To precisely control intrachain π-electron delocalization and interchain interaction simultaneously is the prerequisite to obtain stable and efficient deep-blue light-emitting p-n polymer semiconductors for the polym...To precisely control intrachain π-electron delocalization and interchain interaction simultaneously is the prerequisite to obtain stable and efficient deep-blue light-emitting p-n polymer semiconductors for the polymer light-emitting diodes(PLEDs).Herein,we introduced the steric carbazole-fluorene nanogrid into light-emitting diphenyl sulfone-based p-n polymer semiconductors(PG and PDG) via metal-free C-N coupling polymerization for the fabrication of deep-blue PLEDs.The steric,rigid and twisted configuration between nanogrid and diphenyl sulfone in PG and PDG present the unique characteristic of large steric hindrance interaction to suppress interchain aggregation in solid state.Due to the different length of electron-deficient diphenyl sulfone monomers,PG showed a deep-blue emission with a maximum peak at 428 nm but red-shifted to 480 nm for the PDG films.Interestingly,similar deep-blue emission behavior of PG in diluted non-polar solution and films suggested the extremely weak interchain aggregation.Finally,PLEDs based on PG are fabricated with a stable deep-blue emission of CIE(0.15,0.10),and corresponding EL spectral profile is also completely identical to PL ones of diluted solution,revealed the intrachain emission without obvious interchain excited state,confirmed effectiveness of the steric hindrance functionalization of nanogrid in p-n polymer semiconductor for deep-blue light-emitting organic optoelectronics.展开更多
Background:The bacterial biofilm poses a significant challenge to traditional antibiotic therapy.There is a great need to develop novel antibiofilm agents combined with biofilm disrupting and bacteria-killing without ...Background:The bacterial biofilm poses a significant challenge to traditional antibiotic therapy.There is a great need to develop novel antibiofilm agents combined with biofilm disrupting and bacteria-killing without the dependence of antibiotic.Methods:Herein,we prepared ultrasound/magnetic field-responsive ferroferric oxide nanoparticles(Fe_(3)O_(4))/glucose oxidase microbubbles(FGMB)to form a cascade catalytic system for effective removing methicillin-resistant Staphylococcus aureus biofilms.FGMB were prepared through interfacial self-assembly of Fe_(3)O_(4) nanoparticles(NPs)and glucose oxidase(GOx)at the gas-liquid interface stabilized by surfactants.Under ultrasound/magnetic field stimulation,FGMB disrupted biofilm architecture through microbubble collapse-induced microjets and magnetically driven displacement.Simultaneously,ultrasound-triggered rupture of FGMB released GOx and Fe_(3)O_(4) NPs.Glucose can be oxidized by GOx to generate gluconic acid and hydrogen peroxide which was subsequently catalyzed into hydroxyl radicals by Fe_(3)O_(4) NPs,enabling chemical eradication of biofilm-embedded bacteria.Results:Optical microscopy images demonstrated that FGMB have spherical structure with average size of approximately 17μm.FGMB showed a 65.4%decrease in methicillin-resistant Staphylococcus aureus biofilm biomass and 1.1 log bacterial inactivation efficiency(91.2%),suggesting effective biofilm elimination.In vitro experimental results also indicate that FGMB have good biocompatibility.Conclusion:This antibiofilm strategy integrated dual modes of physical biofilm disruption with chemical bacteria-killing shows great potential as a versatile,non-resistant strategy for bacterial biofilm elimination.展开更多
With the in-depth implementation of sustainable development strategies,hydrogen energy as a clean energy source is receiving increasing attention[1,2].Among the various methods of hydrogen production,the electrocataly...With the in-depth implementation of sustainable development strategies,hydrogen energy as a clean energy source is receiving increasing attention[1,2].Among the various methods of hydrogen production,the electrocatalytic decomposition of abundant seawater into hydrogen utilizing renewable energy has emerged as a green and promising approach.However,natural seawater contains complex components,such as halide ions,which lead to the corrosion of catalysts or the occurrence of competitive side reactions during the electrolysis process[3].展开更多
The field of nanomedicine has been revolutionized by the concept of immunogenic cell death(ICD)-enhanced cancer therapy,which holds immense promise for the efficient treatment of cancer.However,precise delivery of ICD...The field of nanomedicine has been revolutionized by the concept of immunogenic cell death(ICD)-enhanced cancer therapy,which holds immense promise for the efficient treatment of cancer.However,precise delivery of ICD inducer is severely hindered by complex biological barriers.How to design and build intelligent nanoplatform for adaptive and dynamic cancer therapy remains a big challenge.Herein,this article presents the design and preparation of CD44-targeting and ZIF-8 gated gold nanocage(Au@ZH) for programmed delivery of the 1,2-diaminocyclohexane-Pt(Ⅱ)(DACHPt) as ICD inducer.After actively targeting the CD44 on the surface of 4T1 tumor cell,this Pt-Au@ZH can be effectively endocytosed by the 4T1 cell and release the DACHPt in tumor acidic environment,resulting in ICD effect and superior antitumor efficacy both in vitro and in vivo in the presence of mild 808 nm laser irradiation.By integration of internal and external stimuli intelligently,this programmed nanoplatform is poised to become a cornerstone in the pursuit of effective and targeted cancer therapy in the foreseeable future.展开更多
Improving the optoelectronic behavior and stress-deformation stability of conjugated materials is crucial for the realization of their potential applications in flexible optoelectronics.To tune the emission behavior a...Improving the optoelectronic behavior and stress-deformation stability of conjugated materials is crucial for the realization of their potential applications in flexible optoelectronics.To tune the emission behavior and mechanical property of molecular crystals simultaneously via supramolecular salt strategy is rarely reported,which is very important to improve their photophysical behavior and softness for the fabrication of flexible light-emitting device.Herein,supramolecular salt approach has been successfully applied to synthesize two elastic organic fluorescent crystals(CMOH-Py-Cl and CMOH-Py-Br)derived from non-emissive and brittle pyridine-substituted coumarin derivative(CMOH-Py).Their elastic properties can be attributed to the prevalent presence of numerous weak interactions introduced by halogen atoms,which are beneficial to the absorption and release of mechanical energy.Furthermore,density functional theory(DFT)calculations demonstrated a narrowing of the HOMO-LUMO energy gaps from CMOH-Py to CMOH-Py-Cl/CMOH-Py-Br via supramolecular salt approach.Finally,the application of flexible crystal materials in the field of optical waveguides has been investigated.The transformation of crystals in terms of photophysical and mechanical properties,achieved by the supramolecular salt approach,offers novel insights into the design and construction of flexible crystalline materials,providing a new path for the development of next-generation smart materials.展开更多
Shikonin,a naphthoquinone compound derived from the root of Lithospermum erythrorhizon,has been extensively studied for its antibacterial,antioxidant,and anti-inflammatory properties.Increasing evidence highlights its...Shikonin,a naphthoquinone compound derived from the root of Lithospermum erythrorhizon,has been extensively studied for its antibacterial,antioxidant,and anti-inflammatory properties.Increasing evidence highlights its potential in treating inflammation-related diseases.However,its clinical application is hindered by challenges such as poor water solubility,rapid metabolism in vivo,and other limitations.Recent advancements have demonstrated that encapsulating shikonin within nanocarriers can significantly enhance its water solubility and pharmacokinetic profile.Building on this,this perspective paper outlines the current landscape of inflammation treatment,explores the anti-inflammatory mechanisms of shikonin,reviews the latest progress in shikonin-based nanomaterials for anti-inflammatory applications,and discusses the challenges and future directions for the clinical translation of shikonin nanoformulations.展开更多
Surface passivation via two-dimensional(2D)perovskite has emerged as a promising strategy to enhance the performance of perovskite solar cells(PSCs)due to the effective compensation of interfacial states.However,the i...Surface passivation via two-dimensional(2D)perovskite has emerged as a promising strategy to enhance the performance of perovskite solar cells(PSCs)due to the effective compensation of interfacial states.However,the in situ grown 2D perovskite passivation layers typically comprise a mixture of multiple dimensionalities at the interface,where band alignment has only been portrayed qualitatively and empirically.Herein,the interface states for precisely phase-tailored 2D perovskite passivated PSCs are quantitatively investigated.In comparison to traditional passivation molecules,2D perovskite layers based on 4-trifluoromethyl-phenylethylammonium iodide(CF3PEAI)exhibit an increased work function,introducing desirable downward band bending to eliminate the Schottky Barrier.Furthermore,precisely phase-tailored 2D layers could modulate the interface trap density and energetics.The n=1 film delivers optimal performance with a hole extraction efficiency of 95.1%.The optimized n-i-p PSCs in the two-step method significantly improve PCE to 25.40%,along with enhanced photostability and negligible hysteresis.It highlights that tailoring in the composition and phase distribution of the 2D perovskite layer could modulate the interface states at the 2D/3D interface.展开更多
In the field of organic solar cells(OSCs),side-chain engineering is a key strategy for developing high-performance non-fullerene small molecule acceptors(SMAs),which could adjust the material solubility and modulate t...In the field of organic solar cells(OSCs),side-chain engineering is a key strategy for developing high-performance non-fullerene small molecule acceptors(SMAs),which could adjust the material solubility and modulate the intermolecular stacking properties,profoundly impacting the film morphology and thus acting on the final power conversion efficiency(PCE) of the materials.In this study,two asymmetric acceptor molecules,Qx-Ph Br-BO and Qx-Ph Br-X,were synthesized by migrating the branching site of the outer side chain from the β-site to the γ-site.The branching site located at the γ-site could reduce the steric-hindrance effect and enhance the molecular aggregation behavior,giving rise to redshifted absorption and tight π-π stacking.Morphology analysis shows that the Qx-Ph Br-X-based devices have smoother surfaces and a phase-separated structure,which is more favorable for charge transport and extraction.The Qx-Ph Br-X-based devices exhibit balanced hole-electron mobility,efficient exciton dissociation,and low charge recombination.As a result,Qx-Ph Br-X with γ-site branching exhibits superior photovoltaic performance with a PCE of 17.16 %,which is significantly higher than that of Qx-Ph Br-BO at 16.28 %.These results highlight the importance of side-chain modifications for optimizing OSC efficiency and provide an important reference for precise tuning of side-chain structures in future molecular design.展开更多
近些年,通过合理的分子设计将手性基团与室温磷光材料相结合,构建了一系列具有圆偏振发光性质的有机室温磷光材料。圆偏振有机室温磷光(Circularly polarized room temperature phosphorescence,CPRTP)材料的发光原理与有机室温磷光材...近些年,通过合理的分子设计将手性基团与室温磷光材料相结合,构建了一系列具有圆偏振发光性质的有机室温磷光材料。圆偏振有机室温磷光(Circularly polarized room temperature phosphorescence,CPRTP)材料的发光原理与有机室温磷光材料的发光过程保持一致,同时伴随着圆偏振发光性质。这类材料不仅保留了圆偏振发光中能量损耗低的优势,还极大地拓展了有机室温磷光材料在防伪加密、余辉显示等领域的应用。本文从CPRTP材料的发光机理及分子策略出发,依据CPRTP材料构筑方法的不同,概括了其结构设计策略,系统综述了各种类型的CPRTP材料的分子结构和光电性能的关系,最后探讨了CPRTP材料目前存在的问题,并展望了其未来的发展前景及挑战。展开更多
基金the support from the Jiangsu Provincial Senior Talent Program (Dengfeng,Jiangsu University)the support from the National Key R&D Program of China (No.2024YFB3612600)+3 种基金the National Natural Science Foundation of China (Nos.22275098,62288102)Basic Research Program of Jiangsu (No.BK20243057)the Natural Science Research Start-up Foundation of Recruiting Talents of Nanjing University of Posts and Telecommunications (No.NY222097)the National Natural Science Foundation of China (No.62205035)。
文摘To precisely control intrachain π-electron delocalization and interchain interaction simultaneously is the prerequisite to obtain stable and efficient deep-blue light-emitting p-n polymer semiconductors for the polymer light-emitting diodes(PLEDs).Herein,we introduced the steric carbazole-fluorene nanogrid into light-emitting diphenyl sulfone-based p-n polymer semiconductors(PG and PDG) via metal-free C-N coupling polymerization for the fabrication of deep-blue PLEDs.The steric,rigid and twisted configuration between nanogrid and diphenyl sulfone in PG and PDG present the unique characteristic of large steric hindrance interaction to suppress interchain aggregation in solid state.Due to the different length of electron-deficient diphenyl sulfone monomers,PG showed a deep-blue emission with a maximum peak at 428 nm but red-shifted to 480 nm for the PDG films.Interestingly,similar deep-blue emission behavior of PG in diluted non-polar solution and films suggested the extremely weak interchain aggregation.Finally,PLEDs based on PG are fabricated with a stable deep-blue emission of CIE(0.15,0.10),and corresponding EL spectral profile is also completely identical to PL ones of diluted solution,revealed the intrachain emission without obvious interchain excited state,confirmed effectiveness of the steric hindrance functionalization of nanogrid in p-n polymer semiconductor for deep-blue light-emitting organic optoelectronics.
基金supported by the National Natural Science Foundation of China(22375101)the Natural Science of Colleges and Universities in Jiangsu Province(24KJB430027).
文摘Background:The bacterial biofilm poses a significant challenge to traditional antibiotic therapy.There is a great need to develop novel antibiofilm agents combined with biofilm disrupting and bacteria-killing without the dependence of antibiotic.Methods:Herein,we prepared ultrasound/magnetic field-responsive ferroferric oxide nanoparticles(Fe_(3)O_(4))/glucose oxidase microbubbles(FGMB)to form a cascade catalytic system for effective removing methicillin-resistant Staphylococcus aureus biofilms.FGMB were prepared through interfacial self-assembly of Fe_(3)O_(4) nanoparticles(NPs)and glucose oxidase(GOx)at the gas-liquid interface stabilized by surfactants.Under ultrasound/magnetic field stimulation,FGMB disrupted biofilm architecture through microbubble collapse-induced microjets and magnetically driven displacement.Simultaneously,ultrasound-triggered rupture of FGMB released GOx and Fe_(3)O_(4) NPs.Glucose can be oxidized by GOx to generate gluconic acid and hydrogen peroxide which was subsequently catalyzed into hydroxyl radicals by Fe_(3)O_(4) NPs,enabling chemical eradication of biofilm-embedded bacteria.Results:Optical microscopy images demonstrated that FGMB have spherical structure with average size of approximately 17μm.FGMB showed a 65.4%decrease in methicillin-resistant Staphylococcus aureus biofilm biomass and 1.1 log bacterial inactivation efficiency(91.2%),suggesting effective biofilm elimination.In vitro experimental results also indicate that FGMB have good biocompatibility.Conclusion:This antibiofilm strategy integrated dual modes of physical biofilm disruption with chemical bacteria-killing shows great potential as a versatile,non-resistant strategy for bacterial biofilm elimination.
基金financially supported by the Natural Science Research Start-up Foundation of Recruiting Talents of Nanjing University of Posts and Telecommunications(No.NY223016)Qinglan Project of Jiangsu Province of China2024 Nanjing Science and Technology Innovation Program(No.NJKCZYZZ2024-06)。
文摘With the in-depth implementation of sustainable development strategies,hydrogen energy as a clean energy source is receiving increasing attention[1,2].Among the various methods of hydrogen production,the electrocatalytic decomposition of abundant seawater into hydrogen utilizing renewable energy has emerged as a green and promising approach.However,natural seawater contains complex components,such as halide ions,which lead to the corrosion of catalysts or the occurrence of competitive side reactions during the electrolysis process[3].
基金financially supported by the Natural Science Foundation of Jiangsu Province (No.BK20200709)the Natural Science Foundation of China (Nos.62288102,32201127 and 82270113)+2 种基金the Natural Science Foundation of Guangdong Province (No.2023A1515011386)the Natural Science Foundation of the Jiangsu Higher Education Institutes (No.20KJB430031)the startup fund from Nanjing Tech University,and Disciplinary Fund of School of Pharmaceutical Sciences (2024)。
文摘The field of nanomedicine has been revolutionized by the concept of immunogenic cell death(ICD)-enhanced cancer therapy,which holds immense promise for the efficient treatment of cancer.However,precise delivery of ICD inducer is severely hindered by complex biological barriers.How to design and build intelligent nanoplatform for adaptive and dynamic cancer therapy remains a big challenge.Herein,this article presents the design and preparation of CD44-targeting and ZIF-8 gated gold nanocage(Au@ZH) for programmed delivery of the 1,2-diaminocyclohexane-Pt(Ⅱ)(DACHPt) as ICD inducer.After actively targeting the CD44 on the surface of 4T1 tumor cell,this Pt-Au@ZH can be effectively endocytosed by the 4T1 cell and release the DACHPt in tumor acidic environment,resulting in ICD effect and superior antitumor efficacy both in vitro and in vivo in the presence of mild 808 nm laser irradiation.By integration of internal and external stimuli intelligently,this programmed nanoplatform is poised to become a cornerstone in the pursuit of effective and targeted cancer therapy in the foreseeable future.
基金supported by the National Natural Science Foundation of China(Nos.22205105,61874053,22075136)National Key Basic Research Program of China(No.2020YFA0709900)Jiangsu Provincial Postgraduate Scientific Research Innovation Program(No.KYCX24_1649).
文摘Improving the optoelectronic behavior and stress-deformation stability of conjugated materials is crucial for the realization of their potential applications in flexible optoelectronics.To tune the emission behavior and mechanical property of molecular crystals simultaneously via supramolecular salt strategy is rarely reported,which is very important to improve their photophysical behavior and softness for the fabrication of flexible light-emitting device.Herein,supramolecular salt approach has been successfully applied to synthesize two elastic organic fluorescent crystals(CMOH-Py-Cl and CMOH-Py-Br)derived from non-emissive and brittle pyridine-substituted coumarin derivative(CMOH-Py).Their elastic properties can be attributed to the prevalent presence of numerous weak interactions introduced by halogen atoms,which are beneficial to the absorption and release of mechanical energy.Furthermore,density functional theory(DFT)calculations demonstrated a narrowing of the HOMO-LUMO energy gaps from CMOH-Py to CMOH-Py-Cl/CMOH-Py-Br via supramolecular salt approach.Finally,the application of flexible crystal materials in the field of optical waveguides has been investigated.The transformation of crystals in terms of photophysical and mechanical properties,achieved by the supramolecular salt approach,offers novel insights into the design and construction of flexible crystalline materials,providing a new path for the development of next-generation smart materials.
基金supported by the National Natural Science Foundation of China(82373393),Xinjiang Uygur Autonomous Region“Tianchi Yingcai”Project(2023TCYCQNBS02)Xinjiang Uygur Autonomous Region Colleges and Universities Basic Research Operating Expenses Scientific Research Project(XJEDU2022P106).
文摘Shikonin,a naphthoquinone compound derived from the root of Lithospermum erythrorhizon,has been extensively studied for its antibacterial,antioxidant,and anti-inflammatory properties.Increasing evidence highlights its potential in treating inflammation-related diseases.However,its clinical application is hindered by challenges such as poor water solubility,rapid metabolism in vivo,and other limitations.Recent advancements have demonstrated that encapsulating shikonin within nanocarriers can significantly enhance its water solubility and pharmacokinetic profile.Building on this,this perspective paper outlines the current landscape of inflammation treatment,explores the anti-inflammatory mechanisms of shikonin,reviews the latest progress in shikonin-based nanomaterials for anti-inflammatory applications,and discusses the challenges and future directions for the clinical translation of shikonin nanoformulations.
基金supported by the National Natural Science Foundation of China(Nos.62304111,62304110,22579136)the National Key Research and Development Program of China(2024YFE0201800)+6 种基金the China Postdoctoral Science Foundation(No.2024M761492)the Project of State Key Laboratory of Organic Electronics and Information Displays(Nos.GDX2022010009,GZR2023010046)the Natural Science Research Start-up Foundation of Recruiting Talents of Nanjing University of Posts and Telecommunications(No.NY223053)the Science and Technology Project of Jiangsu(Science and Technology Cooperation Project of HongKong,Macao and Taiwan,No.BZ2023059)Shaanxi Fundamental Science Research Project for Mathematics and Physics(No.22jSY015)Young Talent Fund of Xi'an Association for Science and Technology(No.959202313020)Guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic Systems(No.2023B1212010003).
文摘Surface passivation via two-dimensional(2D)perovskite has emerged as a promising strategy to enhance the performance of perovskite solar cells(PSCs)due to the effective compensation of interfacial states.However,the in situ grown 2D perovskite passivation layers typically comprise a mixture of multiple dimensionalities at the interface,where band alignment has only been portrayed qualitatively and empirically.Herein,the interface states for precisely phase-tailored 2D perovskite passivated PSCs are quantitatively investigated.In comparison to traditional passivation molecules,2D perovskite layers based on 4-trifluoromethyl-phenylethylammonium iodide(CF3PEAI)exhibit an increased work function,introducing desirable downward band bending to eliminate the Schottky Barrier.Furthermore,precisely phase-tailored 2D layers could modulate the interface trap density and energetics.The n=1 film delivers optimal performance with a hole extraction efficiency of 95.1%.The optimized n-i-p PSCs in the two-step method significantly improve PCE to 25.40%,along with enhanced photostability and negligible hysteresis.It highlights that tailoring in the composition and phase distribution of the 2D perovskite layer could modulate the interface states at the 2D/3D interface.
基金the financial support by the Beijing Natural Science Foundation (No.Z230018)the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB0520102)CAS Project for Young Scientists in Basic Research (No.YSBR-102)。
文摘In the field of organic solar cells(OSCs),side-chain engineering is a key strategy for developing high-performance non-fullerene small molecule acceptors(SMAs),which could adjust the material solubility and modulate the intermolecular stacking properties,profoundly impacting the film morphology and thus acting on the final power conversion efficiency(PCE) of the materials.In this study,two asymmetric acceptor molecules,Qx-Ph Br-BO and Qx-Ph Br-X,were synthesized by migrating the branching site of the outer side chain from the β-site to the γ-site.The branching site located at the γ-site could reduce the steric-hindrance effect and enhance the molecular aggregation behavior,giving rise to redshifted absorption and tight π-π stacking.Morphology analysis shows that the Qx-Ph Br-X-based devices have smoother surfaces and a phase-separated structure,which is more favorable for charge transport and extraction.The Qx-Ph Br-X-based devices exhibit balanced hole-electron mobility,efficient exciton dissociation,and low charge recombination.As a result,Qx-Ph Br-X with γ-site branching exhibits superior photovoltaic performance with a PCE of 17.16 %,which is significantly higher than that of Qx-Ph Br-BO at 16.28 %.These results highlight the importance of side-chain modifications for optimizing OSC efficiency and provide an important reference for precise tuning of side-chain structures in future molecular design.
文摘近些年,通过合理的分子设计将手性基团与室温磷光材料相结合,构建了一系列具有圆偏振发光性质的有机室温磷光材料。圆偏振有机室温磷光(Circularly polarized room temperature phosphorescence,CPRTP)材料的发光原理与有机室温磷光材料的发光过程保持一致,同时伴随着圆偏振发光性质。这类材料不仅保留了圆偏振发光中能量损耗低的优势,还极大地拓展了有机室温磷光材料在防伪加密、余辉显示等领域的应用。本文从CPRTP材料的发光机理及分子策略出发,依据CPRTP材料构筑方法的不同,概括了其结构设计策略,系统综述了各种类型的CPRTP材料的分子结构和光电性能的关系,最后探讨了CPRTP材料目前存在的问题,并展望了其未来的发展前景及挑战。
