Na-ion O3-type layered oxides are prospective cathodes for Na-ion batteries due to high energy density and low-cost.Nevertheless,such cathodes usually suffer from phase transitions,sluggish kinetics and air instabilit...Na-ion O3-type layered oxides are prospective cathodes for Na-ion batteries due to high energy density and low-cost.Nevertheless,such cathodes usually suffer from phase transitions,sluggish kinetics and air instability,making it difficult to achieve high performance solid-state sodium-ion batteries.Herein,the high-entropy design and Li doping strategy alleviate lattice stress and enhance ionic conductivity,achieving high-rate performance,air stability and electrochemically thermal stability for Na_(0.95)Li_(0.06)Ni_(0.25)Cu_(0.05)Fe_(0.15)Mn_(0.49)O_(2).This cathode delivers a high reversible capacity(141 mAh g^(−1)at 0.2C),excellent rate capability(111 mAh g^(−1)at 8C,85 mAh g^(−1)even at 20C),and long-term stability(over 85%capacity retention after 1000 cycles),which is attributed to a rapid and reversible O3–P3 phase transition in regions of low voltage and suppresses phase transition.Moreover,the compound remains unchanged over seven days and keeps thermal stability until 279℃.Remarkably,the polymer solid-state sodium battery assembled by this cathode provides a capacity of 92 mAh g^(−1)at 5C and keeps retention of 96%after 400 cycles.This strategy inspires more rational designs and could be applied to a series of O3 cathodes to improve the performance of solid-state Na-ion batteries.展开更多
Highly active bifunctional oxygen electrocatalysts accelerate the development of high-performance Zn-air battery,but suffer from the mismatched activities of oxygen evolution reaction(OER)and oxygen reduced reaction(O...Highly active bifunctional oxygen electrocatalysts accelerate the development of high-performance Zn-air battery,but suffer from the mismatched activities of oxygen evolution reaction(OER)and oxygen reduced reaction(ORR).Herein,highly integrated bifunctional oxygen electrocatalysts,cobalt-tin alloys coated by nitrogen doped carbon(CoSn@NC)are prepared by MOFs-derived method.In this hybrid catalyst,the binary CoSn nanoalloys mainly contribute to highly active OER process while the Co(or Sn)-N-C serves as ORR active sites.Rational interaction between CoSn and NC donates more rapid reaction kinetics than Pt/C(ORR)and IrO_(2)(OER).Such CoSn@NC holds a promise as air-cathode electrocatalyst in Zn-air battery,superior to Pt/C+IrO_(2)catalyst.First-principles calculations predict that CoSn alloys can upgrade charge redistribution on NC and promote the transfer to reactants,thus optimizing the adsorption strength of oxygen-containing intermediates to boost the overall reactivity.The tuning of oxygenate adsorption by interactions between alloy and heteroatom-doped carbon can guide the design of bifunctional oxygen electrocatalysts.展开更多
Large surface area,high conductivity,and rich active site of carbon electrode materials are necessary characteristics for energy storage devices.However,high conductivity and high nitrogen doping of carbon electrode m...Large surface area,high conductivity,and rich active site of carbon electrode materials are necessary characteristics for energy storage devices.However,high conductivity and high nitrogen doping of carbon electrode materials are difficult to coordinate.Here,a facile method via the carbonization of nitrogen-containing Schiff base polymer has been developed to prepare high conductivity and high nitrogen-doped hierarchical porous carbon.The organic components with a benzene ring structure in the polymer promote the formation of more sp^(2)-graphitized carbon,which is beneficial for the improvement of electrical conductivity.Nitrogen-doped hierarchical porous carbon calcined at 900℃ under the NH3 atmosphere possesses high nitrogen content of 7.48 at%,a large specific surface area of 1613.2m2/g,and high electrical conductivity of 2.7 S/cm.As electrode materials in an aqueous-based supercapacitor,nitrogen-doped hierarchical porous carbon exhibits superior specific capacitance of 385 F/g at 1 A/g as well as excellent rate performance(242 and 215 F/g at a current density of 100 and 200 A/g,respectively).In addition,the specific capacitance of electrode measured in a two-electrode system is 335 F/g at 1 A/g,and the long-term cycling stability can be achieved with more than 94%initial capacitance after 10000 cycles.The constructed symmetric supercapacitor delivers high energy density and high power density.The outstanding electrochemical performances combined with the novel and scalable synthetic approach make the nitrogen‐doped hierarchical porous carbon potential electrode material for electrochemical devices.展开更多
Metal cyanamides are an emerging class of functional materials with potential applications in sustainable energy conversion and storage technologies such as catalysis,supercapacitors,photoluminescence and next-gen bat...Metal cyanamides are an emerging class of functional materials with potential applications in sustainable energy conversion and storage technologies such as catalysis,supercapacitors,photoluminescence and next-gen batteries.The[NCN]^(2-)as the anion,which is isolobal with[O]^(2-)endows metal cyanamides with similar physicochemical properties as oxides and chalcogenides.Whereas the unique quasI-linear structure and electronic resonance between[N=C=N]^(2-)and[N-C≡N]^(2-)of[NCN]entity bring out superior properties beyond oxides and chalcogenides.In this review,we present research status,challenges,and the recent striking progress on the metal cyanamides in the synthesis and applications.Specifically,the characteristic structures,physicochemical properties,synthetic methods with corresponding merits/demerits and latest applications in energy conversion and storage of cyanamides are summarized.The detailed outlooks for the new compounds design,morphology manipulation and potential applications are also exhibited.展开更多
Iron-based superconductor family FeX(X=S,Se,Te)has been one of the research foci in physics and material science due to their record-breaking superconducting temperature(FeSe film)and rich physical phenomena.Recently,...Iron-based superconductor family FeX(X=S,Se,Te)has been one of the research foci in physics and material science due to their record-breaking superconducting temperature(FeSe film)and rich physical phenomena.Recently,FeS,the least studied Fe X compound(due to the difficulty in synthesizing high quality macroscopic crystals)attracted much attention because of its puzzling superconducting pairing symmetry.In this work,combining scanning tunneling microscopy and angle resolved photoemission spectroscopy(ARPES)with sub-micron spatial resolution,we investigate the intrinsic electronic structures of superconducting FeS from individual single crystalline domains.Unlike FeTe or FeSe,FeS remains identical tetragonal structure from room temperature down to 5 K,and the band structures observed can be well reproduced by our ab-initio calculations.Remarkably,mixed with the 1×1 tetragonal metallic phase,we also observe the coexistence of √5×√5 reconstructed insulating phase in the crystal,which not only helps explain the unusual properties of FeS,but also demonstrates the importance of using spatially resolved experimental tools in the study of this compound.展开更多
The growing demand for new therapeutic strategies in the medical and pharmaceutic fields has resulted in a pressing need for novel druggable targets.Paradoxically,however,the targets of certain drugs that are already ...The growing demand for new therapeutic strategies in the medical and pharmaceutic fields has resulted in a pressing need for novel druggable targets.Paradoxically,however,the targets of certain drugs that are already widely used in clinical practice have largely not been annotated.Because the pharmacologic effects of a drug can only be appreciated when its interactions with cellular components are clearly delineated,an integrated deconvolution of drug-target interactions for each drug is necessary.The emerging field of chemical proteomics represents a powerful mass spectrometry(MS)-based affinity chromatography approach for identifying proteome-wide small molecule-protein interactions and mapping these interactions to signaling and metabolic pathways.This technique could comprehensively characterize drug targets,profile the toxicity of known drugs,and identify possible off-target activities.With the use of this technique,candidate drug molecules could be optimized,and predictable side effects might consequently be avoided.Herein,we provide a holistic overview of the major chemical proteomic approaches and highlight recent advances in this area as well as its potential applications in drug discovery.展开更多
Pyrrolic and pyridinic N dopants can dramatically increase the electrochemical activities of carbon and conducting polymers.Although N-doped conducting polymers suffer from rapid degradation,their carbon counterpart o...Pyrrolic and pyridinic N dopants can dramatically increase the electrochemical activities of carbon and conducting polymers.Although N-doped conducting polymers suffer from rapid degradation,their carbon counterpart of extraordinary capacitance has remarkable rate performance and cycling endurance thanks to carbon’s excellent electrical conductivity.But high nitrogen content and high electrical conductivity are difficult to achieve in a high-surface-area carbon,because the high chemical vapor deposition(CVD)temperature required for obtaining high conductivity also destabilizes under-coordinated pyrrolic and pyridinic nitrogen and tends to lower the surface area.Here we resolve this dilemma by using SiO2 as an effective N-fixation additive,which stabilizes the N-rich nano few-layer sp2-carbon construct in1000℃CVD.This enables a scalable sol-gel/CVD fabrication process for few-layer carbon electrodes of extraordinary capacitance(690 F g^-1).The electrodes have excellent rate performance and can maintain90%of their initial capacitance after 30,000 cycles,thus potentially suitable for practical applications.展开更多
Alloying-type metal sulfides with high sodiation activity and theoretical capacity are promising anode materials for high energy density sodium ion batteries.However,the large volume change and the migratory and aggre...Alloying-type metal sulfides with high sodiation activity and theoretical capacity are promising anode materials for high energy density sodium ion batteries.However,the large volume change and the migratory and aggregation behavior of metal atoms will cause severe capacity decay during the charge/discharge process.Herein,a robust and conductive TiS_(2)framework is integrated with a high-capacity SbS layer to construct a single phase(SbS)_(1.15)TiS_(2)superlattice for both high-capacity and fast Na^(+)storage.The metallic TiS_(2)sublayer with high electron activity acts as a robust and conductive skeleton to buffer the volume expansion caused by conversion and alloying reaction between Na+and SbS sublayer.Hence,high capacity and high rate capability can be synergistically realized in a single phase(SbS)_(1.15)TiS_(2)superlattice.The novel(SbS)_(1.15)TiS_(2)anode has a high charge capacity of 618 mAh g^(-1)at 0.2 C and superior rate performance and cycling stability(205 mAh g^(-1)at 35 C after 2,000 cycles).Furthermore,in situ and ex situ characterizations are applied to get an insight into the multi-step reaction mechanism.The integrity of robust Na-Ti-S skeleton during(dis)charge process can be confirmed.This superlattice construction idea to integrate the Na^(+)-active unit and electron-active unit would provide a new avenue for exploring high-performance anode materials for advanced sodium-ion batteries.展开更多
In-situ polymerized electrolytes significantly enhance the interfacial compatibility of lithium metal batteries(LMBs). Typically,in-situ polymerized 1,3-dioxolane(PDOL) exhibits low interfacial resistance, yet still s...In-situ polymerized electrolytes significantly enhance the interfacial compatibility of lithium metal batteries(LMBs). Typically,in-situ polymerized 1,3-dioxolane(PDOL) exhibits low interfacial resistance, yet still suffers from low ionic conductivity and a narrow electrochemical stability window(ESW). Here, an ultra-stable PDOL-based polymer electrolyte is developed by incorporating plasticizers of tetramethylene sulfone(TMS) and fluorinated ethylene carbonate(FEC) into the 3D cross-linked network, achieving a significant enhancement in the transport capacity and efficiency of Li-ion. The ionic conductivity reaches3.63×10^(-4)S cm^(-1)even at room temperature, and the transference number(tLi^(+)) is even higher at 0.85. Furthermore, the ESW of this electrolyte can be increased to 4.5 V with the addition of TMS, which forms a thin and robust antioxidant cathode-electrolyte interface(CEI) on the surface of high-voltage LiCoO_(2). FEC generates an inorganic-rich solid-electrolyte interface(SEI) on the Li anode, which effectively inhibits the growth of lithium dendrites. Benefiting from the aforementioned advantages, the highvoltage lithium metal battery demonstrates outstanding long-cycle stability, with 93.2% capacity retention after 200 cycles. This work offers a straightforward and accessible method for the practical implementation of high energy density in-situ polymerized solid-state LMBs.展开更多
Crystal structure determines electrochemical energy storage characteristics;this is the underlying logic of material design.To date,hundreds of electrode materials have been developed to pursue superior performance.Ho...Crystal structure determines electrochemical energy storage characteristics;this is the underlying logic of material design.To date,hundreds of electrode materials have been developed to pursue superior performance.However,it remains a great challenge to understand the fundamental structure–performance relationship and achieve quantitative crystal structure design for efficient energy storage.In this review,we introduce the concept of crystal packing factor(PF),which can quantify crystal packing density.We then present and classify the typical crystal structures of attractive cathode/anode materials.Comparative PF analyses of different materials,including polymorphs,isomorphs,and others,are performed to clarify the influence of crystal packing density on energy storage performance through electronic and ionic conductivities.Notably,the practical electronic/ionic conductivities of energy storage materials are based on their intrinsic characteristics related to the PF yet are also affected by extrinsic factors.The PF provides a novel avenue for understanding the electrochemical performance of pristine materials and may offer guidance on designing better materials.Additional approaches involve size regulation,doping,carbon additives,and other methods.We also propose extended PF concepts to understand charge storage and transport behavior at different scales.Finally,we provide our insights on the major challenges and prospective solutions in this highly exciting field.展开更多
有机电极具有结构可设计性强、容量大、可容纳大离子等优点.然而,在钠离子电池中,有机电极材料的容量仍然很低,且其在有机电解质中的高溶解度导致其寿命较短.如何通过化合物设计来提高其性能一直是研究人员关注的问题.本研究通过简单方...有机电极具有结构可设计性强、容量大、可容纳大离子等优点.然而,在钠离子电池中,有机电极材料的容量仍然很低,且其在有机电解质中的高溶解度导致其寿命较短.如何通过化合物设计来提高其性能一直是研究人员关注的问题.本研究通过简单方法将氨基酸接枝到有机化合物上,提高了其容量和循环稳定性.首先,氨基酸之间的氢键使其形成更稳定的层状结构;氨基酸基团在有机电极材料和羧甲基纤维素粘合剂之间形成分子间相互作用,降低界面阻力,显著提高循环稳定性,使得钠离子电池循环次数超过2000次.其次,实验和计算结果表明,氨基酸基团提供了Na^(+)转运途径和额外的可逆存储位点,从而提高了比容量(~300 mA h g^(-1)).本策略可以启发未来钠离子电池的有机分子设计.展开更多
Two‐dimensional(2D)ferroelectrics have attracted considerable attention due to their potential in the development of devices of miniaturization and multifunction.Although several van der Waals(vdW)‐layered materials...Two‐dimensional(2D)ferroelectrics have attracted considerable attention due to their potential in the development of devices of miniaturization and multifunction.Although several van der Waals(vdW)‐layered materials show ferroelectricity,the experimental demonstrations of ferroelectric behavior in monolayers are very limited.Here we report the observation of room‐temperature out‐of‐plane switchable electric polarization in supported MoS_(2) monolayers exfoliated from 3R‐stacked bulk crystals under ambient conditions.Using in situ piezoelectric force microscopy and Kelvin probe force microscopy in a glovebox,we reveal that trapped water/ice molecules are responsible for this switchable electric polarization and this conclusion is strongly supported by theoretical simulations.It is worth noting that the water/ice trapping in the monolayers exfoliated from 2H‐stacked MoS_(2) crystals is not as much as that in 3R monolayers and,consequently,the out‐of‐plane electric polarization is missing there.Our findings indicate that monolayers with a trapped single layer of polar molecules might be emerging alternatives to 2D ferroelectrics.Furthermore,the stacking sequences may bring new properties and applications to 2D vdW materials not only when we stack them up but also when we thin them down.展开更多
Golgi membrane protein 1(GOLM1/GP73)is a serum marker of hepatocellular carcinoma(HCC).We have previously shown that mTOR promoted tumorigenesis of HCC through stimulating GOLM1 expression.In this study,we demonstrate...Golgi membrane protein 1(GOLM1/GP73)is a serum marker of hepatocellular carcinoma(HCC).We have previously shown that mTOR promoted tumorigenesis of HCC through stimulating GOLM1 expression.In this study,we demonstrated that the mammalian target of rapamycin(mTOR)was a negative regulator of microRNA-145(miR-145)expression.miR-145 inhibited GOLM1 expression by targeting a coding sequence of GOLM1 gene.GOLM1 and miR-145 were inversely correlated in human HCC tissues.GOLM1-enriched exosomes activated the glycogen synthase kinase-3β/matrix metalloproteinases(GSK-3β/MMPs)signaling axis of recipient cells and accelerated cell proliferation and migration.In contrast,miR-145 suppressed tumorigenesis and metastasis.We suggest that mTOR/miR-145/GOLM1 signaling pathway should be targeted for HCC treatment.展开更多
Although many materials have been studied for the purpose of microwave absorption,SiO_(2) has never been reported as a good candidate.In this study,we present for the first time that doped,microwave conductive SiO_(2)...Although many materials have been studied for the purpose of microwave absorption,SiO_(2) has never been reported as a good candidate.In this study,we present for the first time that doped,microwave conductive SiO_(2) nanoparticles can possess an excellent microwave absorbing performance.A large microwave reflection loss(RL)of−55.09 dB can be obtained.The large microwave absorption originates mainly from electrical relaxation rather than the magnetic relaxation of the incoming microwave field.The electrical relaxation is attributed to a large electrical conductivity that is enabled by the incorporation of heterogeneous(N,C and Cl)atoms.The removal of the magnetic susceptibility only results in a negligible influence of the microwave absorption.In contrast,the removal of the heterogeneous atoms leads to a large decrease in the electrical conductivity and microwave absorption performance.Meanwhile,the microwave absorption characteristics can be largely adjusted with a change of the thickness,which provides large flexibility for various microwave absorption applications.展开更多
Although single-atom catalysts significantly improve the atom utilization efficiency,the multistep preparation procedures are complicated and difficult to control.Herein,we demonstrate that one-step in situ synthesis ...Although single-atom catalysts significantly improve the atom utilization efficiency,the multistep preparation procedures are complicated and difficult to control.Herein,we demonstrate that one-step in situ synthesis of the single-atom Pt anchored in single-crystal MoC(Pt_(1)/MoC)by using facile and controllable arc-discharge strategy under extreme conditions.The high temperature(up to 4000℃)provides the sufficient energy for atom dispersion and overall stability by forming thermodynamically favourable metal-support interactions.The high-temperature-stabilized Pt1/MoC exhibits outstanding performance and excellent thermal stability as durable catalyst for selective quinoline hydrogenation.The initial turnover frequency of 3710 h^(-1)is greater than those of previously reported samples by an order of magnitude under 2 MPa H_(2)at 100℃.The catalyst also shows broad scope activity toward hydrogenation containing unsaturated groups of C=C,C=N,and C=O.The facile,one-step,and fast arc-discharge method provides an effective avenue for single-atom catalyst fabrication that is conventionally challenging.展开更多
Interactions between incident electromagnetic energy and matter are of critical importance for numerous civil and military applications such as photocatalysis,solar cells,optics,radar detection,communications,informat...Interactions between incident electromagnetic energy and matter are of critical importance for numerous civil and military applications such as photocatalysis,solar cells,optics,radar detection,communications,information processing and transport et al.Traditional mechanisms for such interactions in the microwave frequency mainly rely on dipole rotations and magnetic domain resonance.In this study,we present the first report of the microwave absorption of Al/H2 treated TiO_(2) nanoparticles,where the A_(l)/H_(2) treatment not only induces structural and optical property changes,but also largely improves the microwave absorption performance of TiO_(2) nanoparticles.Moreover,the frequency of the microwave absorption can be finely controlled with the treatment temperature,and the absorption efficiency can reach optimal values with a careful temperature tuning.A large reflection loss of58.02 dB has been demonstrated with 3.1mm TiO_(2) coating when the treating temperature is 700℃.The high efficiency of microwave absorption is most likely linked to the disordering-induced property changes in the materials.Along with the increased microwave absorption properties are largely increased visiblelight and IR absorptions,and enhanced electrical conductivity and reduced skin-depth,which is likely related to the interfacial defects within the TiO_(2) nanoparticles caused by the Al/H2 treatment.展开更多
For energy storage system,it is still a huge challenge to achieve high energy density and high power density simultaneously.One potential solution is to fabricate electrochemical capacitors(ECs),which store electric e...For energy storage system,it is still a huge challenge to achieve high energy density and high power density simultaneously.One potential solution is to fabricate electrochemical capacitors(ECs),which store electric energy through surface ion adsorption or redox reactions.Here we report a new electrode material,heavy nitrogen-doped(9.29 at.%)black titania(TiO2-x:N).This unique hybrid material,consisting of conductive amorphous shells supported on nanocrystalline cores,has rapid N-mediated redox reaction(TiO2-xNy+zH++ze■-TiO2-xNyHz),especially in acidic solutions,providing a specific capacitance of 750 Fg-1at 2 m V s-1(707 Fg-1at 1 A g-1),great rate capability(503 F g-1at 20 Ag-1),and maintain stable after initial fading.Being a new developed supercapacitor material,nitrogen-doped black titania may revive the oxide-based supercapacitors.展开更多
Rationally designed heterostructures provide attractive prospects for energy storage electrodes by combining different active materials with distinct electrochemical properties.Herein,through a phase separation strate...Rationally designed heterostructures provide attractive prospects for energy storage electrodes by combining different active materials with distinct electrochemical properties.Herein,through a phase separation strategy,a heterostructure of SnO_(2) encapsulated by amorphous Nb_(2)O_(5) is spontaneously synthesized.Insertion-type anode Nb_(2)O_(5) outer shell,playing as reaction containers and fast ionic pathways,physically inhibits the Sn atoms’migration and enhances the reaction kinetics.Moreover,strong chemical interactions are found at the SnO_(2)/Nb_(2)O_(5) interfaces,which ensure the solid encapsulation of the SnO_(2) cores even after 500 cycles.When used for lithium-ion batteries,this heterostructured anode exhibits high cycling stability with a capacity of 626 mAhg^(-1) after 1000 cycles at 2Ag^(-1)(85% capacity retention)and good rate performance with the capacity of 340 mAhg^(-1) at 8Ag^(-1).展开更多
With an overall prevalence of about 70%in women at reproductive age,uterine leiomyomas(ULs)are the most prevalent benign tumors in the female reproductive tract[1].Due to high lesion recurrence,the current treatment o...With an overall prevalence of about 70%in women at reproductive age,uterine leiomyomas(ULs)are the most prevalent benign tumors in the female reproductive tract[1].Due to high lesion recurrence,the current treatment of multiple leiomyomas for fertility or uterine preservation is a daunting task and only provides partial or temporary relief[2].展开更多
Aqueous supercapacitors are powerful energy sources,but they are limited by energy density that is much lower than lithium-ion batteries.Since raising the voltage beyond the thermodynamic potential for water splitting...Aqueous supercapacitors are powerful energy sources,but they are limited by energy density that is much lower than lithium-ion batteries.Since raising the voltage beyond the thermodynamic potential for water splitting(1.23 V)can boost the energy density,there has been much effort on water-stabilizing salvation additives such as Li_(2)SO_(4) that can provide an aqueous electrolyte capable of withstanding~1.8 V.Guided by the first-principles calculations that reveal water can promote hydrogen and oxygen evolution reactions,here,we pursue a new strategy of covering the electrode with a dense electroplated polymerized polyacrylic acid,which is an electron insulator but a proton conductor and proton reservoir.The combined effect of salvation and coating expands the electrochemical window throughout pH 3 to pH 10 to 2.4V for both fast and slow proton-mediated redox reactions.This allows activated carbon to quadruple the energy density,a kilogram of nitrogen-doped graphene to provide 127 Watt-hour,and both to have improved endurance because of suppression of water-mediated corrosion.Therefore,aqueous supercapacitors can now achieve energy densities quite comparable to that of a lithium-ion battery,but at 100 times the charging/discharging speed and cycle durability.展开更多
基金National Natural Science Foundation of China(52202327)Science and Technology Commission of Shanghai Municipality(22ZR1471300)+2 种基金National Science Foundation of China(Grant 51972326)Youth Innovation Promotion Association CAS,Foundation Strengthening ProjectProgram of Shanghai Academic Research Leader(Grant 22XD1424300).
文摘Na-ion O3-type layered oxides are prospective cathodes for Na-ion batteries due to high energy density and low-cost.Nevertheless,such cathodes usually suffer from phase transitions,sluggish kinetics and air instability,making it difficult to achieve high performance solid-state sodium-ion batteries.Herein,the high-entropy design and Li doping strategy alleviate lattice stress and enhance ionic conductivity,achieving high-rate performance,air stability and electrochemically thermal stability for Na_(0.95)Li_(0.06)Ni_(0.25)Cu_(0.05)Fe_(0.15)Mn_(0.49)O_(2).This cathode delivers a high reversible capacity(141 mAh g^(−1)at 0.2C),excellent rate capability(111 mAh g^(−1)at 8C,85 mAh g^(−1)even at 20C),and long-term stability(over 85%capacity retention after 1000 cycles),which is attributed to a rapid and reversible O3–P3 phase transition in regions of low voltage and suppresses phase transition.Moreover,the compound remains unchanged over seven days and keeps thermal stability until 279℃.Remarkably,the polymer solid-state sodium battery assembled by this cathode provides a capacity of 92 mAh g^(−1)at 5C and keeps retention of 96%after 400 cycles.This strategy inspires more rational designs and could be applied to a series of O3 cathodes to improve the performance of solid-state Na-ion batteries.
基金This work was financially supported by Shanghai Science and Technology Innovation Action Plan(Program No.20DZ1204400)the Key Research Program of Frontier Science,Chinese Academy of Sciences(Grant No.QYZDJSSW-JSC013).
文摘Highly active bifunctional oxygen electrocatalysts accelerate the development of high-performance Zn-air battery,but suffer from the mismatched activities of oxygen evolution reaction(OER)and oxygen reduced reaction(ORR).Herein,highly integrated bifunctional oxygen electrocatalysts,cobalt-tin alloys coated by nitrogen doped carbon(CoSn@NC)are prepared by MOFs-derived method.In this hybrid catalyst,the binary CoSn nanoalloys mainly contribute to highly active OER process while the Co(or Sn)-N-C serves as ORR active sites.Rational interaction between CoSn and NC donates more rapid reaction kinetics than Pt/C(ORR)and IrO_(2)(OER).Such CoSn@NC holds a promise as air-cathode electrocatalyst in Zn-air battery,superior to Pt/C+IrO_(2)catalyst.First-principles calculations predict that CoSn alloys can upgrade charge redistribution on NC and promote the transfer to reactants,thus optimizing the adsorption strength of oxygen-containing intermediates to boost the overall reactivity.The tuning of oxygenate adsorption by interactions between alloy and heteroatom-doped carbon can guide the design of bifunctional oxygen electrocatalysts.
基金Peng Wang and Xiaohuan Qi contributed equally to this study.This study was supported by the National Key Research and Development Program(Grant No.2016YFB0901600)National Natural Science Foundation of China(Grant Nos.21801247,51672295,51972326,and 21871008)the Key Research Program of Frontier Chinese Academy of Sciences(Grant No.QYZDJ-SSW-JSC013).
文摘Large surface area,high conductivity,and rich active site of carbon electrode materials are necessary characteristics for energy storage devices.However,high conductivity and high nitrogen doping of carbon electrode materials are difficult to coordinate.Here,a facile method via the carbonization of nitrogen-containing Schiff base polymer has been developed to prepare high conductivity and high nitrogen-doped hierarchical porous carbon.The organic components with a benzene ring structure in the polymer promote the formation of more sp^(2)-graphitized carbon,which is beneficial for the improvement of electrical conductivity.Nitrogen-doped hierarchical porous carbon calcined at 900℃ under the NH3 atmosphere possesses high nitrogen content of 7.48 at%,a large specific surface area of 1613.2m2/g,and high electrical conductivity of 2.7 S/cm.As electrode materials in an aqueous-based supercapacitor,nitrogen-doped hierarchical porous carbon exhibits superior specific capacitance of 385 F/g at 1 A/g as well as excellent rate performance(242 and 215 F/g at a current density of 100 and 200 A/g,respectively).In addition,the specific capacitance of electrode measured in a two-electrode system is 335 F/g at 1 A/g,and the long-term cycling stability can be achieved with more than 94%initial capacitance after 10000 cycles.The constructed symmetric supercapacitor delivers high energy density and high power density.The outstanding electrochemical performances combined with the novel and scalable synthetic approach make the nitrogen‐doped hierarchical porous carbon potential electrode material for electrochemical devices.
基金financial support from the National Natural Science Foundation of China(Grants 21871008,21801247 and 21905292)the Shanghai Science and Technology Innovation Action Plan(Program No.20dz1204400)the Key Research Program of Frontier Sciences,Chinese Academy of Sciences(Grant No.QYZDJ-SSWJSC013)。
文摘Metal cyanamides are an emerging class of functional materials with potential applications in sustainable energy conversion and storage technologies such as catalysis,supercapacitors,photoluminescence and next-gen batteries.The[NCN]^(2-)as the anion,which is isolobal with[O]^(2-)endows metal cyanamides with similar physicochemical properties as oxides and chalcogenides.Whereas the unique quasI-linear structure and electronic resonance between[N=C=N]^(2-)and[N-C≡N]^(2-)of[NCN]entity bring out superior properties beyond oxides and chalcogenides.In this review,we present research status,challenges,and the recent striking progress on the metal cyanamides in the synthesis and applications.Specifically,the characteristic structures,physicochemical properties,synthetic methods with corresponding merits/demerits and latest applications in energy conversion and storage of cyanamides are summarized.The detailed outlooks for the new compounds design,morphology manipulation and potential applications are also exhibited.
基金Project supported by CAS-Shanghai Science Research Center,China(Grant No.CAS-SSRC-YH-2015-01)the National Key R&D Program of China(Grant No.2017YFA0305400)+4 种基金the National Natural Science Foundation of China(Grant Nos.11674229,11227902,and 11604207)the EPSRC Platform Grant(Grant No.EP/M020517/1)Hefei Science Center,Chinese Academy of Sciences(Grant No.2015HSC-UE013)Science and Technology Commission of Shanghai Municipality,China(Grant No.14520722100)the Strategic Priority Research Program(B)of the Chinese Academy of Sciences(Grant No.XDB04040200)。
文摘Iron-based superconductor family FeX(X=S,Se,Te)has been one of the research foci in physics and material science due to their record-breaking superconducting temperature(FeSe film)and rich physical phenomena.Recently,FeS,the least studied Fe X compound(due to the difficulty in synthesizing high quality macroscopic crystals)attracted much attention because of its puzzling superconducting pairing symmetry.In this work,combining scanning tunneling microscopy and angle resolved photoemission spectroscopy(ARPES)with sub-micron spatial resolution,we investigate the intrinsic electronic structures of superconducting FeS from individual single crystalline domains.Unlike FeTe or FeSe,FeS remains identical tetragonal structure from room temperature down to 5 K,and the band structures observed can be well reproduced by our ab-initio calculations.Remarkably,mixed with the 1×1 tetragonal metallic phase,we also observe the coexistence of √5×√5 reconstructed insulating phase in the crystal,which not only helps explain the unusual properties of FeS,but also demonstrates the importance of using spatially resolved experimental tools in the study of this compound.
基金supported by grants from the National Basic Research Program of China (No.2011CB910703)the National 863 High Tech Foundation (No.2007AA021205)Chinese NSFC (No.81072022)
文摘The growing demand for new therapeutic strategies in the medical and pharmaceutic fields has resulted in a pressing need for novel druggable targets.Paradoxically,however,the targets of certain drugs that are already widely used in clinical practice have largely not been annotated.Because the pharmacologic effects of a drug can only be appreciated when its interactions with cellular components are clearly delineated,an integrated deconvolution of drug-target interactions for each drug is necessary.The emerging field of chemical proteomics represents a powerful mass spectrometry(MS)-based affinity chromatography approach for identifying proteome-wide small molecule-protein interactions and mapping these interactions to signaling and metabolic pathways.This technique could comprehensively characterize drug targets,profile the toxicity of known drugs,and identify possible off-target activities.With the use of this technique,candidate drug molecules could be optimized,and predictable side effects might consequently be avoided.Herein,we provide a holistic overview of the major chemical proteomic approaches and highlight recent advances in this area as well as its potential applications in drug discovery.
基金supported by the National Key Research and Development Program of China(Grant no.2016YFB0901600)the National Natural Science Foundation of China(Grant nos.51922103 and 51672301)the Key Research Program of Chinese Academy of Sciences(Grant no.QYZDJSSW-JSC013)。
文摘Pyrrolic and pyridinic N dopants can dramatically increase the electrochemical activities of carbon and conducting polymers.Although N-doped conducting polymers suffer from rapid degradation,their carbon counterpart of extraordinary capacitance has remarkable rate performance and cycling endurance thanks to carbon’s excellent electrical conductivity.But high nitrogen content and high electrical conductivity are difficult to achieve in a high-surface-area carbon,because the high chemical vapor deposition(CVD)temperature required for obtaining high conductivity also destabilizes under-coordinated pyrrolic and pyridinic nitrogen and tends to lower the surface area.Here we resolve this dilemma by using SiO2 as an effective N-fixation additive,which stabilizes the N-rich nano few-layer sp2-carbon construct in1000℃CVD.This enables a scalable sol-gel/CVD fabrication process for few-layer carbon electrodes of extraordinary capacitance(690 F g^-1).The electrodes have excellent rate performance and can maintain90%of their initial capacitance after 30,000 cycles,thus potentially suitable for practical applications.
基金supported by the National Key Research and Development Program of China(2019YFA0210600)the National Natural Science Foundation of China(51922103 and 51972326)。
文摘Alloying-type metal sulfides with high sodiation activity and theoretical capacity are promising anode materials for high energy density sodium ion batteries.However,the large volume change and the migratory and aggregation behavior of metal atoms will cause severe capacity decay during the charge/discharge process.Herein,a robust and conductive TiS_(2)framework is integrated with a high-capacity SbS layer to construct a single phase(SbS)_(1.15)TiS_(2)superlattice for both high-capacity and fast Na^(+)storage.The metallic TiS_(2)sublayer with high electron activity acts as a robust and conductive skeleton to buffer the volume expansion caused by conversion and alloying reaction between Na+and SbS sublayer.Hence,high capacity and high rate capability can be synergistically realized in a single phase(SbS)_(1.15)TiS_(2)superlattice.The novel(SbS)_(1.15)TiS_(2)anode has a high charge capacity of 618 mAh g^(-1)at 0.2 C and superior rate performance and cycling stability(205 mAh g^(-1)at 35 C after 2,000 cycles).Furthermore,in situ and ex situ characterizations are applied to get an insight into the multi-step reaction mechanism.The integrity of robust Na-Ti-S skeleton during(dis)charge process can be confirmed.This superlattice construction idea to integrate the Na^(+)-active unit and electron-active unit would provide a new avenue for exploring high-performance anode materials for advanced sodium-ion batteries.
基金supported by the National Natural Science Foundation of China (52202327)Science and Technology Commission of Shanghai Municipality (22ZR1471300)。
文摘In-situ polymerized electrolytes significantly enhance the interfacial compatibility of lithium metal batteries(LMBs). Typically,in-situ polymerized 1,3-dioxolane(PDOL) exhibits low interfacial resistance, yet still suffers from low ionic conductivity and a narrow electrochemical stability window(ESW). Here, an ultra-stable PDOL-based polymer electrolyte is developed by incorporating plasticizers of tetramethylene sulfone(TMS) and fluorinated ethylene carbonate(FEC) into the 3D cross-linked network, achieving a significant enhancement in the transport capacity and efficiency of Li-ion. The ionic conductivity reaches3.63×10^(-4)S cm^(-1)even at room temperature, and the transference number(tLi^(+)) is even higher at 0.85. Furthermore, the ESW of this electrolyte can be increased to 4.5 V with the addition of TMS, which forms a thin and robust antioxidant cathode-electrolyte interface(CEI) on the surface of high-voltage LiCoO_(2). FEC generates an inorganic-rich solid-electrolyte interface(SEI) on the Li anode, which effectively inhibits the growth of lithium dendrites. Benefiting from the aforementioned advantages, the highvoltage lithium metal battery demonstrates outstanding long-cycle stability, with 93.2% capacity retention after 200 cycles. This work offers a straightforward and accessible method for the practical implementation of high energy density in-situ polymerized solid-state LMBs.
基金supported by the National Natural Science Foundation of China(52202327)Science and Technology Commission of Shanghai Municipality(22ZR1471300)the Key Research Program of Frontier Science,Chinese Academy of Sciences(Grant No.QYZDJ-SSW-JSC013 and KGZD-EW-T06).
文摘Crystal structure determines electrochemical energy storage characteristics;this is the underlying logic of material design.To date,hundreds of electrode materials have been developed to pursue superior performance.However,it remains a great challenge to understand the fundamental structure–performance relationship and achieve quantitative crystal structure design for efficient energy storage.In this review,we introduce the concept of crystal packing factor(PF),which can quantify crystal packing density.We then present and classify the typical crystal structures of attractive cathode/anode materials.Comparative PF analyses of different materials,including polymorphs,isomorphs,and others,are performed to clarify the influence of crystal packing density on energy storage performance through electronic and ionic conductivities.Notably,the practical electronic/ionic conductivities of energy storage materials are based on their intrinsic characteristics related to the PF yet are also affected by extrinsic factors.The PF provides a novel avenue for understanding the electrochemical performance of pristine materials and may offer guidance on designing better materials.Additional approaches involve size regulation,doping,carbon additives,and other methods.We also propose extended PF concepts to understand charge storage and transport behavior at different scales.Finally,we provide our insights on the major challenges and prospective solutions in this highly exciting field.
基金supported by the National Key Research and Development Program of China(2019YFA0210600)the National Natural Science Foundation of China(51922103 and BC0500463)。
文摘有机电极具有结构可设计性强、容量大、可容纳大离子等优点.然而,在钠离子电池中,有机电极材料的容量仍然很低,且其在有机电解质中的高溶解度导致其寿命较短.如何通过化合物设计来提高其性能一直是研究人员关注的问题.本研究通过简单方法将氨基酸接枝到有机化合物上,提高了其容量和循环稳定性.首先,氨基酸之间的氢键使其形成更稳定的层状结构;氨基酸基团在有机电极材料和羧甲基纤维素粘合剂之间形成分子间相互作用,降低界面阻力,显著提高循环稳定性,使得钠离子电池循环次数超过2000次.其次,实验和计算结果表明,氨基酸基团提供了Na^(+)转运途径和额外的可逆存储位点,从而提高了比容量(~300 mA h g^(-1)).本策略可以启发未来钠离子电池的有机分子设计.
基金supported by the National Key Research and Development Program of China(No.2021YFA 1200800)the Start‐up Funds of Wuhan Universitysupported by the National Research Foundation,Singapore,under its Competitive Research Programmer(No.NRF‐CRP22‐2019‐0007).
文摘Two‐dimensional(2D)ferroelectrics have attracted considerable attention due to their potential in the development of devices of miniaturization and multifunction.Although several van der Waals(vdW)‐layered materials show ferroelectricity,the experimental demonstrations of ferroelectric behavior in monolayers are very limited.Here we report the observation of room‐temperature out‐of‐plane switchable electric polarization in supported MoS_(2) monolayers exfoliated from 3R‐stacked bulk crystals under ambient conditions.Using in situ piezoelectric force microscopy and Kelvin probe force microscopy in a glovebox,we reveal that trapped water/ice molecules are responsible for this switchable electric polarization and this conclusion is strongly supported by theoretical simulations.It is worth noting that the water/ice trapping in the monolayers exfoliated from 2H‐stacked MoS_(2) crystals is not as much as that in 3R monolayers and,consequently,the out‐of‐plane electric polarization is missing there.Our findings indicate that monolayers with a trapped single layer of polar molecules might be emerging alternatives to 2D ferroelectrics.Furthermore,the stacking sequences may bring new properties and applications to 2D vdW materials not only when we stack them up but also when we thin them down.
基金supported by National Basic Research Program of China 973 Program (2015CB553802)the National Natural Science Foundation of China (81730078)Chinese Academy of Medical Sciences Innovation Fund for Medical Sciences (CIFMS2016-I2M-1-001)
文摘Golgi membrane protein 1(GOLM1/GP73)is a serum marker of hepatocellular carcinoma(HCC).We have previously shown that mTOR promoted tumorigenesis of HCC through stimulating GOLM1 expression.In this study,we demonstrated that the mammalian target of rapamycin(mTOR)was a negative regulator of microRNA-145(miR-145)expression.miR-145 inhibited GOLM1 expression by targeting a coding sequence of GOLM1 gene.GOLM1 and miR-145 were inversely correlated in human HCC tissues.GOLM1-enriched exosomes activated the glycogen synthase kinase-3β/matrix metalloproteinases(GSK-3β/MMPs)signaling axis of recipient cells and accelerated cell proliferation and migration.In contrast,miR-145 suppressed tumorigenesis and metastasis.We suggest that mTOR/miR-145/GOLM1 signaling pathway should be targeted for HCC treatment.
基金the support from the U.S.National Science Foundation(DMR-1609061)the College of Arts and Sciences,University of Missouri–Kansas City+3 种基金the support from the National Science Fund for Distinguished Young Scholars of China(No.61525404)the support from the National Natural Science Foundation of China(Grant No.51372080)the support from the National Natural Science Foundation of China(U1765105)the support from the National Key Research and Development Program of China(2016YFB0901600).
文摘Although many materials have been studied for the purpose of microwave absorption,SiO_(2) has never been reported as a good candidate.In this study,we present for the first time that doped,microwave conductive SiO_(2) nanoparticles can possess an excellent microwave absorbing performance.A large microwave reflection loss(RL)of−55.09 dB can be obtained.The large microwave absorption originates mainly from electrical relaxation rather than the magnetic relaxation of the incoming microwave field.The electrical relaxation is attributed to a large electrical conductivity that is enabled by the incorporation of heterogeneous(N,C and Cl)atoms.The removal of the magnetic susceptibility only results in a negligible influence of the microwave absorption.In contrast,the removal of the heterogeneous atoms leads to a large decrease in the electrical conductivity and microwave absorption performance.Meanwhile,the microwave absorption characteristics can be largely adjusted with a change of the thickness,which provides large flexibility for various microwave absorption applications.
基金This work was financially supported by the National Key Research and Development Program of China(2016YFB0901600)the NSF of China(21872166)the Key Research Program of Chinese Academy of Sciences(QYZDJ-SSW-JSC013 and KGZD-EW-T06).
文摘Although single-atom catalysts significantly improve the atom utilization efficiency,the multistep preparation procedures are complicated and difficult to control.Herein,we demonstrate that one-step in situ synthesis of the single-atom Pt anchored in single-crystal MoC(Pt_(1)/MoC)by using facile and controllable arc-discharge strategy under extreme conditions.The high temperature(up to 4000℃)provides the sufficient energy for atom dispersion and overall stability by forming thermodynamically favourable metal-support interactions.The high-temperature-stabilized Pt1/MoC exhibits outstanding performance and excellent thermal stability as durable catalyst for selective quinoline hydrogenation.The initial turnover frequency of 3710 h^(-1)is greater than those of previously reported samples by an order of magnitude under 2 MPa H_(2)at 100℃.The catalyst also shows broad scope activity toward hydrogenation containing unsaturated groups of C=C,C=N,and C=O.The facile,one-step,and fast arc-discharge method provides an effective avenue for single-atom catalyst fabrication that is conventionally challenging.
基金M.G.and X.C.appreciate the support from the U.S.National Science Foundation(DMR-1609061)the College of Arts and Sciences,University of MissouriKansas City.X.Tan thanks the support from the National Natural Science Foundation of China(11374181)+3 种基金F.Huang acknowledged the support from the National Key Research and Development Program of China(Grant No.2016YFB0901600)the National Science Foundation of China(Grant Nos.51402334 and 51502331)the Science and Technology Commission of Shanghai(Grant No.14520722000)the Key Research Program of Chinese Academy of Sciences(Grant No.KGZD-EW-T06).
文摘Interactions between incident electromagnetic energy and matter are of critical importance for numerous civil and military applications such as photocatalysis,solar cells,optics,radar detection,communications,information processing and transport et al.Traditional mechanisms for such interactions in the microwave frequency mainly rely on dipole rotations and magnetic domain resonance.In this study,we present the first report of the microwave absorption of Al/H2 treated TiO_(2) nanoparticles,where the A_(l)/H_(2) treatment not only induces structural and optical property changes,but also largely improves the microwave absorption performance of TiO_(2) nanoparticles.Moreover,the frequency of the microwave absorption can be finely controlled with the treatment temperature,and the absorption efficiency can reach optimal values with a careful temperature tuning.A large reflection loss of58.02 dB has been demonstrated with 3.1mm TiO_(2) coating when the treating temperature is 700℃.The high efficiency of microwave absorption is most likely linked to the disordering-induced property changes in the materials.Along with the increased microwave absorption properties are largely increased visiblelight and IR absorptions,and enhanced electrical conductivity and reduced skin-depth,which is likely related to the interfacial defects within the TiO_(2) nanoparticles caused by the Al/H2 treatment.
基金financially supported by the National key R&D Program of China(2016YFB0901600)the Key Research Program of Chinese Academy of Sciences(QYZDJ-SSWJSC013)Chen IW was supported by U.S.Department of Energy BES grant DE-FG02-11ER46814used the facilities(Laboratory for Research on the Structure of Matter)supported by NSF grant DMR-1120901。
文摘For energy storage system,it is still a huge challenge to achieve high energy density and high power density simultaneously.One potential solution is to fabricate electrochemical capacitors(ECs),which store electric energy through surface ion adsorption or redox reactions.Here we report a new electrode material,heavy nitrogen-doped(9.29 at.%)black titania(TiO2-x:N).This unique hybrid material,consisting of conductive amorphous shells supported on nanocrystalline cores,has rapid N-mediated redox reaction(TiO2-xNy+zH++ze■-TiO2-xNyHz),especially in acidic solutions,providing a specific capacitance of 750 Fg-1at 2 m V s-1(707 Fg-1at 1 A g-1),great rate capability(503 F g-1at 20 Ag-1),and maintain stable after initial fading.Being a new developed supercapacitor material,nitrogen-doped black titania may revive the oxide-based supercapacitors.
基金supported by China Postdoctoral Science Foundation(2020M671242 and 2021T140688)the Special Research Assistant program of CASthe Super Postdoctoral Fellow Program of Shanghai。
文摘Rationally designed heterostructures provide attractive prospects for energy storage electrodes by combining different active materials with distinct electrochemical properties.Herein,through a phase separation strategy,a heterostructure of SnO_(2) encapsulated by amorphous Nb_(2)O_(5) is spontaneously synthesized.Insertion-type anode Nb_(2)O_(5) outer shell,playing as reaction containers and fast ionic pathways,physically inhibits the Sn atoms’migration and enhances the reaction kinetics.Moreover,strong chemical interactions are found at the SnO_(2)/Nb_(2)O_(5) interfaces,which ensure the solid encapsulation of the SnO_(2) cores even after 500 cycles.When used for lithium-ion batteries,this heterostructured anode exhibits high cycling stability with a capacity of 626 mAhg^(-1) after 1000 cycles at 2Ag^(-1)(85% capacity retention)and good rate performance with the capacity of 340 mAhg^(-1) at 8Ag^(-1).
基金supported by the National Natural Science Foundation of China(81830043)Non-profit Central Research Institute Fund of Chinese Academy of Medical Sciences(2020-PT320-003)。
文摘With an overall prevalence of about 70%in women at reproductive age,uterine leiomyomas(ULs)are the most prevalent benign tumors in the female reproductive tract[1].Due to high lesion recurrence,the current treatment of multiple leiomyomas for fertility or uterine preservation is a daunting task and only provides partial or temporary relief[2].
基金This work was financially supported by the National Key R&D Program of China(Grant no.2016YFB0901600)the Science and Technology Commission of Shanghai Municipality(Grant no.16JC1401700)+4 种基金the Key Research Program of Chinese Academy of Sciences(Grants no.QYZDJ-SSW-JSC013 and KGZD-EW-T06)T.Lin acknowledges support from Outstanding Youth Science Foundation(Grant No.51922103)W.Dong was funded by the China Postdoctoral Science Foundation(Grant No.2020M671242)the Special Research Assistant Program of Chinese Academy of Sciencesthe Super Postdoctoral Fellow Program of Shanghai.
文摘Aqueous supercapacitors are powerful energy sources,but they are limited by energy density that is much lower than lithium-ion batteries.Since raising the voltage beyond the thermodynamic potential for water splitting(1.23 V)can boost the energy density,there has been much effort on water-stabilizing salvation additives such as Li_(2)SO_(4) that can provide an aqueous electrolyte capable of withstanding~1.8 V.Guided by the first-principles calculations that reveal water can promote hydrogen and oxygen evolution reactions,here,we pursue a new strategy of covering the electrode with a dense electroplated polymerized polyacrylic acid,which is an electron insulator but a proton conductor and proton reservoir.The combined effect of salvation and coating expands the electrochemical window throughout pH 3 to pH 10 to 2.4V for both fast and slow proton-mediated redox reactions.This allows activated carbon to quadruple the energy density,a kilogram of nitrogen-doped graphene to provide 127 Watt-hour,and both to have improved endurance because of suppression of water-mediated corrosion.Therefore,aqueous supercapacitors can now achieve energy densities quite comparable to that of a lithium-ion battery,but at 100 times the charging/discharging speed and cycle durability.
