Sodium-ion hybrid capacitor(SIHC)is one of the most promising alternatives for large-scale energy storage due to its high energy and power densities,natural abundance,and low cost.However,overcoming the imbalance betw...Sodium-ion hybrid capacitor(SIHC)is one of the most promising alternatives for large-scale energy storage due to its high energy and power densities,natural abundance,and low cost.However,overcoming the imbalance between slow Na^(+)reaction kinetics of battery-type anodes and rapid ion adsorption/desorption of capacitive cathodes is a significant challenge.Here,we propose the high-rate-performance NiS_(2)@OMGC anode material composed of monodispersed NiS_(2) nanocrystals(8.8±1.7 nm in size)and N,S-co-doped graphenic carbon(GC).The NiS_(2)@OMGC material has a three-dimensionally ordered macroporous(3DOM)morphology,and numerous NiS_(2) nanocrystals are uniformly embedded in GC,forming a core-shell structure in the local area.Ultrafine NiS_(2) nanocrystals and their nano-microstructure demonstrate high pseudocapacitive Na-storage capability and thus excellent rate performance(355.7 mAh/g at 20.0 A/g).A SIHC device fabricated using NiS_(2)@OMGC and commercial activated carbon(AC)cathode exhibits ultrahigh energy densities(197.4 Wh/kg at 398.8 W/kg)and power densities(43.9 kW/kg at 41.3 Wh/kg),together with a long life span.This outcome exemplifies the rational architecture and composition design of this type of anode material.This strategy can be extended to the design and synthesis of a wide range of high-performance electrode materials for energy storage applications.展开更多
Since their seminal discovery in 2011,two-dimensional(2D)transition metal carbides/nitrides known as MXenes,that constitute a large family of 2D materials,have been targeted toward various applications due to their ou...Since their seminal discovery in 2011,two-dimensional(2D)transition metal carbides/nitrides known as MXenes,that constitute a large family of 2D materials,have been targeted toward various applications due to their outstanding electronic properties.MXenes functioning as co-catalyst in combination with certain photocatalysts have been applied in photocatalytic systems to enhance photogenerated charge separation,suppress rapid charge recombination,and convert solar energy into chemical energy or use it in the degradation of organic compounds.The photocatalytic performance greatly depends on the composition and morphology of the photocatalyst,which,in turn,are determined by the method of preparation used.Here,we review the four different synthesis methods(mechanical mixing,self-assembly,in situ decoration,and oxidation)reported for MXenes in view of their application as co-catalyst in photocatalysis.In addition,the working mechanism for MXenes application in photocatalysis is discussed and an outlook for future research is also provided.展开更多
Zoonoses account for the majority of emerging infectious diseases and pose a serious threat to human and animal health.Under global warming and climate change,zoonoses are significantly affected by influencing hosts,v...Zoonoses account for the majority of emerging infectious diseases and pose a serious threat to human and animal health.Under global warming and climate change,zoonoses are significantly affected by influencing hosts,vectors,and pathogen dynamics as well as their in-teractions.Traditional zoonoses surveillance relies on molecular or serological diagnostic methods to monitor pathogens from animal or patient samples,which may miss the early warning signs of pathogens spillover from the environment.Nowadays,new technologies such as remote sensing,environment-based screening,multi-omics,and big data science facilitate comprehensive active surveillance,offering great potential for early warning and prediction.Despite the recent technological advances,there is few reviews that explores the integration of cutting-edge technologies aimed at constructing a robust early warning system.Therefore,we discussed the opportunities,barriers,and limitations of interdisciplinary emerging technologies for exploring early warning and surveillance of zoonoses.This systematic review summarized a practical framework for early surveillance integrated with a modified SEIR model for zoonoses in the context of climate change.It also outlined challenges and future prospects in terms of data sharing,early detection of unknown zoonoses and the move towards global surveillance.展开更多
Over the past decade,all-inorganic metal halide perovskites(MHPs,CsPbX_(3):X=Cl,Br,I)have been widely investigated as promising materials for optoelectronic devices such as solar cells and light-emitting diodes.MHPs a...Over the past decade,all-inorganic metal halide perovskites(MHPs,CsPbX_(3):X=Cl,Br,I)have been widely investigated as promising materials for optoelectronic devices such as solar cells and light-emitting diodes.MHPs are defecttolerant,which allows tuning of their bandgap without altering their photophysical properties.From a fundamental point of view,MHPs are excellent candidates for photocatalytic reactions due to their light-harvesting capability,high photogenerated charge-carrier mobility,long diffusion lengths,and tunable bandgap energy.In this review,we provide an overview of various MHP engineering strategies(e.g.,surface,morphological,and structural modifications,heterojunction coupling,and encapsulation)which are directly linked to the charge-carrier mobility and lifetimes,and then to the photocatalytic efficiency.Specifically,we outline different synthetic approaches resulting in surface and morphological modifications,anion/cation substitution,metallic doping,coupling,and encapsulation that tremendously influence MHPs’stability,optical properties,and charge-carrier dynamics at variable time scales(from fs toμs).We also provide an in-depth evaluation of the MHPs for variable photoredox reactions,discussing how the optical and electronic properties help to improve their stability and efficiency.展开更多
本文设计了基于二维玻璃态石墨烯的多功能器件.与本征石墨烯相比,扭曲的晶格结构打开了玻璃态石墨烯的带隙,表现出与石墨烯类似甚至更优异的光电探测与化学传感性能.由于玻璃态石墨烯与空气中的小分子间较强的相互作用,该器件受到光致...本文设计了基于二维玻璃态石墨烯的多功能器件.与本征石墨烯相比,扭曲的晶格结构打开了玻璃态石墨烯的带隙,表现出与石墨烯类似甚至更优异的光电探测与化学传感性能.由于玻璃态石墨烯与空气中的小分子间较强的相互作用,该器件受到光致脱附的影响更小,呈现出正的光响应.在405 nm的激光照射下,器件的响应率为0.22 A W^(-1),探测率为10^(10)Jones.此外,玻璃态石墨烯中的固有缺陷和应变可增强分析物的吸附,获得良好的化学传感性能.玻璃态石墨烯器件探测丙酮的信噪比为48,比石墨烯器件提高了50%以上.此外,对偏压和厚度有关的挥发性有机化合物(VOC)感测功能的分析表明,少层玻璃态石墨烯更为敏感.这项研究表明玻璃态石墨烯在集成光电探测和化学传感多功能器件方面具有巨大应用前景.展开更多
Recently,increasing attention has been concentrated on negative permittivity with the development of the emerging metamaterials composed of periodic array structures.However,taking facile preparation into consideratio...Recently,increasing attention has been concentrated on negative permittivity with the development of the emerging metamaterials composed of periodic array structures.However,taking facile preparation into consideration,it is important to achieve negative permittivity behavior based on materials'intrinsic properties rather than their artificially periodic structures.In this paper,we proposed to fabricate the percolating composites with copper dispersed in epoxy(EP)resin by a polymerization method to realize the negative permittivity behavior.When Cu content in the composites reached to 80 wt%,the conductivity abruptly went up by three orders of magnitudes,suggesting a percolation behavior.Below the percolation threshold,the conductivity spectra conform to Jonscher's power law;when the Cu/EP composites reached to percolating state,the conductivity gradually reduced in high frequency region due to the skin effect.It is indicated that the conductive mechanism changed from hopping conduction to electron conduction.In addition,the permittivity did not increase monotonously with the increase of Cu content in the vicinity of percolation threshold,due to the presence of leakage current.Meanwhile,the negative permittivity conforming to Drude model was observed above the percolation threshold.Further investigation revealed that there was a constitutive relationship between the permittivity and the reactance.When conductive fillers are slightly above the percolation threshold,the inductive characteristic derived from conductive percolating network leads to the negative permittivity.Such epsilon-negative materials can potentially be applied in novel electrical devices,such as high-power microwave filters,stacked capacitors,negative capacitance field effect transistors and coil-free resonators.In addition,the design strategy based on percolating composites provides an approach to epsilon-negative materials.展开更多
Herein we computationally explore the modulation of the release kinetics of an encapsulated guest molecule from the cucurbit[7]uril(CB7)cavity by ligands binding to the host portal.We uncovered a correlation between t...Herein we computationally explore the modulation of the release kinetics of an encapsulated guest molecule from the cucurbit[7]uril(CB7)cavity by ligands binding to the host portal.We uncovered a correlation between the ligand-binding affinity with CB7 and the guest residence time,allowing us to rapidly predict the release kinetics through straightforward energy minimization calculations.These high-throughput predictions in turn enable a Monte-Carlo Tree Search(MCTS)to de novo design a series of cap-shaped ligand molecules with large binding affinities and boosting guest residence times by up to 7 orders of magnitude.Notably,halogenated aromatic compounds emerge as top-ranking ligands.Detailed modeling suggests the presence of halogen-bonding between the ligands and the CB7 portal.Meanwhile,the binding of top-ranked ligands is supported by^(1)H NMR and 2D DOSY-NMR.Our findings open up possibilities in gating of molecular transport through a nanoscale cavity with potential applications in nanopore technology and controlled drug release.展开更多
基金supported by the National Natural Science Foundation of Tianjin(No.20JCQNJC01280)the National Natural Science Foundation of China(No.21905201)+1 种基金the support of the scientifi c research project from China Three Gorges Corporation(No.202103406)supported by Tohoku University and JSPS KAKENHI(No.JP16J06828).
文摘Sodium-ion hybrid capacitor(SIHC)is one of the most promising alternatives for large-scale energy storage due to its high energy and power densities,natural abundance,and low cost.However,overcoming the imbalance between slow Na^(+)reaction kinetics of battery-type anodes and rapid ion adsorption/desorption of capacitive cathodes is a significant challenge.Here,we propose the high-rate-performance NiS_(2)@OMGC anode material composed of monodispersed NiS_(2) nanocrystals(8.8±1.7 nm in size)and N,S-co-doped graphenic carbon(GC).The NiS_(2)@OMGC material has a three-dimensionally ordered macroporous(3DOM)morphology,and numerous NiS_(2) nanocrystals are uniformly embedded in GC,forming a core-shell structure in the local area.Ultrafine NiS_(2) nanocrystals and their nano-microstructure demonstrate high pseudocapacitive Na-storage capability and thus excellent rate performance(355.7 mAh/g at 20.0 A/g).A SIHC device fabricated using NiS_(2)@OMGC and commercial activated carbon(AC)cathode exhibits ultrahigh energy densities(197.4 Wh/kg at 398.8 W/kg)and power densities(43.9 kW/kg at 41.3 Wh/kg),together with a long life span.This outcome exemplifies the rational architecture and composition design of this type of anode material.This strategy can be extended to the design and synthesis of a wide range of high-performance electrode materials for energy storage applications.
基金supported by the National Natural Science Foundation of China(No.11574111 and No.11974129 to X.-F.W.)“the Fundamental Research Funds for the Central Universities.”.
文摘Since their seminal discovery in 2011,two-dimensional(2D)transition metal carbides/nitrides known as MXenes,that constitute a large family of 2D materials,have been targeted toward various applications due to their outstanding electronic properties.MXenes functioning as co-catalyst in combination with certain photocatalysts have been applied in photocatalytic systems to enhance photogenerated charge separation,suppress rapid charge recombination,and convert solar energy into chemical energy or use it in the degradation of organic compounds.The photocatalytic performance greatly depends on the composition and morphology of the photocatalyst,which,in turn,are determined by the method of preparation used.Here,we review the four different synthesis methods(mechanical mixing,self-assembly,in situ decoration,and oxidation)reported for MXenes in view of their application as co-catalyst in photocatalysis.In addition,the working mechanism for MXenes application in photocatalysis is discussed and an outlook for future research is also provided.
基金supported by the National Natural Science Foundation of China (22104090)the Natural Science Foundation of Shanghai (22ZR1436200).
文摘Zoonoses account for the majority of emerging infectious diseases and pose a serious threat to human and animal health.Under global warming and climate change,zoonoses are significantly affected by influencing hosts,vectors,and pathogen dynamics as well as their in-teractions.Traditional zoonoses surveillance relies on molecular or serological diagnostic methods to monitor pathogens from animal or patient samples,which may miss the early warning signs of pathogens spillover from the environment.Nowadays,new technologies such as remote sensing,environment-based screening,multi-omics,and big data science facilitate comprehensive active surveillance,offering great potential for early warning and prediction.Despite the recent technological advances,there is few reviews that explores the integration of cutting-edge technologies aimed at constructing a robust early warning system.Therefore,we discussed the opportunities,barriers,and limitations of interdisciplinary emerging technologies for exploring early warning and surveillance of zoonoses.This systematic review summarized a practical framework for early surveillance integrated with a modified SEIR model for zoonoses in the context of climate change.It also outlined challenges and future prospects in terms of data sharing,early detection of unknown zoonoses and the move towards global surveillance.
基金the IDEX Paris-SaclayIRS MOMENTOM for financial support+6 种基金the French National Research Agency(ANR),through the IngenCat project(ANR-20-CE43-0014),for the financial supportthe ACT programme(Accelerating CCS Technologies,Horizon 2020 Project No.691712)for the financial support of the NEXTCCUS project(project ID:327327)the Royal Society(RGSR1211068)Cambridge Materials Limited for their funding and technical supportthe Department for Energy Security and Net Zero(Project ID:NEXTCCUS)University College London’s Research,Innovation and Global EngagementUCL Cities Partnerships Programme Award in Paris for their financial support。
文摘Over the past decade,all-inorganic metal halide perovskites(MHPs,CsPbX_(3):X=Cl,Br,I)have been widely investigated as promising materials for optoelectronic devices such as solar cells and light-emitting diodes.MHPs are defecttolerant,which allows tuning of their bandgap without altering their photophysical properties.From a fundamental point of view,MHPs are excellent candidates for photocatalytic reactions due to their light-harvesting capability,high photogenerated charge-carrier mobility,long diffusion lengths,and tunable bandgap energy.In this review,we provide an overview of various MHP engineering strategies(e.g.,surface,morphological,and structural modifications,heterojunction coupling,and encapsulation)which are directly linked to the charge-carrier mobility and lifetimes,and then to the photocatalytic efficiency.Specifically,we outline different synthetic approaches resulting in surface and morphological modifications,anion/cation substitution,metallic doping,coupling,and encapsulation that tremendously influence MHPs’stability,optical properties,and charge-carrier dynamics at variable time scales(from fs toμs).We also provide an in-depth evaluation of the MHPs for variable photoredox reactions,discussing how the optical and electronic properties help to improve their stability and efficiency.
基金supported by the National Natural Science Foundation of China (61974014)the EPSRC Future Compound Semiconductor Manufacturing Hub (EP/P006973/1)。
文摘本文设计了基于二维玻璃态石墨烯的多功能器件.与本征石墨烯相比,扭曲的晶格结构打开了玻璃态石墨烯的带隙,表现出与石墨烯类似甚至更优异的光电探测与化学传感性能.由于玻璃态石墨烯与空气中的小分子间较强的相互作用,该器件受到光致脱附的影响更小,呈现出正的光响应.在405 nm的激光照射下,器件的响应率为0.22 A W^(-1),探测率为10^(10)Jones.此外,玻璃态石墨烯中的固有缺陷和应变可增强分析物的吸附,获得良好的化学传感性能.玻璃态石墨烯器件探测丙酮的信噪比为48,比石墨烯器件提高了50%以上.此外,对偏压和厚度有关的挥发性有机化合物(VOC)感测功能的分析表明,少层玻璃态石墨烯更为敏感.这项研究表明玻璃态石墨烯在集成光电探测和化学传感多功能器件方面具有巨大应用前景.
基金sponsored by the National Natural Science Foundation of China (Grant No.51803119,51871146 and 51771108)the Innovation Program of Shanghai Municipal Education Commission (Grant No.2019-01-07-00-10-E00053)+1 种基金"Chenguang Program" supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission (Grant No.18CG56)the Science and Technology Commission of Shanghai Municipality (Grant No.18DZ1112902,No.18DZ1100802)
文摘Recently,increasing attention has been concentrated on negative permittivity with the development of the emerging metamaterials composed of periodic array structures.However,taking facile preparation into consideration,it is important to achieve negative permittivity behavior based on materials'intrinsic properties rather than their artificially periodic structures.In this paper,we proposed to fabricate the percolating composites with copper dispersed in epoxy(EP)resin by a polymerization method to realize the negative permittivity behavior.When Cu content in the composites reached to 80 wt%,the conductivity abruptly went up by three orders of magnitudes,suggesting a percolation behavior.Below the percolation threshold,the conductivity spectra conform to Jonscher's power law;when the Cu/EP composites reached to percolating state,the conductivity gradually reduced in high frequency region due to the skin effect.It is indicated that the conductive mechanism changed from hopping conduction to electron conduction.In addition,the permittivity did not increase monotonously with the increase of Cu content in the vicinity of percolation threshold,due to the presence of leakage current.Meanwhile,the negative permittivity conforming to Drude model was observed above the percolation threshold.Further investigation revealed that there was a constitutive relationship between the permittivity and the reactance.When conductive fillers are slightly above the percolation threshold,the inductive characteristic derived from conductive percolating network leads to the negative permittivity.Such epsilon-negative materials can potentially be applied in novel electrical devices,such as high-power microwave filters,stacked capacitors,negative capacitance field effect transistors and coil-free resonators.In addition,the design strategy based on percolating composites provides an approach to epsilon-negative materials.
基金H.L.and T.-C.L.are grateful to the studentship funded by the A*STAR-UCL Research Attachment Programme through the EPSRC Centre for Doctoral Training in Molecular Modelling and Materials Science(Grant EP/L015862/1)T.-C.L.is grateful to the Research Project Grant(Grant RPG-2016-393)funded by the Leverhulme Trust+1 种基金We acknowledge the use of the UCL Myriad High Performance Computing Facility(Myriad@UCL),and associated support services,in the completion of this workThis work is partially supported financially by the Agency for Science,Technology and Research(A^(*)STAR)under grant AMDM A1898b0043,and A^(*)STAR SERC CRF Award.
文摘Herein we computationally explore the modulation of the release kinetics of an encapsulated guest molecule from the cucurbit[7]uril(CB7)cavity by ligands binding to the host portal.We uncovered a correlation between the ligand-binding affinity with CB7 and the guest residence time,allowing us to rapidly predict the release kinetics through straightforward energy minimization calculations.These high-throughput predictions in turn enable a Monte-Carlo Tree Search(MCTS)to de novo design a series of cap-shaped ligand molecules with large binding affinities and boosting guest residence times by up to 7 orders of magnitude.Notably,halogenated aromatic compounds emerge as top-ranking ligands.Detailed modeling suggests the presence of halogen-bonding between the ligands and the CB7 portal.Meanwhile,the binding of top-ranked ligands is supported by^(1)H NMR and 2D DOSY-NMR.Our findings open up possibilities in gating of molecular transport through a nanoscale cavity with potential applications in nanopore technology and controlled drug release.