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Electrostatic interaction-mediated 1:1 complexes for high-contrast mitochondrial-targeted phosphorescence bioimaging

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Science China Chemistry 2024年第10期67卷 3406-3413页

作者： Jianshuo Cheng Hao Sun Lulu Zhou Glib VBaryshnikov Mouwei Liu Shen Shen hans ågren Liangliang Zhu State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China Laboratory of Organic Electronics Department of Science and TechnologyLinköping UniversityNorrköping 60174Sweden Department of Physics and Astronomy Uppsala UniversityUppsala SE-75120Sweden

Organelle-targeted imaging can provide information on cellular functions and intracellular interactions,being significant for disease *** use of room-temperature phosphorescence(RTP)in organelle-targeted imaging can fully utilize its unique characteristics of long wavelength and deep ***,this technology has long been plagued by insufficient probe targeting and limited luminous *** this work,we prepared a series of complexes composed of multicationic persulfurated arenes and biomacromolecules via electrostatic interactions in 1:1 stoichiometry for high-contrast mitochondrial-targeted RTP *** an electrostatic interaction design effectively prevented the self-aggregation of the probes,which is not conducive to mitochondrial ***,it suppressed the non-radiative decay to the maximum extent,enabling the probes to exhibit strong RTP signals both in aqueous solution and at the cellular ***,the biomacromolecules can serve as carriers for an electrostatic interaction transfer of the persulfurated arenes to *** leads to high mitochondrial targeting Pearson's correlation coefficients of the probes and high-contrast RTP imaging effects,as well as the independence of the co-incubated probe *** results provide new insights for the development of targeted imaging technologies.

关键词： room-temperature phosphorescence mitochondrial targeting bioimaging complex electrostatic interaction

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Functional characterization,structural basis,and protein engineering of a rare flavonoid 2′-O-glycosyltransferase from Scutellaria baicalensis

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Acta Pharmaceutica Sinica B 2024年第8期14卷 3746-3759页

作者： Zilong Wang Xueqing Du Guo Ye Haotian Wang Yizhan Liu Chenrui Liu Fudong Li hansÅgren Yang Zhou Junhao Li Chao He De-An Guo Min Ye State Key Laboratory of Natural and Biomimetic Drugs School of Pharmaceutical SciencesPeking UniversityBeijing 100191China Anhui Key Laboratory of Modern Biomanufacturing and School of Life Sciences Anhui UniversityHefei 230601China National Science Center for Physical Sciences at Microscale Division of Molecular&Cell Biophysics and School of Life Sciences University of Science and Technology of ChinaHefei 230026China Department of Physics and Astronomy Uppsala UniversityUppsala SE-75120Sweden School of Pharmacy Jinan UniversityGuangzhou 510632China Shanghai Research Center for Modernization of Traditional Chinese Medicine Shanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China

Glycosylation is an important post-modification reaction in plant secondary metabolism,and contributes to structural diversity of bioactive natural *** plants,glycosylation is usually catalyzed by *** 2′-O-glycosides are rare ***,no UGTs have been reported,thus far,to specifically catalyze 2′-O-glycosylation of *** this work,UGT71AP2 was identified from the medicinal plant Scutellaria baicalensis as the first flavonoid 2′-*** could preferentially transfer a glycosyl moiety to 2′-hydroxy of at least nine flavonoids to yield six new *** of the 2′-O-glycosides showed noticeable inhibitory activities against cyclooxygenase *** crystal structure of UGT71AP2(2.15Å)was solved,and mechanisms of its regio-selectivity was interpreted by pKa calculations,molecular docking,MD simulation,MM/GBSA binding free energy,QM/MM,and hydrogen‒deuterium exchange mass spectrometry *** structure-guided rational design,we obtained the L138T/V179D/M180T mutant with remarkably enhanced regio-selectivity(the ratio of 7-O-glycosylation byproducts decreased from 48%to 4%)and catalytic efficiency of 2′-O-glycosylation(kcat/Km,0.23 L/(s·μmol),12-fold higher than the native).Moreover,UGT71AP2 also possesses moderate UDP-dependent de-glycosylation activity,and is a dual function *** work provides an efficient biocatalyst and sets a good example for protein engineering to optimize enzyme catalytic features through rational design.

关键词： Glycosyltransferase Regio-selectivity Crystal structure De-glycosylation Catalytic mechanisms

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Recent research progress for upconversion assisted dye-sensitized solar cells

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Chinese Chemical Letters 2021年第6期32卷 1834-1846页

作者： Xugeng Guo Wenpeng Wu Yuanyuan Li Jinglai Zhang Li Wang hans ågren Institute of Upconversion Nanoscale Materials College of Chemistry and Chemical EngineeringHenan UniversityKaifeng 475004China Henan Center for Outstanding Overseas Scientists Henan UniversityKaifeng 475004China Department of Physics and Astronomy Uppsala UniversityBox 516SE-75120 UppsalaSweden

Upconversion(UC)technology makes it possible to harvest infrared(IR)light from the sun and has increasingly been employed in recent years to improve the efficiency of solar *** progress in the area concerns both research on fundamental principles and processes of UC and technologies of device *** increase of important solar cell parameters,like short-circuit photocurrent density and open-circuit photovoltage as well as the total photon-to-current efficiency,has been *** here review the research published during the last few years in the area,in particular we consider the two most cherished techniques,namely the incorporation of upconverting nanophosphors directly into the photoanodes of the solar cells and the introduction of plasmonic metal nanoparticles co-existing with the UC *** ways to achieve strong field enhancement,and the use of the non-linear nature of UC,is to apply microlenses,with or without assisting plasmonic *** enhanced UC action has been demonstrated by broad band and effective harvesting by organic IR antennas,with subsequent mediation by an intermediate nanoshell of the energy into the upconverting ***,nanohybrid and layer-by-layer technologies involving upconverting particles as well as the use of upconverting nanoparticles in hole-transport and electrolyte layers,tested in recent works,are also *** most of these technologies employ upconverting rare earth metals for sequential photon absorption,the main alternative technique,namely triplet-triplet annihilation UC using organic materials,is also *** is our belief that all these approaches will be further much researched in the near future,with potentially great impact on solar cell technology.

关键词： Upconversion nanoparticles Dye-sensitized solar cells Infrared light Triplet-triplet annihilation Photovoltaic systems

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Dual-ionic imidazolium salts to promote synthesis of cyclic carbonates at atmospheric pressure

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Green Energy & Environment 2022年第6期7卷 1327-1339页

作者： Tengfei Wang Danning Zheng Beibei An Yi Liu Tiegang Ren hansÅgren Li Wang Jinglai Zhang Mårten S.G.Ahlquist Henan Engineering Research Center of Green Anticorrosion Technology for Magnesium Alloys Henan UniversityKaifengHenan475004China Henan Engineering Research Center of Corrosion and Protection for Magnesium Alloys Henan UniversityKaifengHenan475004China College of Chemistry and Chemical Engineering Henan UniversityKaifengHenan475004China Department of Theoretical Chemistry&Biology School of BiotechnologyKTH Royal Institute of Technology10691 StockholmSweden

Novel dual-ionic imidazolium salts are shown to display excellent catalytic activity for cycloaddition of carbon dioxide and epoxides under room temperature and atmospheric pressure(0.1 MPa)without any solvent and co-catalyst leading to 96.1%product *** can be reused five times to keep the product yield over 90%.These intriguing results are attributed to a new reaction mechanism,which is supported by theoretical calculations along with the measurements of ^(13)C NMR spectrum and Fourier transform infrared spectroscopy(FT-IR).The excellent catalytic activity can be traced to a CO_(2)-philic group along with an electrophilic hydrogen *** work shows that incorporation of CO_(2)-philic group is an feasible pathway to develop the new efficient ionic liquids.

关键词： Dual-ionic imidazolium salts CO_(2)-Philic group New mechanism Room temperature Atmospheric pressure

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Conformation Governed Reactivity of Fused Thia-Sapphyrin Dimers Bearing Multiply Fused Heteroaromatic Rings

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CCS Chemistry 2023年第6期5卷 1332-1342页

作者： Qizhao Li Masatoshi Ishida Chengjie Li Glib Baryshnikov Feng Sha Bin Zhu Xinyan Wu hansÅgren Hiroyuki Furuta Yongshu Xie Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237 Department of Chemistry Graduate School of ScienceTokyo Metropolitan UniversityTokyo 192-0397 Department of Science and Technology Laboratory of Organic ElectronicsLinköping UniversityNorrköping SE-60174 Department of Physics and Astronomy Uppsala UniversityUppsala SE-75120 Department of Applied Chemistry Graduate School of EngineeringKyushu UniversityFukuoka 819-0395 Research Organization of Science and Technology Ritsumeikan UniversityKusatsu 525-8577

Suitable conformations and proper alignment of complex natural macrocycles are essential for achieving their unique ***,such artificial macrocycle prototypes are still limited due to synthetic *** this respect,directly linked porphyrin analog dimers display tunable conformations and intriguing properties,and thus,they may be employed as a class of promising ***,we report that one-pot oxidative dimerization of thiahydrosapphyrin 1 yields dimers,2anti and 2syn,comprising a transoid-oriented plate-like bipyrrolo[1,2-a]*** thiophene-containing tetrapyrrole arching subunits in 2 lie at the opposite(anti)and same(syn)sides of the plate,***,multiply fused cisoid-orientated dimer 3 was also obtained;a polycyclic pyrrolo-bridged bipyrroloindole derivative tethered with fullyπ-conjugated bridges was ***,the anti-dimer 2anti underwent subsequent oxidative fusion to furnish a further-fused[6.***.5.7.5.***.5.6]-octacyclic compound *** contrast,the syn-orientated 2syn could not be further fused due to the long distance between the potential reaction *** study provides a unique approach to the fused dimeric porphyrin analogs for potential near-infrared optical materials by a simple oxidation *** also reveals the importance of conformation-modulated reactivity for constructing complex porphyrin arrays.

关键词： porphyrins porphyrinoids sapphyrins π-conjugated systems porphyrin oligomers nearinfrared dyes macrocycles

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Visualizing Material Processing via Photoexcitation-ControlledOrganic-Phase Aggregation-Induced Emission

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Research 2021年第1期2021卷 1402-1412页

作者： Jian Gu Bingbing Yue Glib V.Baryshnikov Zhongyu Li Man Zhang Shen Shen hansÅgren Liangliang Zhu State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China College of Science University of Shanghai for Science and TechnologyShanghai 200093China Division of Theoretical Chemistry and Biology School of Biotechnology KTH Royal Institute of TechnologySE-10691 StockholmSweden Department of Physics and Astronomy Uppsala UniversityBox 516SE-75120 UppsalaSweden

Aggregation-induced emission(AIE)has been much employed for visualizing material aggregation and ***,water is generally required for the preparation of the AIE aggregates,the operation of which limits numerous material processing *** hexathiobenzene-based small molecules,monopolymers,and block copolymers as different material prototypes,we herein achieve AIE in pure organic phases by applying a nonequilibrium strategy,photoexcitationcontrolled *** strategy enabled a dynamic change of molecular conformation rather than chemical structure upon irradiation,leading to a continuous aggregation-dependent luminescent enhancement(up to~200-fold increase of the luminescent quantum yield)in organic *** by the materialization of the nonequilibrium strategy,photoconvertible self-assemblies with a steady-state characteristic can be achieved upon organic solvent *** visual monitoring with the luminescence change covered the whole solution-to-film transition,as well as the in situ photoprocessing of the solid-state materials.

关键词： excitation aggregation nonequilibrium

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Removing trace oxygen to obtain truly intrinsic transport in organic semiconductors

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Science China Materials 2024年第5期67卷 1668-1669页

作者： hans Kleemann Dresden Integrated Center for Applied Physics and Photonic Materials Technische UniversitätDresdenGermany

Organic semiconductor is an emerging generation semiconductor material,which has a broad application prospect in the field of flexible and large-area *** now,tens of thousands of organic semiconductor molecules with diverse functions have been developed through elaborate molecular *** molecules are often classified into n-type and ptype,depending on whether the prevalent charge carriers are electrons or holes[1].

关键词： transport intrinsic moving

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二噻吩乙烯修饰的基于1,3,5-苯三甲酰胺的光响应超分子组装体

二噻吩乙烯修饰的基于1,3,5-苯三甲酰胺的光响应超分子组装体

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全国第十八届大环化学暨第十届超分子化学学术讨论会

作者：李腾李昕汪洁 hans ?gren 马骧田禾华东理工大学精细化工研究所结构可控先进功能材料及其制备教育部重点实验室

＜正＞设计并合成基于非共价键作用力的有序超分子自组装结构是一项充满挑战的课题。1,3,5-苯三甲酰胺（Benzene-1,3,5-tricarboxamide,BTA）是一种在超分子体系中广泛应用的可修饰性内核,其在三重氢键的稳定作用下可以形成微米级的一... 详细信息

＜正＞设计并合成基于非共价键作用力的有序超分子自组装结构是一项充满挑战的课题。1,3,5-苯三甲酰胺（Benzene-1,3,5-tricarboxamide,BTA）是一种在超分子体系中广泛应用的可修饰性内核,其在三重氢键的稳定作用下可以形成微米级的一维超分子结构。在该内核的基础上,我们设计并合成了二噻吩乙烯修饰的1,3,5-苯三甲酰胺分子（C3-BTE）,该分子组

关键词：光响应光致变色二噻吩乙烯超分子自组装

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Suppression of mature TAU isoforms prevents Alzheimer's disease-like amyloid-beta oligomer-induced spine loss in rodent neurons

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Neural Regeneration Research 2024年第8期19卷 1655-1657页

作者： Sarah Buchholz hans Zempel Institute of Human Genetics Faculty of Medicine and University Hospital CologneUniversity of CologneCologneGermany Center for Molecular Medicine Cologne(CMMC) Faculty of Medicine and University Hospital CologneUniversity of CologneCologneGermany

Introduction:TAU isoforms as disease mediators:The microtubule-associated protein TAU is predominantly present in the axons of neurons under physiological *** Alzheimer’s disease(AD)and related tauopathies,TAU also mislocalizes("TAU missorting")to the soma and the dendrites,where it eventually forms aggregates,the so-called neurofibrillary tangles(for review see Zimmer-Bensch and Zempel,2021;Zempel,2023).

关键词： Alzheimer Zimmer tau

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A highly selective C-rhamnosyltransferase from Viola tricolor and insights into its mechanisms

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Acta Pharmaceutica Sinica B 2023年第8期13卷 3535-3544页

作者： Bo-Yun Han Zi-Long Wang Junhao Li Qing Jin Hao-Tian Wang Kuan Chen Yang Yi hansgren Xue Qiao Min Ye State Key Laboratory of Natural and Biomimetic Drugs School of Pharmaceutical SciencesPeking UniversityBeijing 100191China Department of Physics and Astronomy Uppsala UniversityUppsala SE-75120Sweden College of Life Science Anhui Agricultural UniversityHefei 230036China Peking University-Yunnan Baiyao International Medical Research Center Beijing 100191China

C-Glycosides are important natural products with various *** plant biosynthetic pathways,the C-glycosylation step is usually catalyzed by C-glycosyltransferases(CGTs),and most of them prefer to accept uridine 5’-diphosphate glucose(UDP-Glc)as sugar *** CGTs favoring UDP-rhamnose(UDP-Rha)as sugar donor has been reported,thus ***,we report the first selective C-rhamnosyltransferase VtCGTc from the medicinal plant Viola *** could efficiently catalyze C-rhamnosylation of 2-hydroxynaringenin 3-C-glucoside,and exhibited high selectivity towards *** for the sugar donor selectivity of VtCGTc were investigated by molecular dynamics(MD)simulations and molecular mechanics with generalized Born and surface area solvation(MM/GBSA)binding free energy ***144 played a vital role in recognizing UDP-Rha,and the V144T mutant could efficiently utilize *** work provides a new and efficient approach to prepare flavonoid C-rhamnosides such as violanthin and iso-violanthin.

关键词： Flavonoid C-glycoside C-rhamnosyltransferase Biosynthesis Catalytic mechanisms Sugardonorselectivity

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