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Trifluoromethyl enable high-performance single-emitter white organic light-emitting devices based on quinazoline acceptor

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Chinese Chemical Letters 2024年第4期35卷 442-446页

作者： Xiangan Song Shaogang Shen Mengyao Lu Ying Wang Yong Zhang School of Materials Science and engineering Harbin Institute of TechnologyHarbin 150001China Key Laboratory of Photochemical Conversion and Optoelectronic Materials and TIPC-CityU Joint Laboratory of Functional Materials and DeviceChinese Academy of SciencesTechnical Institute of Physics and ChemistryBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Single-emitter white organic light-emitting diode(WOLeD) based on small organic molecule exhibits great potential in simplifying fabrication process of WOLeDs. However, the design and synthesis of molecule for highly efficient single-emitter WOLeD still remains a challenge. Herein, two asymmetric donor-acceptor-acceptor'(D-A-A') type molecule(PTZ-PQ-F and PTZ-PQ-CF3) are developed by employing trifluoromethyl(CF_(3)) or fluorine atom as secondary acceptor, which can exhibit white lighting with dual emission bands consisting of blue traditional fluorescence from quasi-axial(ax) conformer and orange thermally activated delayed fluorescence(TADF) from quasi-equatorial(eq) conformer. The introduction of CF_(3) into PTZ-PQ-CF3 greatly enhanced the photoluminescence quantum yield(PLQY) by suppressing the nonradiative deactivation. Owing to electron-inductive-effect of CF3, the “eq” conformer of PTZ-PQCF3 exhibits a much smaller ΔeSTof 0.01 e v to realize more efficient reverse intersystem crossing(RISC)process, and then enhance the exciton utilization(nearly 100%) of the whole dual emission system. Consequently, single-emitter WOLeDs based on PTZ-PQ-CF3 show nearly standard white emission with eQe of 13.0% and CIe of(0.35, 0.36) in m CP host and show warm white emission with high eQe of 25.5%and CIe of(0.40, 0.47) in 35 Dcz PPy host, which are the best performance among reported single-emitter WOLeDs.

关键词： Single-emitter white organic light-emitting diode Conformational isomerism Thermally activated delayed fluorescence Trifluoromethyl exciton utilization

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Nanomedicine-boosting icaritin-based immunotherapy of advanced hepatocellular carcinoma

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Military Medical Research 2023年第3期10卷 403-414页

作者： Yi Lu Yue Gao Huan Yang Yong Hu Xin Li Department of Polymeric Materials School of Materials Science and EngineeringTongji UniversityShanghai 201804China institute of Biotechnology RWTH Aachen University52074 AachenGermany dwi-Leibniz-institute for Interactive Materials e.v. 52056 AachenGermany College of chemistry Chemical Engineering and BiotechnologyDonghua UniversityShanghai 201620China School of Pharmacy Jiangsu UniversityZhenjiang 212013JiangsuChina institute of technical and macromolecular chemistry RWTH Aachen University52074 AachenGermany

Traditional treatments for advanced hepatocellular carcinoma(HCC),such as surgical resection,transplantation,radiofrequency ablation,and chemotherapy are unsatisfactory,and therefore the exploration of powerful therapeutic strategies is urgently needed.Immunotherapy has emerged as a promising strategy for advanced HCC treatment due to its minimal side effects and long-lasting therapeutic memory effects.Recent studies have demonstrated that icaritin could serve as an immunomodulator for effective immunotherapy of advanced HCC.encouragingly,in 2022,icaritin soft capsules were approved by the National Medical Products Administration(NMPA)of China for the immunotherapy of advanced HCC.However,the therapeutic efficacy of icaritin in clinical practice is impaired by its poor bioavailability and unfavorable in vivo delivery efficiency.Recently,functionalized drug delivery systems including stimuli-responsive nanocarriers,cell membrane-coated nanocarriers,and living cell-nanocarrier systems have been designed to overcome the shortcomings of drugs,including the low bioavailability and limited delivery efficiency as well as side effects.Taken together,the development of icaritin-based nanomedicines is expected to further improve the immunotherapy of advanced HCC.Herein,we compared the different preparation methods for icaritin,interpreted the HCC immune microenvironment and the mechanisms underlying icaritin for treatment of advanced HCC,and discussed both the design of icaritin-based nanomedicines with high icaritin loading and the latest progress in icaritinbased nanomedicines for advanced HCC immunotherapy.Finally,the prospects to promote further clinical translation of icaritin-based nanomedicines for the immunotherapy of advanced HCC were proposed.

关键词： Icaritin Nanomedicine Advanced hepatocellular carcinoma Immunotherapy Clinical translation

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Dysfunction of the adhesion G protein-coupled receptor latrophilin 1(ADGRL1/LPHN1)increases the risk of obesity

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Signal Transduction and Targeted Therapy 2024年第5期9卷 2298-2311页

作者： Heba ZabriTorsten Schöneberg AndréNguyen Dietzsch Hadi Al-Hasani Joachim Altschmied Katharina Bottermann Jana Brendler Judith Haendeler Susanne Horn Isabell Kaczmarek Antje Körner Kerstin Krause Kathrin Landgraf Diana Le Duc Laura Lehmann Stefan Lehr Stephanie Pick Albert Ricken Rene Schnorr Angela Schulz Martina Strnadová Akhil velluva Heba Zabri Torsten Schöneberg Doreen Thor Simone Prömel Rudolf Schönheimer institute of Biochemistry Medical FacultyLeipzig UniversityLeipzigGermany institute for Clinical Biochemistry and Pathobiochemistry Medical FacultyGerman Diabetes CenterLeibniz Center for Diabetes Research at Heinrich Heine University DüsseldorfDüsseldorfGermany German Center for Diabetes Research(DZD e.v.) Munich-NeuherbergGermany Cardiovascular Degeneration Clinical Chemistry and Laboratory DiagnosticsMedical FacultyUniversity Hospital and Heinrich Heine University DüsseldorfDüsseldorfGermany Cardiovascular Research institute(CARID) Medical FacultyUniversity Hospital and Heinrich Heine University DüsseldorfDüsseldorfGermany institute of Pharmacology Medical FacultyUniversity Hospital and Heinrich Heine University DüsseldorfDüsseldorfGermany institute of Anatomy Medical FacultyLeipzig UniversityLeipzigGermany Center for Pediatric Research Hospital for Children and AdolescentsMedical FacultyLeipzig UniversityLeipzigGermany Helmholtz institute for Metabolic Obesity and Vascular Research(HI-MAG)of the Helmholtz Zentrum München at the University of Leipzig and University Hospital LeipzigLeipzigGermany Department of endocrinology NephrologyRheumatologyLeipzig University Medical CenterLeipzigGermany institute of Human Genetics Leipzig University Medical CenterLeipzigGermany institute of Cell Biology Department of BiologyHeinrich Heine University DüsseldorfDüsseldorfGermany School of Medicine University of Global Health EquityKigaliRwanda

Obesity is one of the diseases with severe health consequences and rapidly increasing worldwide prevalence.Understanding the complex network of food intake and energy balance regulation is an essential prerequisite for pharmacological intervention with obesity.G protein-coupled receptors(GPCRs)are among the main modulators of metabolism and energy balance.They,for instance,regulate appetite and satiety in certain hypothalamic neurons,as well as glucose and lipid metabolism and hormone secretion from adipocytes.Mutations in some GPCRs,such as the melanocortin receptor type 4(MC4R),have been associated with early-onset obesity.Here,we identified the adhesion GPCR latrophilin 1(ADGRL1/LPHN1)as a member of the regulating network governing food intake and the maintenance of energy balance.Deficiency of the highly conserved receptor in mice results in increased food consumption and severe obesity,accompanied by dysregulation of glucose homeostasis.Consistently,we identified a partially inactivating mutation in human ADGRL1/LPHN1 in a patient suffering from obesity.Therefore,we propose that LPHN1 dysfunction is a risk factor for obesity development.

关键词： obesity metabolism intake

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Multidisciplinary strategies to enhance therapeutic effects of flavonoids from epimedii Folium:Integration of herbal medicine,enzyme engineering,and nanotechnology

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Journal of Pharmaceutical Analysis 2023年第3期13卷 239-254页

作者： Yi Lu Qiulan Luo Xiaobin Jia James P.Tam Huan Yang Yuping Shen Xin Li School of Pharmacy Jiangsu UniversityZhenjiangJiangsu212013China College of Fashion&Design Jiaxing Nanhu UniversityJiaxingZhejiang314001China School of Traditional Chinese Pharmacy China Pharmaceutical UniversityNanjing211198China School of Biological Sciences Nanyang Technological University637551SingaporeSingapore dwi-Leibniz-institute for Interactive Materials e.v. 52056AachenGermany institute for technical and macromolecular chemistry RWTH Aachen University52074AachenGermany

Flavonoids such as baohuoside I and icaritin are the major active compounds in epimedii Folium(eF)and possess excellent therapeutic effects on various diseases.encouragingly,in 2022,icaritin soft capsules were approved to reach the market for the treatment of hepatocellular carcinoma(HCC)by National Medical Products Administration(NMPA)of China.Moreover,recent studies demonstrate that icaritin can serve as immune-modulating agent to exert anti-tumor effects.Nonetheless,both production efficiency and clinical applications of epimedium flavonoids have been restrained because of their low content,poor bioavailability,and unfavorable in vivo delivery efficiency.Recently,various strategies,including enzyme engineering and nanotechnology,have been developed to increase productivity and activity,improve delivery efficiency,and enhance therapeutic effects of epimedium flavonoids.In this review,the structure-activity relationship of epimedium flavonoids is described.Then,enzymatic engineering strategies for increasing the productivity of highly active baohuoside I and icaritin are discussed.The nanomedicines for overcoming in vivo delivery barriers and improving therapeutic effects of various diseases are summarized.Finally,the challenges and an outlook on clinical translation of epimedium flavonoids are proposed.

关键词： Flavonoids enzymatic hydrolysis Nanomedicine Therapeutic effects Clinical translation epimedii Folium

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Modulating p-type doping of two-dimensional material palladium diselenide

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Nano Research 2024年第4期17卷 3232-3244页

作者： Jiali Yang Yu Liu en-Yang Wang Jinbo Pang Shirong Huang Thomas Gemming Jinshun Bi Alicja Bachmatiuk Hao Jia Shu-Xian Hu Chongyun Jiang Hong Liu Gianaurelio Cuniberti Weijia Zhou Mark H Rümmeli institute for Advanced Interdisciplinary Research(iAIR) University of JinanJinan 250022China institute for Materials chemistry Leibniz Institute for Solid State and Materials Research Dresden(IFW Dresden)20 Helmholtz StrasseDresden 01069Germany State Key Lab of Transducer Technology Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai 200050China College of energy Soochow Institute for Energy and Materials Innovations Soochow UniversitySuzhou 215006China Key Laboratory of Advanced Carbon Materials and Wearable energy Technologies of Jiangsu Province Soochow UniversitySuzhou 215006China School of Integrated Circuits University of Chinese Academy of SciencesBeijing 101408China institute of Microelectronics of Tianjin Binhai New Area Tianjin 300451China institute of Microelectronics Chinese Academy of SciencesBeijing 100029China Lukasiewicz Research Network PORT Polish Center for Technology DevelopmentStablowicka 147Wroclaw 54-066Poland School of Mathematics and Physics University of Science and Technology BeijingBeijing 100083China College of electronic information and optical engineering Nankai UniversityTianjin 300350China Centre of Polymer and Carbon Materials Polish Academy of SciencesM.Curie Sklodowskiej 34Zabrze 41-819Poland Center for energy and environmental Technologies VŠB-Technical University of Ostrava17.Listopadu 15Ostrava 70833Czech Republic State Key Laboratory of Crystal Materials Center of Bio&Micro/Nano Functional MaterialsShandong UniversityJinan 250100China Dresden Center for Computational Materials Science Technische Universität DresdenDresden 01062Germany Dresden Center for Intelligent Materials(GCL DCIM) Technische Universität DresdenDresden 01062Germany institute for Materials Science and Max Bergmann Center of Biomaterials Technische Universität DresdenDresden 01069Germany Center for Advancing electronics Dresden Technische Universität DresdenDresden 01069Germany

The van der Waals heterostructures have evolved as novel materials for complementing the Si-based semiconductor technologies.Group-10 noble metal dichalcogenides(e.g.,PtS_(2),PtSe_(2),PdS_(2),and PdSe_(2))have been listed into two-dimensional(2D)materials toolkit to assemble van der Waals heterostructures.Among them,PdSe_(2) demonstrates advantages of high stability in air,high mobility,and wide tunable bandgap.However,the regulation of p-type doping of PdSe_(2) remains unsolved problem prior to fabricating p–n junction as a fundamental platform of semiconductor physics.Besides,a quantitative method for the controllable doping of PdSe_(2) is yet to be reported.In this study,the doping level of PdSe_(2) was correlated with the concentration of Lewis acids,for example,SnCl_(4),used for soaking.Considering the transfer characteristics,the threshold voltage(the gate voltage corresponding to the minimum drain current)increased after SnCl_(4) soaking treatment.PdSe_(2) transistors were soaked in SnCl_(4) solutions with five different concentrations.The threshold voltages from the as-obtained transfer curves were extracted for linear fitting to the threshold voltage versus doping concentration correlation equation.This study provides in-depth insights into the controllable p-type doping of PdSe_(2).It may also push forward the research of the regulation of conductivity behaviors of 2D materials.

关键词： two-dimensional(2D)materials Lewis acid treatment p-type doping field-effect transistors transfer characteristic

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Nano-and Micro-patterned Biomaterials

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复旦学报（自然科学版） 2007年第5期46卷 706-页

作者： M.C.Lensen M.Diez v.A.Schulte P.Mela M.Mller dwi e.v.and institute of technical and macromolecular chemistry RWTH AachenGermany

1 Results Our objective is two fold: we (ⅰ) aim at the development of novel patterning methodologies in order to (ⅱ) achieve control over the positioning and alignment of living cells.The patterning of the biointerfaces is carried out both at the micro-and nanometer scale and involve (bio)chemical as well as topographic patterns.The former are relatively easily obtained by patterning techniques adapted from (conventional) soft lithography,e.***.by means of micro-contact printing (μ-CP).The topographic pat...

关键词： soft lithography hydrogels nanoimprinting Uv-curing cell adhesion

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electrochemical behavior of Ti-6Al-4v alloy in Hank's solution subjected to deep cryogenic treatment

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Rare Metals 2023年第6期42卷 2037-2046页

作者： Kai-Xuan Gu Kai-Kai Wang Jian-Peng Zheng Liu-Biao Chen Jun-Jie Wang CAS Key Laboratory of Cryogenics Technical Institute of Physics and ChemistryBeijing100190China University of Chinese Academy of Sciences Beijing100049China

The effect of deep cryogenic treatment(DCT)on the electrochemical behavior of Ti-6Al-4v alloy in Hank's solution was experimentally investigated in the present work.Deep cryogenic treatments at-196℃soaking for 24(DCT-24) and 48(DCT-48) hours were conducted on the commercial annealed Ti-6Al-4v alloy.The methods of polarization and electrochemical impedance spectroscopy(eIS) were employed to evaluate the electrochemical behavior and corrosion mechanism.Furthermore,atomic force microscopy(AFM) was used to detect the corrosion surface.The results showed that deep cryogenic treatment shifted the corrosion potentials(e_(corr))to the positive direction.The corrosion current densities(i_(corr))of samples treated by DCT-24 and DCT-48decreased from 153.1 nA·cm^(-2) in the untreated(UT)sample to 86.3 nA·cm^(-2) and 43.3 nA·cm^(-2),respectively.Furthermore,the roughness of corrosion surfaces of samples subjected to DCT was smaller than that of the UT sample,which indeed demonstrated the improvement in corrosion resistance of Ti-6Al-4v alloy in Hank's solution.The results of eIS test indicated that deep cryogenic treatment had no influence on the corrosion mechanism of Ti-6Al-4v alloy in Hank's,while enhanced resistance value of outer porous layer R_p,which makes the surface more efficient to prevent the corrosion.The reduction of β-phase particles,improvement in dislocation density and release of residual stress caused by deep cryogenic treatment had great contribution to the improvement in corrosion resistance of Ti-6Al-4v alloy in Hank's solution.

关键词： Ti-6Al-4v alloy Deep cryogenic treatment Polarization electrochemical impedance spectroscopy(eIS)

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Laser-assisted synthesis of Au NPs on MgO/chitosan:Applications in electrochemical hydrogen storage

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镁合金学报(英文) 2023年第6期11卷 2072-2083页

作者： Babak Jaleh Aida Moradi Mahtab eslamipanah Sadegh Khazalpour Haniyeh Tahzibi Saeid Azizian Manoj B.Gawande Department of Physics Bu-Ali Sina UniversityHamedanIran Faculty of chemistry Bu-Ali Sina University65174HamedanIran Department of Physical chemistry Faculty of ChemistryBu-Ali Sina UniversityHamedanIran Department of Industrial and engineering chemistry Institute of Chemical TechnologyMumbai-Marathwada CampusJalna 431203MaharashtraIndia CeeT Nanotechnology CentreVŠB–Technical University of Ostrava17.listopadu 2172/1570800 Ostrava-PorubaCzech Republic

Hydrogen with high energy density is an environmental alternative to fossil fuels which can respond to the demand for energy considering environmental conditions.It can be stored on porous materials employing physical interaction(e.***.adsorption process).The H2storage capacity of materials can be evaluated through electrochemical methods.Therefore,a fast and straightforward approach was employed to fabricate magnesium oxide/chitosan/Au nanoparticles(Mg O/CS/Au)nanocomposites with porous structure for electrochemical hydrogen storage.Herein,laser ablation in water as a fast and green method was utilized to obtain Au nanoparticles(Au NPs).The obtained Au NPs were loaded on Mg O/CS nanocomposite through physical mixing.Structural and morphological investigation of nanocomposites display spherically shaped Au NPs with a diameter of 49–58 nm agglomerated on the Mg O/CS.Drop casting,the fast and cost-effective method was deployed to deposit the benign,and reusable Mg O/CS/Au-x(x is Au NPs weight percentage of 1,3 and 5 wt.%)nanocomposites on stainless steel mesh and their electrochemical hydrogen storage were measured by cyclic voltammetry(Cv),indicating good stability and significant hydrogen storage capacity(28 C/g)after 300 Cv scans for MgO/CS/Au-1 sample.

关键词： Magnesium oxide(MgO) Chitosan(CS) Gold nanoparticles(Au NPs) Hydrogen storage

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The Mechanochemical Release of Naphthalimide Fluorophores fromβ-Carbonate andβ-Carbamate Disulfide-Centered Polymers

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CCS chemistry 2021年第11期3卷 2333-2344页

作者： Zhiyuan Shi Qingchuan Song Robert Göstl Andreas Herrmann dwi—Leibniz institute for Interactive Materials Aachen 52056 institute of technical and macromolecular chemistry RWTH Aachen UniversityAachen 52074 Department I of Internal Medicine University Hospital of CologneCologne 50937 Zernike institute for Advanced Materials University of Groningen9747 AG Groningen

The covalent attachment of cargo molecules(e.g.,drugs and fluorophores)inβ-position to a disulfide moiety through carbamate and carbonate bonds finds many applications in responsive release systems.Recently,we showed that the combination of this release process with polymer mechanochemistry-induced disulfide scission enabled the remote-controlled release of small molecule drugs and fluorophores from their inactive parent macromolecules using ultrasound.The nature of the linker bond largely governed the subsequent release kinetics,an aspect that has not been investigated so far.To compare the differences,we here employ disulfide-centered polymers releasing either hydroxyl-or amino-naphthalimides from their respectiveβ-carbonate or-carbamate linkers by forceinduced intramolecular 5-exo-trig cyclization.We present the synthesis,characterization,and cell imaging evaluation of three naphthalimides featuring colorimetric and green fluorescence turn-on upon release,allowing monitoring of the release process.We believe that the insights gained from these experiments would advance the tailoring of release rates for force-induced pharmacotherapy.

关键词： mechanochemistry polymers drug delivery bioimaging sonopharmacology

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Dendrimer-decorated nanogels:efficient nanocarriers for biodistribution in vivo and chemotherapy of ovarian carcinoma

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Bioactive Materials 2021年第10期6卷 3244-3253页

作者： Xin Li Zhijun Ouyang Helin Li Chaolei Hu Pabitra Saha Lingxi Xing Xiangyang Shi Andrij Pich dwi-Leibniz-institute for Interactive Materials e.v 52056AachenGermany institute for technical and macromolecular chemistry RWTH Aachen University52074AachenGermany College of chemistry Chemical Engineering and BiotechnologyDonghua UniversityShanghai201620China CQM-Centro de Química da Madeira Universidade da MadeiraCampus da Penteada9000-390FunchalPortugal Department of Gynecology and Obstetrics XinHua HospitalSchool of MedicineShanghai Jiao Tong UniversityShanghai200092China Aachen Maastricht institute for Biobased Materials Maastricht UniversityNL-6167 RDGeleenthe Netherlands

Nanomedicine has revolutionized disease theranostics by the accurate diagnosis and efficient therapy.Here,the PAMAM dendrimer decorated PvCL-GMA nanogels(NGs)were developed for favorable biodistribution in vivo and enhanced antitumor efficacy of ovarian carcinoma.By an ingenious design,the NGs with a unique structure that GMA-rich domains were localized on the surface were synthesized via precipitation polymerization.After G2 dendrimer decoration,the overall charge is changed from neutral to positive,and the NGs-G2 display the whole charge nature of positively charged corona and neutral core.Importantly,the unique architecture and charge conversion of NGs-G2 have a profound impact on the biodistribution and drug delivery in vivo.As a consequence of this alteration,the NGs-G2 as nanocarriers emerge the highly sought biodistribution of reduced liver accumulation,enhanced tumor uptake,and promoted drug release,resulting in the significantly augmented antitumor efficacy with low side effects.Remarkably,this finding is contrary to some reported work that the nanocarriers with positive charge have preferential liver uptake.Moreover,the NGs-G2 also displayed thermal/pH dual-responsive behaviors,excellent biocompatibility,improved cellular uptake,and stimuli-responsive drug release.encouragingly,this work demonstrates a novel insight into the strategy for optimizing design,improving biodistribution and enhancing theranostic efficacy of nanocarriers.

关键词： Nanogels Dendrimer Surface charge Thermal/pH dual-responsiveness Drug delivery

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