Due to its unique layered structure and excellent electrochemical properties,molybdenum disulfide(MoS_(2))demonstrates significant potential for applications in the energy storage field,particularly in supercapacitors...Due to its unique layered structure and excellent electrochemical properties,molybdenum disulfide(MoS_(2))demonstrates significant potential for applications in the energy storage field,particularly in supercapacitors.It is widely regarded as one of the most representative transition metal dichalcogenides.MoS_(2)possesses a high theoretical specific capacitance,abundant edge active sites,and favorable tunability and structural diversity,which provide it with a distinct advantage in the construction of advanced electrode structures.Additionally,the anisotropic characteristics of MoS_(2)concerning electron and ion transport offer more dimensions for regulating its electrochemical behavior.This work will systematically review various synthesis strategies for MoS_(2)and its recent advancements in energy storage,with a particular focus on the mechanisms by which interlayer spacing modulation affects energy storage behavior in supercapacitor configurations.The discussion will encompass a comprehensive logical framework that spans material structure modifications,electronic configuration evolution,and enhancements in macroscopic device performance.This review aims to provide theoretical support and practical guidance for the application of MoS_(2)in the next generation of highperformance energy storage devices.展开更多
1T-MoS_(2)nanosheets,with metallic conductivity and high capacity,hold great potential for lithium-ion capacitors(LICs),but suffer from sluggish reaction kinetics due to dense stacking.Herein,1T-MoS_(2)nanosheets with...1T-MoS_(2)nanosheets,with metallic conductivity and high capacity,hold great potential for lithium-ion capacitors(LICs),but suffer from sluggish reaction kinetics due to dense stacking.Herein,1T-MoS_(2)nanosheets with enlarged interlayer spacing,vertically bonded to reduced graphene oxide(rGO)(1T-MoS_(2)/rGO),were designed using a hydrothermal-assisted dispersion and intercalation strategy.The active nitrogen species derived from N,N-dimethylformamide(DMF)not only bridge the rGO and MoS_(2)through strong Mo-N-C bonds to promote the formation of dispersed MoS_(2)nanosheets,but also intercalate into the MoS_(2)structure,further enlarging the interlayer spacing.This unique structure synergistically enhances meso-and microscale mass transfer outside and inside of the few-layered nanosheets,significantly improving electrochemical reaction kinetics and reducing the kinetic mismatch between the anode and cathode.Consequently,the resulting 1T-MoS_(2)/rGO achieves a capacity of 500 mAh g^(-1)after 500 cycles at 5 A g^(-1)and a high rate performance of 587 mAh g^(-1)at a high rate of 10 A g^(-1).Moreover,the assembled 3D vertical 1T-MoS_(2)/rGO//AC LIC delivers a high energy density of 100.3 Wh kg^(-1)at a power density of1.0 kW kg^(-1),and long cycle stability with capacity retention as high as 91.02%after 5000 cycles at 2 A g^(-1).This work provides a generalizable strategy for engineering two-dimensional material-based electrodes,offering new insights into high-performance energy storage systems.展开更多
The hydrogen-bonded organic frameworks(HOFs)as a new type of porous framework materials have been widely studied in various areas.However,the lack of appropriate active sites,low intrinsic conductivity,and poor stabil...The hydrogen-bonded organic frameworks(HOFs)as a new type of porous framework materials have been widely studied in various areas.However,the lack of appropriate active sites,low intrinsic conductivity,and poor stability limited their performance in the field of electrocatalysis.Herein,we designed two 2D metal hydrogen-bonded organic frameworks(2D–M–HOF,M=Cu^(2+)or Ni^(2+))with coordination compounds based on 2,3,6,7,14,15-hexahydroxyl cyclotricatechylene and transition metal ions(Cu^(2+)and Ni^(2+)),respectively.The crystal structure of 2D–Cu–HOF is determined by continuous rotation electron diffraction,indicating an undulated 2D hydrogen-bond network with interlayeredπ-πstacking.The flexible structure of 2D–M–HOF leads to the formation of self-adaption interlayered sites,resulting in superior activity and selectivity in the electrocatalytic conversion of CO_(2) to C_(2) products,achieving a total Faradaic efficiency exceeding 80%due to the high-efficiency C–C coupling.The experimental results and density functional calculations verify that the undulated 2D–M–HOF enables the energetically favorable formation of*OCCHO intermediate.This work provides a promising strategy for designing HOF catalysts in electrocatalysis and related processes.展开更多
As artificial intelligence and big data become increasingly prevalent, resistive random-access memory (RRAM) has become one of the most promising alternatives for storing massive amounts of data. In this study, we emp...As artificial intelligence and big data become increasingly prevalent, resistive random-access memory (RRAM) has become one of the most promising alternatives for storing massive amounts of data. In this study, we employed high-quality crystalline TiN/Al_(2)O_(3)/BaTiO_(3)/Pt RRAM with an optimized thin Al_(2)O_(3) interlayer around 12 nm thick prepared using atomic layer deposition since the thickness of the interlayer affects the memory window size. After insertion of the Al_(2)O_(3) interlayer, the novel RRAM exhibited outstanding uniform resistive switching voltage and the ON/OFF memory window drastically increased from 10 to 103 without any discernible decline in performance. Moreover, the low-resistance state and high-resistance state operating current values decreased by almost one order and three orders of magnitude, respectively, thereby decreasing the power consumption for the RESET and SET processes by more than three and almost one order of magnitude, respectively. The device also exhibits multilevel resistive switching behavior when varying the applied voltage. Finally, we also developed a 6 6 crossbar array which demonstrated consistent and reliable resistive switching behavior with minimal variation. Hence, our approach holds great promise for producing state-of-the-art non-volatile resistive switching devices.展开更多
As an alternative for lithium-ion batteries(LIBs),sodium-ion batteries(SIBs)have lately received tremendous interest due to their abundant reserves as well as low cost.Nevertheless,the lack of suitable anode materials...As an alternative for lithium-ion batteries(LIBs),sodium-ion batteries(SIBs)have lately received tremendous interest due to their abundant reserves as well as low cost.Nevertheless,the lack of suitable anode materials severely hinders the application of sodium-ion batteries.TiS_(2)is elected as a representative material owing to its unique layered structure.But it always suffers from capacity fade due to poor electrochemical kinetics and structural stability.In this work,we fabricate a pre-potassiated TiS_(2)as a host material for sodium storage by an electrochemical pre-potassiation strategy.The intercalation/extraction mechanism,structural changes and reaction kinetics are completely investigated to reveal the outstanding electrochemical property of pre-potassiated TiS_(2)electrode.It turns out that the large interlayer space of pre-potassiated TiS_(2)is conducive to the diffusion of sodium ions,inducing the reduction of entropic barrier for the electrochemical reactions.In addition,the pre-potassiated host structure is still firmly maintained upon repeated cycles.Therefore,the pre-potassiated TiS_(2)presents superior rate capability(165.9 mA h g^(−1) at 1 C and 132.1 mA h g^(−1) at 20 C)and long-term cycling stability(85.3%capacity retention at 5 C after 500 cycles)for SIBs.This research provides an avenue to construct long-life sodium energy storage systems based on pre-potassiated TiS_(2).展开更多
"Shuttle effect" is detrimental for maintaining the high capacity and cycling reversibility of lithium-sulfur batteries(LSBs).To inhibit polysulfide migration,N-doped carbon nanofibers(N-CNFs) membrane compr..."Shuttle effect" is detrimental for maintaining the high capacity and cycling reversibility of lithium-sulfur batteries(LSBs).To inhibit polysulfide migration,N-doped carbon nanofibers(N-CNFs) membrane comprising TiO_(2)nanoparticles(TiO_(2)/N-CNFs) is fabricated using an electrospinning-calcination method and further applied as interlayer in LSBs.The TiO_(2)/N-CNFs interlayer helps the battery to deliver a high specific capacity of 1155.2 mA·h·g^(-1)at 0.2 C with high Coulombic efficiency,good rate capability and stability.When cycling at 0.5 C,a capacity retention rate of 62.4% is achieved over 300 cycles,which is higher than that of CNFs and TiO_(2)/CNFs counterparts.The excellent performance should mainly be attributed to the alleviated "shuttle effect" deriving from high polysulfide trapping ability of TiO_(2)nanoparticles and N heteroatoms in interwoven CNFs.展开更多
Lithium-sulfur batteries as one of the most promising next-generation high-energy storage system, the shuttle effect, the expansion of cathode and the slow electrode redox kinetics limit its further development. Herei...Lithium-sulfur batteries as one of the most promising next-generation high-energy storage system, the shuttle effect, the expansion of cathode and the slow electrode redox kinetics limit its further development. Herein, we report a two-dimensional, ultrathin and ultra-light bimetal-Ni Co-organic framework as the interlayer for Li-S batteries. This kind of interlayer can effectively block polysulfides and accelerate the conversion with a thickness of only 1 μm and a load of 0.1 mg/cm^(2). Because the MOF nanosheets with a thickness of a few nanometers have a large specific surface and a large number of exposed accessible active sites. At the same time, the intrinsic activity of each site is enhanced and the catalytic performance is improved due to the synergistic effect of mixed metals and the unique coordination environment around the active sites. So, 2D NiCo MOF/CNT totally meets the requirements for the lightweight and effective interlayer. The initial discharge capacity of cell with 2D NiCo MOF/CNT interlayer can reach 1132.7 m Ah/g at 0.5 C. It remained 709.1 m Ah/g after 300 cycles, showing good cycling stability and rate performance.展开更多
High theoretical capacity and unique layered structures make MoS_(2)a promising lithium-ion battery anode material.However,the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS...High theoretical capacity and unique layered structures make MoS_(2)a promising lithium-ion battery anode material.However,the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS_(2)lead to unacceptable ion transport capability.Here,we propose in-situ construction of interlayer electrostatic repulsion caused by Co^(2+)substituting Mo^(4+)between MoS_(2)layers,which can break the limitation of interlayer van der Waals forces to fabricate monolayer MoS_(2),thus establishing isotropic ion transport paths.Simultaneously,the doped Co atoms change the electronic structure of monolayer MoS_(2),thus improving its intrinsic conductivity.Importantly,the doped Co atoms can be converted into Co nanoparticles to create a space charge region to accelerate ion transport.Hence,the Co-doped monolayer MoS_(2)shows ultrafast lithium ion transport capability in half/full cells.This work presents a novel route for the preparation of monolayer MoS_(2)and demonstrates its potential for application in fast-charging lithium-ion batteries.展开更多
Rational electrode structure design is of great significance for realizing superior Na^(+)storage performance.Herein,a metal salt-induced polymer blowing-bubble approach followed by selenization procedure is developed...Rational electrode structure design is of great significance for realizing superior Na^(+)storage performance.Herein,a metal salt-induced polymer blowing-bubble approach followed by selenization procedure is developed to in-situ generate abundant sub-10 nm CoSe_(2) nanocrystals on 3D Se/N co-doped carbon networks(CoSe_(2)@3DSNC).The phase transition from Co to CoSe_(2) and the incorporation of Se into the carbon layer are realized simultaneously to establish above configuration,in which the CoSe_(2) nanocrystals are anchored on interlayer expanded carbon networks.Such unique configuration endows electrode with lower Na+diffusion energy barrier,higher Na+storage capability and better structural durability.Reflected in SIBs,the optimized CoSe_(2)@3 DSNC delivers superior rate capability(310 m Ah g^(-1) at 10 A g^(-1))and excellent longterm cycling stability(409 m Ah g^(-1) after 1200 cycles at 5 A g^(-1)).Moreover,this configuration can also be obtained in other metal selenides-carbon composite through a similar approach.展开更多
To improve operation efficiency,an interlayered thin-film composite forward osmosis(iTFC-FO)membrane was designed by introducing an ultrathin and porous interlayer based on aluminum tetra-(4-carboxyphenyl)porphyrin(a ...To improve operation efficiency,an interlayered thin-film composite forward osmosis(iTFC-FO)membrane was designed by introducing an ultrathin and porous interlayer based on aluminum tetra-(4-carboxyphenyl)porphyrin(a stable metal-organic framework nanosheet,Al-MOF).Surface characterization results revealed that Al-MoF spread evenly in the macro-porous substrate,and provided a flat and smooth reaction interface with moderate hydrophilicity and uniform small aperture.The resultant polyamide(PA)layer had a thin base(without intrusion into substrate)and crumpled surface(with abundant leaves).The leaves size and cross-linking degree of PA layer firstly increased and then decreased with the Al-MOF loading.Compared to the original membrane,the iTFC-FO showed an enhanced water permeability and a reduced reverse sodium flux in both modes of active layer facing feed solution(ALFS)and active layer facing draw solution(AL-DS).To be specific,the specific reverse sodium flux(reverse sodium flux/pure water flux)decreased from 0.27 g/L to 0.04 g/L in the AL-FS mode,while from 1.36 g/L to 0.23 g/L in the AL-DS mode with 2 mol/L NaCl as DS.Moreover,the iTFC-FO maintained high stability and high permeability under high-salinity and contaminated environment.This study offers a new possibility for the rational fabrication of high-performance TFC-FO membranes.展开更多
The intercalation of foreign species into MXene, as an approach of tuning the interlayer environment, is employed to improve electrochemical ion storage behaviors. Herein, to understand the effect of confined ions by ...The intercalation of foreign species into MXene, as an approach of tuning the interlayer environment, is employed to improve electrochemical ion storage behaviors. Herein, to understand the effect of confined ions by the MXene layers on the performance of electrochemical energy storage, Zn^(2+) ions were employed to intercalate into MXene via an electrochemical technique. Zn^(2+) ions induced a shrink of the adjacent MXene layers. Meaningfully, a higher capacity of lithium ion storage was obtained after Zn^(2+) preintercalation. In order to explore the roles of the intercalated Zn^(2+) ions, the structural evolution, and the electronic migration among Zn, Ti and the surface termination were investigated to trace the origination of the higher Li^(+) storage capacity. The pre-intercalated Zn^(2+) ions lost electrons, meanwhile Ti of MXene obtained electrons. Moreover, a low-F surface functional groups was achieved. Contrary to the first shrink, after 200 cycles, a larger interlayer distance was monitored, this can accelerate the ion transport and offer a larger expansile space for lithium storage. This may offer a guidance to understand the roles of the confined ion by two-dimensional(2D) layered materials.展开更多
Lithium rich layered oxide(LRLO) has been considered as one of the promising cathodes for lithium-ion batteries(LIBs). The high voltage and large capacity of LRLO depend on Li2MnO_(3)phase. To ameliorate the electroch...Lithium rich layered oxide(LRLO) has been considered as one of the promising cathodes for lithium-ion batteries(LIBs). The high voltage and large capacity of LRLO depend on Li2MnO_(3)phase. To ameliorate the electrochemical performance of Li2MnO_(3), also written as Li(Li1/3Mn2/3)O_(2), we propose a strategy to substitute Mn4+and Li+in Mn/Li transition metal layer with Ti4+, which can stabilize the structure of Li2MnO_(3)by inhibiting the excessive oxidation of O_(2)-above 4.5 V. More significantly, the unequal-valent substitution brings about the emergence of interlayer Li vacancies, which can promote the Li-ion diffusion based on the enlarged interlayer and increase the capacity by activating the Mn3+/4+redox. We designed Li0.7[Li1/3Mn2/3]0.7Ti0.3O_(2)with high interlayer Li vacancies, which presents a high capacity(290 m Ah/g at 10 m A/g) and stable cycling performance(84% over 60 cycles at 50 m A/g). We predict that this strategy will be helpful to further improve the electrochemical performance of LRLOs.展开更多
Layered transition metal dichalcogenides are promising candidates for sodium storage but suffering from low intrinsic electronic conductivity and limited interlayer spacing for fast electron/ion transport,which restri...Layered transition metal dichalcogenides are promising candidates for sodium storage but suffering from low intrinsic electronic conductivity and limited interlayer spacing for fast electron/ion transport,which restricts their high-rate capability and cycling stability.In this work,rGO@MoSe_(2)/NAC hierarchical architectures,consisting of conductive reduced graphene oxide(rGO)supported by hollow nanospheres that are rolled from superlattices of alternatively overlapped MoSe_(2)and N-doped amorphous carbon(NAC)monolayers,are synthesized as a highperformance sodium storage anode.Theoretical calculations reveal the intercalation of NAC monolayer between two adjacent MoSe_(2)monolayers improving electronic conductivity of MoSe_(2)in both surface and internal bulk to fully accelerate electron transport and enhance Naþadsorption.The interoverlapped MoSe_(2)/NAC superlattice featuring a wide interlayer expansion(72.3%)of MoSe_(2)dramatically decreases Naþdiffusion barriers for fast insertion/extraction.Moreover,the hollow nanospheres and the rGO conductive network contribute to a robust hiberarchy that can well release internal stress and buffer the volume expansion,thereby enabling outstanding structural stability.Consequently,the rGO@MoSe_(2)/NAC anode exhibits excellent high-rate capability of 194 mAh g^(-1)and ultralong cyclability of 12000 cycles with a low capacity fading rate of 0.0038%per cycle at an ultra-high current of 50 A g^(-)1,delivering the best high-rate cycling performance to date.Remarkably,the Na_(3)V_(2)(PO_(4))_(3)||rGO@MoSe_(2)/NAC full cells also present outstanding cycling stability(600 cycles)at 10C rate,which proves the great potential in fast-charging applications.展开更多
Aqueous rechargeable zinc-ion batteries(ARZIBs)have a bright future for energy storage due to their high energy density and safety.However,for traditional ARZIBs,cathode materials always suffer from the limited space ...Aqueous rechargeable zinc-ion batteries(ARZIBs)have a bright future for energy storage due to their high energy density and safety.However,for traditional ARZIBs,cathode materials always suffer from the limited space for large-sized zinc ions storage and transport,leading to low Coulombic efficiency and inferior cycling performance.To build a reliable host with large tunnel,1-butyl-1-methylpyrrolidinium ion(PY14^(+))pre-intercalated TiS_(2)(PY14^(+)-TiS_(2))is designed as an alternative intercalation-type electrode.As the insertion organic vip widens the interlayer space of TiS_(2)and buffers the lattice stress generated during the electrochemical cycles,the structural reversibility,cycling stability and kinetics properties of PY14^(+)-TiS_(2) are enhanced greatly.A specific capacity of 130.9 mAh g^(−1) with 84.3%capacity retention over 500 cycles can be achieved at 0.1 A g^(−1).Therefore,this study paves the way for enhancing the aqueous Zn ions storage capability by organic interlayer engineering.展开更多
Two-dimensional(2D)MoS_(2) nanomaterials have been extensively studied due to their special structure and high theoretical capacity,but it is still a huge challenge to improve its cycle stability and achieve superior ...Two-dimensional(2D)MoS_(2) nanomaterials have been extensively studied due to their special structure and high theoretical capacity,but it is still a huge challenge to improve its cycle stability and achieve superior fast charge and discharge performance.Herein,a facile one-step hydrothermal method is proposed to synthetize an ordered and self-assembled MoS_(2) nanoflower(MoS_(2)/C NF)with expanded interlayer spacing via embedding a carbon layer into the interlayer.The carbon layer in the MoS_(2) interlayer can speed the transfer of electrons,while the nanoflower structure promotes the ions transport and improves the structural stability during the charging/discharging process.Therefore,MoS_(2)/C NF electrode exhibits exceptional rate performance(318.2 and 302.3 mA·h·g^(-1) at 5.0 and 10.0 A·g^(-1),respectively)and extraordinary cycle durability(98.8%retention after 300 cycles at a current density of 1.0 A·g^(-1)).This work provides a simple and feasible method for constructing high-performance anode composites for sodium ion batteries with excellent cycle durability and fast charge/discharge ability.展开更多
In the interlayer expansion of the layered zeolite precursor COK-5, a Sn, salt, bis（2,4-pentanedionate）- dichlorotin [Sn（acac）2CL2], instead of a silylating agent was used to link the layers at 180 ℃. The obtaine...In the interlayer expansion of the layered zeolite precursor COK-5, a Sn, salt, bis（2,4-pentanedionate）- dichlorotin [Sn（acac）2CL2], instead of a silylating agent was used to link the layers at 180 ℃. The obtained material, which is designed as Sn-COE-5, shows a shift of the first XRD reflection, which is very similar to that of COK-5 interlayer expanded with dichlorodimethylsilane （DCDMS）, indicating an increase in interlayer distance. X-ray diffraction （XRD）, N2 sorption isotherms, inductively coupled plasma （ICP）, and X-ray photo- electron spectroscopy （XPS） support the incorporation of isolated Sn sites in the sample. In the conversion of glucose to levulinic acid. Sn-COE-5 exhibits much higher activity than COK-5, which is due to the presence of Lewis acidic sites in the Sn-COE-5.展开更多
文摘Due to its unique layered structure and excellent electrochemical properties,molybdenum disulfide(MoS_(2))demonstrates significant potential for applications in the energy storage field,particularly in supercapacitors.It is widely regarded as one of the most representative transition metal dichalcogenides.MoS_(2)possesses a high theoretical specific capacitance,abundant edge active sites,and favorable tunability and structural diversity,which provide it with a distinct advantage in the construction of advanced electrode structures.Additionally,the anisotropic characteristics of MoS_(2)concerning electron and ion transport offer more dimensions for regulating its electrochemical behavior.This work will systematically review various synthesis strategies for MoS_(2)and its recent advancements in energy storage,with a particular focus on the mechanisms by which interlayer spacing modulation affects energy storage behavior in supercapacitor configurations.The discussion will encompass a comprehensive logical framework that spans material structure modifications,electronic configuration evolution,and enhancements in macroscopic device performance.This review aims to provide theoretical support and practical guidance for the application of MoS_(2)in the next generation of highperformance energy storage devices.
基金the financial support from the National Natural Science Foundation of China(No.52225208 and 51802131)the Training Program for academic and technical leaders in major disciplines of Jiangxi Province-Young Talents(No.20212BCJ23021)the Natural Science Foundation of Jiangxi Province,China(No.20232BAB204020).
文摘1T-MoS_(2)nanosheets,with metallic conductivity and high capacity,hold great potential for lithium-ion capacitors(LICs),but suffer from sluggish reaction kinetics due to dense stacking.Herein,1T-MoS_(2)nanosheets with enlarged interlayer spacing,vertically bonded to reduced graphene oxide(rGO)(1T-MoS_(2)/rGO),were designed using a hydrothermal-assisted dispersion and intercalation strategy.The active nitrogen species derived from N,N-dimethylformamide(DMF)not only bridge the rGO and MoS_(2)through strong Mo-N-C bonds to promote the formation of dispersed MoS_(2)nanosheets,but also intercalate into the MoS_(2)structure,further enlarging the interlayer spacing.This unique structure synergistically enhances meso-and microscale mass transfer outside and inside of the few-layered nanosheets,significantly improving electrochemical reaction kinetics and reducing the kinetic mismatch between the anode and cathode.Consequently,the resulting 1T-MoS_(2)/rGO achieves a capacity of 500 mAh g^(-1)after 500 cycles at 5 A g^(-1)and a high rate performance of 587 mAh g^(-1)at a high rate of 10 A g^(-1).Moreover,the assembled 3D vertical 1T-MoS_(2)/rGO//AC LIC delivers a high energy density of 100.3 Wh kg^(-1)at a power density of1.0 kW kg^(-1),and long cycle stability with capacity retention as high as 91.02%after 5000 cycles at 2 A g^(-1).This work provides a generalizable strategy for engineering two-dimensional material-based electrodes,offering new insights into high-performance energy storage systems.
基金financially supported by the National Natural Science Foundation of China(nos.21971012,61933002,21601015,21625102,21674012,and 81601549)the National Key Research and Development Program of China(2020YFB1506300)Beijing Institute of Technology Research Fund Program for Young Scholars。
文摘The hydrogen-bonded organic frameworks(HOFs)as a new type of porous framework materials have been widely studied in various areas.However,the lack of appropriate active sites,low intrinsic conductivity,and poor stability limited their performance in the field of electrocatalysis.Herein,we designed two 2D metal hydrogen-bonded organic frameworks(2D–M–HOF,M=Cu^(2+)or Ni^(2+))with coordination compounds based on 2,3,6,7,14,15-hexahydroxyl cyclotricatechylene and transition metal ions(Cu^(2+)and Ni^(2+)),respectively.The crystal structure of 2D–Cu–HOF is determined by continuous rotation electron diffraction,indicating an undulated 2D hydrogen-bond network with interlayeredπ-πstacking.The flexible structure of 2D–M–HOF leads to the formation of self-adaption interlayered sites,resulting in superior activity and selectivity in the electrocatalytic conversion of CO_(2) to C_(2) products,achieving a total Faradaic efficiency exceeding 80%due to the high-efficiency C–C coupling.The experimental results and density functional calculations verify that the undulated 2D–M–HOF enables the energetically favorable formation of*OCCHO intermediate.This work provides a promising strategy for designing HOF catalysts in electrocatalysis and related processes.
基金supported by the National Research Foundation of Korea funded by the Korean Government(grant No.RS-2023-00208801).
文摘As artificial intelligence and big data become increasingly prevalent, resistive random-access memory (RRAM) has become one of the most promising alternatives for storing massive amounts of data. In this study, we employed high-quality crystalline TiN/Al_(2)O_(3)/BaTiO_(3)/Pt RRAM with an optimized thin Al_(2)O_(3) interlayer around 12 nm thick prepared using atomic layer deposition since the thickness of the interlayer affects the memory window size. After insertion of the Al_(2)O_(3) interlayer, the novel RRAM exhibited outstanding uniform resistive switching voltage and the ON/OFF memory window drastically increased from 10 to 103 without any discernible decline in performance. Moreover, the low-resistance state and high-resistance state operating current values decreased by almost one order and three orders of magnitude, respectively, thereby decreasing the power consumption for the RESET and SET processes by more than three and almost one order of magnitude, respectively. The device also exhibits multilevel resistive switching behavior when varying the applied voltage. Finally, we also developed a 6 6 crossbar array which demonstrated consistent and reliable resistive switching behavior with minimal variation. Hence, our approach holds great promise for producing state-of-the-art non-volatile resistive switching devices.
基金sponsored by NSAF joint Fund(U1830106)Science and Technology Innovation 2025 Major Program of Ningbo(2018B10061)+1 种基金National Natural Science Foundation of China(U1632114,51901205)K.C.Wong Magna Fund in Ningbo University。
文摘As an alternative for lithium-ion batteries(LIBs),sodium-ion batteries(SIBs)have lately received tremendous interest due to their abundant reserves as well as low cost.Nevertheless,the lack of suitable anode materials severely hinders the application of sodium-ion batteries.TiS_(2)is elected as a representative material owing to its unique layered structure.But it always suffers from capacity fade due to poor electrochemical kinetics and structural stability.In this work,we fabricate a pre-potassiated TiS_(2)as a host material for sodium storage by an electrochemical pre-potassiation strategy.The intercalation/extraction mechanism,structural changes and reaction kinetics are completely investigated to reveal the outstanding electrochemical property of pre-potassiated TiS_(2)electrode.It turns out that the large interlayer space of pre-potassiated TiS_(2)is conducive to the diffusion of sodium ions,inducing the reduction of entropic barrier for the electrochemical reactions.In addition,the pre-potassiated host structure is still firmly maintained upon repeated cycles.Therefore,the pre-potassiated TiS_(2)presents superior rate capability(165.9 mA h g^(−1) at 1 C and 132.1 mA h g^(−1) at 20 C)and long-term cycling stability(85.3%capacity retention at 5 C after 500 cycles)for SIBs.This research provides an avenue to construct long-life sodium energy storage systems based on pre-potassiated TiS_(2).
基金financially supported by the National Natural Science Foundation of China(52102100,52072330)Industry-University-Research Cooperation Project of Jiangsu Province(BY2021525)Guangdong Basic and Applied Basic Research Foundation(2020A1515110035)。
文摘"Shuttle effect" is detrimental for maintaining the high capacity and cycling reversibility of lithium-sulfur batteries(LSBs).To inhibit polysulfide migration,N-doped carbon nanofibers(N-CNFs) membrane comprising TiO_(2)nanoparticles(TiO_(2)/N-CNFs) is fabricated using an electrospinning-calcination method and further applied as interlayer in LSBs.The TiO_(2)/N-CNFs interlayer helps the battery to deliver a high specific capacity of 1155.2 mA·h·g^(-1)at 0.2 C with high Coulombic efficiency,good rate capability and stability.When cycling at 0.5 C,a capacity retention rate of 62.4% is achieved over 300 cycles,which is higher than that of CNFs and TiO_(2)/CNFs counterparts.The excellent performance should mainly be attributed to the alleviated "shuttle effect" deriving from high polysulfide trapping ability of TiO_(2)nanoparticles and N heteroatoms in interwoven CNFs.
基金financially supported by the National Natural Science Foundation of China (No. 22179007)。
文摘Lithium-sulfur batteries as one of the most promising next-generation high-energy storage system, the shuttle effect, the expansion of cathode and the slow electrode redox kinetics limit its further development. Herein, we report a two-dimensional, ultrathin and ultra-light bimetal-Ni Co-organic framework as the interlayer for Li-S batteries. This kind of interlayer can effectively block polysulfides and accelerate the conversion with a thickness of only 1 μm and a load of 0.1 mg/cm^(2). Because the MOF nanosheets with a thickness of a few nanometers have a large specific surface and a large number of exposed accessible active sites. At the same time, the intrinsic activity of each site is enhanced and the catalytic performance is improved due to the synergistic effect of mixed metals and the unique coordination environment around the active sites. So, 2D NiCo MOF/CNT totally meets the requirements for the lightweight and effective interlayer. The initial discharge capacity of cell with 2D NiCo MOF/CNT interlayer can reach 1132.7 m Ah/g at 0.5 C. It remained 709.1 m Ah/g after 300 cycles, showing good cycling stability and rate performance.
基金financially supported by Shenzhen Key Laboratory of Advanced Energy Storage(No.ZDSYS20220401141000001)the Research Grants Council of the Hong Kong Special Administrative Region,China(Project No.R6005-20)。
文摘High theoretical capacity and unique layered structures make MoS_(2)a promising lithium-ion battery anode material.However,the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS_(2)lead to unacceptable ion transport capability.Here,we propose in-situ construction of interlayer electrostatic repulsion caused by Co^(2+)substituting Mo^(4+)between MoS_(2)layers,which can break the limitation of interlayer van der Waals forces to fabricate monolayer MoS_(2),thus establishing isotropic ion transport paths.Simultaneously,the doped Co atoms change the electronic structure of monolayer MoS_(2),thus improving its intrinsic conductivity.Importantly,the doped Co atoms can be converted into Co nanoparticles to create a space charge region to accelerate ion transport.Hence,the Co-doped monolayer MoS_(2)shows ultrafast lithium ion transport capability in half/full cells.This work presents a novel route for the preparation of monolayer MoS_(2)and demonstrates its potential for application in fast-charging lithium-ion batteries.
基金financially supported by the National Natural Science Foundation of China(21471040)。
文摘Rational electrode structure design is of great significance for realizing superior Na^(+)storage performance.Herein,a metal salt-induced polymer blowing-bubble approach followed by selenization procedure is developed to in-situ generate abundant sub-10 nm CoSe_(2) nanocrystals on 3D Se/N co-doped carbon networks(CoSe_(2)@3DSNC).The phase transition from Co to CoSe_(2) and the incorporation of Se into the carbon layer are realized simultaneously to establish above configuration,in which the CoSe_(2) nanocrystals are anchored on interlayer expanded carbon networks.Such unique configuration endows electrode with lower Na+diffusion energy barrier,higher Na+storage capability and better structural durability.Reflected in SIBs,the optimized CoSe_(2)@3 DSNC delivers superior rate capability(310 m Ah g^(-1) at 10 A g^(-1))and excellent longterm cycling stability(409 m Ah g^(-1) after 1200 cycles at 5 A g^(-1)).Moreover,this configuration can also be obtained in other metal selenides-carbon composite through a similar approach.
基金supported by the National Natural Science Foundation of China(Nos.52100089 and 51978312)the Program to Cultivate Middle-aged and Young Science Leaders of Colleges and Universities of Jiangsu Province and Youth Fund of Basic Research Program of Jiangnan University(No.JUSRP121058).
文摘To improve operation efficiency,an interlayered thin-film composite forward osmosis(iTFC-FO)membrane was designed by introducing an ultrathin and porous interlayer based on aluminum tetra-(4-carboxyphenyl)porphyrin(a stable metal-organic framework nanosheet,Al-MOF).Surface characterization results revealed that Al-MoF spread evenly in the macro-porous substrate,and provided a flat and smooth reaction interface with moderate hydrophilicity and uniform small aperture.The resultant polyamide(PA)layer had a thin base(without intrusion into substrate)and crumpled surface(with abundant leaves).The leaves size and cross-linking degree of PA layer firstly increased and then decreased with the Al-MOF loading.Compared to the original membrane,the iTFC-FO showed an enhanced water permeability and a reduced reverse sodium flux in both modes of active layer facing feed solution(ALFS)and active layer facing draw solution(AL-DS).To be specific,the specific reverse sodium flux(reverse sodium flux/pure water flux)decreased from 0.27 g/L to 0.04 g/L in the AL-FS mode,while from 1.36 g/L to 0.23 g/L in the AL-DS mode with 2 mol/L NaCl as DS.Moreover,the iTFC-FO maintained high stability and high permeability under high-salinity and contaminated environment.This study offers a new possibility for the rational fabrication of high-performance TFC-FO membranes.
基金supported by the Development Plan of Science and Technology of Jilin Province (20190201309JC,YDZJ202101ZYTS187)the Project of Development and Reform Commission of Jilin Provinve (2019C042-1)+3 种基金the Science and Technology Research Project of Education Department of Jilin Province(JJKH20210453KJ, JJKH20210449KJ)the National Natural Science Foundation of China (51932005)the Liaoning Revitalization Talents Program (XLYC1807175)the Research Fund of Shenyang National Laboratory for Materials Science。
文摘The intercalation of foreign species into MXene, as an approach of tuning the interlayer environment, is employed to improve electrochemical ion storage behaviors. Herein, to understand the effect of confined ions by the MXene layers on the performance of electrochemical energy storage, Zn^(2+) ions were employed to intercalate into MXene via an electrochemical technique. Zn^(2+) ions induced a shrink of the adjacent MXene layers. Meaningfully, a higher capacity of lithium ion storage was obtained after Zn^(2+) preintercalation. In order to explore the roles of the intercalated Zn^(2+) ions, the structural evolution, and the electronic migration among Zn, Ti and the surface termination were investigated to trace the origination of the higher Li^(+) storage capacity. The pre-intercalated Zn^(2+) ions lost electrons, meanwhile Ti of MXene obtained electrons. Moreover, a low-F surface functional groups was achieved. Contrary to the first shrink, after 200 cycles, a larger interlayer distance was monitored, this can accelerate the ion transport and offer a larger expansile space for lithium storage. This may offer a guidance to understand the roles of the confined ion by two-dimensional(2D) layered materials.
基金financially supported by the National Natural Science Foundation of China (Nos. 51972258 and 22109186)Open Fund by Sanya Science and Education Innovation Park of Wuhan University of Technology (No. 2021KF0021)supported by 21C Innovation Laboratory,Contemporary Amperex Technology Ltd. by Project No. 21C-OP-202002。
文摘Lithium rich layered oxide(LRLO) has been considered as one of the promising cathodes for lithium-ion batteries(LIBs). The high voltage and large capacity of LRLO depend on Li2MnO_(3)phase. To ameliorate the electrochemical performance of Li2MnO_(3), also written as Li(Li1/3Mn2/3)O_(2), we propose a strategy to substitute Mn4+and Li+in Mn/Li transition metal layer with Ti4+, which can stabilize the structure of Li2MnO_(3)by inhibiting the excessive oxidation of O_(2)-above 4.5 V. More significantly, the unequal-valent substitution brings about the emergence of interlayer Li vacancies, which can promote the Li-ion diffusion based on the enlarged interlayer and increase the capacity by activating the Mn3+/4+redox. We designed Li0.7[Li1/3Mn2/3]0.7Ti0.3O_(2)with high interlayer Li vacancies, which presents a high capacity(290 m Ah/g at 10 m A/g) and stable cycling performance(84% over 60 cycles at 50 m A/g). We predict that this strategy will be helpful to further improve the electrochemical performance of LRLOs.
基金This work was financially supported by the National Natural Science Foundation of China(Grant Nos.51972092 and 52271208)。
文摘Layered transition metal dichalcogenides are promising candidates for sodium storage but suffering from low intrinsic electronic conductivity and limited interlayer spacing for fast electron/ion transport,which restricts their high-rate capability and cycling stability.In this work,rGO@MoSe_(2)/NAC hierarchical architectures,consisting of conductive reduced graphene oxide(rGO)supported by hollow nanospheres that are rolled from superlattices of alternatively overlapped MoSe_(2)and N-doped amorphous carbon(NAC)monolayers,are synthesized as a highperformance sodium storage anode.Theoretical calculations reveal the intercalation of NAC monolayer between two adjacent MoSe_(2)monolayers improving electronic conductivity of MoSe_(2)in both surface and internal bulk to fully accelerate electron transport and enhance Naþadsorption.The interoverlapped MoSe_(2)/NAC superlattice featuring a wide interlayer expansion(72.3%)of MoSe_(2)dramatically decreases Naþdiffusion barriers for fast insertion/extraction.Moreover,the hollow nanospheres and the rGO conductive network contribute to a robust hiberarchy that can well release internal stress and buffer the volume expansion,thereby enabling outstanding structural stability.Consequently,the rGO@MoSe_(2)/NAC anode exhibits excellent high-rate capability of 194 mAh g^(-1)and ultralong cyclability of 12000 cycles with a low capacity fading rate of 0.0038%per cycle at an ultra-high current of 50 A g^(-)1,delivering the best high-rate cycling performance to date.Remarkably,the Na_(3)V_(2)(PO_(4))_(3)||rGO@MoSe_(2)/NAC full cells also present outstanding cycling stability(600 cycles)at 10C rate,which proves the great potential in fast-charging applications.
基金supported by the NSAF joint Fund(No.U1830106)the National Natural Science Foundation of China(No.U1632114).
文摘Aqueous rechargeable zinc-ion batteries(ARZIBs)have a bright future for energy storage due to their high energy density and safety.However,for traditional ARZIBs,cathode materials always suffer from the limited space for large-sized zinc ions storage and transport,leading to low Coulombic efficiency and inferior cycling performance.To build a reliable host with large tunnel,1-butyl-1-methylpyrrolidinium ion(PY14^(+))pre-intercalated TiS_(2)(PY14^(+)-TiS_(2))is designed as an alternative intercalation-type electrode.As the insertion organic vip widens the interlayer space of TiS_(2)and buffers the lattice stress generated during the electrochemical cycles,the structural reversibility,cycling stability and kinetics properties of PY14^(+)-TiS_(2) are enhanced greatly.A specific capacity of 130.9 mAh g^(−1) with 84.3%capacity retention over 500 cycles can be achieved at 0.1 A g^(−1).Therefore,this study paves the way for enhancing the aqueous Zn ions storage capability by organic interlayer engineering.
基金National Natural Science Foundation of China(51874142)Pearl River S&T Nova Program of Guangzhou(201806010031)+3 种基金the Fundamental Research Funds for the Central Universities(2019JQ09)Guangdong Innovative and Entrepreneurial Research Team Program(2016ZT06N569)Tip-top Scientific and Technical Innovative Youth Talents of Guangdong Special Support Program(2019TQ05L903)Young Elite Scientists Sponsorship Program by CAST(2019QNRC001).
文摘Two-dimensional(2D)MoS_(2) nanomaterials have been extensively studied due to their special structure and high theoretical capacity,but it is still a huge challenge to improve its cycle stability and achieve superior fast charge and discharge performance.Herein,a facile one-step hydrothermal method is proposed to synthetize an ordered and self-assembled MoS_(2) nanoflower(MoS_(2)/C NF)with expanded interlayer spacing via embedding a carbon layer into the interlayer.The carbon layer in the MoS_(2) interlayer can speed the transfer of electrons,while the nanoflower structure promotes the ions transport and improves the structural stability during the charging/discharging process.Therefore,MoS_(2)/C NF electrode exhibits exceptional rate performance(318.2 and 302.3 mA·h·g^(-1) at 5.0 and 10.0 A·g^(-1),respectively)and extraordinary cycle durability(98.8%retention after 300 cycles at a current density of 1.0 A·g^(-1)).This work provides a simple and feasible method for constructing high-performance anode composites for sodium ion batteries with excellent cycle durability and fast charge/discharge ability.
基金supported by the National Natural Science Foundation of China (21422306 and 21403192)Zhejiang Provincial Natural Science Foundation of China under grant no. LR15B030001the Fundamental Research Funds for the Central Universities (2015XZZX004-04)
文摘In the interlayer expansion of the layered zeolite precursor COK-5, a Sn, salt, bis（2,4-pentanedionate）- dichlorotin [Sn（acac）2CL2], instead of a silylating agent was used to link the layers at 180 ℃. The obtained material, which is designed as Sn-COE-5, shows a shift of the first XRD reflection, which is very similar to that of COK-5 interlayer expanded with dichlorodimethylsilane （DCDMS）, indicating an increase in interlayer distance. X-ray diffraction （XRD）, N2 sorption isotherms, inductively coupled plasma （ICP）, and X-ray photo- electron spectroscopy （XPS） support the incorporation of isolated Sn sites in the sample. In the conversion of glucose to levulinic acid. Sn-COE-5 exhibits much higher activity than COK-5, which is due to the presence of Lewis acidic sites in the Sn-COE-5.
