The search for photoactive materials that are able to efficiently produce solar fuels is a growing research field to tackle the current energy crisis.Herein,we have prepared two ionic non-noble metallo-supramolecular ...The search for photoactive materials that are able to efficiently produce solar fuels is a growing research field to tackle the current energy crisis.Herein,we have prepared two ionic non-noble metallo-supramolecular polymers Se-MTpy(M=Co or Ni),and constructed their composites with single-walled carbon nanotubes(CNTs)via electrostatic attraction andπ-πinteractions for efficient and stable photocatalytic hydrogen evolution.In the photocatalytic system,the cationic Se-MTpy as host and anionic CNTs as vip are assembled into a binary composite,which exhibits superior photocatalytic activity under visible light irradiation(>420 nm).The optimized CNT@Se-CoTpy composite,containing 1.2 wt%metal loading,achieves 7 times higher hydrogen evolution rate(2.47 mmol g^(-1)h^(-1))than bare Se-CoTpy(0.35 mmol g^(-1)h^(-1)).This is attributed to the constructive formation of junctions between polymer and CNTs,facilitating interfacial charge transfer and transport for efficient proton reduction.The composite system also shows high photostability after continuous irradiation for~30 h.The combination of experimental and theoretical analysis demonstrates the higher activity for reducing H_(2)O to H_(2)of Se-CoTpy than Se-NiTpy.The feasible interfacial architecture proposed in this study represents an effective approach to achieve high photocatalytic performance.展开更多
In this study,we present a novel multicomponent self-assembly approach that offers good potential for crafting heterometallic complexes with exceptional constitutional control.This method generates metal ions from a s...In this study,we present a novel multicomponent self-assembly approach that offers good potential for crafting heterometallic complexes with exceptional constitutional control.This method generates metal ions from a sacrificial anode by using an electric field,which then coordinates with a metal complex precursor.As a proof-of-concept demonstration,we successfully synthesized single crystals of a heterometallic platinum(Ⅱ)-copper(Ⅰ)(Pt[Ⅱ]-Cu[Ⅰ])complex at an exceptionally rapid rate within 30 s by applying a voltage to an acetonitrile solution of[Pt(ppy)(CN)_(2)]^(−)Bu_(4)N^(+),using copper foil as the anode.Intriguingly,by finely adjusting the intensity and duration of the electric field,we achieved a variety of supramolecular structures,spanning from spherical to rod-like and even flower-like morphologies.Additionally,we found that the photoluminescence property of the resultant crystal can be reversibly shifted among green,orange,and cyan by merely altering the solvent environment.Finally,the crafted heterometallic Pt(Ⅱ)-Cu(Ⅰ)complex has shown great promise in advanced anti-counterfeiting applications.展开更多
Organic persistent room-temperature phosphorescent(RTP)materials are promising for applications requiring the secure recording and anti-counterfeiting features owing to their appealing optical properties.Several criti...Organic persistent room-temperature phosphorescent(RTP)materials are promising for applications requiring the secure recording and anti-counterfeiting features owing to their appealing optical properties.Several critical challenges,such as the difficulty to obtain high-quality patterns over large areas and low security levels,need to be addressed to meet the requirements for commercial purpose.Here,we prepared a series of quaternary phosphonium salts with different alkyl chains,which showed interesting organic persistent RTP.The ionic characteristics and the alkyl chains of these molecules impart abundant weak intermolecular interactions.This confers the molecules a high crystallinity,which helps to preserve the persistent RTP properties and cover large areas.Moreover,the RTP lifetime of these organic salts varies over a wide range(1.27 to 884.71 ms)and can be tuned by simply changing the alkyl chain length and counterions,which opens new possibilities in multi-level information encryption applications.It is believed that the engineering of organic salts with tunable persistent RTP lifetimes and large-area printing can promote early-stage demonstrations of security applications into mature commercialization.展开更多
Organic-ligand-containing frameworks have drawn considerable attention due to their multifunctional properties as well as tunable structures for broad applications.Among numerous synthesis methods developed in the pas...Organic-ligand-containing frameworks have drawn considerable attention due to their multifunctional properties as well as tunable structures for broad applications.Among numerous synthesis methods developed in the past two decades,electrochemical processing has been demonstrated as one of the most efficient,safe,and facile ways to realize the large-scale and highly controllable production of organic-ligand-containing frameworks.In this review,the progress of electrochemically induced crystallization and thin film fabrication of organic-ligand-containing frameworks is summarized in a well-rounded way.Besides,the mechanism and processing parameters are also discussed.Moreover,the main challenges are also expounded for providing some guidance on the future development of organic-ligand-containing frameworks,especially for covalent-organic frameworks and hydrogen-bonded organic frameworks.展开更多
Objective:Pseudomonas aeruginosa(P.aeruginosa)contains a hierarchy of quorum sensing(QS)network,consisting of the las,rhl and pqs systems,which play a key role in coordinating the expression of virulence factors.PA214...Objective:Pseudomonas aeruginosa(P.aeruginosa)contains a hierarchy of quorum sensing(QS)network,consisting of the las,rhl and pqs systems,which play a key role in coordinating the expression of virulence factors.PA2146 was found to be associated with P.aeruginosa pathogenicity in macrophage and host Immune response.The aim of this study was to investigate the effects of PA2146 on the virulence of P.aeruginosa and explore its mechanism.Methods:PA2146 gene knockout strain and complement strain of P.aeruginosa PAO1 were constructed.The biomass of biofilm was detected by crystal violet staining;the virulence factors were measured,including pyocyanin,rhamnolipid,LasA elastase,LasB elastase and hemolytic activity;RNA-seq and label-free relative quantitative proteomics analyses were carried out to test the influence of PA2146 on transcriptomics and proteomics.This study was approved by the Institutional Review Board of the Third Xiangya Hospital,Central South University,China(approval No.2019-S021).Results:PA2146-deficient strains showed reduced biofilm formation and increased pyocyanin,rhamnolipid,LasA elastase,LasB elastase,and hemolytic activity,as well as increased motility,compared with the wild-type strain.RNA-seq and label-free relative quantitative proteomics analyses revealed that PA2146 repressed the transcription of several genes that are integral to the pqs system and to pyocyanin biosynthesis,and increased the expression of MexEF-OprN efflux pump components at the gene and protein level.Conclusion:PA2146 gene was found to inhibit the pqs system.PA2146 may affect quorum sensing by directly inhibiting the pqs system or by enhancing the expression of MexEF-OprN efflux pump components,thereby promoting efflux of 2-heptyl-4(1H)-quinolone,a Pseudomonas quinolone signal precursor,and thus affecting P.aeruginosa virulence.展开更多
Controlling multicolor luminescence in a single chromophore is of fundamental significance but remains a great challenge.In this study,a carbazole group was incorporated into terpyridine through acylamide to produce a...Controlling multicolor luminescence in a single chromophore is of fundamental significance but remains a great challenge.In this study,a carbazole group was incorporated into terpyridine through acylamide to produce a novel chromophore(N-{4-[(2,2′:6′,2″-terpyridine)-4′-yl]benzyl}-9-hexyl-9H-carbazole-3-carboxamide,TBCC)for achieving programmable luminescence switches.Significantly different emission states,such as nonemissive,blue,green,yellow,red,and white,were achieved in situ by controlling sol–gel transformation with sonication/heat and the reversible metal–ligand coordination between TBCC and various metal salts.展开更多
基金supported by the RGC Senior Research Fellowship Scheme(Grant No.SRFS2021-5S01)the Hong Kong Research Grants Council(Grant No.PolyU 15307321)+2 种基金Research Institute for Smart Energy(CDAQ),Research Centre for Nanoscience and Nanotechnology(CE2H),Research Centre for Carbon-Strategic Catalysis(CE2L)Miss Clarea Au for the Endowed Professorship in Energy(Grant No.847S)National Natural Science Foundation of China(Grant No.62205277).
文摘The search for photoactive materials that are able to efficiently produce solar fuels is a growing research field to tackle the current energy crisis.Herein,we have prepared two ionic non-noble metallo-supramolecular polymers Se-MTpy(M=Co or Ni),and constructed their composites with single-walled carbon nanotubes(CNTs)via electrostatic attraction andπ-πinteractions for efficient and stable photocatalytic hydrogen evolution.In the photocatalytic system,the cationic Se-MTpy as host and anionic CNTs as vip are assembled into a binary composite,which exhibits superior photocatalytic activity under visible light irradiation(>420 nm).The optimized CNT@Se-CoTpy composite,containing 1.2 wt%metal loading,achieves 7 times higher hydrogen evolution rate(2.47 mmol g^(-1)h^(-1))than bare Se-CoTpy(0.35 mmol g^(-1)h^(-1)).This is attributed to the constructive formation of junctions between polymer and CNTs,facilitating interfacial charge transfer and transport for efficient proton reduction.The composite system also shows high photostability after continuous irradiation for~30 h.The combination of experimental and theoretical analysis demonstrates the higher activity for reducing H_(2)O to H_(2)of Se-CoTpy than Se-NiTpy.The feasible interfacial architecture proposed in this study represents an effective approach to achieve high photocatalytic performance.
基金Wai-Yeung Wong acknowledges the financial support from the National Key R&D Program of China(2022YFE0104100)the National Natural Science Foundation of China(52073242)+4 种基金the RGC Senior Research Fellowship Scheme(SRFS2021-5S01)General Research Fund(PolyU 15301922)the Research Institute for Smart Energy(CDAQ)the Research Centre for Nanoscience and Nanotechnology(CE2H),the Research Centre for Carbon-Strategic Catalysis(CE01 and CE2L)Miss Clarea Au for the Endowed Professorship in Energy(847S).
文摘In this study,we present a novel multicomponent self-assembly approach that offers good potential for crafting heterometallic complexes with exceptional constitutional control.This method generates metal ions from a sacrificial anode by using an electric field,which then coordinates with a metal complex precursor.As a proof-of-concept demonstration,we successfully synthesized single crystals of a heterometallic platinum(Ⅱ)-copper(Ⅰ)(Pt[Ⅱ]-Cu[Ⅰ])complex at an exceptionally rapid rate within 30 s by applying a voltage to an acetonitrile solution of[Pt(ppy)(CN)_(2)]^(−)Bu_(4)N^(+),using copper foil as the anode.Intriguingly,by finely adjusting the intensity and duration of the electric field,we achieved a variety of supramolecular structures,spanning from spherical to rod-like and even flower-like morphologies.Additionally,we found that the photoluminescence property of the resultant crystal can be reversibly shifted among green,orange,and cyan by merely altering the solvent environment.Finally,the crafted heterometallic Pt(Ⅱ)-Cu(Ⅰ)complex has shown great promise in advanced anti-counterfeiting applications.
基金financial support from the National Funds for Distinguished Young Scientists (61825503)the National Natural Science Foundation of China (62075101, 21701087 and 61775101)+1 种基金the National Program for Support of Top-Notch Young Professionalsthe Postgraduate Research & Practice Innovation Program of Jiangsu Province (46030CX18010)
文摘Organic persistent room-temperature phosphorescent(RTP)materials are promising for applications requiring the secure recording and anti-counterfeiting features owing to their appealing optical properties.Several critical challenges,such as the difficulty to obtain high-quality patterns over large areas and low security levels,need to be addressed to meet the requirements for commercial purpose.Here,we prepared a series of quaternary phosphonium salts with different alkyl chains,which showed interesting organic persistent RTP.The ionic characteristics and the alkyl chains of these molecules impart abundant weak intermolecular interactions.This confers the molecules a high crystallinity,which helps to preserve the persistent RTP properties and cover large areas.Moreover,the RTP lifetime of these organic salts varies over a wide range(1.27 to 884.71 ms)and can be tuned by simply changing the alkyl chain length and counterions,which opens new possibilities in multi-level information encryption applications.It is believed that the engineering of organic salts with tunable persistent RTP lifetimes and large-area printing can promote early-stage demonstrations of security applications into mature commercialization.
基金supported by the National Funds for Distinguished Young Scientists(61825503)the National Natural Science Foundation of China(62288102,62205277 and 62322508).
基金Qichun Zhang acknowledges the starting fund from City University of Hong Kong and 111 Project(D20015).
文摘Organic-ligand-containing frameworks have drawn considerable attention due to their multifunctional properties as well as tunable structures for broad applications.Among numerous synthesis methods developed in the past two decades,electrochemical processing has been demonstrated as one of the most efficient,safe,and facile ways to realize the large-scale and highly controllable production of organic-ligand-containing frameworks.In this review,the progress of electrochemically induced crystallization and thin film fabrication of organic-ligand-containing frameworks is summarized in a well-rounded way.Besides,the mechanism and processing parameters are also discussed.Moreover,the main challenges are also expounded for providing some guidance on the future development of organic-ligand-containing frameworks,especially for covalent-organic frameworks and hydrogen-bonded organic frameworks.
基金This study was supported by the National Natural Science Foundation of China(grant No.82072350 to YW).
文摘Objective:Pseudomonas aeruginosa(P.aeruginosa)contains a hierarchy of quorum sensing(QS)network,consisting of the las,rhl and pqs systems,which play a key role in coordinating the expression of virulence factors.PA2146 was found to be associated with P.aeruginosa pathogenicity in macrophage and host Immune response.The aim of this study was to investigate the effects of PA2146 on the virulence of P.aeruginosa and explore its mechanism.Methods:PA2146 gene knockout strain and complement strain of P.aeruginosa PAO1 were constructed.The biomass of biofilm was detected by crystal violet staining;the virulence factors were measured,including pyocyanin,rhamnolipid,LasA elastase,LasB elastase and hemolytic activity;RNA-seq and label-free relative quantitative proteomics analyses were carried out to test the influence of PA2146 on transcriptomics and proteomics.This study was approved by the Institutional Review Board of the Third Xiangya Hospital,Central South University,China(approval No.2019-S021).Results:PA2146-deficient strains showed reduced biofilm formation and increased pyocyanin,rhamnolipid,LasA elastase,LasB elastase,and hemolytic activity,as well as increased motility,compared with the wild-type strain.RNA-seq and label-free relative quantitative proteomics analyses revealed that PA2146 repressed the transcription of several genes that are integral to the pqs system and to pyocyanin biosynthesis,and increased the expression of MexEF-OprN efflux pump components at the gene and protein level.Conclusion:PA2146 gene was found to inhibit the pqs system.PA2146 may affect quorum sensing by directly inhibiting the pqs system or by enhancing the expression of MexEF-OprN efflux pump components,thereby promoting efflux of 2-heptyl-4(1H)-quinolone,a Pseudomonas quinolone signal precursor,and thus affecting P.aeruginosa virulence.
基金National Funds for Distinguished Young of China(no.61825503)and National Natural Science Foundation of China(nos.62075101,21701087 and 61775101).
文摘Controlling multicolor luminescence in a single chromophore is of fundamental significance but remains a great challenge.In this study,a carbazole group was incorporated into terpyridine through acylamide to produce a novel chromophore(N-{4-[(2,2′:6′,2″-terpyridine)-4′-yl]benzyl}-9-hexyl-9H-carbazole-3-carboxamide,TBCC)for achieving programmable luminescence switches.Significantly different emission states,such as nonemissive,blue,green,yellow,red,and white,were achieved in situ by controlling sol–gel transformation with sonication/heat and the reversible metal–ligand coordination between TBCC and various metal salts.
