The low-energy electrochemical production of hydrogen peroxide(H_(2)O_(2))has garnered significant attention as a viable alternative to traditional industrial routes,with the goal of achieving carbon neutrality.For th...The low-energy electrochemical production of hydrogen peroxide(H_(2)O_(2))has garnered significant attention as a viable alternative to traditional industrial routes,with the goal of achieving carbon neutrality.For their H_(2)O_(2) selectivity in the two-electron oxygen reduction reaction(ORR),the coordination environment of tungsten(W)-based materials is critical.In this study,atomically dispersed W single atoms were immobilized on N-doped carbon substrates by a facile pyrolysis method to obtain a W single-atom catalyst(W-SAC).The coordination environment of an isolated W single atom with a tetra-coordinated porphyrin-like structure in W-SAC was determined by X-ray photoelectron spectroscopy and X-ray absorption spectroscopy analysis.Notably,the as-prepared W-SAC showed superior two-electron ORR activity in 0.1 M KOH solution,including high onset potential(0.89 V),high H_(2)O_(2) selectivity(82.5%),and excellent stability.By using differential phase contrast-scanning transmission electron microscopy and density functional theory calculations,it is revealed that the charge symmetry-breaking of W atoms changes the adsorption behavior of the intermediates,leading to enhanced reactivity and selectivity for two-electron ORR.This work broadens the avenue for understanding the charge transfer of W-based electrocatalytic materials and the in-depth reaction mechanism of SACs in two-electron ORR.展开更多
Utilization of the body’s regenerative potential for tissue repair is known as in situ tissue regeneration.However,the use of exogenous growth factors requires delicate control of the dose and delivery strategies and...Utilization of the body’s regenerative potential for tissue repair is known as in situ tissue regeneration.However,the use of exogenous growth factors requires delicate control of the dose and delivery strategies and may be accompanied by safety,efficacy and cost concerns.In this study,we developed,for the first time,a biomaterial-based strategy to activate endogenous transforming growth factor beta 1(TGFβ1)under alkaline conditions for effective in situ tissue regeneration.We demonstrated that alkaline-activated TGFβ1 from blood serum,bone marrow fluids and soaking solutions of meniscus and tooth dentin was capable of increasing cell recruitment and early differentiation,implying its broad practicability.Furthermore,we engineered an injectable hydrogel(MS-Gel)consisting of gelatin microspheres for loading strong alkaline substances and a modified gelatin matrix for hydrogel click crosslinking.In vitro models showed that alkaline MS-Gel controllably and sustainably activated endogenous TGFβ1 from tooth dentin for robust bone marrow stem cell migration.More importantly,infusion of in vivo porcine prepared root canals with alkaline MS-Gel promoted significant pulp-dentin regeneration with neurovascular stroma and mineralized tissue by endogenous proliferative cells.Therefore,this work offers a new bench-to-beside translation strategy using biomaterial-activated endogenous biomolecules to achieve in situ tissue regeneration without the need for cell or protein delivery.展开更多
During the last few years, the preparation of novel fluorescent probes for the detection of carbon dioxide has attracted considerable attention since carbon dioxide plays extremely important roles in widespread fields...During the last few years, the preparation of novel fluorescent probes for the detection of carbon dioxide has attracted considerable attention since carbon dioxide plays extremely important roles in widespread fields including chemical, environmental, clinical analysis, and agri-food industry. This review focuses on the recent advances in the design principles, recognition mechanisms, and preparation of small-molecule fluorescent probes for the selective detection and monitoring of CO;. Moreover, their properties and functions will be discussed detailedly as well.展开更多
During the past few years, the construction of BODIPY-based supramolecular fluorescent metallacages through coordination-driven self-assembly has gained increasing interest due to their unique photophysical properties...During the past few years, the construction of BODIPY-based supramolecular fluorescent metallacages through coordination-driven self-assembly has gained increasing interest due to their unique photophysical properties and applications in catalysis, sensing, and bioimaging. In consideration of the rapid development of this field, it is time to summarize recent developments involving BODIPY-based metallacages.In this review, a comprehensive summary of the construction of BODIPY-based metallacages as well as their photophysical properties and applications will be presented.展开更多
The fabrication of highly effective photosensitizers has received considerable attention because of their attractive functions and applications in the fields of photodynamic therapy, photosynthesis, photocatalysis, et...The fabrication of highly effective photosensitizers has received considerable attention because of their attractive functions and applications in the fields of photodynamic therapy, photosynthesis, photocatalysis, etc. Thus, it is highly desirable to develop a new approach to enhance photosensitization efficiency.Herein, through coordination-driven self-assembly, a series of metallacycles with efficient fluorescence resonance energy transfer(FRET) were effectively constructed, which displayed higher photosensitization efficiency and photocatalytic activity than their model metallacycles without FRET due to broadband absorption and singlet energy transfer from the energy acceptor to the energy donor. Moreover, iodization of fluorophores induced a significant enhancement of the photosensitization efficiency and photocatalytic activity of the metallacycles. This research provides an efficient strategy for improving photosensitization efficiency and a promising platform for the preparation of effective photosensitizers and photocatalysts.展开更多
Alzheimer's disease is a neurodegenerative disease that signals for excessβ-amyloid(Aβ)aggregation.Although people have made great attempts to control the aggregation of Aβ,no effective medications have been pr...Alzheimer's disease is a neurodegenerative disease that signals for excessβ-amyloid(Aβ)aggregation.Although people have made great attempts to control the aggregation of Aβ,no effective medications have been produced yet.Due to its excellent temporal and spatial selectivity,photodynamic treatment has been gradually employed and interfered in the aggregation process of Aβ,with some achievement.To enhance the research and application of photodynamic therapy in Alzheimer's disease,this paper reviews the progress of small-molecule photosensitizers in the treatment of Alzheimer's disease in recent years and outlines existing tactics and potential obstacles.展开更多
Plasmonic devices using periodic metallic nanostructures have recently gained tremendous interest for color filters,sensing,surface enhanced spectroscopy,and enhanced photoluminescence,etc.However,the performance of s...Plasmonic devices using periodic metallic nanostructures have recently gained tremendous interest for color filters,sensing,surface enhanced spectroscopy,and enhanced photoluminescence,etc.However,the performance of such plasmonic devices is severely hampered by the solid substrates supporting the metallic nanostructures.Here,a strategy for freestanding metallic nanomembranes is introduced by taking advantages of hollow substrate structures.Large-area and highly uniform gold nanomembranes with nanohole array are fabricated via a flexible and simple replication-releasing method.The hollow structures include a hollow core fiber with 30μm core diameter and two ferrules with their hole diameter as 125 and 500μm,respectively.As a proof-of-concept demonstration,2 times higher sensitivity of the bulk refractive index is obtained with this platform compared to that of a counterpart on a solid silica substrate.Such a portable and compact configuration provides unique opportunities to explore the intrinsic properties of the metal nanomembranes and paves a new way to fabricate high-performance plasmonic devices for biomolecule sensing and color filter.展开更多
基金National Natural Science Foundation of China,Grant/Award Number:51971157Science and Technology Commission of Shanghai Municipality,Grant/Award Number:22ZR1415700+5 种基金Shanghai Rising Star Program,Grant/Award Number:20QA1402400Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher LearningFundamental Research Funds for the Central UniversitiesFrontiers Science Center for Materiobiology and Dynamic ChemistryFeringa Nobel Prize Scientist Joint Research Center at East China University of Science and TechnologyShenzhen Science and Technology Program,Grant/Award Numbers:JCYJ20210324115412035,JCYJ20210324122803009,ZDSYS20210813095534001,J10M00172307180001,JCYJ20210324123202008。
文摘The low-energy electrochemical production of hydrogen peroxide(H_(2)O_(2))has garnered significant attention as a viable alternative to traditional industrial routes,with the goal of achieving carbon neutrality.For their H_(2)O_(2) selectivity in the two-electron oxygen reduction reaction(ORR),the coordination environment of tungsten(W)-based materials is critical.In this study,atomically dispersed W single atoms were immobilized on N-doped carbon substrates by a facile pyrolysis method to obtain a W single-atom catalyst(W-SAC).The coordination environment of an isolated W single atom with a tetra-coordinated porphyrin-like structure in W-SAC was determined by X-ray photoelectron spectroscopy and X-ray absorption spectroscopy analysis.Notably,the as-prepared W-SAC showed superior two-electron ORR activity in 0.1 M KOH solution,including high onset potential(0.89 V),high H_(2)O_(2) selectivity(82.5%),and excellent stability.By using differential phase contrast-scanning transmission electron microscopy and density functional theory calculations,it is revealed that the charge symmetry-breaking of W atoms changes the adsorption behavior of the intermediates,leading to enhanced reactivity and selectivity for two-electron ORR.This work broadens the avenue for understanding the charge transfer of W-based electrocatalytic materials and the in-depth reaction mechanism of SACs in two-electron ORR.
文摘Utilization of the body’s regenerative potential for tissue repair is known as in situ tissue regeneration.However,the use of exogenous growth factors requires delicate control of the dose and delivery strategies and may be accompanied by safety,efficacy and cost concerns.In this study,we developed,for the first time,a biomaterial-based strategy to activate endogenous transforming growth factor beta 1(TGFβ1)under alkaline conditions for effective in situ tissue regeneration.We demonstrated that alkaline-activated TGFβ1 from blood serum,bone marrow fluids and soaking solutions of meniscus and tooth dentin was capable of increasing cell recruitment and early differentiation,implying its broad practicability.Furthermore,we engineered an injectable hydrogel(MS-Gel)consisting of gelatin microspheres for loading strong alkaline substances and a modified gelatin matrix for hydrogel click crosslinking.In vitro models showed that alkaline MS-Gel controllably and sustainably activated endogenous TGFβ1 from tooth dentin for robust bone marrow stem cell migration.More importantly,infusion of in vivo porcine prepared root canals with alkaline MS-Gel promoted significant pulp-dentin regeneration with neurovascular stroma and mineralized tissue by endogenous proliferative cells.Therefore,this work offers a new bench-to-beside translation strategy using biomaterial-activated endogenous biomolecules to achieve in situ tissue regeneration without the need for cell or protein delivery.
基金the National Natural Science Foundation of China (Nos. 21871092, 21672070, 31570360)Shanghai Pujiang Program (No. 18PJD015)+1 种基金STCSM (Nos. 16XD1401000, 17XD14230000)Shanghai Rising-Star Program (No. 16QB1403800) for the financial support
文摘During the last few years, the preparation of novel fluorescent probes for the detection of carbon dioxide has attracted considerable attention since carbon dioxide plays extremely important roles in widespread fields including chemical, environmental, clinical analysis, and agri-food industry. This review focuses on the recent advances in the design principles, recognition mechanisms, and preparation of small-molecule fluorescent probes for the selective detection and monitoring of CO;. Moreover, their properties and functions will be discussed detailedly as well.
基金supported by the Program of Shanghai Outstanding Academic Leaders(No.21XD1421200)the Fundamental Research Funds for the Central Universities+1 种基金the financial support sponsored by the National Natural Science Foundation of China(No.22101183)China Postdoctoral Science Foundation(No.2021M702251)。
文摘During the past few years, the construction of BODIPY-based supramolecular fluorescent metallacages through coordination-driven self-assembly has gained increasing interest due to their unique photophysical properties and applications in catalysis, sensing, and bioimaging. In consideration of the rapid development of this field, it is time to summarize recent developments involving BODIPY-based metallacages.In this review, a comprehensive summary of the construction of BODIPY-based metallacages as well as their photophysical properties and applications will be presented.
基金supported by the National Nature Science Foundation of China (No. 21871092)Program of Shanghai Outstanding Academic Leaders (No. 21XD1421200)+1 种基金the Fundamental Research Funds for the Central Universities2021 Academic Innovation Ability Enhancement Plan for Excellent Doctoral Students of East China Normal University (No. YBNLTS2021-025)。
文摘The fabrication of highly effective photosensitizers has received considerable attention because of their attractive functions and applications in the fields of photodynamic therapy, photosynthesis, photocatalysis, etc. Thus, it is highly desirable to develop a new approach to enhance photosensitization efficiency.Herein, through coordination-driven self-assembly, a series of metallacycles with efficient fluorescence resonance energy transfer(FRET) were effectively constructed, which displayed higher photosensitization efficiency and photocatalytic activity than their model metallacycles without FRET due to broadband absorption and singlet energy transfer from the energy acceptor to the energy donor. Moreover, iodization of fluorophores induced a significant enhancement of the photosensitization efficiency and photocatalytic activity of the metallacycles. This research provides an efficient strategy for improving photosensitization efficiency and a promising platform for the preparation of effective photosensitizers and photocatalysts.
基金financially supported by the Fundamental Research Funds for the Central Universitiesthe Research Program on the Relationship between Nicotine and Alzheimer’s Disease(No.110201801035(JY-09))。
文摘Alzheimer's disease is a neurodegenerative disease that signals for excessβ-amyloid(Aβ)aggregation.Although people have made great attempts to control the aggregation of Aβ,no effective medications have been produced yet.Due to its excellent temporal and spatial selectivity,photodynamic treatment has been gradually employed and interfered in the aggregation process of Aβ,with some achievement.To enhance the research and application of photodynamic therapy in Alzheimer's disease,this paper reviews the progress of small-molecule photosensitizers in the treatment of Alzheimer's disease in recent years and outlines existing tactics and potential obstacles.
基金Innovation Foundation for Doctor Dissertation of Northwestern Polytechnical University(CX201818)China Scholarship Council(201706290163)+1 种基金ARC Centre of Excellence for Nanoscale Biophotonics(CE14010003)State Key Laboratory of Advanced Optical Communication Systems and Networks,China.
文摘Plasmonic devices using periodic metallic nanostructures have recently gained tremendous interest for color filters,sensing,surface enhanced spectroscopy,and enhanced photoluminescence,etc.However,the performance of such plasmonic devices is severely hampered by the solid substrates supporting the metallic nanostructures.Here,a strategy for freestanding metallic nanomembranes is introduced by taking advantages of hollow substrate structures.Large-area and highly uniform gold nanomembranes with nanohole array are fabricated via a flexible and simple replication-releasing method.The hollow structures include a hollow core fiber with 30μm core diameter and two ferrules with their hole diameter as 125 and 500μm,respectively.As a proof-of-concept demonstration,2 times higher sensitivity of the bulk refractive index is obtained with this platform compared to that of a counterpart on a solid silica substrate.Such a portable and compact configuration provides unique opportunities to explore the intrinsic properties of the metal nanomembranes and paves a new way to fabricate high-performance plasmonic devices for biomolecule sensing and color filter.
