Atorvastatin Calcium. Chem. Cent. J. 2015, 9 (1). https://doi.org/10.1186/s13065-015-0082-7. 2. Artico, M.; Corelli, F.; Massa, S.; Stefancich, G. Non-steroidal antiinflammatory agents. A novel synthesis of 1-methyl-5-p-tolylpyrrole- 2-acetic acid (tolmetin). J. Het. Chem. 1982, 19 (6), 1493 – 1495. https://doi.org/10.1002/jhet.5570190647. 3. Müller, P.; Polleux, Ph. Synthesis of a Ketorolac Model via Aromatic Carbenoid Insertion. Helv. Chim. Acta. 1998, 81 (2), 317 – 323. https://doi.org/10.1002/hlca.19980810212. 4. Ulrich, G.; Ziessel, R.; Harriman, A. The Chemistry of Fluorescent Bodipy Dyes: Versatility Unsurpassed. Angew. Chem. Int. Ed. 2008, 47 (7), 1184 – 1201. https://doi.org/10.1002/anie.200702070. 5. Hantzsch, A. Neue Bildungsweise von Pyrrolderivaten. Ber. Dtsch. Chem. Ges. 1890, 23 (1), 1474 – 1476. https://doi.org/10.1002/cber.189002301243. 6. Knorr, L. Synthese von Pyrrolderivaten. Ber. Dtsch. Chem. Ges. 1884, 17 (2), 1635 – 1642. https://doi.org/10.1002/cber.18840170220. 7. Paal, C. Synthese von Thiophen‐ und Pyrrolderivaten. Ber. Dtsch. Chem. Ges. 1885, 18 (1), 367 – 371. https://doi.org/10.1002/cber.18850180175. 8. Katritzky, A. R.; Jiang, J.; Steel, P. J. 1-Aza-1,3-bis(triphenylphosphoranylidene)propane: A Novel :CHCH2N: Synthon. J. Org. Chem. 1994, 59, 4551. https://doi.org/10.1021/jo00095a034. Ph NO2 + Me O Me O N H Ph O Me Me 49 MeONa NH3 51, 93 % O Ph Me Ph Me OH N O MeOH, 0 Cº MeOH, 0 Cº 50, 92 % Me O Me O -HNO2, -H2O Scheme 16. The synthesis of anomalous Michael’s product 50 and pyrrole 51 52 N Ph R 2 O R 1 Me a: R 1 = OMe, R 2 = H b: R 1 = OEt, R 2 = H c: R 1 = Me, R 2 = H d: R 1 = OMe, R 2 = CH2Ph e: R 1 = OMe, R 2 = Ph f: R 1 = O Bu, Rt 2 = H Ph NO2 + Me O R 1 O 49 1. MeONa / MeOH, 0 Cº 2. R 2 -NH2 / MeOH, 0 Cº 50 80 %– Scheme 17. The one-pot pyrrole synthesis by Gómez-Sánchez 52 N H O EtO Me R 1 = 4-NC-C6H4, 2-O2N-C6H4 NO2 + Me O OEt O 49 1. MeONa / MeOH, 0 Cº 2. NH3 / MeOH, 0 Cº 25 30 %– R 1 R 1 Scheme 18. The synthesis of other pyrrole derivatives by the Gómez-Sánchez-like procedure ISSN 2308-8303 (Print) / 2518-1548 (Online) 57 Journal of Organic and Pharmaceutical Chemistry 2025, 23 (2) 9. Plaskon, A. S.; Ryabukhin, S. V.; Volochnyuk, D. M.; Shivanyuk, A. N.; Tolmachev, A. A. The Synthesis of 5-Hetaryl-3-(2-Hydroxybenzoyl) Pyrroles. Tetrahedron 2008, 64 (25), 5933 – 5943. https://doi.org/10.1016/j.tet.2008.04.041. 10. González-Olvera, R.; Vergara-Arenas, B. I.; Negrón-Silva, G. E.; Angeles-Beltrán, D.; Lomas-Romero, L.; Gutiérrez-Carrillo, A.; Lara, V. H.; Morales-Serna, J. A. Synthesis of β-Nitrostyrenes in the Presence of Sulfated Zirconia and Secondary Amines. RSC Adv. 2015, 5 (120), 99188 – 99192. https://doi.org/10.1039/c5ra17168g. 11. Stowe, G. N.; Janda, K. D. A Diels-Alder Reaction Conducted within the Parameters of Aqueous Organocatalysis: Still Just Smoke and Mirrors. Tetrahedron Lett. 2011, 52 (17), 2085 – 2087. https://doi.org/10.1016/j.tetlet.2010.10.134. 12. Halimehjani, A. Z.; Namboothiri, I. N. N.; Hooshmand, S. E. Part I: Nitroalkenes in the Synthesis of Heterocyclic Compounds. RSC Adv. 2014, 4 (89) 48022 – 48084. https://doi.org/10.1039/c4ra08828j. 13. Grob, C. A.; Camenish, K. Eine neue Pyrrolring-Synthese, Helv. Chim. Acta. 1953, 36 (1), 49 – 58. https://doi.org/10.1002/hlca.19530360109. 14. Meyer, H. Dihydropyridine, VI. Diimidomalonsäurederivate in der Hantzsch‐Pyridin‐Synthese. Liebigs Ann. Chem. 1981, 1981 (9). 1523 – 1533. https://doi.org/10.1002/jlac.198119810902. 15. Yavari, I.; Ghazvini, M.; Aminkhani, A. Solvent-Free Synthesis of 1,2,3,4-Tetrasubstituted Pyrroles from Enaminones and β-Nitrostyrenes. J. Chem. Res. 2011, 35 (10), 558 – 560. https://doi.org/10.3184/174751911X13164434098696. 16. Guan, Z. H.; Li, L.; Ren, Z. H.; Li, J.; Zhao, M. N. A Facile and Efficient Synthesis of Multisubstituted Pyrroles from Enaminoesters and Nitroolefins. Green Chem. 2011, 13 (7), 1664 – 1668. https://doi.org/10.1039/c1gc15278e. 17. Xu, H.; Li, Y.; Xing, M.; Jia, J.; Han, L.; Ye, Q.; Gao, J. Synthesis of Pyrroles from β-Enamines and Nitroolefins Catalyzed by I2 under High- Speed Vibration Milling (HSVM). Chem. Lett. 2015, 44 (4), 574 – 576. https://doi.org/10.1246/cl.141102. 18. Abdukader, A.; Xue, Q.; Lin, A.; Zhang, M.; Cheng, Y.; Zhu, C. Gold-Catalyzed Cascade C-C and C-N Bond Formation: Synthesis of Poly- substituted Indolequinones and Pyrroles. Tetrahedron Lett. 2013, 54 (44), 5898 – 5900. https://doi.org/10.1016/j.tetlet.2013.08.100. 19. Ponduri, R.; Kumar, P.; Vadali, L. R. PEG-400 Promoted a Simple, Efficient, and Recyclable Catalyst for the One-Pot Eco-Friend- ly Synthesis of Functionalized Isoxazole Substituted Pyrroles in Aqueous Medium. Synth. Commun. 2018, 48 (24), 3113 – 3122. https://doi.org/10.1080/00397911.2018.1535078. 20. Trautwein, A. W.; Jung, G. Solid-phase synthesis of pyrroles from enaminones and nitroalkenes. Tetrahedron Lett. 1998, 39, 8263 – 8266. https://doi.org/10.1016/S0040-4039(98)01887-5. 21. Akbaslar, D.; Giray, E. S.; Algul, O. Revisit to the Synthesis of 1,2,3,4-Tetrasubstituted Pyrrole Derivatives in Lactic Acid Media as a Green Solvent and Catalyst. Mol. Divers. 2021, 25 (4), 2321 – 2338. https://doi.org/10.1007/s11030-020-10122-1. 22. Sarkar, S.; Bera, K.; Maiti, S.; Biswas, S.; Jana, U. Three-Component Coupling Synthesis of Diversely Substituted N-Aryl Pyrroles Cata- lyzed by Iron(III) Chloride. Synth. Commun. 2013, 43 (11), 1563 – 1570. https://doi.org/10.1080/00397911.2011.650273. 23. Sarkar, S.; Bera, K.; Jalal, S.; Jana, U. Synthesis of Structurally Diverse Polyfunctional Pyrrolo[1,2-a]Quinolines by Sequential Iron- Catalyzed Three-Component Coupling and Gold-Catalyzed Hydroarylation Reactions. Eur. J. Org. Chem. 2013, 27, 6055 – 6061. https://doi.org/10.1002/ejoc.201300659. 24. Jad, Y. E.; Gudimella, S. K.; Govender, T.; De La Torre, B. G.; Albericio, F. Solid-Phase Synthesis of Pyrrole Derivatives through a Multicompo- nent Reaction Involving Lys-Containing Peptides. ACS Comb. Sci. 2018, 20 (4), 187 – 191. https://doi.org/10.1021/acscombsci.8b00006. 25. Rostami, H.; Shiri, L. Fe3O4@SiO2—CPTMS—Guanidine—SO3H-Catalyzed One-Pot Multicomponent Synthesis of Polysubstituted Pyrrole Derivatives under Solvent-Free Conditions. Russian J. Org. Chem. 2019, 55 (8), 1204 – 1211. https://doi.org/10.1134/S1070428019080207. 26. Silveira, C. C.; Mendes, S. R.; Martins, G. M.; Schlösser, S. C.; Kaufman, T. S. Modular CeCl3·7H2O-Catalyzed Multi-Component Synthesis of 1,2,3,4-Tetrasubstituted Pyrroles under Microwave Irradiation and Their Further Trichloroisocyanuric Acid-Mediated Conversion into 5-Sulfenylpyrrole Derivatives. Tetrahedron 2013, 69 (43), 9076 – 9085. https://doi.org/10.1016/j.tet.2013.08.035. 27. Magar, D. R.; Ke, Y. J.; Chen, K. Three-Component Synthesis of Functionalized N-Protected Tetrasubstituted Pyrroles by an Addition- Elimination-Aromatization Process. Asian J. Org. Chem. 2013, 2 (4), 330 – 335. https://doi.org/10.1002/ajoc.201200193. 28. Li, L.; Chen, Q.; Xiong, X.; Zhang, C.; Qian, J.; Shi, J.; An, Q.; Zhang, M. Synthesis of Polysubstituted Pyrroles via a Gold(I)-Catalyzed Tandem Three- Component Reaction at Room Temperature. Chinese Chem. Lett. 2018, 29 (12), 1893 – 1896. https://doi.org/10.1016/j.cclet.2018.09.004. 29. Goyal, S.; Patel, J. K.; Gangar, M.; Kumar, K.; Nair, V. A. Zirconocene Dichloride Catalysed One-Pot Synthesis of Pyrroles through Nitroalkene- Enamine Assembly. RSC Adv. 2015, 5 (5), 3187 – 3195. https://doi.org/10.1039/c4ra09873k. 30. Jadhav, N. C.; Pahelkar, A. R.; Desai, N. V.; Telvekar, V. N. Design, Synthesis and Molecular Docking Study of Novel Pyrrole-Based α-Amylase and α-Glucosidase Inhibitors. Med. Chem. Res. 2017, 26 (10), 2675 – 2691. https://doi.org/10.1007/s00044-017-1965-z. 31. Jadhav, N. C.; Jagadhane, P. B.; Patile, H. V.; Telvekar, V. N. Three-Component Direct Synthesis of Substituted Pyrroles from Easily Accessible Chemi- cal Moieties Using Hypervalent Iodine Reagent. Tetrahedron Lett. 2013, 54 (23), 3019 – 3021. https://doi.org/10.1016/j.tetlet.2013.04.014. 32. Pachechne, L. A.; Pereira, V. F.; Martins, G. M.; Martendal, E.; Xavier, F. R.; Mendes, S. R. One-Pot Multicomponent Synthesis of 1,2,3,4-Tetra- substituted Pyrroles Catalyzed by [NMPH]CH3SO3. Tetrahedron Lett. 2019, 60 (38), 151043. https://doi.org/10.1016/j.tetlet.2019.151043. 33. Maiti, S.; Biswas, S.; Jana, U. Iron(III)-Catalyzed Four-Component Coupling Reaction of 1,3-Dicarbonyl Compounds, Amines, Aldehydes, and Ni- troalkanes: A Simple and Direct Synthesis of Functionalized Pyrroles. J. Org. Chem. 2010, 75 (5), 1674 – 1683. https://doi.org/10.1021/jo902661y. 34. Reddy, G. R.; Reddy, T. R.; Joseph, S. C.; Reddy, K. S.; Reddy, L. S.; Kumar, P. M.; Krishna, G. R.; Reddy, C. M.; Rambabu, D.; Kapavarapu, R.; Lakshmi, C.; Meda, T.; Priya, K. K.; Parsa, K. V. L.; Pal, M. Pd-Mediated New Synthesis of Pyrroles: Their Evaluation as Potential Inhibitors of Phosphodiesterase 4. Chem. Commun. 2011, 47 (27), 7779 – 7781. https://doi.org/10.1039/c1cc12321a. 35. Atar, A. B.; Jeong, Y. T. Heterogenized Tungsten Complex: An Efficient and High Yielding Catalyst for the Synthesis of Structur- ally Diverse Tetra Substituted Pyrrole Derivatives via Four-Component Assembly. Tetrahedron Lett. 2013, 54 (41), 5624 – 5628. https://doi.org/10.1016/j.tetlet.2013.08.016. 36. Saeidian, H.; Abdoli, M.; Salimi, R. One-Pot Synthesis of Highly Substituted Pyrroles Using Nano Copper Oxide as an Effective Hetero- geneous Nanocatalyst. C. R. Chim. 2013, 16 (11), 1063 – 1070. https://doi.org/10.1016/j.crci.2013.02.008. 37. Meshkatalsadat, M. H.; Mahmoudi, A.; Lotfi, S.; Pouramiri, B.; Foroumadi, A. Green and Four-Component Cyclocondensation Synthesis and in Silico Docking of New Polyfunctionalized Pyrrole Derivatives as the Potential Anticholinesterase Agents. Mol. Div. 2022, 26 (6), 3021 – 3035. https://doi.org/10.1007/s11030-021-10362-9. 38. Meshram, H. M.; Madhu Babu, B.; Santosh Kumar, G.; Thakur, P. B.; Bangade, V. M. Catalyst-Free Four-Component Protocol for the Synthesis of Substituted Pyrroles under Reusable Reaction Media. Tetrahedron Lett. 2013, 54 (19), 2296 – 2302. https://doi.org/10.1016/j.tetlet.2013.01.098. ISSN 2308-8303 (Print) / 2518-1548 (Online) 58 Журнал органічної та фармацевтичної хімії 2025, 23 (2) 39. Reddy, G. R.; Reddy, T. R.; Joseph, S. C.; Reddy, K. S.; Pal, M. Iodine Catalyzed Four-Component Reaction: A Straightforward One-Pot Syn- thesis of Functionalized Pyrroles under Metal-Free Conditions. RSC Adv. 2012, 2 (8), 3387 – 3395. https://doi.org/10.1039/c2ra00982j. 40. Bharate, J. B.; Sharma, R.; Aravinda, S.; Gupta, V. K.; Singh, B.; Bharate, S. B.; Vishwakarma, R. A. Montmorillonite Clay Catalyzed Syn- thesis of Functionalized Pyrroles through Domino Four-Component Coupling of Amines, Aldehydes, 1,3-Dicarbonyl Compounds and Nitroalkanes. RSC Adv. 2013, 3 (44), 21736 – 21742. https://doi.org/10.1039/c3ra43324b. 41. Khan, A. T.; Lal, M.; Ray Bagdi, P.; Sidick Basha, R.; Saravanan, P.; Patra, S. Synthesis of Tetra-Substituted Pyrroles, a Potential Phospho- diesterase 4B Inhibitor, through Nickel(II) Chloride Hexahydrate Catalyzed One-Pot Four-Component Reaction. Tetrahedron Let.t 2012, 53 (32), 4145 – 4150. https://doi.org/10.1016/j.tetlet.2012.05.133. 42. Li, B. Le; Li, P. H.; Fang, X. N.; Li, C. X.; Sun, J. L.; Mo, L. P.; Zhang, Z. H. One-Pot Four-Component Synthesis of Highly Substituted Pyrroles in Gluconic Acid Aqueous Solution. Tetrahedron 2013, 69 (34), 7011 – 7018. https://doi.org/10.1016/j.tet.2013.06.049. 43. Gómez-Sánchez, A.; Stiefel, B. M.; Fernbndez-Ferngndez, R.; Bellanato, J. Unusual Michael Reaction of Acyclic 1,S-Dicarbonyl Compounds with Nitro-Olefins. A Novel Pyrrole Synthesis. J. Chem. Soc., Perkin Trans., 1982, 1, 441 – 447. https://doi.org/10.1039/P19820000441. 44. Yamamoto, S.; Matsunaga, N.; Hitaka, T.; Yamada, M.; Hara, T.; Miyazaki, J.; Santou, T.; Kusaka, M.; Yamaoka, M.; Kanzaki, N.; Furuya, S.; Tasaka, A.; Hamamura, K.; Ito, M. Design, Synthesis, and Biological Evaluation of 4-Phenylpyrrole Derivatives as Novel Androgen Recep- tor Antagonists. Bioorg. Med. Chem. 2012, 20 (1), 422 – 434. https://doi.org/10.1016/j.bmc.2011.10.067. 45. Okamoto, M.; Kojima, H.; Saito, N.; Okabe, T.; Masuda, Y.; Furuya, T.; Nagano, T. Virtual Screening and Further Development of Novel ALK Inhibitors. Bioorg. Med. Chem. 2011, 19 (10), 3086 – 3095. https://doi.org/10.1016/j.bmc.2011.04.008. Information about the authors: Andrii H. Hotynchan (corresponding author), Ph.D. student of the Department of Colour and Structure of Organic Compounds, Institute of Organic Chemistry of the National Academy of Sciences of Ukraine. https://orcid.org/0000-0002-1569-8590; e-mail for correspondence: ahotynchan@gmail.com. Olena M. Kovtun, Associate Professor of the Chemistry Department, Natural Faculty, Dragomanov Ukrainian State University. Yuriy P. Kovtun, Dr. Sci. in Chemistry, Professor, Leading Researcher of the Department of Colour and Structure of Organic Compounds, Institute of Organic Chemistry of the National Academy of Sciences of Ukraine. https://orcid.org/0000-0002-2673-5342.
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spelling oai:ojs.journals.uran.ua:article-3237752026-08-22T19:54:27Z The Synthesis of Pyrroles from Nitroolefins Синтез піролів з нітроолефінів Hotynchan, Andrii H. Kovtun, Olena M. Kovtun, Yuriy P. pyrrole Grob–Camenisch reaction nitroolefines пірол реакція Гроба-Каменіша нітроолефіни The synthesis of pyrroles occupies a key place in synthetic organic chemistry due to the numerous biological properties of pyrrole derivatives, in particular antimicrobial, antibacterial, antifungal, antimalarial, anticancer activities, etc. Therefore, pyrroles serve as building blocks in the creation of potential pharmaceuticals and also serve as the basis for the synthesis of boradipyrromethene dyes. One of the most well-known approaches to the synthesis of pyrroles is the reaction between nitroolefins, 1,3-dicarbonyl compounds, and amines, also known as the Grob-Camenisch reaction. This review is devoted to the historical chronology from the discovery of this transformation dating back to 1950s to the present, and covers the development of various modifications of the above reaction in the synthesis of pyrroles. Синтез піролів займає ключове місце в синтетичній органічній хімії завдяки численним біологічним властивостям похідних піролу, зокрема антимікробній, антибактеріальній, протигрибковій, антималярійній, протираковій тощо. Саме тому піроли слугують будівельними блоками у створенні потенційних фармацевтичних препаратів, а також є основою для синтезу барвників бордипірометенового ряду. Одним із найвідоміших підходів до синтезу піролів є реакція між нітроолефінами, 1,3-дикарбонільними сполуками та амінами, відома як реакція Гроба-Каменіша. Цей огляд висвітлює історичну хронологію від відкриття цього перетворення, датованого 1950-ми роками, до сьогодення та охоплює розробку різноманітних модифікацій вищезгаданої реакції в синтезі піролів. National University of Pharmacy 2025-06-11 Article Article application/pdf https://ophcj.nuph.edu.ua/article/view/323775 10.24959/ophcj.25.323775 Journal of Organic and Pharmaceutical Chemistry; Vol. 23 No. 2 (2025); 48-58 Журнал органической и фармацевтической химии; Том 23 № 2 (2025); 48-58 Журнал органічної та фармацевтичної хімії; Том 23 № 2 (2025); 48-58 2518-1548 2308-8303 en https://ophcj.nuph.edu.ua/article/view/323775/322354 Copyright (c) 2025 Andrii H. Hotynchan, Olena M. Kovtun, Yuriy P. Kovtun http://creativecommons.org/licenses/by/4.0
spellingShingle пірол
реакція Гроба-Каменіша
нітроолефіни
Hotynchan, Andrii H.
Kovtun, Olena M.
Kovtun, Yuriy P.
Синтез піролів з нітроолефінів
title Синтез піролів з нітроолефінів
title_alt The Synthesis of Pyrroles from Nitroolefins
title_full Синтез піролів з нітроолефінів
title_fullStr Синтез піролів з нітроолефінів
title_full_unstemmed Синтез піролів з нітроолефінів
title_short Синтез піролів з нітроолефінів
title_sort синтез піролів з нітроолефінів
topic пірол
реакція Гроба-Каменіша
нітроолефіни
topic_facet pyrrole
Grob–Camenisch reaction
nitroolefines
пірол
реакція Гроба-Каменіша
нітроолефіни
url https://ophcj.nuph.edu.ua/article/view/323775
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