PL440866A1 - 6-Methyl-8-nitro-4-O-β-D-(4"-O-methylglucopyranosyl)-flavanone and method for producing 6-methyl-8-nitro-4-O-β-D-(4"-O -methylglucopyranosyl)-flavanone - Google Patents

6-Methyl-8-nitro-4-O-β-D-(4"-O-methylglucopyranosyl)-flavanone and method for producing 6-methyl-8-nitro-4-O-β-D-(4"-O -methylglucopyranosyl)-flavanone Download PDF

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PL440866A1
PL440866A1 PL440866A PL44086622A PL440866A1 PL 440866 A1 PL440866 A1 PL 440866A1 PL 440866 A PL440866 A PL 440866A PL 44086622 A PL44086622 A PL 44086622A PL 440866 A1 PL440866 A1 PL 440866A1
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methyl
nitro
methylglucopyranosyl
flavanone
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Martyna Krzywda
Edyta Kostrzewa-Susłow
Monika Dymarska
Tomasz Janeczko
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Wrocław University Of Environmental And Life Sciences
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Abstract

Przedmiotem zgłoszenia jest 6-Metylo-8-nitro-4-O-β-D-(4"-O-metyloglukopiranozylo)-flawanon o wzorze 2. Przedmiotem zgłoszenia jest również sposób wytwarzania 6-metylo-8-nitro-4-O-β-D-(4"-O-metyloglukopiranozylo)-flawanonu, charakteryzujący się tym, że do podłoża odpowiedniego dla grzybów strzępkowych wprowadza się szczep Isaria fumosorosea KCH J2, następnie po upływie co najmniej 72 godzin do hodowli wprowadza się substrat, którym jest 6-metylo-8-nitroflawanon o wzorze 1, rozpuszczony w rozpuszczalniku organicznym mieszającym się z wodą, transformację prowadzi się w temperaturze od 20 do 30 stopni Celsjusza, przy ciągłym wstrząsaniu, co najmniej 96 godzin, po czym produkt ekstrahuje się rozpuszczalnikiem organicznym niemieszającym się z wodą i oczyszcza chromatograficznie, przy czym 6-metylo-8-nitro-4-O-β-D-(4"-O-metyloglukopiranozylo)-flawanon o wzorze 2 znajduje się we frakcji o pośredniej polarności w czwartym paśmie od linii startu.The subject of the application is 6-Methyl-8-nitro-4-O-β-D-(4"-O-methylglucopyranosyl)-flavanone of formula 2. The subject of the application is also a method for preparing 6-methyl-8-nitro-4-O -β-D-(4"-O-methylglucopyranosyl)-flavanone, characterized by the introduction of the Isaria fumosorosea KCH J2 strain into a medium suitable for filamentous fungi, then after at least 72 hours, the substrate is introduced into the culture, which is 6-methyl-8-nitroflavanone of formula 1, dissolved in an organic solvent miscible with water, the transformation is carried out at a temperature of 20 to 30 degrees Celsius, with constant shaking, for at least 96 hours, after which the product is extracted with an organic solvent immiscible with water and purified chromatographically, wherein 6-methyl-8-nitro-4-O-β-D-(4"-O-methylglucopyranosyl)-flavanone of formula 2 is found in the fraction of intermediate polarity in the fourth band from the starting line .

Description

6-Metylo-8-nitro-4-O-,8-0-( 4" -O-metyloglukopi ranozylo )-flawanon i sposób wytwarzania 6-m etylo-8-n itro-4-O-,8-0-( 4" -O-metylog lu kopi ranozylo )-flawanon u Przedmiotem wynalazku jest 6-metylo-8-nitro-4-O-,8-0-( 4" -O- metyloglukopiranozylo )-flawanon o wzorze 2 przedstawionym na rysunku. Przedmiotem wynalazku jest równiez sposób wytwarzania 6-metylo- 8-nitro-4-O-,8-0-( 4" -O-metyloglukopiranozylo )-flawanonu. 6-Metylo-8-nitro-4-O-,8-0-( 4" -O-metyloglukopiranozylo )-flawanon moze znalezc zastosowanie jako zwiazek kontrolujacy wzrost bakterii opornych na antybiotyki, przeciwnowotworowy oraz przeciwwirusowy w preparatach farmaceutycznych. Znany jest szczep lsaria fumosorosea KCH J2 ujawniony w zgloszeniu patentowym o numerze P.416996. W ostatnich latach, w leczeniu róznych chorób i ich zapobieganiu, coraz wieksze znaczenie zyskuja zwiazki pochodzenia naturalnego oraz ich odpowiedniki uznawane za naturalne, które uzyskano na drodze przeksztalcen mikrobiologicznych. Dlatego istotne jest opracowywanie nowych metod wytwarzania zwiazków aktywnych biologicznie na drodze biotransformacji, uzytecznych dla przemyslu farmaceutycznego, kosmetycznego. W dostepnej literaturze brak jest informacji na temat otrzymywania 6-metylo-8-nitro-4-O-,8-0-(4"-O-metyloglukopiranozylo)-flawanonu. Istota wynalazku jest 6-metylo-8-nitro-4-O-,8-0-( 4" -0- metyloglukopiranozylo )-flawanon. PL 440866 A1 2/11Istota sposobu polega na tym, ze do podloza odpowiedniego dla grzybów strzepkowych wprowadza sie szczep lsaria fumosorosea KCH J2. Po uplywie co najmniej 72 godzin do hodowli wprowadza sie substrat, którym jest 6-metylo-8-nitroflawanon, rozpuszczony w rozpuszczalniku organicznym mieszajacym sie z woda. Transformacje prowadzi sie w temperaturze od 20 do 30 stopni Celsjusza, przy ciaglym wytrzasaniu, przez co najmniej 96 godzin. Nastepnie produkt ekstrahuje sie rozpuszczalnikiem organicznym nie mieszajacym sie z woda oraz oczyszcza chromatograficznie. 6-metylo-8-nitro-4-O-,6-D-( 4" -O- metyloglukopiranozylo )-flawanon znajduje sie we frakcji o posredniej polarnosci w czwartym pasmie od linii startu. Korzystnie jest, gdy stosunek masy dodawanego substratu do objetosci hodowli wynosi O, 1 mg: 1 cm 3. Korzystnie takze jest, gdy proces prowadzi sie w temperaturze 25 stopni Celsjusza. Dodatkowo, korzystnie takze jest, gdy transformacje prowadzi sie przez 9 dni. Korzystnie równiez jest, gdy oczyszczanie prowadzi sie wykorzystujac cienkowarstwowa chromatografie preparatywna w ukladzie eluujacym z chloroformem i metanolem w stosunku objetosciowym 9:1. Postepujac zgodnie z wynalazkiem, w wyniku dzialania ukladu enzymatycznego zawartego w komórkach szczepu lsaria fumosorosea KCH J2, nastepuje redukcja grupy karbonylowej i przylaczenie 4-metoksy­ ,B-D-glukozy przy C-4. Uzyskany w ten sposób produkt wydziela sie z wodnej kultury mikroorganizmu, znanym sposobem, przez ekstrakcje rozpuszczalnikiem organicznym niemieszajacym sie z woda. Zasadnicza zaleta wynalazku jest otrzymanie 6-metylo-8-nitro-4-O­ ,6-D-( 4"-O-metyloglukopiranozylo )-flawanonu w temperaturze pokojowej i przy pH naturalnym dla szczepu oraz wykorzystujac mikroorganizm niebedacy patogenem ludzkim. PL 440866 A1 3/11Wykorzystanie biotransformacji, zamiast syntezy chemicznej, umozliwia, w sposób przyjazny dla srodowiska, uzyskanie zwiazków o wiekszej biodostepnosci i aktywnosci biologicznej, niz uzyte substraty. Wynalazek jest blizej objasniony na przykladzie wykonania. Przyklad. Do kolby stozkowej o pojemnosci 2000cm 3 , w której znajduje sie 500cm 3 sterylnej pozywki zawierajacej 1 0g am inobaku i 30g sacharozy wprowadza sie szczep lsaria fumosorosea KCH J2. Po 72 godzinach jego wzrostu dodaje sie 50 mg 6-metylo-8-nitroflawanonu o wzorze 1, rozpuszczonego w 1 cm 3 dimetylosulfotlenku. Transformacje prowadzi sie w 25 stopniach Celsjusza przy ciaglym wstrzasaniu przez 9 dni. Nastepnie mieszanine poreakcyjna ekstrahuje sie dwukrotnie octanem etylu, osusza bezwodnym siarczanem magnezu i odparowuje rozpuszczalnik. Otrzymany ekstrakt oczyszcza sie chromatograficznie z zastosowaniem jako eluentu mieszaniny chloroformu i metanolu w stosunku objetosciowym 9: 1. Produkt znajduje sie we frakcji o posredniej polarnosci, czwartym pasmie od linii startu. Na tej drodze otrzymuje sie 4,3 mg 6-metylo-8-nitro-4-O-/3-D-(4"-O­ metyloglukopiranozylo)-flawanonu (wydajnosc 5,3%) oraz pozostalosc, w sklad, której wchodzi 6-metyleno-O-/3-D-(4"-O-metyloglukopiranozylo)-8- nitroflawan-4-ol. Stopien konwersji substratu wedlug HPLC 87%. Uzyskany produkt charakteryzuje sie nastepujacymi danymi spektralnymi. Opis sygnalów pochodzacych z widma 1 H NMR (601 MHz, Aceton-d6) PL 440866 A1 4/11Sygnaly pochodzace od szkieletu Sygnaly pochodzace od jednostki flawonoidowego cukrowej o [ppm] J [Hz] H o [ppm] J [Hz] H ,55 (dd) 12, 1; 2,0 2 4,50 (d) 7,7 1" 2,15(m) 3eq 3,30 (ddd) 9,0; 8,0; 2" 3,8 2,60 (dt) 14,4; 2,5 3ax 3,50 (dd) 8,9; 3,8 3" ,06 (t) 2,9 4 3,12(dd) 9,6; 9,0 4" 7,69 (d) 1,6 5 3,36 (ddd) 9,8; 5,6; 5" 2, 1 7,59 (d) 2, 1 7 3,72 (dt) 11,7; 6,0 6" 3,91 (ddd) 11,4; 5,6; 2, 1 7,55 (d) 7,2 2', 6' 3,54 (s) 4"-O-CH3 7,42 (t) 7,6 3', 5' 3,86 (m) 6"-OH 7,35 (m) 4' 4,25 (d) 3,9 3"-OH 2,37 (s) 6-CH3 4,43 (d) 3,9 2"-OH Wykonane badania modelowania aktywnosci 6-metylo-8-nitro-4-O­ j3-0-( 4"-O-metyloglukopiranozylo )-flawanonu przy uzyciu platformy PASS online wykazaly, ze zwiazek moze byc inhibitorem glicerofosfotransferazy COP-glicerol z wysokim prawdopodobienstwem 90,6%. Glicerofosfotransferaza COP-glicerol odpowiada za polimeryzacje glównego lancucha kwasu tejchojowego zwiazanego ze sciana komórkowa bakterii gram-dodatnich. Kwas tejchojowy jest wazny w patogenezie i odgrywa kluczowa role w opornosci bakterii na antybiotyki (Brown, S., Santa Maria Jr, J. P., & Walker, S. (2013). Wall teichoic acids of gram­ positive bacteria. Annual review of microbiology, 67, 313-336). Garcia PL 440866 A1 /11i wspólpracownicy wykazali, ze 3'-metoksy-4'-hydroksy-3-nitrochalkon wykazywal dzialanie przeciwbakteryjne przeciwko wieloopornym szczepom Staphylococcus aureus 1 O i Escherichia coli 06, gdy byl powiazany odpowiednio z antybiotykami cyprofloksacyna i gentamycyna, co wskazuje, ze zwiazek ten moze przyczyniac sie do kontroli opornosci przeciwbakteryjnej (Garcia, T. R., de Freitas, T. S., dos Santos, H. S., Bandeira, P. N., Juliao, M. S.S., Rocha, J_ E., Nogueira, C. E.S., Pereira, R. L.S., Barreto, A. C.H., Freire, P. T.C., Coutinho, H. D.M., Teixeira, A. M.R. (2020). Structural, vibrational and electrochemical analysis and antibiotic activity study of chalcone (2E)-1-(3',-methoxy-4',-hydroxyphenyl)-3-(3- nitrophenyl) prop-2-en-1-one. Journal of Molecular Structure, 1216, 128358.) Maghal i wspólpracownicy potwierdzili, ze grupa nitrowa i siarkowa zwiekszaja wlasciwosci przeciwbakteryjne co za tym idzie, dzialaja negatywnie na wzrost E. coli, S. flexneri, P. aeruginosa and S. typhi. (Mughal, E. U., Ayaz, M., Hussain, Z., Hasan, A., Sadiq, A., Riaz, M., ... & Choudhary, M. I. (2006). Synthesis and antibacterial activity of substituted flavones, 4-thioflavones and 4-iminoflavones. Bioorganic & medicinal chemistry, 14(14), 4704-4711.) W badaniach in silico wykazano, ze z prawdopodobienstwem 77,9% 6-metylo-8-nitro-4-O-,B-D-( 4" -O-metyloglukopi ranozylo )-flawanon jest substratem CYP2H, nalezacego do rodziny cytochromu P450. Enzymy cytochromu P450 sa szeroko zaangazowane w procesy fizjologiczne i toksykologiczne, takie jak metabolizm czasteczek endogennych i egzogennych oraz reakcje obronne organizmu. Dowiedziono, ze CYP2H wystepujacy u ptaków jest ortologiczny do ludzkiego CYP2C62P. Co wiecej enzymy z rodziny CYP2 moga dzialac jako 25-hydroksylaza witaminy 02 i 03 (CYP2R1 ), z kolei CYP2U1 dziala w hydroksylacji kwasu arachidonowego i dlugolancuchowych kwasów tluszczowych, sugerujac ich wazna i znaczaca role w procesach fizjologicznych (Kubota, A., Stegeman, J. J., Goldstone, J. V., Nelson, D. R., Kim, E. Y., Tanabe, S., & lwata, H. PL 440866 A1 6/11(2011 ). Cytochrome P450 CYP2 genes in the common cormorant: Evolutionary relationships with 130 diapsid CYP2 elan sequences and chemical effects on their expression. Comparative Biochemistry and Physiology Part C: Toxicology & Pharmacology, 153(3), 280-289). Badania in silico wykazaly równiez, ze zwiazek moze posiadac wlasciwosci przeciwnowotworowe z prawdopodobienstwem 81,7%. Nowotwór jest uwazany za chorobe zwiazana z przewleklym stanem zapalnym. Jednym z mechanizmów zwalczania stanu zapalnego i proliferacji komórek nowotworowych przez flawonoidy jest stymulacja szlaku Nrf2, który odgrywa kluczowa role w zapewnianiu odpornosci na stres oksydacyjny i stany zapalne poprzez hamowanie NF-kB. (Farni, C., Rossi, M., Borromeo, I., Feriotto, G., Platamone, G., Tabolacci, C., ... & Beninati, S. (2021 ). Flavonoids: A Myth or a Reality for Cancer Therapy?. Molecules, 26(12), 3583). W badaniach nad (2S)-8-formylo-5- hydroksy-7-metoksy-6-metyloflawanonem Ye i wspólpracownicy wykazali wlasciwosci antykancerogenne zwiazku przeciwko ludzkim liniom komórek nowotworowym: SMMC-7721, 8898, K562, Hela i 95-D (Ye, C. L., Liu, Y., & Wei, D. Z. (2007). Antioxidant and anticancer activity of 3'-formyl-4',6'­ dihydroxy-2' -methoxy-5'-methylchalcone and (2S)-8-formyl-5-hydroxy-7- methoxy-6-methylflavanone. Journal pharmacology, 59(4), 553-559). of pharmacy and Badania aktywnosci 6-metylo-8-nitro-4-O-,B-D-( 4"-0- metyloglukopiranozylo)-flawanonu wykazaly, ze z prawdopodobienstwem 70,6% moze byc stosowany jako srodek przeciwwirusowy np. przeciwko grypie. Ai-Lin Liu i wspólpracownicy przeprowadzili test redukcji CPE (efektu cytopatycznego) indukowanego wirusem grypy A/Jinan/15/90 (H3N2) w komórkach nerki psów Madina-Darby'ego (MDCK). Wykazali, ze apigenina, dinatyna, luteolina i 2-((E)-4'-hydroksyfenylideno)-6-hydroksy- 2,3-dihydrobenzofuran-3-on nalezace do zwiazków flawonoidowych wykazaly znaczaca aktywnosc przeciw wirusowi grypy z IC50 od 4, 7 4µM do 24,?0µM (Liu, A. L., Wang, H. D., Lee, S. M., Wang, Y. T., & Du, G. H. PL 440866 A1 7/11(2008). Structure-activity relationship of flavonoids as influenza virus neuraminidase inhibitors and their in vitro anti-viral activities. Bioorganic & medicinal chemistry, 16(15), 7141-7147). Metylacja flawonoidów poprzez ich wolne grupy hydroksylowe lub atom C radykalnie zwieksza ich stabilnosc metaboliczna i usprawnia transport blonowy, prowadzac do latwiejszego wchlaniania i znacznie zwiekszonej biodostepnosci po podaniu doustnym. Na przyklad 7-O­ metyloapigenina ma dzialanie przeciwbakteryjne, przeciwzapalne i jest zmiataczem wolnych rodników. Równiez 4'-metylofarrerol dziala przeciwnowotworowa przeciwko komórkom HL60, KB, Bel7402 oraz cytotoksycznie przeciwko liniom komórkowym HL-60 i SMMC-7721 (Koirala, N., Thuan, N. H., Ghimire, G. P., Van Thang, O., & Sohng, J. K. (2016). Methylation of flavonoids: Chemical structures, bioactivities, progress and perspectives for biotechnological production. Enzyme and microbial technology, 86, 103-116.). PL 440866 A1 8/11Zastrzezenia patentowe 1. 6-Metylo-8-nitro-4-O-,8-0-( 4"-O-metyloglukopiranozylo )-flawanon o wzorze 2. 2. Sposób wytwarzania 6-metylo-8-nitro-4-O-,8-0-( 4" -O- metyloglukopiranozylo )-flawanonu znamienny tym, ze do podloza odpowiedniego dla grzybów strzepkowych wprowadza sie szczep lsaria fumosorosea KCH J2, nastepnie po uplywie co najmniej 72 godzin do hodowli wprowadza sie substrat, którym jest 6-metylo-8-nitroflawanon o wzorze 1, rozpuszczony w rozpuszczalniku organicznym mieszajacym sie z woda, transformacje prowadzi sie w temperaturze od do 30 stopni Celsjusza, przy ciaglym wstrzasaniu, co najmniej 96 godzin, po czym produkt ekstrahuje sie rozpuszczalnikiem organicznym niemieszajacym sie z woda i oczyszcza chromatograficznie, przy czym 6-metylo-8-nitro-4-O-,8-D-( 4" -O-metyloglukopi ranozylo )-flawanon o wzorze 2 znajduje sie we frakcji o posredniej polarnosci w czwartym pasmie od linii startu. 3. Sposób wedlug zastrz. 2., znamienny tym, ze stosunek masy dodawanego substratu do objetosci hodowli wynosi O, 1 mg:1 cm 3 . 4. Sposób wedlug zastrz. 2., znamienny tym, ze proces prowadzi sie w temperaturze 25 stopni Celsjusza. . Sposób wedlug zastrz. 2., znamienny tym, ze transformacje prowadzi sie przez 9 dni. 6. Sposób wedlug zastrz. 2., znamienny tym, ze oczyszczanie prowadzi sie wykorzystujac cienkowarstwowa chromatografie preparatywna w ukladzie eluujacym chloroform:metanol w stosunku objetosciowym 9: 1 PL 440866 A1 9/113' 3' N02 N02 6' lsaria fumosorosea KCH J2 H 3 C H 3 C o H 3 C, ~ .. 6 .. QH Q 5" Q Q HO 3" 2"QH 1" wzór1 wzór2 PL 440866 A1 /11al. Niepodleglosci 188/192 00-950 Warszawa. skr. poczt. 203 URZAD PATENTOWY RZECZYPOSPOLITEJ POLSKIEJ tel.: (+48) 22 579 05 55 I fax: (+48) 22 579 00 01 e-mail: kontakt@uprp.gov.pl I www.uprp.gov.pl SPRAWOZDANIE O STANIE TECHNIKI DO ZGLOSZENIA NR P.-1--1-0866 Klasyfikacja zgloszenia: C07H 17 /065 (2006.01), Cl2P 19/60 (2006.01), Cl2R 1/6-1-5 (2006.01) Poszukiwania prowadzone w klasach: C07H, Cl2P, Cl2R Bazy komputcrmYc w któr: eh prowadzono poszuki,, ania: EPODOC, WPI. Patcntscopc, STNcxt: REGISTRY, bazy UPRP Kategoria dokumentu A Dokumenty - z podana idcnty fikacja PL-1-32958 Al (UNIWERSYTET PRZYRODNICZY WE WROCLAWIU) 2021- 08-23 D Dalszy ciag wvkam dokumentów na nastepnej stronie A- dokument okreslaJacy ogólny stan techniki, h.tóry me jest uwa.L.any za posiada1acJ szcLególne z1racLeme, _[ doh.umcnt sta110½1acy V\CzcSnicJszc zgloszcmc lub patent, ak opubhko\\a11y v\ lub pu dacie zgluszenia. Odniesienie do zastrz. 1-6 L - clol'-umc11l, klÓI) lll0"1.c poddawac w ,., atpli\.\,osc /.a~tr/.cganc picrws'f.ct'lst,.vn(-\·\ a), lub pr1.y· toC'/Dll)' w celu us1alc11ia dat) publiL1cji innc;;.o C) lowancgo doku111c11t11 hib 7 innego S7Czc_góh1c_!20 powodu O - cloknment odnos74cy sie do ll_j3wnienia ustnego przez zastosowanie. wystawienie lnb ujawnienie''" inny sposób. P - dokument opubhkowam przed data zgloszema, ale póznieJ niz zastrzegana data piemszenstwa. T - dokument pózme_isz). opubllkowany po dac1e zgloszema lub w dac1e p1er11 szenstwa 1 mebeclac, 11 konlhb.c1e ze zgloszemem ale C) to11 am w celu zrozunuema zasad lub teorii lcz<-1{:: eh u pod~Lav, w: nalaz.ku, X - dol.u111cnt o Si'.C'i'.Cgóln)' 111 /nac1.c11iu; 1.astu.cga11: ,_, )' 11ala/.cl. nic mo1.c b)' c ll\-\-a/.a11)' i'.a 110w: lub nic mo/.c b: c u,-vai:a11: /:t posiadaj:\C)' po/.io111 w: na la/Ci'.)'. jc/.cli ten dolrnmcnt hrrm:v _jest pod uv,·nge smnodziclnic. Y - dokument o szczególnym znaczeniu; z.astrze_gany v,·yn3Jazek nie mo?.e byc nw3zany za posi3dajacy pozfom ·ayn;ilazc:zy. jezeli ten dokument zostanie polaczony z Jedmm lub kilkoma tego typu dokumentami, a takie potaczeme bedz1e oczJw1ste dla znawc,. & - clob.umelll nalezacy do tej samej rodzmy patentoweJ Sprawozdanie wykonal/-a: Agnieszka Ucinska Ekspert Koordynator Data: .12.2022 Uwagi do zgloszenia Sprawozdanie zostalo wykonane w oparciu o zastrz. z dnia 06.04.2022 r. Podpis: /podpisano kwalifikowanym podpisem elektronicznym/ Pismo wydane w formie dokumentu elektronicznego PL 440866 A1 11/11 PL6-Methyl-8-nitro-4-O-,8-O-(4"-O-methylglucopyranosyl)-flavanone and a method for preparing 6-methyl-8-nitro-4-O-,8-O-(4"-O-methylglucopyranosyl)-flavanone The subject of the invention is 6-methyl-8-nitro-4-O-,8-O-(4"-O-methylglucopyranosyl)-flavanone of formula 2 shown in the drawing. The subject of the invention is also a method for preparing 6-methyl-8-nitro-4-O-,8-O-(4"-O-methylglucopyranosyl)-flavanone. 6-Methyl-8-nitro-4-O-,8-O-(4"-O-methylglucopyranosyl)-flavanone can be used as a compound controlling the growth of antibiotic-resistant bacteria, as an anticancer and antiviral agent in pharmaceutical preparations. The strain Isaria fumosorosea KCH J2 is known, disclosed in the patent application no. P.416996. In recent years, in the treatment and prevention of various diseases, compounds of natural origin and their equivalents considered to be natural, obtained through microbiological transformations, have been gaining increasing importance. Therefore, it is important to develop new methods for the production of biologically active compounds through biotransformation, useful for the pharmaceutical and cosmetic industries. There is no information in the available literature on the production of 6-methyl-8-nitro-4-O-,8-O-(4"-O-methylglucopyranosyl)-flavanone. The essence of the invention is 6-methyl-8-nitro-4-O-,8-O-(4"-O-methylglucopyranosyl)-flavanone. PL 440866 A1 2/11The essence of the method is that the strain Isaria fumosorosea KCH J2 is introduced into a medium suitable for filamentous fungi. After at least 72 hours, the substrate, which is 6-methyl-8-nitroflavanone, dissolved in an organic solvent miscible with water, is introduced into the culture. The transformation is carried out at a temperature of 20 to 30 degrees Celsius, with continuous shaking, for at least 96 hours. Then the product is extracted with an organic solvent immiscible with water and purified chromatographically. 6-methyl-8-nitro-4-O-,6-D-( 4"-O- Methylglucopyranosyl)-flavanone is found in the intermediate polarity fraction in the fourth band from the starting line. It is preferred that the mass ratio of added substrate to culture volume is 0.1 mg:1 cm3. It is also preferred that the process is carried out at 25 degrees Celsius. Additionally, it is also preferred that the transformation is carried out for 9 days. It is also preferred that purification is carried out using thin-layer preparative chromatography eluting with chloroform and methanol in a 9:1 volume ratio. In accordance with the invention, as a result of the action of the enzymatic system contained in cells of the Isaria fumosorosea KCH J2 strain, the carbonyl group is reduced and 4-methoxy, B-D-glucose is added at C-4. The product thus obtained is separated from the aqueous culture of the microorganism in a known manner by extraction with an organic solvent immiscible with water. The main advantage of the invention is the production of 6-methyl-8-nitro-4-O,6-D-(4"-O-methylglucopyranosyl)-flavanone at room temperature and at the natural pH of the strain and using a microorganism that is not a human pathogen. PL 440866 A1 3/11 The use of biotransformation, instead of chemical synthesis, allows, in an environmentally friendly way, obtaining compounds with greater bioavailability and biological activity than the substrates used. The invention is explained in more detail on the example of its embodiment. Example. The Isaria fumosorosea KCH J2 strain is introduced into a conical flask with a capacity of 2000 cm3, containing 500 cm3 of sterile medium containing 10 g of amino acid and 30 g of sucrose. After 72 hours of its growth, 50 mg of 6-methyl-8-nitroflavanone of formula 1, dissolved in 1 cm3 of dimethyl sulfoxide, is added. The transformation is carried out at 25 degrees Celsius with constant shaking for 9 days. Then the reaction mixture is extracted twice with ethyl acetate, dried with anhydrous magnesium sulfate and the solvent is evaporated. The obtained extract is purified by chromatography using a mixture of chloroform and methanol in a volume ratio of 9:1 as eluent. The product is found in the fraction of intermediate polarity, the fourth band from the starting line. In this way, 4.3 mg of 6-methyl-8-nitro-4-O-/3-D-(4"-O-methylglucopyranosyl)-flavanone are obtained (yield 5.3%) and a residue consisting of 6-methylene-O-/3-D-(4"-O-methylglucopyranosyl)-8-nitroflavan-4-ol. Substrate conversion rate according to HPLC 87%. The obtained product is characterized by the following spectral data. Description of signals from the 1 H NMR spectrum (601 MHz, Acetone-d6) PL 440866 A1 4/11 Signals from the skeleton Signals from the flavonoid sugar unit o [ppm] J [Hz] H o [ppm] J [Hz] H .55 (dd) 12.1; 2.0 2 4.50 (d) 7.7 1" 2.15 (m) 3eq 3.30 (ddd) 9.0; 8.0; 2" 3.8 2.60 (dt) 14.4; 2.5 3ax 3.50 (dd) 8.9; 3.8 3" .06 (t) 2.9 4 3.12(dd) 9.6; 9.0 4" 7.69 (d) 1.6 5 3.36 (ddd) 9.8; 5.6; 5" 2. 1 7.59 (d) 2. 1 7 3.72 (dt) 11.7; 6.0 6" 3.91 (ddd) 11.4; 5.6; 2, 1 7.55 (d) 7.2 2', 6' 3.54 (s) 4"-O-CH3 7.42 (t) 7.6 3', 5' 3.86 (m) 6"-OH 7.35 (m) 4' 4.25 (d) 3.9 3"-OH 2.37 (s) 6-CH3 4.43 (d) 3.9 2"-OH The modeling studies of the activity of 6-methyl-8-nitro-4-O j3-O-( 4"-O-methylglucopyranosyl )-flavanone using the PASS online platform showed that the compound can be an inhibitor of COP-glycerol glycerophosphotransferase with high probability of 90.6%. Glycerophosphotransferase COP-glycerol is responsible for the polymerization of the main chain of teichoic acid associated with the cell wall of gram-positive bacteria. Teichoic acid is important in pathogenesis and plays a key role in bacterial resistance to antibiotics (Brown, S., Santa Maria Jr, J. P., & Walker, S. (2013). Wall teichoic acids of gram-positive bacteria. Annual review of microbiology, 67, 313-336). Garcia PL 440866 A1/11i and co-workers demonstrated that 3'-methoxy-4'-hydroxy-3-nitrochalcone exhibited antibacterial activity against multiresistant Staphylococcus aureus 1O and Escherichia coli 06 strains when associated with the antibiotics ciprofloxacin and gentamicin, respectively, indicating that this compound may contribute to the control of antimicrobial resistance (Garcia, T. R., de Freitas, T. S., dos Santos, H. S., Bandeira, P. N., Juliao, M. S. S., Rocha, J_ E., Nogueira, C. E. S., Pereira, R. L. S., Barreto, A. C. H., Freire, P. T. C., Coutinho, H. D.M., Teixeira, A. M.R. (2020). Structural, vibrational and electrochemical analysis and antibiotic activity study of chalcone (2E)-1-(3',-methoxy-4',-hydroxyphenyl)-3-(3-nitrophenyl) prop-2-en-1-one. Journal of Molecular Structure, 1216, 128358. Maghal et al. confirmed that the nitro and sulfur groups increase antibacterial properties and, consequently, negatively affect the growth of E. coli, S. flexneri, P. aeruginosa and S. typhi. (Mughal, E. U., Ayaz, M., Hussain, Z., Hasan, A., Sadiq, A., Riaz, M., ... & Choudhary, M. I. (2006). Synthesis and antibacterial activity of substituted flavones, 4-thioflavones and 4-iminoflavones. Bioorganic & medicinal chemistry, 14(14), 4704-4711.) In silico studies have shown that with a probability of 77.9%, 6-methyl-8-nitro-4-O-,B-D-(4"-O-methylglucopi ranosyl)-flavanone is a substrate of CYP2H, belonging to the cytochrome P450 family. Cytochrome P450 enzymes are widely involved in physiological processes and toxicological, such as metabolism of endogenous and exogenous molecules and reactions It has been proven that CYP2H found in birds is orthologous to human CYP2C62P. Moreover, enzymes from the CYP2 family can act as 25-hydroxylase of vitamins O2 and O3 (CYP2R1), while CYP2U1 acts in the hydroxylation of arachidonic acid and long-chain fatty acids, suggesting their important and significant role in physiological processes (Kubota, A., Stegeman, J. J., Goldstone, J. V., Nelson, D. R., Kim, E. Y., Tanabe, S., & lwata, H. PL 440866 A1 6/11(2011). Cytochrome P450 CYP2 genes in the common cormorant: Evolutionary relationships with 130 diapsid CYP2 elan sequences and chemical effects on their expression. Comparative Biochemistry and Physiology Part C: Toxicology & Pharmacology, 153(3), 280-289). In silico studies also showed that the compound may possess anticancer properties with a probability of 81.7%. Cancer is considered a disease associated with chronic inflammation. One of the mechanisms by which flavonoids combat inflammation and cancer cell proliferation is the stimulation of the Nrf2 pathway, which plays a key role in providing resistance to oxidative stress and inflammation by inhibiting NF-kB. (Farni, C., Rossi, M., Borromeo, I., Feriotto, G., Platamone, G., Tabolacci, C., ... & Beninati, S. (2021). Flavonoids: A Myth or a Reality for Cancer Therapy?. Molecules, 26(12), 3583). In studies on (2S)-8-formyl-5-hydroxy-7-methoxy-6-methylflavanone, Ye and co-workers demonstrated anticarcinogenic properties of the compound against human cancer cell lines: SMMC-7721, 8898, K562, Hela and 95-D (Ye, C. L., Liu, Y., & Wei, D. Z. (2007). Antioxidant and anticancer activity of 3'-formyl-4',6' dihydroxy-2'-methoxy-5'-methylchalcone and (2S)-8-formyl-5-hydroxy-7-methoxy-6-methylflavanone. Journal of pharmacy and pharmacology, 59(4), 553-559). Studies on the activity of 6-methyl-8-nitro-4-O-,B-D-( 4"-O-methylglucopyranosyl)-flavanone showed that it can be used as an antiviral agent, e.g. against influenza, with a probability of 70.6%. Ai-Lin Liu and colleagues carried out a test to reduce CPE (cytopathic effect) induced by the influenza virus A/Jinan/15/90 (H3N2) in Madin-Darby canine kidney (MDCK) cells. They showed that apigenin, dinatin, luteolin and 2-((E)-4'-hydroxyphenylidene)-6-hydroxy-2,3-dihydrobenzofuran-3-one belonging to flavonoid compounds showed significant activity against influenza virus with IC50 from 4.74µM to 24.0µM (Liu, A. L., Wang, H. D., Lee, S. M., Wang, Y. T., & Du, G. H. PL 440866 A1 7/11(2008). Structure-activity relationship of flavonoids as influenza virus neuraminidase inhibitors and their in vitro anti-viral activities. Bioorganic & medicinal chemistry, 16(15), 7141-7147). Methylation of flavonoids via their free hydroxyl groups or C atom dramatically increases their metabolic stability and improves membrane transport, leading to easier absorption and significantly increased oral bioavailability. For example, 7-O-methylapigenin has antibacterial, anti-inflammatory, and free radical scavenging effects. 4'-Methylfarrerol also exhibits anticancer activity against HL60, KB, Bel7402 cells and cytotoxic activity against HL-60 and SMMC-7721 cell lines (Koirala, N., Thuan, N. H., Ghimire, G. P., Van Thang, O., & Sohng, J. K. (2016). Methylation of flavonoids: Chemical structures, bioactivities, progress and perspectives for biotechnological production. Enzyme and microbial technology, 86, 103-116.). PL 440866 A1 8/11 Patent claims 1. 6-Methyl-8-nitro-4-O-,8-O-(4"-O-methylglucopyranosyl)-flavanone of formula 2. 2. A method for producing 6-methyl-8-nitro-4-O-,8-O-(4"-O-methylglucopyranosyl)-flavanone, characterized in that the strain Isaria fumosorosea KCH J2 is introduced into a medium suitable for filamentous fungi, then after at least 72 hours a substrate is introduced into the culture, which is 6-methyl-8-nitroflavanone of formula 1, dissolved in an organic solvent miscible with water, the transformation is carried out at a temperature of up to 30 degrees Celsius, with constant shaking, for at least 96 hours, after which the product extracted with a water-immiscible organic solvent and purified by chromatography, wherein 6-methyl-8-nitro-4-O-,8-D-(4"-O-methylglucopyranosyl)-flavanone of formula 2 is found in the fraction of intermediate polarity in the fourth band from the starting line. 3. The method according to claim 2, characterized in that the ratio of the mass of the added substrate to the volume of the culture is 0.1 mg:1 cm3. 4. The method according to claim 2, characterized in that the process is carried out at a temperature of 25 degrees Celsius. The method according to claim 2, characterized in that the transformation is carried out for 9 days. 6. The method according to claim 2, characterized in that the purification is carried out using preparative thin-layer chromatography in the eluting system chloroform:methanol in a volume ratio of 9: 1 PL 440866 A1 9/113' 3' N02 N02 6' lsaria fumosorosea KCH J2 H 3 C H 3 C o H 3 C, ~ .. 6 .. QH Q 5" Q Q HO 3" 2"QH 1" formula1 formula2 PL 440866 A1 /11al. Niepodległosci 188/192 00-950 Warsaw. PO box 203 PATENT OFFICE OF THE REPUBLIC OF POLAND tel.: (+48) 22 579 05 55 I fax: (+48) 22 579 00 01 e-mail: kontakt@uprp.gov.pl I www.uprp.gov.pl STATUS REPORT TECHNIQUES FOR NOTIFICATION NO. P.-1--1-0866 Classification of application: C07H 17 / 065 (2006.01), Cl2P 19/60 (2006.01), Cl2R 1/6-1-5 (2006.01) Searches conducted in classes: C07H, Cl2P, Cl2R Computer databases in which the search was conducted: EPODOC, WPI. Patentscopc, STNcxt: REGISTRY, UPRP databases Document category A Documents - with given ID PL-1-32958 Al (WROCŁAW UNIVERSITY OF ENVIRONMENTAL LIFE) 2021- 08-23 D Continuation of document lists on the next page A- document defining the general state of the art, which is not considered to have particular rights, - [ doh.umcnt standing in a particular application or patent, as published on or after the filing date. Reference to claims 1-6 L - clol'-umc11l, klÓI) lll0"1.c to be submitted in,., atpl.\,osc /.a~tr/.cganc picrws'f.ct'lst,.vn(-\·\ a), or pr1.y· toC'/Dll)' in order to establish the publication date of other documents or other S7Czc_góh1c_!20 because of O - cloknment relating to oral communication by use. issuance or disclosure" in another way. P - I will publish the document before the filing date, but later than the stipulated notice date. T - the document will be published after the filing date or in the event of a prior notice. I will be informed of the circumstances and the nature of the matter. C) I am writing this document in order to understand the principles or theories of the invention, ... 110w: or nothing can/cannot be possessed:\C)' po/.io111 w: na la/Ci'.)'. jc/.cli this document hrrm:v _is under the protection of the patentee. Y - a document of special importance; reserved v,·yn3Jazek cannot be considered as possessing the right to trademark if this document is combined with one or more documents of this type, and such combinations will be obvious to experts, & - clob.umell belonging to the same patent family. Report prepared by: Agnieszka Ucinska Expert Coordinator Date: .12.2022 Comments to the application Report was made on the basis of the reservation of April 6, 2022. Signature: /signed with a qualified electronic signature/ Letter issued in the form of an electronic document PL 440866 A1 11/11 PL

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