Highly thermally conductive graphitic film(GF)materials have become a competitive solution for the thermal management of high-power electronic devices.However,their catastrophic structural failure under extreme altern...Highly thermally conductive graphitic film(GF)materials have become a competitive solution for the thermal management of high-power electronic devices.However,their catastrophic structural failure under extreme alternating thermal/cold shock poses a significant challenge to reliability and safety.Here,we present the first investigation into the structural failure mechanism of GF during cyclic liquid nitrogen shocks(LNS),which reveals a bubbling process characterized by“permeation-diffusion-deformation”phenomenon.To overcome this long-standing structural weakness,a novel metal-nanoarmor strategy is proposed to construct a Cu-modified graphitic film(GF@Cu)with seamless heterointerface.This well-designed interface ensures superior structural stability for GF@Cu after hundreds of LNS cycles from 77 to 300 K.Moreover,GF@Cu maintains high thermal conductivity up to 1088 W m^(−1)K^(−1)with degradation of less than 5%even after 150 LNS cycles,superior to that of pure GF(50%degradation).Our work not only offers an opportunity to improve the robustness of graphitic films by the rational structural design but also facilitates the applications of thermally conductive carbon-based materials for future extreme thermal management in complex aerospace electronics.展开更多
Photosynthesis affects crop growth and yield.The roles of microRNAs(miRNAs)in photosynthesis are little known.In the present study,the role of the OsNF-YB7–OsMIR5810–OsMRLP6 regulatory module in photosynthesis was i...Photosynthesis affects crop growth and yield.The roles of microRNAs(miRNAs)in photosynthesis are little known.In the present study,the role of the OsNF-YB7–OsMIR5810–OsMRLP6 regulatory module in photosynthesis was investigated.The malectin-like protein gene OsMRLP6 was identified as a target gene of osa-miR5810(miR5810).Overexpression in rice of miR5810 or down-expression of OsMRLP6 resulted in reduced expression of genes involved in chloroplast development and photosynthesis and decreased net photosynthetic rate,finally leading to lower shoot biomass and grain yield.Down-expression of miR5810 and overexpression of OsMRLP6 showed the opposite effect.Overexpression of transcription factor OsNF-YB7 elevated expression of OsMIR5810 in rice seedlings by binding to its promoter.The OsNFYB7–OsMIR5810–OsMRLP6 regulatory module affects photosynthesis to mediate growth and grain yield.展开更多
The interest in using therapeutic nanoparticles to bind with harmful molecules or pathogens and subsequently neutralize their bioactivity has grown tremendously.Among various nanomedicine platforms,cell membrane-coate...The interest in using therapeutic nanoparticles to bind with harmful molecules or pathogens and subsequently neutralize their bioactivity has grown tremendously.Among various nanomedicine platforms,cell membrane-coated nanoparticles,namely,“cellular nanosponges,”stand out for their broadspectrum neutralization capability challenging to achieve in traditional countermeasure technologies.Such ability is attributable to their cellular function-based rather than target structure-based working principle.Integrating cellular nanosponges with various synthetic substrates further makes their applications exceptionally versatile and adaptive.This review discusses the latest cellular nanosponge technology focusing on how the structure–function relationship in different designs has led to versatile and potent medical countermeasures.Four design strategies are discussed,including harnessing native cell membrane functions for biological neutralization,functionalizing cell membrane coatings to enhance neutralization capabilities,combining cell membranes and functional cores for multimodal neutralization,and integrating cellular nanosponges with hydrogels for localized applications.Examples in each design strategy are selected,and the discussion is to highlight their structure–function relationships in complex disease settings.The review may inspire additional design strategies for cellular nanosponges and fulfill even broader medical applications.展开更多
The prognosis of patients with previously treated tuberculosis (TB) was suggested to be dependent on whether the initial treatment was in compliance with the established guidelines. The aim of this retrospective multi...The prognosis of patients with previously treated tuberculosis (TB) was suggested to be dependent on whether the initial treatment was in compliance with the established guidelines. The aim of this retrospective multicenter study was to determine the proportion of new TB patients who received standard doses of rifampicin in multiple provinces of China, and the relationship between low doses of rifampicin and frequency of rifampicin-resistance as well as treatment outcomes. A total of 713 new TB patients were treated with either once-daily dose of bulk anti-TB drugs (group I) or every other day combination blister packs of anti-TB drugs containing rifampicin (group II) at more than 30 TB treatment centers/hospitals in China. Treatment history, therapeutic doses of rifampicin, and information about patients were extracted from their medical records and analyzed, and rifampicin-resistance of isolates collected from patients following the treatment as well as treatment outcomes were compared between two treatment groups. Among 522 patients in treatment group I, 154 (29.5%) received standard and 363 (69.5%) received low doses of rifampicin;238 (45.6%) isolates were rifampicin-resistant, and 243 (46.6%) were successfully treated. Among 191 patients in treatment group II, 175 (91.6%) received standard and 15 (7.9%) received low doses of rifampicin;72 (37.7%) isolates were rifampicin-resistant, and 105 (55%) were successfully treated. When patients who received low doses of rifampicin were compared to others within the same treatment group, increased rates for rifampicin-resistance and treatment failure were observed. Results from this study showed that most new TB patients in treatment group I (69.5%) received low doses of rifampicin, and their treatment outcomes were worse than those in treatment group II, indicating that low doses of rifampicin used for the initial treatment of new TB patients were correlated to increased frequency of rifampicin-resistance and poorer treatment outcomes.展开更多
The single planar routing protocol has a slow convergence rate in the large-scale Wireless Sensor Network(WSN).Although the hierarchical routing protocol can effectively cope with large-scale application scenarios,how...The single planar routing protocol has a slow convergence rate in the large-scale Wireless Sensor Network(WSN).Although the hierarchical routing protocol can effectively cope with large-scale application scenarios,how to elect a secure cluster head and balance the network load becomes an enormous challenge.In this paper,a Trust Management-based and Low Energy Adaptive Clustering Hierarchy protocol(LEACH-TM)is proposed.In LEACH-TM,by using the number of dynamic decision cluster head nodes,residual energy and density of neighbor nodes,the size of the cluster can be better constrained to improve energy efficiency,and avoid excessive energy consumption of a node.Simultaneously,the trust management scheme is introduced into LEACH-TM to defend against internal attacks.The simulation results show that,compared with LEACH-SWDN protocol and LEACH protocol,LEACH-TM outperforms in prolonging the network lifetime and balancing the energy consumption,and can effectively mitigate the influence of malicious nodes on cluster head selection,which can greatiy guarantee the security of the overall network.展开更多
Energy-absorbing materials are widely used in transportations,sports,and the military applications.Particularly,porous materials,including natural and artificial materials,have attracted tremendous attentions due to t...Energy-absorbing materials are widely used in transportations,sports,and the military applications.Particularly,porous materials,including natural and artificial materials,have attracted tremendous attentions due to their light weight and excellent energy absorption capability.This review summarizes the recent progresses in the natural and artificial energy-absorbing porous materials.First,we review the typical natural porous materials including cuttlebone,bighorn sheep horn,pomelo peel,and sunflower stem pith.The architectures,energy absorption abilities,and mechanisms of these typical natural materials and their bioinspired materials are summarized.Then,we provide a review on the fabrication methods of artificial energy-absorbing porous materials,such as conventional foaming and three-dimensional(3D)printing.Finally,we address the challenges and prospects for the future development of energy-absorbing porous materials.More importantly,our review provides a direct guidance for the design and fabrication of energy-absorbing porous materials required for various engineering applications.展开更多
Chalcogenide perovskites(CPs) exhibiting lower band gaps than oxide perovskites and higher stability than halide perovskites are promising materials for photovoltaic and optoelectronic applications. For such applicati...Chalcogenide perovskites(CPs) exhibiting lower band gaps than oxide perovskites and higher stability than halide perovskites are promising materials for photovoltaic and optoelectronic applications. For such applications, the absence of deep defect levels serving as recombination centers(dubbed defect tolerance) is a highly desirable property. Here,using density functional theory(DFT) calculations, we study the intrinsic defects in BaZrS_(3), a representative CP material.We compare Hubbard-U and hybrid functional methods, both of which have been widely used in addressing the band gap problem of semi-local functionals in DFT. We find that tuning the U value to obtain experimental bulk band gap and then using the obtained U value for defect calculations may result in over-localization of defect states. In the hybrid functional calculation, the band gap of BaZrS_(3)can be accurately obtained. We observe the formation of small S-atom clusters in both methods, which tend to self-passivate the defects from forming mid-gap levels. Even though in the hybrid functional calculations several relatively deep defects are observed, all of them exhibit too high formation energy to play a significant role if the materials are prepared under thermal equilibrium.BaZrS_(3)is thus expected to exhibit sufficient defect tolerance promising for photovoltaic and optoelectronic applications.展开更多
CONSPECTUS:Biological porous materials,such as polar bear hair,wood,bamboo,and cuttlebone,exhibit outstanding thermal and mechanical properties due to their hierarchical architectures.Specifically,polar bears can reta...CONSPECTUS:Biological porous materials,such as polar bear hair,wood,bamboo,and cuttlebone,exhibit outstanding thermal and mechanical properties due to their hierarchical architectures.Specifically,polar bears can retain thermal homeostasis in the extremely cold Arctic due to outstanding thermal insulation property of their porous hairs;wood and bamboo exhibit excellent mechanical strength,highly efficient water and nutrient transport capacity,and low density due to their hierarchically aligned porous architecture;cuttlebone can resist large hydrostatic pressure in the deep-sea environment due to its mechanically efficient porous structure with lamellar septa connected by asymmetrically S-shaped walls.展开更多
Graphene-polyaniline(GP)composites are promising electrode materials for supercapacitors but possessing unsatisfied stability,especially under high mass loading,due to the low ion transmission efficiency and serious p...Graphene-polyaniline(GP)composites are promising electrode materials for supercapacitors but possessing unsatisfied stability,especially under high mass loading,due to the low ion transmission efficiency and serious pulverization effect.To address this issue,we propose a scalable method to achieve highly wettable GP electrodes,showing excellent stability.In addition,our results demonstrate that the performance of electrodes is nearly independent of the mass loading,indicating the great potential of such GP electrodes for practical devices.We attribute the remarkable performance of GP to the delicate precursor of nitrogen doped graphene film assembled by wet-spinning technology.This report provides a strategy to promote the ion penetrating efficiency across the electrodes and deter the pulverization effect,aiming at the practical GP supercapacitor electrodes of high mass loading.展开更多
Accurate and efficient predictions of the quasiparticle properties of complex materials remain a major challenge due to the convergence issue and the unfavorable scaling of the computational cost with respect to the s...Accurate and efficient predictions of the quasiparticle properties of complex materials remain a major challenge due to the convergence issue and the unfavorable scaling of the computational cost with respect to the system size.Quasiparticle GW calculations for two-dimensional(2D)materials are especially difficult.The unusual analytical behaviors of the dielectric screening and the electron self-energy of 2D materials make the conventional Brillouin zone(BZ)integration approach rather inefficient and require an extremely dense k-grid to properly converge the calculated quasiparticle energies.In this work,we present a combined nonuniform subsampling and analytical integration method that can drastically improve the efficiency of the BZ integration in 2D GW calculations.展开更多
Catalytic diastereodivergent hydrosilylative enyne cyclization with high generality and broad scope was achieved using electronic ac-tivated N-heterocyclic carbene-Ni(O)as a catalyst and R_(3)SiH as silane(IPr^(Cl),sy...Catalytic diastereodivergent hydrosilylative enyne cyclization with high generality and broad scope was achieved using electronic ac-tivated N-heterocyclic carbene-Ni(O)as a catalyst and R_(3)SiH as silane(IPr^(Cl),syn-:anti-selectivity from up to 98:2 to 7:93 by Z=0,NH vs.NMs,R^(1)=n-pentyl).Heterocycles bearing homoallylsilane rather than vinylsilane was obtained chemoselectively.The undesired yet highly competitive reactivity was suppressed,like direct hydrosilylation of alkene and alkyne concurrently.Optionally,the homoallylsilane products could be reduced further in one-pot using IPr^(Me) as ligand and(EtO)_(3)SiH as silane under otherwise the same standard condition as the above,offering practical access to additional stereocenters and more diverse product structures from enynes.展开更多
1Introduction and main contributions Recently,community search over Heterogeneous Information Networks(HINs)has attracted much attention in graph analysis,which aims to search for local communities containing query no...1Introduction and main contributions Recently,community search over Heterogeneous Information Networks(HINs)has attracted much attention in graph analysis,which aims to search for local communities containing query node.Although existing community search studies in HINs have proved effective in converting heterogeneous graphs to homogeneous graphs via pre-defined meta-paths with consistent head and tail node types,two major limitations stilexist.First,they fail to properly utilize the intermediate nodes to assign weights on the edges of the induced homogeneous graph.展开更多
The electronic structure of two-dimensional(2D)materials are inherently prone to environmental perturbations,which may pose significant challenges to their applications in electronic or optoelectronic devices.A 2D mat...The electronic structure of two-dimensional(2D)materials are inherently prone to environmental perturbations,which may pose significant challenges to their applications in electronic or optoelectronic devices.A 2D material couples with its environment through two mechanisms:local chemical coupling and nonlocal dielectric screening effects.The local chemical coupling is often difficult to predict or control experimentally.Nonlocal dielectric screening,on the other hand,can be tuned by choosing the substrates or layer thickness in a controllable manner.Therefore,a compelling 2D electronic material should offer band edge states that are robust against local chemical coupling effects.Here it is demonstrated that the recently synthesized MoSi_(2)N_(4)is an ideal 2D semiconductor with robust band edge states protected from capricious environmental chemical coupling effects.Detailed many-body perturbation theory calculations are carried out to illustrate how the band edge states of MoSi_(2)N_(4)are shielded from the direct chemical coupling effects,but its quasiparticle and excitonic properties can be modulated through the nonlocal dielectric screening effects.This unique property,together with the moderate band gap and the thermodynamic and mechanical stability of this material,paves the way for a range of applications of MoSi_(2)N_(4)in areas including energy,2D electronics,and optoelectronics.展开更多
Inflammatory cytokines are key players in modulating immune responses to mount effective host defense.However,excessive production of inflammatory cytokines contributes to the destructive components responsible for va...Inflammatory cytokines are key players in modulating immune responses to mount effective host defense.However,excessive production of inflammatory cytokines contributes to the destructive components responsible for various inflammatory disorders.As a result,treatment strategies have been developed to lower the cytokine levels or block their bioactivity.In particular,therapeutic agents that directly capture and neutralize cytokines have gained significant attention as they bypass the interactions with the host cells,and therefore,are less likely to induce immunogenic response and clearance.Among them,“monoplex”platforms such as cytokine-neutralizing antibodies(CNAs)are commonly designed to target a specific cytokine for neutralization.Meanwhile,to address the multiplexity of the cytokine targets in diseases,multiplex platforms such as glycosaminoglycan-containing biomaterials and cell-membrane-coated nanoparticles are emerging.Herein,we have reviewed the recent progress of these cytokine-neutralizing platforms(CNPs)and discussed their applications in treating inflammatory disorders.Overall,understanding the structure–function relationships underlying these CNPs would lead to the design of novel therapeutics toward effective management of inflammatory diseases.展开更多
基金the National Natural Science Foundation of China(Nos.52272046,52090030,52090031,52122301,51973191)the Natural Science Foundation of Zhejiang Province(LR23E020003)+4 种基金Shanxi-Zheda Institute of New Materials and Chemical Engineering(2021SZ-FR004,2022SZ-TD011,2022SZ-TD012,2022SZ-TD014)Hundred Talents Program of Zhejiang University(188020*194231701/113,112300+1944223R3/003,112300+1944223R3/004)the Fundamental Research Funds for the Central Universities(Nos.226-2023-00023,226-2023-00082,2021FZZX001-17,K20200060)National Key R&D Program of China(NO.2022YFA1205300,NO.2022YFA1205301,NO.2020YFF0204400,NO.2022YFF0609801)“Pioneer”and“Leading Goose”R&D Program of Zhejiang 2023C01190.
文摘Highly thermally conductive graphitic film(GF)materials have become a competitive solution for the thermal management of high-power electronic devices.However,their catastrophic structural failure under extreme alternating thermal/cold shock poses a significant challenge to reliability and safety.Here,we present the first investigation into the structural failure mechanism of GF during cyclic liquid nitrogen shocks(LNS),which reveals a bubbling process characterized by“permeation-diffusion-deformation”phenomenon.To overcome this long-standing structural weakness,a novel metal-nanoarmor strategy is proposed to construct a Cu-modified graphitic film(GF@Cu)with seamless heterointerface.This well-designed interface ensures superior structural stability for GF@Cu after hundreds of LNS cycles from 77 to 300 K.Moreover,GF@Cu maintains high thermal conductivity up to 1088 W m^(−1)K^(−1)with degradation of less than 5%even after 150 LNS cycles,superior to that of pure GF(50%degradation).Our work not only offers an opportunity to improve the robustness of graphitic films by the rational structural design but also facilitates the applications of thermally conductive carbon-based materials for future extreme thermal management in complex aerospace electronics.
基金We thank Dr.Baixiao Niu(Yangzhou University)for providing YB7-ox transgenic rice plants.the Guangzhou Science and Technology Project(202102021003,2023B03J0742)the National Natural Science Foundation of China(32171933).
文摘Photosynthesis affects crop growth and yield.The roles of microRNAs(miRNAs)in photosynthesis are little known.In the present study,the role of the OsNF-YB7–OsMIR5810–OsMRLP6 regulatory module in photosynthesis was investigated.The malectin-like protein gene OsMRLP6 was identified as a target gene of osa-miR5810(miR5810).Overexpression in rice of miR5810 or down-expression of OsMRLP6 resulted in reduced expression of genes involved in chloroplast development and photosynthesis and decreased net photosynthetic rate,finally leading to lower shoot biomass and grain yield.Down-expression of miR5810 and overexpression of OsMRLP6 showed the opposite effect.Overexpression of transcription factor OsNF-YB7 elevated expression of OsMIR5810 in rice seedlings by binding to its promoter.The OsNFYB7–OsMIR5810–OsMRLP6 regulatory module affects photosynthesis to mediate growth and grain yield.
基金This work is supported by the Defense Threat Reduction Agency Joint Science and Technology Office for Chemical and Biological Defense under Award Numbers HDTRA1-21-1-0010 and HDTRA1-21-C-0019.
文摘The interest in using therapeutic nanoparticles to bind with harmful molecules or pathogens and subsequently neutralize their bioactivity has grown tremendously.Among various nanomedicine platforms,cell membrane-coated nanoparticles,namely,“cellular nanosponges,”stand out for their broadspectrum neutralization capability challenging to achieve in traditional countermeasure technologies.Such ability is attributable to their cellular function-based rather than target structure-based working principle.Integrating cellular nanosponges with various synthetic substrates further makes their applications exceptionally versatile and adaptive.This review discusses the latest cellular nanosponge technology focusing on how the structure–function relationship in different designs has led to versatile and potent medical countermeasures.Four design strategies are discussed,including harnessing native cell membrane functions for biological neutralization,functionalizing cell membrane coatings to enhance neutralization capabilities,combining cell membranes and functional cores for multimodal neutralization,and integrating cellular nanosponges with hydrogels for localized applications.Examples in each design strategy are selected,and the discussion is to highlight their structure–function relationships in complex disease settings.The review may inspire additional design strategies for cellular nanosponges and fulfill even broader medical applications.
文摘The prognosis of patients with previously treated tuberculosis (TB) was suggested to be dependent on whether the initial treatment was in compliance with the established guidelines. The aim of this retrospective multicenter study was to determine the proportion of new TB patients who received standard doses of rifampicin in multiple provinces of China, and the relationship between low doses of rifampicin and frequency of rifampicin-resistance as well as treatment outcomes. A total of 713 new TB patients were treated with either once-daily dose of bulk anti-TB drugs (group I) or every other day combination blister packs of anti-TB drugs containing rifampicin (group II) at more than 30 TB treatment centers/hospitals in China. Treatment history, therapeutic doses of rifampicin, and information about patients were extracted from their medical records and analyzed, and rifampicin-resistance of isolates collected from patients following the treatment as well as treatment outcomes were compared between two treatment groups. Among 522 patients in treatment group I, 154 (29.5%) received standard and 363 (69.5%) received low doses of rifampicin;238 (45.6%) isolates were rifampicin-resistant, and 243 (46.6%) were successfully treated. Among 191 patients in treatment group II, 175 (91.6%) received standard and 15 (7.9%) received low doses of rifampicin;72 (37.7%) isolates were rifampicin-resistant, and 105 (55%) were successfully treated. When patients who received low doses of rifampicin were compared to others within the same treatment group, increased rates for rifampicin-resistance and treatment failure were observed. Results from this study showed that most new TB patients in treatment group I (69.5%) received low doses of rifampicin, and their treatment outcomes were worse than those in treatment group II, indicating that low doses of rifampicin used for the initial treatment of new TB patients were correlated to increased frequency of rifampicin-resistance and poorer treatment outcomes.
基金supported by the National Natural Science Foundation of China(Grant No.61571303,No.61571004)the Shanghai Natural Science Foundation(Grant No.21ZR1461700)+3 种基金the Shanghai Sailing Program(Grant No.19YF1455800)the National Science and Technology Major Project of China(No.2018ZX03001031)the Fundamental Research Funds for State Key Laboratory of Synthetical Automation for Process Industries(Grant No.PAL-N201703)the National Key Research and Development Program of China-Internet of Things and Smart City Key Program(No.2019YFB2101600,NO.2019YFB2101602,No.2019YFB2101602-03).
文摘The single planar routing protocol has a slow convergence rate in the large-scale Wireless Sensor Network(WSN).Although the hierarchical routing protocol can effectively cope with large-scale application scenarios,how to elect a secure cluster head and balance the network load becomes an enormous challenge.In this paper,a Trust Management-based and Low Energy Adaptive Clustering Hierarchy protocol(LEACH-TM)is proposed.In LEACH-TM,by using the number of dynamic decision cluster head nodes,residual energy and density of neighbor nodes,the size of the cluster can be better constrained to improve energy efficiency,and avoid excessive energy consumption of a node.Simultaneously,the trust management scheme is introduced into LEACH-TM to defend against internal attacks.The simulation results show that,compared with LEACH-SWDN protocol and LEACH protocol,LEACH-TM outperforms in prolonging the network lifetime and balancing the energy consumption,and can effectively mitigate the influence of malicious nodes on cluster head selection,which can greatiy guarantee the security of the overall network.
基金supported by the National Natural Science Foundation of China(No.22075244)the Zhejiang Provincial Innovation Center of Advanced Chemicals Technology(No.ACTIC-2022-004)+2 种基金the Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering(No.2021SZ-TD009)the Zhejiang Provincial Natural Science Foundation of China(No.LZ22E030001)the Science and Technology Program of Institute of Zhejiang University-Quzhou(Nos.IZQ2021KJ2001 and IZQ2022KJ3013).
文摘Energy-absorbing materials are widely used in transportations,sports,and the military applications.Particularly,porous materials,including natural and artificial materials,have attracted tremendous attentions due to their light weight and excellent energy absorption capability.This review summarizes the recent progresses in the natural and artificial energy-absorbing porous materials.First,we review the typical natural porous materials including cuttlebone,bighorn sheep horn,pomelo peel,and sunflower stem pith.The architectures,energy absorption abilities,and mechanisms of these typical natural materials and their bioinspired materials are summarized.Then,we provide a review on the fabrication methods of artificial energy-absorbing porous materials,such as conventional foaming and three-dimensional(3D)printing.Finally,we address the challenges and prospects for the future development of energy-absorbing porous materials.More importantly,our review provides a direct guidance for the design and fabrication of energy-absorbing porous materials required for various engineering applications.
基金supported by the National Natural Science Foundation of China (11774365)the Natural Science Foundation of Shanghai (19ZR1421800)+4 种基金Shanghai International Cooperation Project (20520760900)the Opening Project and Science Foundation for Youth Scholar of State Key Laboratory of High Performance Ceramics and Superfine Microstructures (SKL201804 and SKL201803SIC) support by US National Science Foundation (NSF) (CBET1510121)US Department of Energy (DOE) (DEEE0007364)support by US NSF (CBET-1510948).support by US NSF (DMR-1506669)support by the Fundamental Research Funds for the Central Universities (DUT21RC(3) 033)。
文摘Chalcogenide perovskites(CPs) exhibiting lower band gaps than oxide perovskites and higher stability than halide perovskites are promising materials for photovoltaic and optoelectronic applications. For such applications, the absence of deep defect levels serving as recombination centers(dubbed defect tolerance) is a highly desirable property. Here,using density functional theory(DFT) calculations, we study the intrinsic defects in BaZrS_(3), a representative CP material.We compare Hubbard-U and hybrid functional methods, both of which have been widely used in addressing the band gap problem of semi-local functionals in DFT. We find that tuning the U value to obtain experimental bulk band gap and then using the obtained U value for defect calculations may result in over-localization of defect states. In the hybrid functional calculation, the band gap of BaZrS_(3)can be accurately obtained. We observe the formation of small S-atom clusters in both methods, which tend to self-passivate the defects from forming mid-gap levels. Even though in the hybrid functional calculations several relatively deep defects are observed, all of them exhibit too high formation energy to play a significant role if the materials are prepared under thermal equilibrium.BaZrS_(3)is thus expected to exhibit sufficient defect tolerance promising for photovoltaic and optoelectronic applications.
基金supported by the National Natural Science Foundation of China(No.22075244)Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering(No.2021SZ-TD009)+1 种基金Zhejiang Provincial Natural Science Foundation of China(No.LZ22E030001)Science and Technology Program of Institute of Zhejiang University-Quzhou(No.IZQ2021KJ2001).
文摘CONSPECTUS:Biological porous materials,such as polar bear hair,wood,bamboo,and cuttlebone,exhibit outstanding thermal and mechanical properties due to their hierarchical architectures.Specifically,polar bears can retain thermal homeostasis in the extremely cold Arctic due to outstanding thermal insulation property of their porous hairs;wood and bamboo exhibit excellent mechanical strength,highly efficient water and nutrient transport capacity,and low density due to their hierarchically aligned porous architecture;cuttlebone can resist large hydrostatic pressure in the deep-sea environment due to its mechanically efficient porous structure with lamellar septa connected by asymmetrically S-shaped walls.
基金This work is supported by the National Natural Science Foundation of China(51533008,21325417,51603183,51703194,51803177 and 21805242)the National Key R&D Program of China(2016YFA0200200)+3 种基金Fujian Provincial Science and Technology Major Projects(2018HZ0001-2)Hundred Talents Program of Zhejiang University(188020*194231701/113)the Key Research and Development Plan of Zhejiang Province(2018C01049)the Fundamental Research Funds for the Central Universities(2017QNA4036 and 2017XZZX001-04).
文摘Graphene-polyaniline(GP)composites are promising electrode materials for supercapacitors but possessing unsatisfied stability,especially under high mass loading,due to the low ion transmission efficiency and serious pulverization effect.To address this issue,we propose a scalable method to achieve highly wettable GP electrodes,showing excellent stability.In addition,our results demonstrate that the performance of electrodes is nearly independent of the mass loading,indicating the great potential of such GP electrodes for practical devices.We attribute the remarkable performance of GP to the delicate precursor of nitrogen doped graphene film assembled by wet-spinning technology.This report provides a strategy to promote the ion penetrating efficiency across the electrodes and deter the pulverization effect,aiming at the practical GP supercapacitor electrodes of high mass loading.
基金This work is supported by the NSF under Grant Nos DMR-1506669 and DMREF-1626967P.Z.acknowledges the Southern University of Science and Technology(SUSTech)for hosting his extended visit during spring 2019 when he was on sabbatical+3 种基金Work at SUSTech and SHU is supported by the National Natural Science Foundation of China(Nos 51632005,51572167,and 11929401)W.Z.also acknowledges the support from the Guangdong Innovation Research Team Project(No.2017ZT07C062)Guangdong Provincial Key-Lab program(No.2019B030301001)Shenzhen Municipal Key-Lab program(ZDSYS20190902092905285),and the Shenzhen Pengcheng-Scholarship Program.
文摘Accurate and efficient predictions of the quasiparticle properties of complex materials remain a major challenge due to the convergence issue and the unfavorable scaling of the computational cost with respect to the system size.Quasiparticle GW calculations for two-dimensional(2D)materials are especially difficult.The unusual analytical behaviors of the dielectric screening and the electron self-energy of 2D materials make the conventional Brillouin zone(BZ)integration approach rather inefficient and require an extremely dense k-grid to properly converge the calculated quasiparticle energies.In this work,we present a combined nonuniform subsampling and analytical integration method that can drastically improve the efficiency of the BZ integration in 2D GW calculations.
基金the Guangdong Provincial Key Laboratory of Catalysis(No.2020B121201002)NSFC(No.22071096)SUSTech(Nos.Y01501808 and Y01506014).
文摘Catalytic diastereodivergent hydrosilylative enyne cyclization with high generality and broad scope was achieved using electronic ac-tivated N-heterocyclic carbene-Ni(O)as a catalyst and R_(3)SiH as silane(IPr^(Cl),syn-:anti-selectivity from up to 98:2 to 7:93 by Z=0,NH vs.NMs,R^(1)=n-pentyl).Heterocycles bearing homoallylsilane rather than vinylsilane was obtained chemoselectively.The undesired yet highly competitive reactivity was suppressed,like direct hydrosilylation of alkene and alkyne concurrently.Optionally,the homoallylsilane products could be reduced further in one-pot using IPr^(Me) as ligand and(EtO)_(3)SiH as silane under otherwise the same standard condition as the above,offering practical access to additional stereocenters and more diverse product structures from enynes.
基金supported by the National Natural Science Foundation of China(Grant Nos.61762078,61363058,61966004)Natural Science Foundation of Gansu(21JR7RA114)Northwest Normal University Young Teachers Research Capacity Promotion Plan(NWNULKQN2019-2).
文摘1Introduction and main contributions Recently,community search over Heterogeneous Information Networks(HINs)has attracted much attention in graph analysis,which aims to search for local communities containing query node.Although existing community search studies in HINs have proved effective in converting heterogeneous graphs to homogeneous graphs via pre-defined meta-paths with consistent head and tail node types,two major limitations stilexist.First,they fail to properly utilize the intermediate nodes to assign weights on the edges of the induced homogeneous graph.
基金This work is supported in part by the National Natural Science Foundation of China(Nos.51632005,51572167,11929401,and 12104207)the National Key Research and Development Program of China(No.2017YFB0701600)+4 种基金Guangdong Innovative and Entrepreneurial Research Team Program(Grant No.2019ZT08C044)Shenzhen Science and Technology Program(KQTD20190929173815000)Work at UB is supported by the US National Science Foundation under Grant No.DMREF-1626967W.Z.also acknowledges the support from the Guangdong Innovation Research Team Project(Grant No.2017ZT07C062)the Shenzhen Pengcheng-Scholarship Program.W.G.acknowledges the supports by the Fundamental Research Funds for the Central Universities,grant DUT21RC(3)033.
文摘The electronic structure of two-dimensional(2D)materials are inherently prone to environmental perturbations,which may pose significant challenges to their applications in electronic or optoelectronic devices.A 2D material couples with its environment through two mechanisms:local chemical coupling and nonlocal dielectric screening effects.The local chemical coupling is often difficult to predict or control experimentally.Nonlocal dielectric screening,on the other hand,can be tuned by choosing the substrates or layer thickness in a controllable manner.Therefore,a compelling 2D electronic material should offer band edge states that are robust against local chemical coupling effects.Here it is demonstrated that the recently synthesized MoSi_(2)N_(4)is an ideal 2D semiconductor with robust band edge states protected from capricious environmental chemical coupling effects.Detailed many-body perturbation theory calculations are carried out to illustrate how the band edge states of MoSi_(2)N_(4)are shielded from the direct chemical coupling effects,but its quasiparticle and excitonic properties can be modulated through the nonlocal dielectric screening effects.This unique property,together with the moderate band gap and the thermodynamic and mechanical stability of this material,paves the way for a range of applications of MoSi_(2)N_(4)in areas including energy,2D electronics,and optoelectronics.
基金supported by the National Science Foundation Grant DMR-1904702the Defense Threat Reduction Agency Joint Science and Technology Office for ChemicalBiological Defense under grant number HDTRA1-18-1-0014.
文摘Inflammatory cytokines are key players in modulating immune responses to mount effective host defense.However,excessive production of inflammatory cytokines contributes to the destructive components responsible for various inflammatory disorders.As a result,treatment strategies have been developed to lower the cytokine levels or block their bioactivity.In particular,therapeutic agents that directly capture and neutralize cytokines have gained significant attention as they bypass the interactions with the host cells,and therefore,are less likely to induce immunogenic response and clearance.Among them,“monoplex”platforms such as cytokine-neutralizing antibodies(CNAs)are commonly designed to target a specific cytokine for neutralization.Meanwhile,to address the multiplexity of the cytokine targets in diseases,multiplex platforms such as glycosaminoglycan-containing biomaterials and cell-membrane-coated nanoparticles are emerging.Herein,we have reviewed the recent progress of these cytokine-neutralizing platforms(CNPs)and discussed their applications in treating inflammatory disorders.Overall,understanding the structure–function relationships underlying these CNPs would lead to the design of novel therapeutics toward effective management of inflammatory diseases.