Hierarchical SAPO‐34 crystals were synthesized by a facile acid etching post‐treatment. Butterfly‐shaped porous patterns on four side faces and hierarchical pores composed of micropores,mesopores and macropores wer...Hierarchical SAPO‐34 crystals were synthesized by a facile acid etching post‐treatment. Butterfly‐shaped porous patterns on four side faces and hierarchical pores composed of micropores,mesopores and macropores were formed after a nitric acid or oxalic acid treatment. The catalyticperformance of the hierarchical SAPO‐34 for the methanol to olefins (MTO) process showed that thesynergistic effect of the hierarchical pores and acid sites resulted in a longer catalyst lifetime (from210 to 390 min for the acid treated SAPO‐34) and higher selectivity to light olefins of 92%–94%.The ethylene selectivity can be adjusted between 37.4% and 51.5% by the pore size. No hierarchical SAPO‐34 was obtained after a treatment with butanedioic acid, and with this sample, fast deactivation was detected after 100 min.展开更多
Spinal cord injury(SCI)causes motor,sensory,and autonomic dysfunctions.The gut microbiome has an important role in SCI,while short-chain fatty acids(SCFAs)are one of the main bioactive mediators of microbiota.In the p...Spinal cord injury(SCI)causes motor,sensory,and autonomic dysfunctions.The gut microbiome has an important role in SCI,while short-chain fatty acids(SCFAs)are one of the main bioactive mediators of microbiota.In the present study,we explored the effects of oral administration of exogenous SCFAs on the recovery of locomotor function and tissue repair in SCI.Allen’s method was utilized to establish an SCI model in Sprague-Dawley(SD)rats.The animals received water containing a mixture of 150 mmol/L SCFAs after SCI.After 21 d of treatment,the Basso,Beattie,and Bresnahan(BBB)score increased,the regularity index improved,and the base of support(BOS)value declined.Spinal cord tissue inflammatory infiltration was alleviated,the spinal cord necrosis cavity was reduced,and the numbers of motor neurons and Nissl bodies were elevated.Enzyme-linked immunosorbent assay(ELISA),real-time quantitative polymerase chain reaction(qPCR),and immunohistochemistry assay revealed that the expression of interleukin(IL)-10 increased and that of IL-17 decreased in the spinal cord.SCFAs promoted gut homeostasis,induced intestinal T cells to shift toward an anti-inflammatory phenotype,and promoted regulatory T(Treg)cells to secrete IL-10,affecting Treg cells and IL-17^(+)γδT cells in the spinal cord.Furthermore,we observed that Treg cells migrated from the gut to the spinal cord region after SCI.The above findings confirm that SCFAs can regulate Treg cells in the gut and affect the balance of Treg and IL-17^(+)γδT cells in the spinal cord,which inhibits the inflammatory response and promotes the motor function in SCI rats.Our findings suggest that there is a relationship among gut,spinal cord,and immune cells,and the“gut-spinal cord-immune”axis may be one of the mechanisms regulating neural repair after SCI.展开更多
Background:Osteoporosis(OP)has become a major public health issue,threatening the bone health of middle-aged and elderly people from all around the world.Changes in the gut microbiota(GM)are correlated with the mainte...Background:Osteoporosis(OP)has become a major public health issue,threatening the bone health of middle-aged and elderly people from all around the world.Changes in the gut microbiota(GM)are correlated with the maintenance of bone mass and bone quality.However,research results in this field remain highly controversial,and no systematic review or meta-analysis of the relationship between GM and OP has been conducted.This paper addresses this shortcoming,focusing on the difference in the GM abundance between OP patients and healthy controls based on previous 16S ribosomal RNA(rRNA)gene sequencing results,in order to provide new clinical reference information for future customized prevention and treatment options of OP.Methods:According to the Preferred Reporting Items for Systematic Reviews and Meta-Analyses(PRISMA),we comprehensively searched the databases of Pub Med,Web of Science,Embase,Cochrane Library,and China National Knowledge Infrastructure(CNKI).In addition,we applied the R programming language version 4.0.3 and Stata 15.1 software for data analysis.We also implemented the Newcastle-Ottawa Scale(NOS),funnel plot analysis,sensitivity analysis,Egger’s test,and Begg’s test to assess the risk of bias.Results:This research ultimately considered 12 studies,which included the fecal GM data of 2033 people(604 with OP and 1429 healthy controls).In the included research papers,it was observed that the relative abundance of Lactobacillus and Ruminococcus increased in the OP group,while the relative abundance for Bacteroides of Bacteroidetes increased(except for Ireland).Meanwhile,Firmicutes,Blautia,Alistipes,Megamonas,and Anaerostipes showed reduced relative abundance in Chinese studies.In the linear discriminant analysis Effect Size(LEfSe)analysis,certain bacteria showed statistically significant results consistently across different studies.Conclusions:This observational meta-analysis revealed that changes in the GM were correlated with OP,and variations in some advantageous GM might involve regional differences.展开更多
Metal-organic frameworks and covalent organic frameworks have been widely employed in electrochemical catalysis owing to their designable skeletons,controllable porosities,and well-defined catalytic centers.However,th...Metal-organic frameworks and covalent organic frameworks have been widely employed in electrochemical catalysis owing to their designable skeletons,controllable porosities,and well-defined catalytic centers.However,the poor chemical stability and low electron conductivity limited their activity,and single-functional sites in these frameworks hindered them to show multifunctional roles in catalytic systems.Herein,we have constructed novel metal organic polymers(Co-HAT-CN and Ni-HAT-CN)with dual catalytic centers(metal-N_(4) and metal-N_(2))to catalyze oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).By using different metal centers,the catalytic activity and selectivity were well-tuned.Among them,Co-HAT-CN catalyzed the ORR in a 4e^(-)pathway,with a half-wave potential of 0.8 V versus RHE,while the Ni-HAT-CN catalyze ORR in a 2e^(-)pathway with H_(2)O_(2) selectivity over 90%.Moreover,the Co-HAT-CN delivered an overpotential of 350 mV at 10 mA cm^(-2) with a corresponding Tafel slope of 24 mV dec^(-1) for OER in a 1.0 M KOH aqueous solution.The experimental results revealed that the activities toward ORR were due to the M-N_(4) sites in the frameworks,and both M-N_(4) and M-N_(2) sites contributed to the OER.This work gives us a new platform to construct bifunctional catalysts.展开更多
The on-board methanol steam reforming(MSR) has long been considered as an effective approach to insitu produce hydrogen for fuel cell vehicles(FCVs). However, the conventional MSR catalyst pellets suffer from easy bre...The on-board methanol steam reforming(MSR) has long been considered as an effective approach to insitu produce hydrogen for fuel cell vehicles(FCVs). However, the conventional MSR catalyst pellets suffer from easy breakage during the vehicle movement, leading to increased pressure drop and reduced system stability. Herein, we introduce an integrated method to prepare the highly controlled structured catalysts based on coupled processes: direct prototyping the structured substrate using digital light processing(DLP) 3D printing technology, in-situ dynamic crystallization of active components assisted by magnetic resonance imaging(MRI) and calcination. The synthesized catalyst owns a gradient layer of active component, and exhibits better MSR performance, higher mechanical strength, reduced pressure drop, higher Cu dispersion and better adhesion of active compounds when compared with the conventional powder and pellet catalysts. The demonstrated successful application proves the feasibility of developed method,which has great potential to be used for preparing precisely other monolithic catalysts with customized structures.展开更多
The electrochemical carbon dioxide reduction reaction(CO_(2)RR)for highvalue-added products is a promising strategy to tackle excessive CO_(2) emissions.However,the activity of and selectivity for catalysts for CO_(2)...The electrochemical carbon dioxide reduction reaction(CO_(2)RR)for highvalue-added products is a promising strategy to tackle excessive CO_(2) emissions.However,the activity of and selectivity for catalysts for CO_(2)RR still need to be improved because of the competing reaction(hydrogen evolution reaction).In this study,for the first time,we have demonstrated dual atomic catalytic sites for CO_(2)RR from a core-shell hybrid of the covalent-organic framework and the metal-organic framework.Due to abundant dual atomic sites(with CoN_(4)O and ZnN_(4) of 2.47 and 11.05 wt.%,respectively)on hollow carbon,the catalyst promoted catalysis of CO_(2)RR,with the highest Faradic efficiency for CO of 92.6%at-0.8 V and a turnover frequency value of 1370.24 h^(-1) at-1.0 V.More importantly,the activity and selectivity of the catalyst were well retained for 30 h.The theoretical calculation further revealed that CoN_(4)O was the main site for CO_(2)RR,and the activity of and selectivity for Zn sites were also improved because of the synergetic roles.展开更多
Developing an effective and mechanically durable biomimetic membrane for the separation of highly emulsified aqueous oil is significant but challenging owing to its low water flux and serious membrane fouling.In this ...Developing an effective and mechanically durable biomimetic membrane for the separation of highly emulsified aqueous oil is significant but challenging owing to its low water flux and serious membrane fouling.In this work,a biomimetic membrane with superhydrophobicity and superoleophilicity was rationally developed via co-electrospinning of polysulfonamide/polyacrylonitrile(PSA/PAN)emulsion solution,followed by decorating of a-Fe2 O_(3) nanowire onto the membrane surface to create membrane roughness,and grafting of 1 H,1 H,2 H,2 H-perfluorododecyltrichlorosilane(FTCS)to lower membrane surface free energy.Benefiting from the nanowire-wrapped rough membrane structure and the low surface free energy FTCS,the resultant membrane showed superhydrophobicity with a high water contact angle(WCA)of 156°,superoleophilicity with a low oil contact angle(OCA)of 0°,which can separate the highly emulsified aqueous oil with an ultrahigh permeation flux over 7000 L m2 h-1 and high separation efficiency of about 99%.Significantly,the biomimetic membrane also displayed robust stability for long-te rm separation owing to its adva ntage of antifouling property,showing great potential applications in large-scale aqueous oil treatment.展开更多
“我们能人工合成一个细胞吗?Can a cell be artificially synthesized?”——这是2021年《科学》期刊新发布的世界最前沿的125个重大科学问题之一。科学家为了揭示“生命起源”的奥秘以及解决世界关注的重大基础科学问题,设计出人造细...“我们能人工合成一个细胞吗?Can a cell be artificially synthesized?”——这是2021年《科学》期刊新发布的世界最前沿的125个重大科学问题之一。科学家为了揭示“生命起源”的奥秘以及解决世界关注的重大基础科学问题,设计出人造细胞这类仿生材料。它们最明显的特点就是具有与生物细胞类似的结构与功能。因此,深入研究人造细胞,不仅有利于研究真实细胞的结构与功能机制,还有助于建立非生物物质与真实细胞之间的联系,从而搭建非生命系统与生命系统之间的桥梁,为生命起源等相关研究提供实验与理论依据。而磷脂囊泡作为目前应用最为广泛的人造细胞更是有着广阔的应用前景。为了使“磷脂囊泡”这类材料以及相关研究技术得到更广泛的认识,本文基于耳熟能详的四大名著之一——《西游记》,讲述了孙悟空凭借火眼金睛帮助磷脂囊泡战胜癌细胞的故事,介绍了磷脂囊泡的设计和制备、代表功能以及体内治疗案例,以期促进广大读者对该技术的理解,并激发更多该技术潜在的应用可能。展开更多
Objective:To investigate the effects and mechanisms of Polygonatum sibiricum polysaccharide(PSP)on osteogenic differentiation of bone marrow mesenchymal stem cells(BMSCs).Methods:The mouse BMSCs were cultured and indu...Objective:To investigate the effects and mechanisms of Polygonatum sibiricum polysaccharide(PSP)on osteogenic differentiation of bone marrow mesenchymal stem cells(BMSCs).Methods:The mouse BMSCs were cultured and induced in osteoblast medium(OBM)containing finalconcentrations(0 mg/L,12.5 mg/L,25 mg/L,and 50 mg/L)of PSP.The proliferation and cytotoxicity of BMSCs were detected by MTT assay.Alkaline phosphatase(ALP)and Alizarin red S staining were performed after 7 days' ossification-inducing culture.The mRNA expressions of ALP,Runx2 and osteocalcin(OCN)were determined by fluorescence quantitative PCR(qPCR).The mRNA and protein expressions of Tafazzin(TAZ)(a key effector of Hippo pathway)were measured by qPCR and western blotting,respectively.Results:PSP was non-cytotoxicwithin the dose range of 12.5-50 mg/L and had no impact on the proliferation of BMSCs.The activity of ALP,the intensity of ALP staining,and the formation of mineralized nodules were increased by PSP treatment(25 and50 mg/L)(P<0.01).Moreover,administration of 25 mg/L PSP significantly enhanced the mRNA levels of osteoblastic differentiation makers ALP,Runx2 and OCN as well as the mRNA and protein expressions of TAZ(P<0.01).Conclusion:PSP could promote osteogenic differentiation of BMSCs,and the mechanisms might be related to the activation of TAZ in the Hippo signaling pathway.展开更多
Comprehensive Summary The construction of luminescent two-dimensional(2D)imine-linked covalent organic frameworks(COFs)is a formidable challenge due to the strong interlayer stacking and bond rotations that typically ...Comprehensive Summary The construction of luminescent two-dimensional(2D)imine-linked covalent organic frameworks(COFs)is a formidable challenge due to the strong interlayer stacking and bond rotations that typically suppress intramolecular charge transfer(ICT),leading to nonradiative energy dissipation.Herein,three COFs with tailored interlayer distances and bond rotations are designed to modulate the ICT behaviours.The targeted COF(TPAZ-TPE-COF)achieved a significantly enhanced photoluminescence quantum yield(PLQY)of 21.22%in the solid state by restricting bond rotation and enlarging the layer distance.This represents a 3.5-fold and 530.5-fold improvement over TPAZ-PYTA-COF(6.15%),which has a shortened interlayer space,and TPAZ-PATA-COF(0.04%),which exhibits strong bond rotations,respectively.Importantly,TPAZ-TPE-COF also exhibits exceptional sensing performance for iron ions,with a detection limit at the ppb level.Both experimental and theoretical analyses reveal that the prominent luminescent performance of TPAZ-TPE-COF is assigned to the effective suppression of nonradiative pathways,especially those arising from interlayer stacking and bond vibrations.These findings pave the way for deliberate construction of imine-linked 2D COFs with high PL intensity,thereby expanding the portfolio of luminescent COFs with potential applications in sensing and optoelectronics.展开更多
Covalent organic frameworks(COFs)have been developed as the precursors to construct porous carbons for electrocatalytic systems.However,the influences of carbon dimensions on the catalytic performance are still undere...Covalent organic frameworks(COFs)have been developed as the precursors to construct porous carbons for electrocatalytic systems.However,the influences of carbon dimensions on the catalytic performance are still underexplored.In this work,we have first constructed COF-derived carbons by template-synthesis strategy in different dimensions to catalyze the carbon dioxide reduction(CO_(2)RR).By using different templates,the one-dimensional(1D),two-dimensional(2D),and three-dimensional(3D)COF-derived carbons have been employed to anchor Co-porphyrin to form the Co-N5 sites to catalyze CO_(2)RR.The 1D catalyst templated by carbon nano tubes presents high binding ability of CO_(2),more defective sites,and higher electronic conductivity,resulting in a higher catalytic activity for CO_(2)and selectivity of CO than 2D and 3D carbon-based catalysts.The 1D catalyst delivers the turnover frequency values of 1150 h^(−1)and the FECO of 94.5%at 0.7 V versus RHE,which is significantly better than those of 2D and 3D carbon-based catalysts.展开更多
Ion conduction plays key roles in electrochemical systems,including fuel cells,lithium ion batteries,and metal-air batteries.Covalent organic frameworks(COFs),as a new class of porous polymers,constructed by pre-desig...Ion conduction plays key roles in electrochemical systems,including fuel cells,lithium ion batteries,and metal-air batteries.Covalent organic frameworks(COFs),as a new class of porous polymers,constructed by pre-designable building blocks,are ideal hosts to accommodate ionic carries for conduction because of their straightforward pore channels,tunable pore size,controllable pore environment,and good chemical and thermal stability.Different from proton conduction,how to achieve high lithium ion conduction is still a challenge as it is difficult to dissociate ionic bonds of the lithium salts.To facilitate the dissociation of lithium salts,COFs with different pores and skeletons are well designed and constructed.This review focuses on emerging developments of lithium ion conduction in COFs,and discusses the structures of these COFs and conductive performance to elucidate the structure-property correlations.Furthermore,we have concluded the remaining challenge and future direction in these COF-based lithium conductive areas.This review provides deeper insight into COFs for ionic conduction.展开更多
Photo‐/electro‐catalysis has the characteristics of low cost,high perfor-mance,and zero pollution,which meet the policies on environment and energy.Covalent organic frameworks(COFs),a type of crystalline organic ske...Photo‐/electro‐catalysis has the characteristics of low cost,high perfor-mance,and zero pollution,which meet the policies on environment and energy.Covalent organic frameworks(COFs),a type of crystalline organic skeleton polymers,have been widely applied and investigated in the area of photo‐/electro‐catalysis owing to their advantages of large specific surface area,regular pore size,excellent stability,flexible structural design,and massive active sites.This article reviews the structural characteristics of COFs and the strategies for strengthening the photo‐/electro‐catalytic activity of COF materials.Subsequently,deep insights were put into the photo‐/electro‐catalysis application of COF materials.In the end,the development prospects and challenges faced by COF materials in photo‐/electro‐catalysis are discussed.展开更多
基金supported by the National Natural Science Foundation of China (21403279, 21507141, 21506243)the Science and Technology Commission of Shanghai Municipality (14DZ1207602, 14DZ1203700)~~
文摘Hierarchical SAPO‐34 crystals were synthesized by a facile acid etching post‐treatment. Butterfly‐shaped porous patterns on four side faces and hierarchical pores composed of micropores,mesopores and macropores were formed after a nitric acid or oxalic acid treatment. The catalyticperformance of the hierarchical SAPO‐34 for the methanol to olefins (MTO) process showed that thesynergistic effect of the hierarchical pores and acid sites resulted in a longer catalyst lifetime (from210 to 390 min for the acid treated SAPO‐34) and higher selectivity to light olefins of 92%–94%.The ethylene selectivity can be adjusted between 37.4% and 51.5% by the pore size. No hierarchical SAPO‐34 was obtained after a treatment with butanedioic acid, and with this sample, fast deactivation was detected after 100 min.
基金National Natural Science Foundation of China(No.82060399)Guangxi Medical High-level Key Talents Training“139”Program Training Project(No.[2020]15),China.
文摘Spinal cord injury(SCI)causes motor,sensory,and autonomic dysfunctions.The gut microbiome has an important role in SCI,while short-chain fatty acids(SCFAs)are one of the main bioactive mediators of microbiota.In the present study,we explored the effects of oral administration of exogenous SCFAs on the recovery of locomotor function and tissue repair in SCI.Allen’s method was utilized to establish an SCI model in Sprague-Dawley(SD)rats.The animals received water containing a mixture of 150 mmol/L SCFAs after SCI.After 21 d of treatment,the Basso,Beattie,and Bresnahan(BBB)score increased,the regularity index improved,and the base of support(BOS)value declined.Spinal cord tissue inflammatory infiltration was alleviated,the spinal cord necrosis cavity was reduced,and the numbers of motor neurons and Nissl bodies were elevated.Enzyme-linked immunosorbent assay(ELISA),real-time quantitative polymerase chain reaction(qPCR),and immunohistochemistry assay revealed that the expression of interleukin(IL)-10 increased and that of IL-17 decreased in the spinal cord.SCFAs promoted gut homeostasis,induced intestinal T cells to shift toward an anti-inflammatory phenotype,and promoted regulatory T(Treg)cells to secrete IL-10,affecting Treg cells and IL-17^(+)γδT cells in the spinal cord.Furthermore,we observed that Treg cells migrated from the gut to the spinal cord region after SCI.The above findings confirm that SCFAs can regulate Treg cells in the gut and affect the balance of Treg and IL-17^(+)γδT cells in the spinal cord,which inhibits the inflammatory response and promotes the motor function in SCI rats.Our findings suggest that there is a relationship among gut,spinal cord,and immune cells,and the“gut-spinal cord-immune”axis may be one of the mechanisms regulating neural repair after SCI.
基金supported by the National Natural Science Foundation of China(No.81860391)the Guangxi Medical High-level Backbone Talents Training“139”Program Training Project(No.[2020]15)the Guangxi Hundred Thousand Talents Project(No.[2019]32),China.
文摘Background:Osteoporosis(OP)has become a major public health issue,threatening the bone health of middle-aged and elderly people from all around the world.Changes in the gut microbiota(GM)are correlated with the maintenance of bone mass and bone quality.However,research results in this field remain highly controversial,and no systematic review or meta-analysis of the relationship between GM and OP has been conducted.This paper addresses this shortcoming,focusing on the difference in the GM abundance between OP patients and healthy controls based on previous 16S ribosomal RNA(rRNA)gene sequencing results,in order to provide new clinical reference information for future customized prevention and treatment options of OP.Methods:According to the Preferred Reporting Items for Systematic Reviews and Meta-Analyses(PRISMA),we comprehensively searched the databases of Pub Med,Web of Science,Embase,Cochrane Library,and China National Knowledge Infrastructure(CNKI).In addition,we applied the R programming language version 4.0.3 and Stata 15.1 software for data analysis.We also implemented the Newcastle-Ottawa Scale(NOS),funnel plot analysis,sensitivity analysis,Egger’s test,and Begg’s test to assess the risk of bias.Results:This research ultimately considered 12 studies,which included the fecal GM data of 2033 people(604 with OP and 1429 healthy controls).In the included research papers,it was observed that the relative abundance of Lactobacillus and Ruminococcus increased in the OP group,while the relative abundance for Bacteroides of Bacteroidetes increased(except for Ireland).Meanwhile,Firmicutes,Blautia,Alistipes,Megamonas,and Anaerostipes showed reduced relative abundance in Chinese studies.In the linear discriminant analysis Effect Size(LEfSe)analysis,certain bacteria showed statistically significant results consistently across different studies.Conclusions:This observational meta-analysis revealed that changes in the GM were correlated with OP,and variations in some advantageous GM might involve regional differences.
基金support from the Natural Science Foundation of Shanghai (20ZR1464000)G.Zeng acknowledges the support from the National Natural Science Foundation of China (21878322,22075309)the Science and Technology Commission of Shanghai Municipality (19ZR1479200,22ZR1470100)。
文摘Metal-organic frameworks and covalent organic frameworks have been widely employed in electrochemical catalysis owing to their designable skeletons,controllable porosities,and well-defined catalytic centers.However,the poor chemical stability and low electron conductivity limited their activity,and single-functional sites in these frameworks hindered them to show multifunctional roles in catalytic systems.Herein,we have constructed novel metal organic polymers(Co-HAT-CN and Ni-HAT-CN)with dual catalytic centers(metal-N_(4) and metal-N_(2))to catalyze oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).By using different metal centers,the catalytic activity and selectivity were well-tuned.Among them,Co-HAT-CN catalyzed the ORR in a 4e^(-)pathway,with a half-wave potential of 0.8 V versus RHE,while the Ni-HAT-CN catalyze ORR in a 2e^(-)pathway with H_(2)O_(2) selectivity over 90%.Moreover,the Co-HAT-CN delivered an overpotential of 350 mV at 10 mA cm^(-2) with a corresponding Tafel slope of 24 mV dec^(-1) for OER in a 1.0 M KOH aqueous solution.The experimental results revealed that the activities toward ORR were due to the M-N_(4) sites in the frameworks,and both M-N_(4) and M-N_(2) sites contributed to the OER.This work gives us a new platform to construct bifunctional catalysts.
基金supported by the Youth Innovation Promotion Association of Chinese Academy of Sciencesthe Key Technical Personnel of Chinese Academy of Sciences+1 种基金the STS Program of Chinese Academy of Sciences (No. KFJJ-STS-SCYD-302)the National Natural Science Foundation of China (22108288)。
文摘The on-board methanol steam reforming(MSR) has long been considered as an effective approach to insitu produce hydrogen for fuel cell vehicles(FCVs). However, the conventional MSR catalyst pellets suffer from easy breakage during the vehicle movement, leading to increased pressure drop and reduced system stability. Herein, we introduce an integrated method to prepare the highly controlled structured catalysts based on coupled processes: direct prototyping the structured substrate using digital light processing(DLP) 3D printing technology, in-situ dynamic crystallization of active components assisted by magnetic resonance imaging(MRI) and calcination. The synthesized catalyst owns a gradient layer of active component, and exhibits better MSR performance, higher mechanical strength, reduced pressure drop, higher Cu dispersion and better adhesion of active compounds when compared with the conventional powder and pellet catalysts. The demonstrated successful application proves the feasibility of developed method,which has great potential to be used for preparing precisely other monolithic catalysts with customized structures.
基金Q.Xu acknowledges financial support from the Natural Science Foundation of Shanghai(20ZR1464000)G.Zeng is grateful for the support from the National Natural Science Foundation of China(21878322,22075309)the Science and Technology Commission of Shanghai(19ZR1479200).The authors also thank the Shanghai Synchrotron Radiation Facility for XAFS measurements at Beamline BL14w1.
文摘The electrochemical carbon dioxide reduction reaction(CO_(2)RR)for highvalue-added products is a promising strategy to tackle excessive CO_(2) emissions.However,the activity of and selectivity for catalysts for CO_(2)RR still need to be improved because of the competing reaction(hydrogen evolution reaction).In this study,for the first time,we have demonstrated dual atomic catalytic sites for CO_(2)RR from a core-shell hybrid of the covalent-organic framework and the metal-organic framework.Due to abundant dual atomic sites(with CoN_(4)O and ZnN_(4) of 2.47 and 11.05 wt.%,respectively)on hollow carbon,the catalyst promoted catalysis of CO_(2)RR,with the highest Faradic efficiency for CO of 92.6%at-0.8 V and a turnover frequency value of 1370.24 h^(-1) at-1.0 V.More importantly,the activity and selectivity of the catalyst were well retained for 30 h.The theoretical calculation further revealed that CoN_(4)O was the main site for CO_(2)RR,and the activity of and selectivity for Zn sites were also improved because of the synergetic roles.
基金the National Natural Science Foundation of China(No.51873047)the Fundamental Research Funds for the Central Unive rsities(No.30919011266)+1 种基金the Key Laboratory of Low-Carbon Conversion Science&Engineering,Shanghai Advanced Research Institute,Chinese Academy of Sciences(No.KLLCCSE-201906)the Open Founds for LargeScale Instruments and Equipment of Nanjing University of Science and Technology。
文摘Developing an effective and mechanically durable biomimetic membrane for the separation of highly emulsified aqueous oil is significant but challenging owing to its low water flux and serious membrane fouling.In this work,a biomimetic membrane with superhydrophobicity and superoleophilicity was rationally developed via co-electrospinning of polysulfonamide/polyacrylonitrile(PSA/PAN)emulsion solution,followed by decorating of a-Fe2 O_(3) nanowire onto the membrane surface to create membrane roughness,and grafting of 1 H,1 H,2 H,2 H-perfluorododecyltrichlorosilane(FTCS)to lower membrane surface free energy.Benefiting from the nanowire-wrapped rough membrane structure and the low surface free energy FTCS,the resultant membrane showed superhydrophobicity with a high water contact angle(WCA)of 156°,superoleophilicity with a low oil contact angle(OCA)of 0°,which can separate the highly emulsified aqueous oil with an ultrahigh permeation flux over 7000 L m2 h-1 and high separation efficiency of about 99%.Significantly,the biomimetic membrane also displayed robust stability for long-te rm separation owing to its adva ntage of antifouling property,showing great potential applications in large-scale aqueous oil treatment.
文摘“我们能人工合成一个细胞吗?Can a cell be artificially synthesized?”——这是2021年《科学》期刊新发布的世界最前沿的125个重大科学问题之一。科学家为了揭示“生命起源”的奥秘以及解决世界关注的重大基础科学问题,设计出人造细胞这类仿生材料。它们最明显的特点就是具有与生物细胞类似的结构与功能。因此,深入研究人造细胞,不仅有利于研究真实细胞的结构与功能机制,还有助于建立非生物物质与真实细胞之间的联系,从而搭建非生命系统与生命系统之间的桥梁,为生命起源等相关研究提供实验与理论依据。而磷脂囊泡作为目前应用最为广泛的人造细胞更是有着广阔的应用前景。为了使“磷脂囊泡”这类材料以及相关研究技术得到更广泛的认识,本文基于耳熟能详的四大名著之一——《西游记》,讲述了孙悟空凭借火眼金睛帮助磷脂囊泡战胜癌细胞的故事,介绍了磷脂囊泡的设计和制备、代表功能以及体内治疗案例,以期促进广大读者对该技术的理解,并激发更多该技术潜在的应用可能。
基金supported by grants from National Natural Science Foundation of China(No.81360279)Guangxi Natural Science Foundation(No.2015GXNSFAA139150)
文摘Objective:To investigate the effects and mechanisms of Polygonatum sibiricum polysaccharide(PSP)on osteogenic differentiation of bone marrow mesenchymal stem cells(BMSCs).Methods:The mouse BMSCs were cultured and induced in osteoblast medium(OBM)containing finalconcentrations(0 mg/L,12.5 mg/L,25 mg/L,and 50 mg/L)of PSP.The proliferation and cytotoxicity of BMSCs were detected by MTT assay.Alkaline phosphatase(ALP)and Alizarin red S staining were performed after 7 days' ossification-inducing culture.The mRNA expressions of ALP,Runx2 and osteocalcin(OCN)were determined by fluorescence quantitative PCR(qPCR).The mRNA and protein expressions of Tafazzin(TAZ)(a key effector of Hippo pathway)were measured by qPCR and western blotting,respectively.Results:PSP was non-cytotoxicwithin the dose range of 12.5-50 mg/L and had no impact on the proliferation of BMSCs.The activity of ALP,the intensity of ALP staining,and the formation of mineralized nodules were increased by PSP treatment(25 and50 mg/L)(P<0.01).Moreover,administration of 25 mg/L PSP significantly enhanced the mRNA levels of osteoblastic differentiation makers ALP,Runx2 and OCN as well as the mRNA and protein expressions of TAZ(P<0.01).Conclusion:PSP could promote osteogenic differentiation of BMSCs,and the mechanisms might be related to the activation of TAZ in the Hippo signaling pathway.
基金the National Natural Science Foundation of China(52303288,22075309,22378413,22161132010)National Key R&D Program of China Ministry of Science and Technology(2024YFE0206900)+4 种基金Science and Technology Innovation Plan of the Science and Technology Commission of Shanghai Municipality(22ZR1470100,23DZ1202600,23DZ1201804)the Youth Innovation Promotion Association of Chinese Academy of Sciences(E324441401)Biomaterials and Regenerative Medicine Institute Cooperative Research Project Shanghai Jiao Tong University School of Medicine(2022LHA09)Dr.Y.Fu gratefully acknowledge the GWK support for funding this project by providing computing time through the Center for Information Services and HPC(ZIH)at TU DresdenDr.S.Bi thanks the financial support by a fellowship award from the Research Grants Council of the Hong Kong Special Administrative Region,China(Project No.CityU PDFS2324-1S08).
文摘Comprehensive Summary The construction of luminescent two-dimensional(2D)imine-linked covalent organic frameworks(COFs)is a formidable challenge due to the strong interlayer stacking and bond rotations that typically suppress intramolecular charge transfer(ICT),leading to nonradiative energy dissipation.Herein,three COFs with tailored interlayer distances and bond rotations are designed to modulate the ICT behaviours.The targeted COF(TPAZ-TPE-COF)achieved a significantly enhanced photoluminescence quantum yield(PLQY)of 21.22%in the solid state by restricting bond rotation and enlarging the layer distance.This represents a 3.5-fold and 530.5-fold improvement over TPAZ-PYTA-COF(6.15%),which has a shortened interlayer space,and TPAZ-PATA-COF(0.04%),which exhibits strong bond rotations,respectively.Importantly,TPAZ-TPE-COF also exhibits exceptional sensing performance for iron ions,with a detection limit at the ppb level.Both experimental and theoretical analyses reveal that the prominent luminescent performance of TPAZ-TPE-COF is assigned to the effective suppression of nonradiative pathways,especially those arising from interlayer stacking and bond vibrations.These findings pave the way for deliberate construction of imine-linked 2D COFs with high PL intensity,thereby expanding the portfolio of luminescent COFs with potential applications in sensing and optoelectronics.
基金National Natural Science Foundation of China,Grant/Award Numbers:52303288,21878322,22075309,22378413Youth Innovation Promotion Association of Chinese Academy of Sciences and Biomaterials and Regenerative Medicine Institute Cooperative Research Project Shanghai Jiao Tong University School of Medicine,Grant/Award Number:2022LHA09。
文摘Covalent organic frameworks(COFs)have been developed as the precursors to construct porous carbons for electrocatalytic systems.However,the influences of carbon dimensions on the catalytic performance are still underexplored.In this work,we have first constructed COF-derived carbons by template-synthesis strategy in different dimensions to catalyze the carbon dioxide reduction(CO_(2)RR).By using different templates,the one-dimensional(1D),two-dimensional(2D),and three-dimensional(3D)COF-derived carbons have been employed to anchor Co-porphyrin to form the Co-N5 sites to catalyze CO_(2)RR.The 1D catalyst templated by carbon nano tubes presents high binding ability of CO_(2),more defective sites,and higher electronic conductivity,resulting in a higher catalytic activity for CO_(2)and selectivity of CO than 2D and 3D carbon-based catalysts.The 1D catalyst delivers the turnover frequency values of 1150 h^(−1)and the FECO of 94.5%at 0.7 V versus RHE,which is significantly better than those of 2D and 3D carbon-based catalysts.
基金financial support from the Natural Science Foundation of Shanghai(20ZR1464000)supports from the National Natural Science Foundation of China(21878322,22075309)the Science and Technology Commission of Shanghai Municipality(19ZR1479200,22ZR1470100)。
文摘Ion conduction plays key roles in electrochemical systems,including fuel cells,lithium ion batteries,and metal-air batteries.Covalent organic frameworks(COFs),as a new class of porous polymers,constructed by pre-designable building blocks,are ideal hosts to accommodate ionic carries for conduction because of their straightforward pore channels,tunable pore size,controllable pore environment,and good chemical and thermal stability.Different from proton conduction,how to achieve high lithium ion conduction is still a challenge as it is difficult to dissociate ionic bonds of the lithium salts.To facilitate the dissociation of lithium salts,COFs with different pores and skeletons are well designed and constructed.This review focuses on emerging developments of lithium ion conduction in COFs,and discusses the structures of these COFs and conductive performance to elucidate the structure-property correlations.Furthermore,we have concluded the remaining challenge and future direction in these COF-based lithium conductive areas.This review provides deeper insight into COFs for ionic conduction.
基金National Natural Science Foundation of China,Grant/Award Numbers:21878322,22075309,22378413,52303288Youth Innovation Promotion Association of the Chinese Academy of Sciences+1 种基金Science and Technology Commission of Shanghai Municipality,Grant/Award Numbers:22ZR1470100,23DZ1202600,23DZ1201804Shanghai Jiao Tong University School of Medicine,Grant/Award Number:2022LHA09。
文摘Photo‐/electro‐catalysis has the characteristics of low cost,high perfor-mance,and zero pollution,which meet the policies on environment and energy.Covalent organic frameworks(COFs),a type of crystalline organic skeleton polymers,have been widely applied and investigated in the area of photo‐/electro‐catalysis owing to their advantages of large specific surface area,regular pore size,excellent stability,flexible structural design,and massive active sites.This article reviews the structural characteristics of COFs and the strategies for strengthening the photo‐/electro‐catalytic activity of COF materials.Subsequently,deep insights were put into the photo‐/electro‐catalysis application of COF materials.In the end,the development prospects and challenges faced by COF materials in photo‐/electro‐catalysis are discussed.
