Metal-N_(4)(M-N_(4))macrocyclic complexes are interesting electrocatalysts due to their well-defined structures and rich molecular tuning.Among them,metal phthalocyanines have been widely studied for the carbon dioxid...Metal-N_(4)(M-N_(4))macrocyclic complexes are interesting electrocatalysts due to their well-defined structures and rich molecular tuning.Among them,metal phthalocyanines have been widely studied for the carbon dioxide reduction reaction(CO_(2)RR)in heterogeneous systems and demonstrated good electrocatalytic performance.However,other complexes like metal corroles and metal porphyrins are much less explored,and often show inferior performances.In this study,three cobalt macrocyclic complexes,cobalt phthalocyanine,cobalt meso-tetraphenylporphyrin,and cobalt meso-triphenylcorrole(CoPc,CoTPP and CoTPC)are investigated in heterogeneous electrocatalysis of CO_(2)RR.Although CoPc/carbon nanotube(CNT)hybrid exhibits high electrocatalytic activity,CNT hybridization does not work for CoTPC and CoTPP that hold weak interactions with CNTs.By the drop-dry method with a high molecular loading of 5.4×10^(–7) mol cm^(–2),CoTPC and CoTPP could deliver appreciable electrode activities.Poly(4-vinylpyridine)(PVP)introduction is further demonstrated as a facile method to afford enhanced activities for CoTPP at low molecular loadings through enhancing molecule-substrate interactions.The partial current density of carbon monoxide for CoTPP+CNT/PVP is around 8 times higher than the sample without PVP at–0.67 V versus reversible hydrogen electrode.This work provides solutions to enhance the electrode activities of molecular electrocatalysts with weak substrate interactions in heterogeneous systems.展开更多
It is of vital importance to improve the long-term and photostability of organic photovoltaics,including organic solar cells(OSCs)and organic photodetectors(OPDs),for their ultimate industrialization.Herein,two series...It is of vital importance to improve the long-term and photostability of organic photovoltaics,including organic solar cells(OSCs)and organic photodetectors(OPDs),for their ultimate industrialization.Herein,two series of terpolymers featuring with an antioxidant butylated hydroxytoluene(BHT)-terminated side chain,PTzBI-EHp-BTBHTx and N2200-BTBHTx(x=0.05,0.1,0.2),are designed and synthesized.It was found that incorporating appropriate ratio of benzothiadiazole(BT)with BHT side chains on the conjugated backbone would induce negligible effect on the molecular weight,absorption spectra and energy levels of polymers,however,which would obviously enhance the photostability of these polymers.Consequently,all-polymer solar cells(all-PSCs)and photodetectors were fabricated,and the all-PSC based on PTzBI-EHp-BTBHT0.05:N2200 realized an optimal power conversion efficiency(PCE)approaching~10%,outperforming the device based on pristine PTzBI-EHp:N2200.Impressively,the all-PSCs based on BHT-featuring terpolymers displayed alleviated PCEs degradation under continuous irradiation for 300 h due to the improved morphological and photostability of active layers.The OPDs based on BHT-featuring terpolymers achieved a lower dark current at−0.1 bias,which could be stabilized even after irradiation over 400 h.This study provides a feasible approach to develop terpolymers with antioxidant efficacy for improving the lifetime of OSCs and OPDs.展开更多
Algicidal bacteria have been frequently isolated from algal blooming areas.However,knowledge regarding the microbial communities coexisting with microalgae and their potential application in preventing harmful algal b...Algicidal bacteria have been frequently isolated from algal blooming areas.However,knowledge regarding the microbial communities coexisting with microalgae and their potential application in preventing harmful algal blooms(HABs)is limited.In this study,we investigated the composition of the microbial community coexisting with harmful alga Karenia mikimotoi and its responses to algal control via nutrient stimulation or by adding algicidal strain in microcosms.The microorganisms inhabiting the K.mikimotoi culture consisted of 24 identifi ed phyla,including dominant Proteobacteria(relative abundance 76.24%±7.28%)and Bacteroidetes(22.67%±8.32%).Rhodobacteraceae,Phaeodactylibacter,and Maritimibacter predominated during the algal cultivation.Both the added nutrient and fermentation broth of algicidal strain Pseudoalteromonas QF1 caused a massive death of K.mikimotoi and substantial changes in the coexisting microbial community,in which Rhodobacteraceae and Phaeodactylibacter signifi cantly decreased,while Halomonas and Alteromonas increased.Core operational taxonomic units(OTUs)analysis indicated that 13 OTUs belonging to Rhodobacteraceae,Maritimibacter,Marivita,Nisaea,Phaeodactylibacter,Citreicella,Halomonas,Alteromonas,Marinobacter,Muricauda,and Pseudoalteromonas dominated the changes of the microbial communities observed in the K.mikimotoi culture with or without treatments.Collectively,this study indicated that microbial community inhabiting K.mikimotoi culture includes potential algicidal bacteria,and improves our knowledge about microbial community succession during biocontrol of K.mikimotoi via nutrient stimulation or by adding isolated algicidal strains.展开更多
The stability of organic solar cells(OSCs)remains a major concern for their ultimate industrialization due to the photo,oxygen,and water susceptibility of organic photoactive materials.Usually,antioxidant additives ar...The stability of organic solar cells(OSCs)remains a major concern for their ultimate industrialization due to the photo,oxygen,and water susceptibility of organic photoactive materials.Usually,antioxidant additives are blended as radical scavengers into the active layer.However,it will induce the intrinsic morphology instability and adversely affect the efficiency and long-term stability.Herein,the antioxidant dibutylhydroxytoluene(BHT)group has been covalently linked onto the side chain of benzothiadiazole(BT)unit,and a series of ternary copolymers D18-Cl-BTBHTx(x=0,0.05,0.1,0.2)with varied ratio of BHT-containing side chains have been synthesized.It was found that the introduction of BHT side chains would have a negligible effect on the photophysical properties and electronic levels,and the D18-Cl-BTBHT0.05:Y6-based OSC achieved the highest power conversion efficiency(PCE)of 17.6%,which is higher than those based active layer blended with BHT additives.More importantly,the unencapsulated device based on D18-Cl-BTBHTx(x=0.05,0.1,0.2)retained approximately 50%of the initial PCE over 30 hours operation under ambient conditions,significantly outperforming the control device based on D18-Cl(90%degradation in PCE after 30 h).This work provides a new structural design strategy of copolymers for OSCs with simultaneously improved efficiency and stability.展开更多
Herein,we have designed the all-nanoporous composite(ANC)membranes with metal-organic framework(MOF)fillers and hydrogen-bonded organic framework(HOF)matrix,achieving high-permeance H_(2) purification.The hetero-MOF f...Herein,we have designed the all-nanoporous composite(ANC)membranes with metal-organic framework(MOF)fillers and hydrogen-bonded organic framework(HOF)matrix,achieving high-permeance H_(2) purification.The hetero-MOF facilitates the heterogeneous nucleation,offsetting the need for a highly supersaturated solution to achieve sufficient nucleation density during solution processing.Continuous MOF/HOF ANC membranes are realized by suppressing the homogeneous nucleation,equilibrating the nucleation driving force with the molecular attachment rate,and balancing the nutrient supply and demand.The optimized copper 1,4-benzene dicarboxylate nanosheets(ns-CuBDC)/HOF-30-100(30 means that HOF monomer concentration is 30 mg·mL^(−1) and 100 represents that the temperature for solvent evaporation is 100℃)ANC membrane shows synchronously improved H_(2) permeance and H_(2)/CH4 selectivity by 562%and 241%compared to the pristine HOF membrane.The ns-CuBDC/HOF-30-100 ANC membrane inherits the pressure-responsive behavior from the parent HOF,exhibiting further improved H_(2) permeance up to 9842 gas permeation units(GPU)and slightly changed H_(2)/CH4 selectivity of 30.01 at 2.0 bar.The MOF/HOF ANC membrane manifests that incorporating a porous hetero-phase effectively upgrades the gas separation performance,and the HOF matrix circumvents the performance constraints of the traditional polymer matrix while preserving the solution-processability.展开更多
Maintainance of sulfomucin is a key end point in the treatment of diarrhea and inflammatory bowel disease(IBD).However,the mechanisms underlying the microbial sense to sulfomucin are poorly understood,and to date,ther...Maintainance of sulfomucin is a key end point in the treatment of diarrhea and inflammatory bowel disease(IBD).However,the mechanisms underlying the microbial sense to sulfomucin are poorly understood,and to date,there are no therapies targeting the secretion and maturation of sulfomucin in IBD.Herein,we biosynthesized poly-β-hydroxybutyrate(PHB)and found that PHB could alleviate inflammation caused by diarrhea and colitis by enhancing the differentiation of sulfomucin.Microbiota transplantation and clearance together demonstrate that PHB promoting sulfomucin is mediated by Lactobacillus johnsonii(L.johnsonii).Further studies revealed that PHB provides a favorable niche for L.johnsonii biofilm formation to resist disturbance and support its growth.L.johnsonii-biofilm alleviates colitis by regulating fucose residues to promote goblet cell differentiation and subsequent sulfomucin maturation.Importantly,PHB alleviates colitis by enhancing sulfomucin secretion and maturation in a L.johnsonii-dependent manner.PHB represents a class of guardians,acting as a safe probiotic-biofilm delivery system that significantly promotes probiotic proliferation.Altogether,this study adds weight to the possible role of probiotics and functional materials in the treatment of intestinal inflammation.The application of PHB and biofilm self-coating L.johnsonii carries high translational potential and may be of clinical relevance.展开更多
The second near-infrared(NIR-II,1,000 to 1,700 nm)molecular fluorophores containing donor–acceptor–donor conjugated backbone have attracted substantial attention due to their outstanding advantages,such as stable em...The second near-infrared(NIR-II,1,000 to 1,700 nm)molecular fluorophores containing donor–acceptor–donor conjugated backbone have attracted substantial attention due to their outstanding advantages,such as stable emission and facilely tuned photophysical properties.However,it is still challenging for them to simultaneously achieve high brightness and red-shifted absorption and emission.Herein,furan is adopted as the D unit to construct NIR-II fluorophores,demonstrating red shift of absorption,enhanced absorption coefficient,and fluorescent quantum yield when compared with the generally used thiophene counterparts.The high brightness and desirable pharmacokinetics of the optimized fluorophore,IR-FFCHP,endows improved performance for angiography and tumor-targeting imaging.Furthermore,dual-NIR-II imaging of tumor and sentinel lymph nodes(LNs)has been achieved with IR-FFCHP and PbS/CdS quantum dots,enabling the in vivo imaging navigated LN surgery in tumor-bearing mice.This work demonstrates the potential of furan for constructing bright NIR-II fluorophores for biological imaging.展开更多
Organic solar cells(OSCs) have drawn considerable attention in the last decade due to the great potential of light weight,flexibility, and low-cost solution processing. Particularly, Y-series non-fullerene acceptors(N...Organic solar cells(OSCs) have drawn considerable attention in the last decade due to the great potential of light weight,flexibility, and low-cost solution processing. Particularly, Y-series non-fullerene acceptors(NFAs) including small molecular acceptors(SMAs) and polymerized small molecular acceptors(PSMAs) have become research hot spots due to their excellent power conversion efficiency. Side chain engineering is crucial to adjust the solubility and crystallinity of NFAs, which will significantly affect the morphology of active layers and the efficiency of OSCs. However, the understanding of side chain engineering on NFAs is still limited and lacks a systematic review. This review aims to provide a brief summary of the recent developments in side chain engineering of NFAs, with a special focus on the design and application of Y-series SMAs and PSMAs for high-efficiency non-fullerene organic solar cells(NF-OSCs). In addition, the review also points out challenges and provides useful guidance regarding side chain regulation for Y-series NFAs.展开更多
It is challenging to develop molecular fluorophores in the second near-infrared(NIR-Ⅱ)window with long wavelength emission and high brightness,which can improve the performance of biological imaging.Herein,we report ...It is challenging to develop molecular fluorophores in the second near-infrared(NIR-Ⅱ)window with long wavelength emission and high brightness,which can improve the performance of biological imaging.Herein,we report a molecular engineering approach to afford NIR-Ⅱ fluorophores with these merits based on fused-ring acceptor(FRA)molecules.Dioctyl 3,4-propylenedioxy thiophene(PDOT-C8)is utilized as the bridging donor to replace 3-ethylhexyloxy thiophene(3-EHOT),leading to more than 20 times enhancement of brightness.The nanofluorophores(NFs)based on the optimized CPTIC-4F molecule exhibit an emission peak of 1,110 nm with a fluorescence quantum yield(QY)of 0.39%(QY of IR-26 is 0.050%in dichloroethane as reference)and peak absorption coefficient of 14.5 x 10^4 M^-1·cm^-1 in aqueous solutions,which are significantly higher than those of 3-EHOT based COTIC-4F NFs.It is found that PDOT-C8 can weaken intermolecular aggregation,enhance protection of molecular backbone from water,and decrease backbone distortion,beneficial for the high brightness.Compared with indocyanine green with same injection dose,CPTIC-4F NFs show 10 times higher signal-to-background ratio for whole body vessels imaging at 1,300 nm long pass filters.展开更多
Conductive polymers have recently drawn tremendous attention due to their promising applications in electronic and energy-related devices.While p-type conductive polymers such as poly(3,4-ethylenedioxythiophene):poly(...Conductive polymers have recently drawn tremendous attention due to their promising applications in electronic and energy-related devices.While p-type conductive polymers such as poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)have achieved commercialization,the development of stable,high-performance n-type polymers has lagged.Recently,the discovery of n-type polymer poly(benzodifurandione)(PBFDO)has greatly promoted the development and application of n-type conductive polymers.However,the synthesis process involves cumbersome post-processing,which greatly increases the cost and difficulty of mass production.Herein,a novel synthesis method for PBFDO has been developed,which was promoted by the combination of solvent dimethyl sulfoxide(DMSO)and acetic anhydride(Ac_(2)O).This method exploits the oxidative capability of DMSO,activated by Ac_(2)O,which can promote the keto-enol tautomerism of 3,7-dihydrobenzo[1,2-b:4,5-b′]difuran-2,6-dione(BFDO)and induce the rapid polymerization.The resulting PBFDO ink exhibits a high electronic conductivity of more than 2000 S cm^(-1)and excellent ambient stability.Significantly,the additives and by-products remain in a liquid state during the polymerization process and possess low boiling points,allowing for the production of pure PBFDO films through straightforward heating and drying.Furthermore,this approach holds considerable promise for in situ polymerization,as functional conductive films can be prepared by merely combining the monomers with the DMSO/Ac_(2)O mixture and applying heat.This efficient,purification-free strategy represents a significant step toward the industrial application of the highperformance n-type conductive polymer PBFDO.展开更多
文摘Metal-N_(4)(M-N_(4))macrocyclic complexes are interesting electrocatalysts due to their well-defined structures and rich molecular tuning.Among them,metal phthalocyanines have been widely studied for the carbon dioxide reduction reaction(CO_(2)RR)in heterogeneous systems and demonstrated good electrocatalytic performance.However,other complexes like metal corroles and metal porphyrins are much less explored,and often show inferior performances.In this study,three cobalt macrocyclic complexes,cobalt phthalocyanine,cobalt meso-tetraphenylporphyrin,and cobalt meso-triphenylcorrole(CoPc,CoTPP and CoTPC)are investigated in heterogeneous electrocatalysis of CO_(2)RR.Although CoPc/carbon nanotube(CNT)hybrid exhibits high electrocatalytic activity,CNT hybridization does not work for CoTPC and CoTPP that hold weak interactions with CNTs.By the drop-dry method with a high molecular loading of 5.4×10^(–7) mol cm^(–2),CoTPC and CoTPP could deliver appreciable electrode activities.Poly(4-vinylpyridine)(PVP)introduction is further demonstrated as a facile method to afford enhanced activities for CoTPP at low molecular loadings through enhancing molecule-substrate interactions.The partial current density of carbon monoxide for CoTPP+CNT/PVP is around 8 times higher than the sample without PVP at–0.67 V versus reversible hydrogen electrode.This work provides solutions to enhance the electrode activities of molecular electrocatalysts with weak substrate interactions in heterogeneous systems.
基金The work was financially supported by National Key Research and Development Program of China(2019YFA0705900,2022YFB4200400)funded by MOSTthe Basic and Applied Basic Research Major Program of Guangdong Province(No.2019B030302007)+2 种基金the National Natural Science Foundation of China(No.U21A6002)Guangdong-Hong Kong-Macao joint laboratory of optoelectronic and magnetic functional materials(No.2019B121205002)C.Z.acknowledges the financial support by Basic and Applied Basic Research Major Program of Guangdong Province(No.202201010270).
文摘It is of vital importance to improve the long-term and photostability of organic photovoltaics,including organic solar cells(OSCs)and organic photodetectors(OPDs),for their ultimate industrialization.Herein,two series of terpolymers featuring with an antioxidant butylated hydroxytoluene(BHT)-terminated side chain,PTzBI-EHp-BTBHTx and N2200-BTBHTx(x=0.05,0.1,0.2),are designed and synthesized.It was found that incorporating appropriate ratio of benzothiadiazole(BT)with BHT side chains on the conjugated backbone would induce negligible effect on the molecular weight,absorption spectra and energy levels of polymers,however,which would obviously enhance the photostability of these polymers.Consequently,all-polymer solar cells(all-PSCs)and photodetectors were fabricated,and the all-PSC based on PTzBI-EHp-BTBHT0.05:N2200 realized an optimal power conversion efficiency(PCE)approaching~10%,outperforming the device based on pristine PTzBI-EHp:N2200.Impressively,the all-PSCs based on BHT-featuring terpolymers displayed alleviated PCEs degradation under continuous irradiation for 300 h due to the improved morphological and photostability of active layers.The OPDs based on BHT-featuring terpolymers achieved a lower dark current at−0.1 bias,which could be stabilized even after irradiation over 400 h.This study provides a feasible approach to develop terpolymers with antioxidant efficacy for improving the lifetime of OSCs and OPDs.
基金Supported by the National Natural Science Foundation of China(Nos.31971503,31901188)the Shandong Provincial Agricultural Fine Species Project(No.2019LZGC020)+5 种基金the Jining Key Research and Development Project of Shandong Province(No.2019ZDGH019)the Shandong Provincial Natural Science Foundation(Nos.ZR2019BB040,ZR2020MC042)the Interdisciplinary Project of Qufu Normal University(No.XKJJC201903)the Key Research and Development Project of Liaoning Province(No.2018228004)the Revitalization Talents Program of Liaoning Province(No.XLYC1907109),the Shandong Provincial Key Research and Development Project(No.2018GSF117035)the Shandong Provincial Higher Educational Science and Technology Program(No.J17KA112)。
文摘Algicidal bacteria have been frequently isolated from algal blooming areas.However,knowledge regarding the microbial communities coexisting with microalgae and their potential application in preventing harmful algal blooms(HABs)is limited.In this study,we investigated the composition of the microbial community coexisting with harmful alga Karenia mikimotoi and its responses to algal control via nutrient stimulation or by adding algicidal strain in microcosms.The microorganisms inhabiting the K.mikimotoi culture consisted of 24 identifi ed phyla,including dominant Proteobacteria(relative abundance 76.24%±7.28%)and Bacteroidetes(22.67%±8.32%).Rhodobacteraceae,Phaeodactylibacter,and Maritimibacter predominated during the algal cultivation.Both the added nutrient and fermentation broth of algicidal strain Pseudoalteromonas QF1 caused a massive death of K.mikimotoi and substantial changes in the coexisting microbial community,in which Rhodobacteraceae and Phaeodactylibacter signifi cantly decreased,while Halomonas and Alteromonas increased.Core operational taxonomic units(OTUs)analysis indicated that 13 OTUs belonging to Rhodobacteraceae,Maritimibacter,Marivita,Nisaea,Phaeodactylibacter,Citreicella,Halomonas,Alteromonas,Marinobacter,Muricauda,and Pseudoalteromonas dominated the changes of the microbial communities observed in the K.mikimotoi culture with or without treatments.Collectively,this study indicated that microbial community inhabiting K.mikimotoi culture includes potential algicidal bacteria,and improves our knowledge about microbial community succession during biocontrol of K.mikimotoi via nutrient stimulation or by adding isolated algicidal strains.
基金This work was financially supported by National Key Research and Development Program of China(No.2019YFA0705900)funded by MOSTthe Basic and Applied Basic Research Major Program of Guangdong Province(No.2019B030302007)+1 种基金the National Natural Science Foundation of China(No.U21A6002)Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials(No.2019B121205002).
文摘The stability of organic solar cells(OSCs)remains a major concern for their ultimate industrialization due to the photo,oxygen,and water susceptibility of organic photoactive materials.Usually,antioxidant additives are blended as radical scavengers into the active layer.However,it will induce the intrinsic morphology instability and adversely affect the efficiency and long-term stability.Herein,the antioxidant dibutylhydroxytoluene(BHT)group has been covalently linked onto the side chain of benzothiadiazole(BT)unit,and a series of ternary copolymers D18-Cl-BTBHTx(x=0,0.05,0.1,0.2)with varied ratio of BHT-containing side chains have been synthesized.It was found that the introduction of BHT side chains would have a negligible effect on the photophysical properties and electronic levels,and the D18-Cl-BTBHT0.05:Y6-based OSC achieved the highest power conversion efficiency(PCE)of 17.6%,which is higher than those based active layer blended with BHT additives.More importantly,the unencapsulated device based on D18-Cl-BTBHTx(x=0.05,0.1,0.2)retained approximately 50%of the initial PCE over 30 hours operation under ambient conditions,significantly outperforming the control device based on D18-Cl(90%degradation in PCE after 30 h).This work provides a new structural design strategy of copolymers for OSCs with simultaneously improved efficiency and stability.
基金supported by the National Key Research and Development Program of China(No.2024YFE0210200)the National Natural Science Foundation of China(Nos.22171288 and 22231305)+1 种基金the Natural Science Foundation of Shandong Province(No.ZR2024MB128)the Outstanding Youth Science Fund Projects of Shandong Province(No.ZR2022YQ15).
文摘Herein,we have designed the all-nanoporous composite(ANC)membranes with metal-organic framework(MOF)fillers and hydrogen-bonded organic framework(HOF)matrix,achieving high-permeance H_(2) purification.The hetero-MOF facilitates the heterogeneous nucleation,offsetting the need for a highly supersaturated solution to achieve sufficient nucleation density during solution processing.Continuous MOF/HOF ANC membranes are realized by suppressing the homogeneous nucleation,equilibrating the nucleation driving force with the molecular attachment rate,and balancing the nutrient supply and demand.The optimized copper 1,4-benzene dicarboxylate nanosheets(ns-CuBDC)/HOF-30-100(30 means that HOF monomer concentration is 30 mg·mL^(−1) and 100 represents that the temperature for solvent evaporation is 100℃)ANC membrane shows synchronously improved H_(2) permeance and H_(2)/CH4 selectivity by 562%and 241%compared to the pristine HOF membrane.The ns-CuBDC/HOF-30-100 ANC membrane inherits the pressure-responsive behavior from the parent HOF,exhibiting further improved H_(2) permeance up to 9842 gas permeation units(GPU)and slightly changed H_(2)/CH4 selectivity of 30.01 at 2.0 bar.The MOF/HOF ANC membrane manifests that incorporating a porous hetero-phase effectively upgrades the gas separation performance,and the HOF matrix circumvents the performance constraints of the traditional polymer matrix while preserving the solution-processability.
基金supported by the National Key Research and Development Program of China(2022YFD1300400)the National Natural Science Foundation of China(31930106 and 31829004)+3 种基金the Chinese Universities Scientific Fund(2022TC033)the 2115 Talent Development Program of China Agricultural University(1041-00109019)the Henan Province Public Benefit Research Foundation(201300111200-05)the 111 Project(B16044)。
文摘Maintainance of sulfomucin is a key end point in the treatment of diarrhea and inflammatory bowel disease(IBD).However,the mechanisms underlying the microbial sense to sulfomucin are poorly understood,and to date,there are no therapies targeting the secretion and maturation of sulfomucin in IBD.Herein,we biosynthesized poly-β-hydroxybutyrate(PHB)and found that PHB could alleviate inflammation caused by diarrhea and colitis by enhancing the differentiation of sulfomucin.Microbiota transplantation and clearance together demonstrate that PHB promoting sulfomucin is mediated by Lactobacillus johnsonii(L.johnsonii).Further studies revealed that PHB provides a favorable niche for L.johnsonii biofilm formation to resist disturbance and support its growth.L.johnsonii-biofilm alleviates colitis by regulating fucose residues to promote goblet cell differentiation and subsequent sulfomucin maturation.Importantly,PHB alleviates colitis by enhancing sulfomucin secretion and maturation in a L.johnsonii-dependent manner.PHB represents a class of guardians,acting as a safe probiotic-biofilm delivery system that significantly promotes probiotic proliferation.Altogether,this study adds weight to the possible role of probiotics and functional materials in the treatment of intestinal inflammation.The application of PHB and biofilm self-coating L.johnsonii carries high translational potential and may be of clinical relevance.
基金the National Natural Science Foundation of China(Nos.21772084 and 12034008)Fundamental Research Layout of Shenzhen(No.JCY20180504165657443)+3 种基金Guangdong Provincial Natural Science Foundation-Yueshen Joint Funding(Youth Project)(No.2019A1515110464)the Shenzhen Science and Technology Commission-free exploration/general project(No.JCYJ20190812151209348)Special fund for local science and technology development guided by central government is acknowledged.The support from Shanghai Rising Star Program(No.21QA1402600)the graduate fellowship(201808440345)from Chinese Scholarship Council are also acknowledged.
文摘The second near-infrared(NIR-II,1,000 to 1,700 nm)molecular fluorophores containing donor–acceptor–donor conjugated backbone have attracted substantial attention due to their outstanding advantages,such as stable emission and facilely tuned photophysical properties.However,it is still challenging for them to simultaneously achieve high brightness and red-shifted absorption and emission.Herein,furan is adopted as the D unit to construct NIR-II fluorophores,demonstrating red shift of absorption,enhanced absorption coefficient,and fluorescent quantum yield when compared with the generally used thiophene counterparts.The high brightness and desirable pharmacokinetics of the optimized fluorophore,IR-FFCHP,endows improved performance for angiography and tumor-targeting imaging.Furthermore,dual-NIR-II imaging of tumor and sentinel lymph nodes(LNs)has been achieved with IR-FFCHP and PbS/CdS quantum dots,enabling the in vivo imaging navigated LN surgery in tumor-bearing mice.This work demonstrates the potential of furan for constructing bright NIR-II fluorophores for biological imaging.
基金supported by the Science Foundation of Henan University of Technology(2021BS044)。
文摘Organic solar cells(OSCs) have drawn considerable attention in the last decade due to the great potential of light weight,flexibility, and low-cost solution processing. Particularly, Y-series non-fullerene acceptors(NFAs) including small molecular acceptors(SMAs) and polymerized small molecular acceptors(PSMAs) have become research hot spots due to their excellent power conversion efficiency. Side chain engineering is crucial to adjust the solubility and crystallinity of NFAs, which will significantly affect the morphology of active layers and the efficiency of OSCs. However, the understanding of side chain engineering on NFAs is still limited and lacks a systematic review. This review aims to provide a brief summary of the recent developments in side chain engineering of NFAs, with a special focus on the design and application of Y-series SMAs and PSMAs for high-efficiency non-fullerene organic solar cells(NF-OSCs). In addition, the review also points out challenges and provides useful guidance regarding side chain regulation for Y-series NFAs.
基金Y.L.acknowledges financial supports from the National Natural Science Foundation of China(No.21772084)Fundamental Research Layout of Shenzhen(No.JCY20180504165657443)+2 种基金H.S.thanks the National Natural Science Foundation of China(Nos.11727810,61720106009 and 21603074)the Science and Technology Commission of Shanghai Municipality(No.19JC1412200)for funding support and the ECNU Multifunctional Platform for Innovation(001)and HPC Research Computing Team for providing computational and storage resourcesX.Z thanks the funding supports from the National Natural Science Foundation of China(Nos.91859101,81971744,and U1932107).
文摘It is challenging to develop molecular fluorophores in the second near-infrared(NIR-Ⅱ)window with long wavelength emission and high brightness,which can improve the performance of biological imaging.Herein,we report a molecular engineering approach to afford NIR-Ⅱ fluorophores with these merits based on fused-ring acceptor(FRA)molecules.Dioctyl 3,4-propylenedioxy thiophene(PDOT-C8)is utilized as the bridging donor to replace 3-ethylhexyloxy thiophene(3-EHOT),leading to more than 20 times enhancement of brightness.The nanofluorophores(NFs)based on the optimized CPTIC-4F molecule exhibit an emission peak of 1,110 nm with a fluorescence quantum yield(QY)of 0.39%(QY of IR-26 is 0.050%in dichloroethane as reference)and peak absorption coefficient of 14.5 x 10^4 M^-1·cm^-1 in aqueous solutions,which are significantly higher than those of 3-EHOT based COTIC-4F NFs.It is found that PDOT-C8 can weaken intermolecular aggregation,enhance protection of molecular backbone from water,and decrease backbone distortion,beneficial for the high brightness.Compared with indocyanine green with same injection dose,CPTIC-4F NFs show 10 times higher signal-to-background ratio for whole body vessels imaging at 1,300 nm long pass filters.
基金supported by the National Natural Science Foundation of China(52433012)the National Key R&D Program of China(2024YFF1500300)the China Postdoctoral Science Foundation(2023M741201,2024T170286)。
文摘Conductive polymers have recently drawn tremendous attention due to their promising applications in electronic and energy-related devices.While p-type conductive polymers such as poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)have achieved commercialization,the development of stable,high-performance n-type polymers has lagged.Recently,the discovery of n-type polymer poly(benzodifurandione)(PBFDO)has greatly promoted the development and application of n-type conductive polymers.However,the synthesis process involves cumbersome post-processing,which greatly increases the cost and difficulty of mass production.Herein,a novel synthesis method for PBFDO has been developed,which was promoted by the combination of solvent dimethyl sulfoxide(DMSO)and acetic anhydride(Ac_(2)O).This method exploits the oxidative capability of DMSO,activated by Ac_(2)O,which can promote the keto-enol tautomerism of 3,7-dihydrobenzo[1,2-b:4,5-b′]difuran-2,6-dione(BFDO)and induce the rapid polymerization.The resulting PBFDO ink exhibits a high electronic conductivity of more than 2000 S cm^(-1)and excellent ambient stability.Significantly,the additives and by-products remain in a liquid state during the polymerization process and possess low boiling points,allowing for the production of pure PBFDO films through straightforward heating and drying.Furthermore,this approach holds considerable promise for in situ polymerization,as functional conductive films can be prepared by merely combining the monomers with the DMSO/Ac_(2)O mixture and applying heat.This efficient,purification-free strategy represents a significant step toward the industrial application of the highperformance n-type conductive polymer PBFDO.
