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Monoribbed-Functionalized Macrobicyclic Iron(Ⅱ) Complexes Decorated with Terminal Reactive and Vector Groups: Synthetic Strategy, Chemical Transformations and Structural Characterization

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Chinese Journal of Chemistry 2022年第17期40卷 2089-2105页

作者： Ilya P.Limarev genrikh e.zelinskii Svetlana A.Belova Pavel V.Dorovatovskii Anna V.Vologzhanina ekaterina G.Lebed Yan Z.Voloshin Nesmeyanov Institute of Organoelement Compounds of the Russian Academy of Sciences 28 Vavilova stMoscow119991 Russia Kurnakov Institute of General and Inorganic Chemistry of the Russian Academy of Sciences 31 Leninsky prMoscow119991 Russia National Research Center Kurchatov Institute 1 Kurchatova plMoscow123098 Russia

General and straightforward synthetic strategy towards the iron(Ⅱ)clathrochelates with functionalizing substituents in their apical capping and one of the three chelate ribbed fragments was *** hexachloroclathrochelate precursors were prepared by the direct template condensation of dichloroglyoxime with a suitable boronic acid on the Fe^(2+) ion as a matrix and underwent a stepwise nucleophilic substitution with S_(2)-,N_(2)- or O_(2)-bis-nucleophiles,forming the alicyclic or aromatic N_(2)-,S_(2)-or O_(2)-six-membered *** on the reaction conditions and precursor-to-dinucleophile molar ratios,iron(Ⅱ)clathrochelates with one(S,O and N),two(S,O and N)or three(S and O)X_(2)-six-membered ribbed substituent(s)were *** reactivity substantially decreases in a row:Cl_(6)-Cage>Cl_(4)X_(2)-Cage(where X=S,O or,especially,N)>Cl_(2)X_(4)-Cage(where X=S or O).The reactive monoribbed-functionalized clathrochelates underwent further chemical transformations giving the target macrobicyclic complexes with terminal vector *** follows from the single crystal XRD data,their FeN_(6)-coordination polyhedra possess the geometry intermediate between a trigonal prism and a trigonal antiprism(φ=21.3°—25.20°).Fe-N distances vary from 1.887(6)to 1.933(8)Å.Their 3D-molecules,the hydrophobic–hydrophilic balance in which can be tuned using a ribbed functionalization,form in the crystals the intermolecular specific halogen bonds and/or hydrophobic interactions.

关键词： Macrocyclic compounds Clathrochelates Iron complexes Ligand reactivity Targetdelivery

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efficacy of the new therapeutic approach in curing malignant neoplasms on the model of human glioblastoma

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Cancer Biology & Medicine 2021年第3期18卷 910-930页

作者： evgeniya V.Dolgova Oleg M.Andrushkevich Polina e.Kisaretova Anastasia S.Proskurina genrikh S.Ritter Tatyana D.Dubatolova Margarita V.Romanenko Oleg S.Taranov Yaroslav R.efremov evgeniy L.Zavyalov Alexandr V.Romaschenko Sergey V.Mishinov Svetlana S.Kirikovich evgeniy V.Levites ekaterina A.Potter Alexandr A.Ostanin elena R.Chernykh Stanislav Yu.Roshchin Anatoliy V.Bervitskiy Galina I.Moysak Jamil A.Rzaev Sergey S.Bogachev Institute of Cytology and Genetics SB RAS Novosibirsk 630090Russia A.I.evdokimov Moscow State University of Medicine and Dentistry Moscow 127473Russia Institute of Molecular and Cellular Biology Novosibirsk 630090Russia Novosibirsk State University Novosibirsk 630090Russia The State Research Center of Virology and Biotechnology"Vector" KoltsovoNovosibirsk 630559Russia First Department of Neurosurgery Ya.L.Tsivian Novosibirsk Research Institute of Traumatology and OrthopaedicsNovosibirsk 630091Russia Institute of Fundamental and Clinical immunology Novosibirsk 630099Russia Sklifosovsky Research Institute of emergency Medicine Moscow 129010Russia Federal Center of Neurosurgery Novosibirsk 630048Russia

Objective:Glioma is a highly invasive tumor,frequently disposed in essential areas of the brain,which makes its surgical excision extremely difficult;meanwhile adjuvant therapy remains quite ***:In the current report,a new therapeutic approach in curing malignant neoplasms has been performed on the U87 human glioblastoma *** approach,termed"Karanahan",is aimed at the eradication of cancer stem cells(CSCs),which were recently shown to be capable of internalizing fragments of extracellular double-stranded *** being internalized,these fragments interfere in the process of repairing interstrand cross-links caused by exposure to appropriate cytostatics,and such an interference results either in elimination of CSCs or in the loss of their tumorigenic *** of the approach requires a scheduled administration of cytostatic and complex composite double-stranded DNA ***:U87 cells treated in vitro in accordance with the Karanahan approach completely lost their tumorigenicity and produced no grafts upon intracerebral transplantation into immunodeficient *** SCID mice with developed subcutaneous grafts,the treatment resulted in reliable slowing down of tumor growth rate(Pe experiment with intracerebral transplantation of U87 cells followed by surgical excision of the developed graft and subsequent therapeutic treatment,the Karanahan approach was shown to reliably slow down the tumor growth rate and increase the median survival of the mice twofold relative to the ***:The effectiveness of the Karanahan approach has been demonstrated both in vitro and in vivo in treating developed subcutaneous grafts as well as orthotopic grafts after surgical excision of the tumor.

关键词： Glioblastoma U87 cell line mytomycin C cancer stem cells TAMRA

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