Pitch produced by the lique-faction of coal was divided into two frac-tions:soluble in toluene(TS)and insol-uble in toluene but soluble in pyridine(TI-PS),and their differences in molecu-lar structure and oxidation ac...Pitch produced by the lique-faction of coal was divided into two frac-tions:soluble in toluene(TS)and insol-uble in toluene but soluble in pyridine(TI-PS),and their differences in molecu-lar structure and oxidation activity were studied.Several different carbon materi-als were produced from them by oxida-tion in air(350℃,300 mL/min)fol-lowed by carbonization(1000℃ in Ar),and the effect of the cross-linked structure on their structure and sodium storage properties was investigated.The results showed that the two pitch fractions were obviously different after the air oxidation.The TS fraction with a low degree of condensation and abundant side chains had a stronger oxidation activity and thus introduced more cross-linked oxygen-containing functional groups C(O)―O which prevented carbon layer rearrangement during the carbonization.As a result,a disordered hard carbon with more defects was formed,which improved the electrochemical performance.Therefore,the carbon materials derived from TS(O-TS-1000)had an obvious disordered structure and a larger layer spacing,giving them better sodium storage perform-ance than those derived from the TI-PS fraction(O-TI-PS-1000).The specific capacity of O-TS-1000 was about 250 mAh/g at 20 mA/g,which was 1.67 times higher than that of O-TI-PS-1000(150 mAh/g).展开更多
The development of high-performance and cost-effective electrocatalysts towards oxygen reduction reaction(ORR) is of significant importance,but still challenging for the practical applications in related energy system...The development of high-performance and cost-effective electrocatalysts towards oxygen reduction reaction(ORR) is of significant importance,but still challenging for the practical applications in related energy systems.ORR process typically suffers from sluggish kinetics,the exploration of ORR electrocatalyst thus requires elaborate design.Herein,an effective strategy is developed for growing Co/N-doped carbon nanotube arrays on 2D MOFs-derived matrix via the pyrolysis of Co/Zn metalorganic-framework(MOF) nanosheets.The Co/Zn-MOF nanosheets serve as both the self-template for the 2D carbonized framework morphology and C/N source for the in-situ growth of 1D N-doped carbon nanotubes.The constructed hie rarchical architecture effectively integrates the OD/1D Co nanoparticle/Ndoped carbon nanotube interface and 1D(nanotubes)/2D(nanosheets) junction into frameworks with highly exposed active surface,enhanced mass-transport kinetics and electrical conductivity.As a result,the designed composite exhibits superior ORR activity and durability in alkaline media as compared to commercial Pt/C.Particularly,it shows promising ORR performance with a half-wave potential of 0.78 V versus reversible hydrogen electrode and negligible activity attenuation after 5000 potential cycles in acidic electrolyte.The designed strategy can be extended to construct other MOFs-derived carbon matrixes with diverse hierarchical structures and provide an efficient avenue for searching highperformance electrocatalysts.展开更多
we have synthesised a series of new optically nonlinear organic materials of cinnamylidene-acetophenone derivatives which have large nonl inear optical susceptibilities and short cut-off wavelengths.
A series of star-shaped molecules with benzene core and naphthalimides derivatives end groups have been designed to explore their optical,electronic,and charge transport properties as charge transport and/or luminesce...A series of star-shaped molecules with benzene core and naphthalimides derivatives end groups have been designed to explore their optical,electronic,and charge transport properties as charge transport and/or luminescent materials for organic light-emitting diodes（OLEDs）. The frontier molecular orbitals（FMOs） analysis has turned out that the vertical electronic transitions of absorption and emission are characterized as intramolecular charge transfer（ICT）. The calculated results show that the optical and electronic properties of star-shaped molecules are affected by the substituent groups in N-position of 1,8-naphthalimide ring. Our results suggest that star-shaped molecules with n-butyl（1）,benzene（2）,thiophene（3）,thiophene S？,S？-dioxide（4）,benzo[c][1,2,5]thiadiazole（5）,and 2,7a-dihydrobenzo[d]thiazole（6） fragments are expected to be promising candidates for luminescent and electron transport materials for OLEDs. This study should be helpful in further theoretical investigations on such kind of systems and also to the experimental study for charge transport and/or luminescent materials for OLEDs.展开更多
Objective:We aim to develop a dual-functional bone regeneration scaffold(Qx-D)with antibacterial and osteogenic properties for infected bone defect treatment.Impact Statement:This study provides insights into antibact...Objective:We aim to develop a dual-functional bone regeneration scaffold(Qx-D)with antibacterial and osteogenic properties for infected bone defect treatment.Impact Statement:This study provides insights into antibacterial components that could be combined with naturally derived materials through a facile Schiff base reaction,offering a potential strategy to enhance antibacterial properties.Introduction:Naturally derived decalcified bone matrix(DBM)has been reported to be porous and biodegradable.DBM can induce various cell differentiations and participate in immune regulation,making it an ideal bone regeneration scaffold for bone defects.However,DBM does not exhibit antimicrobial properties.Therefore,it is essential to develop antibacterial functionalization method for DBM.Methods:DBM was modified with a macromolecular quaternary ammonium salt(QPEI).A series of Qx-D with tunable feeding ratios were synthesized through Schiff base reaction.The morphology,chemical property,in vitro antibacterial efficiency,in vitro biocompatibility,osteogenic property,and in vivo anti-infection performances were characterized.Results:All Qx-D exhibited marked antibacterial properties.Small adjustments in feed concentration could not induce changes in antibacterial properties.However,cell viability slightly decreased with increasing feed concentration.Q10-D demonstrated significant antibacterial properties and could promote recovery of infected bone defect in an animal model.Conclusion:Qx-D shows marked antibacterial properties and good biocompatibility.Moreover,Q10-D could be a potential choice for infected bone defects.展开更多
For complicated geometries, it is ineflicient to integrate over the entire domain. A new approach for optimization is presented here, based on sensitivity analysis of local do- main and deformation of full domain. Acc...For complicated geometries, it is ineflicient to integrate over the entire domain. A new approach for optimization is presented here, based on sensitivity analysis of local do- main and deformation of full domain. Accurate results of design sensitivity analysis are ob- tained with this approach in shape optimization. This method is shown to be efficient when used in optimization programs and results in less distortion of the mesh.展开更多
This review provides a recompilation of the most important and recent strategies employed to increase the efficiency of metal-organic framework(MOF)-based systems toward the photocatalytic hydrogen evolution(PHE)react...This review provides a recompilation of the most important and recent strategies employed to increase the efficiency of metal-organic framework(MOF)-based systems toward the photocatalytic hydrogen evolution(PHE)reaction through specific strategies:tailoring the photocatalytic activity of bare MOFs and vip@MOF composites,formation of heterojunctions based on MOFs and various photocatalysts,and inorganic photocatalysts derived from MOFs.According to the data reported in this mini-review,the most effective strategy to improve the PHE of MOFs relies on modifying the linkers with new secondary building units(SBUs).Although several reviews have investigated the photocatalytic activity of MOFs from a general point of view,many of these studies relate this activity to the physicochemical and catalytic properties of MOFs.However,they did not consider the interactions between the components of the photocatalytic material.This study highlights the effects of strength of the supramolecular interactions on the photocatalytic performance of bare and MOF-based materials during PHE.A thorough review and comparison of the results established that metal-nanoparticle@MOF composites have weak van der Waals forces between components,whereas heterostructures only interact with MOFs at the surface of bare materials.Regarding material derivatives from MOFs,we found that pyrolysis destroyed some beneficial properties of MOFs for PHE.Thus,we conclude that adding SBUs to organic linkers is the most efficient strategy to perform the PHE because the SBUs added to the MOFs promote synergy between the two materials through strong coordination bonds.展开更多
In this paper we present some results concerning the optimal shape design problem governed by the fourth-order variational inequalities. The problem can be considered as a model example for the design of the shapes fo...In this paper we present some results concerning the optimal shape design problem governed by the fourth-order variational inequalities. The problem can be considered as a model example for the design of the shapes for elastic-plastic problem. The computations are done by finite element method, and the performance criterion is minimized by the material derivative method. We also discuss the error estimates in the appropriate norm and present some numerical results. An example is used to clearly illustrate the essential elements of shape design problems.展开更多
文摘Pitch produced by the lique-faction of coal was divided into two frac-tions:soluble in toluene(TS)and insol-uble in toluene but soluble in pyridine(TI-PS),and their differences in molecu-lar structure and oxidation activity were studied.Several different carbon materi-als were produced from them by oxida-tion in air(350℃,300 mL/min)fol-lowed by carbonization(1000℃ in Ar),and the effect of the cross-linked structure on their structure and sodium storage properties was investigated.The results showed that the two pitch fractions were obviously different after the air oxidation.The TS fraction with a low degree of condensation and abundant side chains had a stronger oxidation activity and thus introduced more cross-linked oxygen-containing functional groups C(O)―O which prevented carbon layer rearrangement during the carbonization.As a result,a disordered hard carbon with more defects was formed,which improved the electrochemical performance.Therefore,the carbon materials derived from TS(O-TS-1000)had an obvious disordered structure and a larger layer spacing,giving them better sodium storage perform-ance than those derived from the TI-PS fraction(O-TI-PS-1000).The specific capacity of O-TS-1000 was about 250 mAh/g at 20 mA/g,which was 1.67 times higher than that of O-TI-PS-1000(150 mAh/g).
基金supported by the National Natural Science Foundation of China (NSFC,Nos.21701124 and 51702236)Tianjin Municipal Science and Technology Commission (Nos. 18TCQNJC71500 and 17JCZDJC38000)the National Key R&D Program of China (No.2017YFA0700104)。
文摘The development of high-performance and cost-effective electrocatalysts towards oxygen reduction reaction(ORR) is of significant importance,but still challenging for the practical applications in related energy systems.ORR process typically suffers from sluggish kinetics,the exploration of ORR electrocatalyst thus requires elaborate design.Herein,an effective strategy is developed for growing Co/N-doped carbon nanotube arrays on 2D MOFs-derived matrix via the pyrolysis of Co/Zn metalorganic-framework(MOF) nanosheets.The Co/Zn-MOF nanosheets serve as both the self-template for the 2D carbonized framework morphology and C/N source for the in-situ growth of 1D N-doped carbon nanotubes.The constructed hie rarchical architecture effectively integrates the OD/1D Co nanoparticle/Ndoped carbon nanotube interface and 1D(nanotubes)/2D(nanosheets) junction into frameworks with highly exposed active surface,enhanced mass-transport kinetics and electrical conductivity.As a result,the designed composite exhibits superior ORR activity and durability in alkaline media as compared to commercial Pt/C.Particularly,it shows promising ORR performance with a half-wave potential of 0.78 V versus reversible hydrogen electrode and negligible activity attenuation after 5000 potential cycles in acidic electrolyte.The designed strategy can be extended to construct other MOFs-derived carbon matrixes with diverse hierarchical structures and provide an efficient avenue for searching highperformance electrocatalysts.
文摘we have synthesised a series of new optically nonlinear organic materials of cinnamylidene-acetophenone derivatives which have large nonl inear optical susceptibilities and short cut-off wavelengths.
基金Support by the National Natural Science Foundation of China(No.21563002)the Natural Science Foundation of Inner Mongolia Autonomous Region(No.2015MS0201)the Research Program of Sciences at Universities of Inner Mongolia Autonomous Region(No.NJZZ235)
文摘A series of star-shaped molecules with benzene core and naphthalimides derivatives end groups have been designed to explore their optical,electronic,and charge transport properties as charge transport and/or luminescent materials for organic light-emitting diodes（OLEDs）. The frontier molecular orbitals（FMOs） analysis has turned out that the vertical electronic transitions of absorption and emission are characterized as intramolecular charge transfer（ICT）. The calculated results show that the optical and electronic properties of star-shaped molecules are affected by the substituent groups in N-position of 1,8-naphthalimide ring. Our results suggest that star-shaped molecules with n-butyl（1）,benzene（2）,thiophene（3）,thiophene S？,S？-dioxide（4）,benzo[c][1,2,5]thiadiazole（5）,and 2,7a-dihydrobenzo[d]thiazole（6） fragments are expected to be promising candidates for luminescent and electron transport materials for OLEDs. This study should be helpful in further theoretical investigations on such kind of systems and also to the experimental study for charge transport and/or luminescent materials for OLEDs.
基金supported by the National Natural Science Foundation of China(grant nos.52122304,52293382,52221006,and 52073024)the Beijing Municipal Administration of Hospitals Incubating Program(grant no.PX2021005).
文摘Objective:We aim to develop a dual-functional bone regeneration scaffold(Qx-D)with antibacterial and osteogenic properties for infected bone defect treatment.Impact Statement:This study provides insights into antibacterial components that could be combined with naturally derived materials through a facile Schiff base reaction,offering a potential strategy to enhance antibacterial properties.Introduction:Naturally derived decalcified bone matrix(DBM)has been reported to be porous and biodegradable.DBM can induce various cell differentiations and participate in immune regulation,making it an ideal bone regeneration scaffold for bone defects.However,DBM does not exhibit antimicrobial properties.Therefore,it is essential to develop antibacterial functionalization method for DBM.Methods:DBM was modified with a macromolecular quaternary ammonium salt(QPEI).A series of Qx-D with tunable feeding ratios were synthesized through Schiff base reaction.The morphology,chemical property,in vitro antibacterial efficiency,in vitro biocompatibility,osteogenic property,and in vivo anti-infection performances were characterized.Results:All Qx-D exhibited marked antibacterial properties.Small adjustments in feed concentration could not induce changes in antibacterial properties.However,cell viability slightly decreased with increasing feed concentration.Q10-D demonstrated significant antibacterial properties and could promote recovery of infected bone defect in an animal model.Conclusion:Qx-D shows marked antibacterial properties and good biocompatibility.Moreover,Q10-D could be a potential choice for infected bone defects.
文摘For complicated geometries, it is ineflicient to integrate over the entire domain. A new approach for optimization is presented here, based on sensitivity analysis of local do- main and deformation of full domain. Accurate results of design sensitivity analysis are ob- tained with this approach in shape optimization. This method is shown to be efficient when used in optimization programs and results in less distortion of the mesh.
基金supported by CONACYT through the following projects:Cátedras CONACYT-ID7708,CONACYT-FC-1725Luis.A.Alfonso-Herrera thanks CONACYT for the M.C.scholarship 844207UANL also supported this research through projects PAICYT CE1352-20 and PAICYT 601-CE-2022.
文摘This review provides a recompilation of the most important and recent strategies employed to increase the efficiency of metal-organic framework(MOF)-based systems toward the photocatalytic hydrogen evolution(PHE)reaction through specific strategies:tailoring the photocatalytic activity of bare MOFs and vip@MOF composites,formation of heterojunctions based on MOFs and various photocatalysts,and inorganic photocatalysts derived from MOFs.According to the data reported in this mini-review,the most effective strategy to improve the PHE of MOFs relies on modifying the linkers with new secondary building units(SBUs).Although several reviews have investigated the photocatalytic activity of MOFs from a general point of view,many of these studies relate this activity to the physicochemical and catalytic properties of MOFs.However,they did not consider the interactions between the components of the photocatalytic material.This study highlights the effects of strength of the supramolecular interactions on the photocatalytic performance of bare and MOF-based materials during PHE.A thorough review and comparison of the results established that metal-nanoparticle@MOF composites have weak van der Waals forces between components,whereas heterostructures only interact with MOFs at the surface of bare materials.Regarding material derivatives from MOFs,we found that pyrolysis destroyed some beneficial properties of MOFs for PHE.Thus,we conclude that adding SBUs to organic linkers is the most efficient strategy to perform the PHE because the SBUs added to the MOFs promote synergy between the two materials through strong coordination bonds.
文摘In this paper we present some results concerning the optimal shape design problem governed by the fourth-order variational inequalities. The problem can be considered as a model example for the design of the shapes for elastic-plastic problem. The computations are done by finite element method, and the performance criterion is minimized by the material derivative method. We also discuss the error estimates in the appropriate norm and present some numerical results. An example is used to clearly illustrate the essential elements of shape design problems.
