Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this...Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this issue with a double benefit.Herein,the amino-functionalized lotus root-like carbon nanofibers(NH_(2)-PLCNFs)are prepared by the amination of electrospinning carbon nanofibers under dielectric barrier discharge plasma.Selective catalytic oxidation of H_(2)S to elemental sulfur(S)is achieved over the metalfree NH_(2)-PLCNFs catalyst,and the obtained composite S@NH_(2)-PLCNFs is further used as cathode in LSBs.NH_(2)-PLCNFs enable efficient desulfurization(removal capacity as high as 3.46 g H_(2)S g^(−1) catalyst)and strongly covalent stabilization of S on modified carbon nanofibers.LSBs equipped with S@NH_(2)-PLCNFs deliver a high specific capacity of 705.8 mA h g^(−1) at 1 C after 1000 cycles based on the spatial confinement and the covalent stabilization of electroactive materials on amino-functionalized porous carbon matrix.It is revealed that S@NH_(2)-PLCNFs obtained by this kind of chemical vapor deposition leads to a more homogeneous S distribution and superior electrochemical performance to the sample S/NH_(2)-PLCNF-M prepared by the traditional molten infusion.This work opens a new avenue for the combination of environment protection and energy storage.展开更多
Developing host materials with high specific surface area, good electron conductivity, and fast ion transportation channel is critical for high performance lithium-selenium(Li-Se) batteries. Herein, a series of three ...Developing host materials with high specific surface area, good electron conductivity, and fast ion transportation channel is critical for high performance lithium-selenium(Li-Se) batteries. Herein, a series of three dimensional ordered hierarchically porous carbon(3D OHPC) materials with micro/meso/macropores are designed and synthesized for Li-Se battery. The porous structure is tuned by following the concept of the generalized Murray’s law to facilitate the mass diffusion and reduce ion transport resistance.The optimized 3D Se/OHPC cathode exhibits a very high 2 nd discharge capacity of 651 m Ah/g and retains 361 m Ah/g after 200 cycles at 0.2 C. Even at a high current rate of 5 C, the battery still shows a discharge capacity as high as 155 m Ah/g. The improved electrochemical performance is attributed to the synergy effect of the interconnected and well-designed micro, meso and macroporosity while shortened ions diffusion pathways of such Murray materials accelerate its ionic and electronic conductivities leading to the enhanced electrochemical reaction. The diffusivity coefficient in Se/OHPC can reach a very high value of 1.3 × 10^(-11)cm^(2)/s, much higher than those in single pore size carbon hosts. Their effective volume expansion accommodation capability and reduced dissolution of polyselenides ensure the high stability of the battery. This work, for the first time, established the clear relationship between textural properties of cathode materials and their performance and demonstrates that the concept of the generalized Murray’s law can be used as efficient guidance for the rational design and synthesis of advanced hierarchically porous materials and the great potential of 3D OHPC materials as a practical high performance cathode material for Li-Se batteries.展开更多
Foam glass is a kind of green building material that is widely used because of its excellent thermal insulation and mechanical properties.In this study,the borosilicate foam glass was fabricated by powder sintering me...Foam glass is a kind of green building material that is widely used because of its excellent thermal insulation and mechanical properties.In this study,the borosilicate foam glass was fabricated by powder sintering method using recycled soda lime waste glass,quartz,and borax as the primary raw materials.CaCO_(3)was used as a foaming agent and Na_(2)CO_(3)as a flux agent.Results showed that as the quartz content decreases from 30 to 17.5 wt.%and borax content increases from 5 to 17.5 wt.%,the pore size,porosity,and thermal insulation of borosilicate foam glass increase significantly,while the compressive strength decreases slightly.When the content of quartz and borax are both 17.5 wt.%,borosilicate foam glass with outstanding performance can be prepared,whose pore distribution is uniform,mean pore size is 1.93 mm,total porosity is 83.44%,thermal conductivity is 0.0711W/(m⋅K),and compressive strength is 2.37 MPa.Finally,the influences of foaming agent content,flux agent content,foaming temperature,and holding time on the pore structure and various properties of borosilicate foam glass were investigated by orthogonal test.According to the results,the foaming temperature has a significant effect,and appropriate foaming agent content,flux agent content,and holding time help to form a uniform pore structure,thereby improving the thermal insulation and mechanical strength of the borosilicate foam glass.展开更多
In combination with the augmented reality (AR) technology and Hololens device, an electric power work assist system is developed to provide a more realistic and convenient training experience for electric power traini...In combination with the augmented reality (AR) technology and Hololens device, an electric power work assist system is developed to provide a more realistic and convenient training experience for electric power training. The training effect was improved, and help guidance information was provided in the actual operation of electric power work. Experimental results show that difficulty of electric power work is reduced and the efficiency of actual work is improved.展开更多
Great interests have arisen over the last decade in the development of hierarchically porous materials. The hierarchical structure enables materials to have maximum structural functions owing to enhanced accessibility...Great interests have arisen over the last decade in the development of hierarchically porous materials. The hierarchical structure enables materials to have maximum structural functions owing to enhanced accessibility and mass transport properties, leading to improved perfor- mances in various applications. Hierarchical porous materials are in high demand for applications in catalysis, adsorption, separation, energy and biochemistry. In the present review, recent advances in synthesis routes to hierarchically porous materials are reviewed together with their catalytic contributions.展开更多
Hierarchical single-crystal ZSM-5 zeolites with different Si/Al ratios(Hier-ZSM-5-x,where x=50,100,150 and 200)were synthesized using an ordered mesoporous carbon-silica composite as hard template.Hier-ZSM-5-x exhibit...Hierarchical single-crystal ZSM-5 zeolites with different Si/Al ratios(Hier-ZSM-5-x,where x=50,100,150 and 200)were synthesized using an ordered mesoporous carbon-silica composite as hard template.Hier-ZSM-5-x exhibits improved mass transport properties,excellent mechanical and hydrothermal stability,and higher catalytic activity than commercial bulk zeolites in the benzyl alcohol self-etherification reaction.Results show that a decrease in the Si/Al ratio in hierarchical single-crystal ZSM-5 zeolites leads to a significant increase in the acidity and the density of micropores,which increases the final catalytic conversion.The effect of porous hierarchy on the diffusion of active sites and the final catalytic activity was also studied by comparing the catalytic conversion after selectively designed poisoned acid sites.These poisoned Hier-ZSM-5-x shows much higher catalytic conversion than the poisoned commercial ZSM-5 zeolite,which indicates that the numerous intracrystalline mesopores significantly reduce the diffusion path of the reactant,leading to the faster diffusion inside the zeolite to contact with the acid sites in the micropores predominating in ZSM-5 zeolites.This study can be extended to develop a series of hierarchical single-crystal zeolites with expected catalytic performance.展开更多
1Introduction and main contributions In the field of social networks and knowledge graphs,semi-supervised learning models based on graph convolutional networks have achieved great success in node classification[1],ind...1Introduction and main contributions In the field of social networks and knowledge graphs,semi-supervised learning models based on graph convolutional networks have achieved great success in node classification[1],inductive node embedding[2],link prediction[3],and recommend.These semi-supervised models based on graph convolutional network(GCN)[4]expect to obtain more feature information of a graph or accelerate the training.展开更多
Both cholinergic dysfunction and protein citrullination are the hallmarks of rheumatoid arthritis(RA),but the relationship between the two phenomena remains unclear.We explored whether and how cholinergic dysfunction ...Both cholinergic dysfunction and protein citrullination are the hallmarks of rheumatoid arthritis(RA),but the relationship between the two phenomena remains unclear.We explored whether and how cholinergic dysfunction accelerates protein citrullination and consequently drives the development of RA.Cholinergic function and protein citrullination levels in patients with RA and collageninduced arthritis(CIA)mice were collected.In both neuron-macrophage coculture system and CIA mice,the effect of cholinergic dysfunction on protein citrullination and expression of peptidylarginine deiminases(PADs)was assessed by immunofluorescence.The key transcription factors for PAD4 expression were predicted and validated.Cholinergic dysfunction in the patients with RA and CIA mice negatively correlated with the degree of protein citrullination in synovial tissues.The cholinergic or alpha7 nicotinic acetylcholine receptor(a7nAChR)deactivation and activation resulted in the promotion and reduction of protein citrullination in vitro and in vivo,respectively.Especially,the activation deficiency of a7nAChR induced the earlier onset and aggravation of CIA.Furthermore,deactivation of a7nAChR increased the expression of PAD4 and specificity protein-3(SP3)in vitro and in vivo.Our results suggest that cholinergic dysfunction-induced deficient a7nAChR activation,which induces the expression of SP3 and its downstream molecule PAD4,accelerating protein citrullination and the development of RA.展开更多
Thioredoxin reductase 1(TrxR1)is over activity in tumor cell to maintain their redox balance.Although gold clusters have great potential in antitumor drug as they could well inhibit TrxR1,the molecular mechanism has n...Thioredoxin reductase 1(TrxR1)is over activity in tumor cell to maintain their redox balance.Although gold clusters have great potential in antitumor drug as they could well inhibit TrxR1,the molecular mechanism has not been disclosed yet.In this work,we revealed gold clusters can well inhibit the activity of TrxR1 in lung tumor cells and further disclosed the inhibition mechanism by using computational simulation methods.We firstly inferred the binding sites of gold in the hydrophobic cavities on TrxR1.The simulation results show that the gold ion(released from Au cluster)interact with–SH of Cys189 in TrxR1,this greatly increase the distance between the C-terminal redox center of TrxR1 and the Trx redox center,thereby destroy the electron transfer pathway between them.Our electron transfer destroying mechanism is different from the previous hypothesis that gold binds to the Sec498 of TrxR1 which has never been proved by experimental and theory studies.This work provides a new understanding of the gold clusters to inhibit TrxR1 activity.展开更多
Herein,we describe an iron-catalyzed borylation and silylation of unactivated alkyl chlorides,delivering the tertiary,secondary,and primary alkylboronic esters,and secondary,primary alkylsilanes with high efficiency.T...Herein,we describe an iron-catalyzed borylation and silylation of unactivated alkyl chlorides,delivering the tertiary,secondary,and primary alkylboronic esters,and secondary,primary alkylsilanes with high efficiency.This protocol exhibits broad substrate scope and good functional group compatibility,allowing the efficient late-stage borylation of biorelevant compounds,thus offering an excellent platform in drug discovery and development.Preliminary mechanistic studies suggest that an alkyl radical was involved in this catalytic system.展开更多
基金financial support from projects funded by the National Natural Science Foundation of China(22179017,52172038).
文摘Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this issue with a double benefit.Herein,the amino-functionalized lotus root-like carbon nanofibers(NH_(2)-PLCNFs)are prepared by the amination of electrospinning carbon nanofibers under dielectric barrier discharge plasma.Selective catalytic oxidation of H_(2)S to elemental sulfur(S)is achieved over the metalfree NH_(2)-PLCNFs catalyst,and the obtained composite S@NH_(2)-PLCNFs is further used as cathode in LSBs.NH_(2)-PLCNFs enable efficient desulfurization(removal capacity as high as 3.46 g H_(2)S g^(−1) catalyst)and strongly covalent stabilization of S on modified carbon nanofibers.LSBs equipped with S@NH_(2)-PLCNFs deliver a high specific capacity of 705.8 mA h g^(−1) at 1 C after 1000 cycles based on the spatial confinement and the covalent stabilization of electroactive materials on amino-functionalized porous carbon matrix.It is revealed that S@NH_(2)-PLCNFs obtained by this kind of chemical vapor deposition leads to a more homogeneous S distribution and superior electrochemical performance to the sample S/NH_(2)-PLCNF-M prepared by the traditional molten infusion.This work opens a new avenue for the combination of environment protection and energy storage.
基金financial support from the China Scholarship Council (CSC) and a scholarship from the Laboratory of Inorganic Materials Chemistry,Universitéde Namur,Belgiumfinancially supported by the National Postdoctoral Program (Grant No. 2020M672782)+2 种基金the National Natural Science Foundation of China (Grant No. U1663225)the the Program of Introducing Talents of Discipline to Universities-National 111 Project from the Ministry of Science and Technology and the Ministry of Education of China (Grant No. B20002)the National Key R&D Program of China (Grant No. 2016YFA0202602)。
文摘Developing host materials with high specific surface area, good electron conductivity, and fast ion transportation channel is critical for high performance lithium-selenium(Li-Se) batteries. Herein, a series of three dimensional ordered hierarchically porous carbon(3D OHPC) materials with micro/meso/macropores are designed and synthesized for Li-Se battery. The porous structure is tuned by following the concept of the generalized Murray’s law to facilitate the mass diffusion and reduce ion transport resistance.The optimized 3D Se/OHPC cathode exhibits a very high 2 nd discharge capacity of 651 m Ah/g and retains 361 m Ah/g after 200 cycles at 0.2 C. Even at a high current rate of 5 C, the battery still shows a discharge capacity as high as 155 m Ah/g. The improved electrochemical performance is attributed to the synergy effect of the interconnected and well-designed micro, meso and macroporosity while shortened ions diffusion pathways of such Murray materials accelerate its ionic and electronic conductivities leading to the enhanced electrochemical reaction. The diffusivity coefficient in Se/OHPC can reach a very high value of 1.3 × 10^(-11)cm^(2)/s, much higher than those in single pore size carbon hosts. Their effective volume expansion accommodation capability and reduced dissolution of polyselenides ensure the high stability of the battery. This work, for the first time, established the clear relationship between textural properties of cathode materials and their performance and demonstrates that the concept of the generalized Murray’s law can be used as efficient guidance for the rational design and synthesis of advanced hierarchically porous materials and the great potential of 3D OHPC materials as a practical high performance cathode material for Li-Se batteries.
基金This work was supported by the Shanghai Municipal Natural Science Foundation,China(Granted No.[19ZR1418500]).
文摘Foam glass is a kind of green building material that is widely used because of its excellent thermal insulation and mechanical properties.In this study,the borosilicate foam glass was fabricated by powder sintering method using recycled soda lime waste glass,quartz,and borax as the primary raw materials.CaCO_(3)was used as a foaming agent and Na_(2)CO_(3)as a flux agent.Results showed that as the quartz content decreases from 30 to 17.5 wt.%and borax content increases from 5 to 17.5 wt.%,the pore size,porosity,and thermal insulation of borosilicate foam glass increase significantly,while the compressive strength decreases slightly.When the content of quartz and borax are both 17.5 wt.%,borosilicate foam glass with outstanding performance can be prepared,whose pore distribution is uniform,mean pore size is 1.93 mm,total porosity is 83.44%,thermal conductivity is 0.0711W/(m⋅K),and compressive strength is 2.37 MPa.Finally,the influences of foaming agent content,flux agent content,foaming temperature,and holding time on the pore structure and various properties of borosilicate foam glass were investigated by orthogonal test.According to the results,the foaming temperature has a significant effect,and appropriate foaming agent content,flux agent content,and holding time help to form a uniform pore structure,thereby improving the thermal insulation and mechanical strength of the borosilicate foam glass.
文摘In combination with the augmented reality (AR) technology and Hololens device, an electric power work assist system is developed to provide a more realistic and convenient training experience for electric power training. The training effect was improved, and help guidance information was provided in the actual operation of electric power work. Experimental results show that difficulty of electric power work is reduced and the efficiency of actual work is improved.
基金Acknowledgements This work was carried out in the framework of a program for Changjiang Scholars and Innovative Research Team (IRT_I 5R52) of the Chinese Ministry of Education. B. L. Su acknowledges the Chinese Central Government for an "Expert of the State" position in the Program of the "Thousand Talents", the Chinese Ministry of Education for a "Changjiang Chaire Professor' position and a Clare Hall Life Membership at the Clare Hall College and the financial support of the Department of Chemistry, University of Cambridge. L.H. Chen acknowledges Hubei Provincial Department of Education for the "Chutian Scholar" program. This work was also financially supported by NFSC-21301133, NFSC- 51472190, ISTC-2015DFE52870, SRF for ROCS SEM ([20151311), Hubei Provincial Natural Science Foundation (2015CFB428, 2014CFB160).
文摘Great interests have arisen over the last decade in the development of hierarchically porous materials. The hierarchical structure enables materials to have maximum structural functions owing to enhanced accessibility and mass transport properties, leading to improved perfor- mances in various applications. Hierarchical porous materials are in high demand for applications in catalysis, adsorption, separation, energy and biochemistry. In the present review, recent advances in synthesis routes to hierarchically porous materials are reviewed together with their catalytic contributions.
基金This work was also financially supported by the National Natural Science Foundation of China(Grant Nos.21671155,U1663225,21805216,21902122)Major programs of technical innovation in Hubei(No.2018AAA012)+1 种基金Hubei Provincial Natural Science Foundation(No.2018CFA054)Postdoctoral Science Foundation of China(No.2019M652723)。
文摘Hierarchical single-crystal ZSM-5 zeolites with different Si/Al ratios(Hier-ZSM-5-x,where x=50,100,150 and 200)were synthesized using an ordered mesoporous carbon-silica composite as hard template.Hier-ZSM-5-x exhibits improved mass transport properties,excellent mechanical and hydrothermal stability,and higher catalytic activity than commercial bulk zeolites in the benzyl alcohol self-etherification reaction.Results show that a decrease in the Si/Al ratio in hierarchical single-crystal ZSM-5 zeolites leads to a significant increase in the acidity and the density of micropores,which increases the final catalytic conversion.The effect of porous hierarchy on the diffusion of active sites and the final catalytic activity was also studied by comparing the catalytic conversion after selectively designed poisoned acid sites.These poisoned Hier-ZSM-5-x shows much higher catalytic conversion than the poisoned commercial ZSM-5 zeolite,which indicates that the numerous intracrystalline mesopores significantly reduce the diffusion path of the reactant,leading to the faster diffusion inside the zeolite to contact with the acid sites in the micropores predominating in ZSM-5 zeolites.This study can be extended to develop a series of hierarchical single-crystal zeolites with expected catalytic performance.
基金the National Natural Science Foundation of China(Grant Nos.61272209,61872164)in part by the Program of Science and Technology Development Plan of Jilin Province of China(20190302032GX)in part by the Fundamental Research Funds for the Central Universities(Jilin University).
文摘1Introduction and main contributions In the field of social networks and knowledge graphs,semi-supervised learning models based on graph convolutional networks have achieved great success in node classification[1],inductive node embedding[2],link prediction[3],and recommend.These semi-supervised models based on graph convolutional network(GCN)[4]expect to obtain more feature information of a graph or accelerate the training.
基金supported by the“Double First-Class”University Project(CPU2022QZ31,China)。
文摘Both cholinergic dysfunction and protein citrullination are the hallmarks of rheumatoid arthritis(RA),but the relationship between the two phenomena remains unclear.We explored whether and how cholinergic dysfunction accelerates protein citrullination and consequently drives the development of RA.Cholinergic function and protein citrullination levels in patients with RA and collageninduced arthritis(CIA)mice were collected.In both neuron-macrophage coculture system and CIA mice,the effect of cholinergic dysfunction on protein citrullination and expression of peptidylarginine deiminases(PADs)was assessed by immunofluorescence.The key transcription factors for PAD4 expression were predicted and validated.Cholinergic dysfunction in the patients with RA and CIA mice negatively correlated with the degree of protein citrullination in synovial tissues.The cholinergic or alpha7 nicotinic acetylcholine receptor(a7nAChR)deactivation and activation resulted in the promotion and reduction of protein citrullination in vitro and in vivo,respectively.Especially,the activation deficiency of a7nAChR induced the earlier onset and aggravation of CIA.Furthermore,deactivation of a7nAChR increased the expression of PAD4 and specificity protein-3(SP3)in vitro and in vivo.Our results suggest that cholinergic dysfunction-induced deficient a7nAChR activation,which induces the expression of SP3 and its downstream molecule PAD4,accelerating protein citrullination and the development of RA.
基金financially supported by the National Science Foundation of China(Nos.21727817,U2067214,11621505,31971311)the National Key Basic Research Program of China(No.2020YFA0710700)。
文摘Thioredoxin reductase 1(TrxR1)is over activity in tumor cell to maintain their redox balance.Although gold clusters have great potential in antitumor drug as they could well inhibit TrxR1,the molecular mechanism has not been disclosed yet.In this work,we revealed gold clusters can well inhibit the activity of TrxR1 in lung tumor cells and further disclosed the inhibition mechanism by using computational simulation methods.We firstly inferred the binding sites of gold in the hydrophobic cavities on TrxR1.The simulation results show that the gold ion(released from Au cluster)interact with–SH of Cys189 in TrxR1,this greatly increase the distance between the C-terminal redox center of TrxR1 and the Trx redox center,thereby destroy the electron transfer pathway between them.Our electron transfer destroying mechanism is different from the previous hypothesis that gold binds to the Sec498 of TrxR1 which has never been proved by experimental and theory studies.This work provides a new understanding of the gold clusters to inhibit TrxR1 activity.
基金support from the National Natural Science Foundation of China(no.21801029)the Fundamental Research Funds for the Central Universities(no.2020CDJQY-A043)+4 种基金the Sichuan Key Laboratory of Medical Imaging(North Sichuan Medical College,no.SKLMI201901)the Strategic Cooperation of Science and Technology between Nanchong City and North Sichuan Medical College(nos.19SXHZ0441 and 19SXHZ0227)the Chongqing Postdoctoral Science Foundation(no.cstc2020jcyj-bsh0061)the China Postdoctoral Science Foundation(no.2020M673121)the Natural Science Foundation of Chongqing(no.cstc2019jcyj-msxmX0048).
文摘Herein,we describe an iron-catalyzed borylation and silylation of unactivated alkyl chlorides,delivering the tertiary,secondary,and primary alkylboronic esters,and secondary,primary alkylsilanes with high efficiency.This protocol exhibits broad substrate scope and good functional group compatibility,allowing the efficient late-stage borylation of biorelevant compounds,thus offering an excellent platform in drug discovery and development.Preliminary mechanistic studies suggest that an alkyl radical was involved in this catalytic system.