The development of flexible zinc-ion batteries(ZIBs)faces a threeway trade-off among the ionic conductivity,Zn^(2+)mobility,and the electrochemical stability of hydrogel electrolytes.To address this challenge,we desig...The development of flexible zinc-ion batteries(ZIBs)faces a threeway trade-off among the ionic conductivity,Zn^(2+)mobility,and the electrochemical stability of hydrogel electrolytes.To address this challenge,we designed a cationic hydrogel named PAPTMA to holistically improve the reversibility of ZIBs.The long cationic branch chains in the polymeric matrix construct express pathways for rapid Zn^(2+)transport through an ionic repulsion mechanism,achieving simultaneously high Zn^(2+)transference number(0.79)and high ionic conductivity(28.7 mS cm−1).Additionally,the reactivity of water in the PAPTMA hydrogels is significantly inhibited,thus possessing a strong resistance to parasitic reactions.Mechanical characterization further reveals the superior tensile and adhesion strength of PAPTMA.Leveraging these properties,symmetric batteries employing PAPTMA hydrogel deliver exceeding 6000 h of reversible cycling at 1 mA cm^(−2) and maintain stable operation for 1000 h with a discharge of depth of 71%.When applied in 4×4 cm2 pouch cells with MnO_(2) as the cathode material,the device demonstrates remarkable operational stability and mechanical robustness through 150 cycles.This work presents an eclectic strategy for designing advanced hydrogels that combine high ionic conductivity,enhanced Zn^(2+)mobility,and strong resistance to parasitic reactions,paving the way for long-lasting flexible ZIBs.展开更多
Lithium metal attracts growing attention as an ideal anode candidate for next generation lithium battery systems owing to its high capacity,low density,and low working potential.However,the volume expansion of the bul...Lithium metal attracts growing attention as an ideal anode candidate for next generation lithium battery systems owing to its high capacity,low density,and low working potential.However,the volume expansion of the bulk and dendrite growth on the surface of lithium anode limits its practical application.Herein,we fabricate a composite lithium host featuring both multiple scaled structure and lithiophilic property to address obstacles at both aspects of bulk and surface simultaneously.In which,the multiple scaled structure provides void space to accommodate lithium volume change while zinc and cobalt oxides sites derived from Zeolitic Imidazolate Frameworks can react with lithium and form a stable solid electrolyte interphase,leading to a stable cycling of lithium symmetrical cell for more than 500 cycles with voltage hysteresis of only 88 mV at 2 mAcm^-2 and 5 mAh cm^-2.Moreover,full cells paired with LiFePO4 cathode can realize 500 cycles with 99.2%capacity retention,showing great potential for practical applications.The excellent electrochemical performance of the composite lithium anode proves the effectiveness of our anode design with multiple scaled structure and lithiophilic feature,which can be also expanded to other metal anodes for batteries.展开更多
The photocatalytic production of syngas using a noble-metal-free catalytic system is a promising approach for renewable energy and environmental sustainability.In this study,we demonstrate an efficient catalytic syste...The photocatalytic production of syngas using a noble-metal-free catalytic system is a promising approach for renewable energy and environmental sustainability.In this study,we demonstrate an efficient catalytic system formed by integrating Co single sites,which act as the active sites,in covalent triazine frameworks(CTFs),which act as the photoabsorber,for the photocatalytic production of syngas from CO2 in aqueous solution.The enhanced light absorption of the CTFs,which contain intramolecular heterojunctions,in conjunction with 0.8 mmol L^‒1 of the Co complex enables excellent syngas production with a yield of 3303μmol g‒1(CO:H2=1.4:1)in 10 h,which is about three times greater than that achieved using CTF without a heterojunction.In the photocatalytic reaction,the coordinated single Co centers accept the photogenerated electrons from the CTF,and serve as active sites for CO2 conversion through an adsorption-activation-reaction mechanism.Theoretical calculations further reveal that the intramolecular heterojunctions highly promote photogenerated charge separation,thus boosting photocatalytic syngas production.This work reveals the promising potential of CTFs for single-metal-site-based photocatalysis.展开更多
The Er3+doped double perovskite Ba_(2)CaWO_(6) crystal is a promising ratiometric thermometer based on the fluorescence intensity ratio(FIR) of transitions from ^(2)H_(11/2) and ^(4)S_(3/2) to the lowered ^(4)I_(15/2)...The Er3+doped double perovskite Ba_(2)CaWO_(6) crystal is a promising ratiometric thermometer based on the fluorescence intensity ratio(FIR) of transitions from ^(2)H_(11/2) and ^(4)S_(3/2) to the lowered ^(4)I_(15/2) level.However,the Ca^(2+) vacancy defect caused by the charge difference between rare-earth ions and the substituted alkaline-earth ions gives rise to the non-radiative probability and limits the thermal sensitivity.Here,the up-conversion luminescence and thermometric performance of Er^(3+),Yb^(3+) dopedBa_(2)CaWO_(6) are tuned by tri-doping with alkaline ions.The Ca^(2+) vacancy defect can be eliminated by the introduction of Na^(+),which occupies the Ca^(2+) site when it is doped into Ba_(2)CaWO_(6) with Er^(3+) and Yb^(3+).On the contrary,the doping of Cs^(+) into Ba_(2)CaWO_(6) with Er^(3+) and Yb^(3+) enhances the defect concentration because it occupies the site of Ba^(2+).Thus,the tri-doping of Na^(+) reduces the non-radiative probability and enhances the quantum efficiency of Er^(3+),leading to the improvement of the thermometric sensitivity of Ba_(2)CaWO_(6).As a result,we get an excellent thermometric Ba_(2)CaWO_(6):8%Yb^(3+),3.5%Er^(3+),6%Na^(+) powder with a luminescence lifetime of 515 μs and maximum thermal sensitivity(S_(r)) of 1.45%/K,which is more than three times higher than that of the BCWO:Er^(3+) powder.展开更多
Metal skeletons,such as Nickel Foam(NF) has attracted worldwide interests as stable host for lithium metal anode because of its high stability,large specific surface area and high conductivity.However,most metal skele...Metal skeletons,such as Nickel Foam(NF) has attracted worldwide interests as stable host for lithium metal anode because of its high stability,large specific surface area and high conductivity.However,most metal skeletons have lithophobic surface and uneven current distribution that result in sporadic lithium nucleation and uncontrolled dendrites growth.Herein,we describe a sequential immersing strategy to generate interwoven Nickel(Ⅱ)-dimethylglyoxime(Ni-DMG) nanowires at NF to obtain composite skeleton(NDNF),which can be used as an stable host for Li metal storage.The Ni-DMG has proved effective to realize uniform lithium nucleation and dendrite-free lithium deposition.Combing with the three dimensional(3 D) hierarchical porous structure,the composite host shows a significantly improved coulombic efficiency(CE) than pristine commercial nickel foam.Moreover,the corresponding Li‖Li symmetrical cells can run more than 700 h with low voltage hysteresis 22 mV at 1.0 mA/cm^(2),and Li@NDNF‖LiFePO;full-cell exhibits a high capacity retention of 82.03% at 1.0 C during 630 cycles.These results proved the effectiveness of metal-organic complexes in governing Li metal growth and can be employed as a new strategy for dendrite-free Li metal anode and safe Li metal batteries(LMBs).展开更多
The two-dimensional (2D) structure of layered transition metal dichalcogenides (TMDs) provides unusual physical properties [1,2]and chemical reactivity [3,4], which can be influenced by defects such as dislocations [5...The two-dimensional (2D) structure of layered transition metal dichalcogenides (TMDs) provides unusual physical properties [1,2]and chemical reactivity [3,4], which can be influenced by defects such as dislocations [5,6]. For example, dislocations can act as nucleation sites for the onset of deformation when subjected to stress [7].展开更多
Side reactions and dendrite growth triggered by the unstable interface and inhomogeneous deposition have become the biggest obstacle to the commercialization for lithium metal batteries.In this study,a highly-chlorina...Side reactions and dendrite growth triggered by the unstable interface and inhomogeneous deposition have become the biggest obstacle to the commercialization for lithium metal batteries.In this study,a highly-chlorinated organic-inorganic hybrid interfacial protective layer is developed by rationally tuning the interfacial passivation and robustness to achieve the convenient and efficient Li metal anode.The polyvinyl chloride(PVC)can effectively resist water and oxygen,which is confirmed by density functional theory.The organic-dominant solid electrolyte interphases(SEI)with lithium chloride are investigated by the X-ray photoelectron spectroscopy(XPS)with little mineralization of oxide,such as Li_(2)O and Li_(2)CO_(3).With such artificial SEI,a uniform and dense lithium deposition morphology are formed and an ultra-long stable cycle of over 500 h are achieved even at an ultra-high current density of 10 m A/cm^(2).Moreover,the simple and convenient protected anode also exhibits excellent battery stability when paired with the LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)and LiFePO_(4)(LFP)cathode,showing great potential for the commercial application of lithium metal batteries.展开更多
The development of lithium-metal batteries(LMBs)is seriously restricted by the out-of-control dendrites growth and infinite volume expansion.Herein,a pervasive organic-inorganic layer construction strategy is reported...The development of lithium-metal batteries(LMBs)is seriously restricted by the out-of-control dendrites growth and infinite volume expansion.Herein,a pervasive organic-inorganic layer construction strategy is reported for the composite lithium metal anode with congener-derived organic-inorganic solid electrolyte interphase(SEI).In this strategy,the organic-inorganic Ag@polydopamine(Ag@PDA)layer is coated on the arbitrary substrates by a simple two-step method.The thin and stable congener-derived SEI is insitu formed with fewer inorganic components and more organic components during charging/discharging.The polydopamine with sufficient adhesion groups and lithiophilic Ag layer realize near-zero nucleation overpotential during lithium deposition.The low interface resistance and stable lithium deposition are achieved.Moreover,the practical areal and volumetric capacities of the composite anode with three-dimensional copper(3DCu)as the substrate are 10 mAh/cm^(2)and 1538 mAh/cm^3(vs.the mass of anode).The symmetrical cell shows very low polarization voltage(10 mV)and more than 2500 h cycles life at 1 mA/cm^(2)(1 mAh/cm^(2)).The LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)-based full cells show improved capacity retention(82%)after 100 cycles at 0.5 C.The modified lithiophilic anode with congener-derived interphase provides a promising strategy to realize the next-generation dendrite-free LMBs.展开更多
Lithium-metal batteries with high energy/power densities have significant applications in electronics,electric vehicles,and stationary power plants.However,the unstable lithium-metal-anode/electrolyte interface has in...Lithium-metal batteries with high energy/power densities have significant applications in electronics,electric vehicles,and stationary power plants.However,the unstable lithium-metal-anode/electrolyte interface has induced insufficient cycle life and safety issues.To improve the cycle life and safety,understanding the formation of the solid electrolyte interphase(SEI)and growth of lithium dendrites near the anode/electrolyte interface,regulating the electrodeposition/electrostripping processes of Li^(+),and developing multiple approaches for protecting the lithium-metal surface and SEI layer are crucial and necessary.This paper comprehensively reviews the research progress in SEI and lithium dendrite growth in terms of their classical electrochemical lithium plating/stripping processes,interface interaction/nucleation processes,anode geometric evolution,fundamental electrolyte reduction mechanisms,and effects on battery performance.Some important aspects,such as charge transfer,the local current distribution,solvation,desolvation,ion diffusion through the interface,inhibition of dendrites by the SEI,additives,models for dendrite formation,heterogeneous nucleation,asymmetric processes during stripping/plating,the host matrix,and in situ nucleation characterization,are also analyzed based on experimental observations and theoretical calculations.Several technical challenges in improving SEI properties and reducing lithium dendrite growth are analyzed.Furthermore,possible future research directions for overcoming the challenges are also proposed to facilitate further research and development toward practical applications.展开更多
CO_(2)electroreduction has been regarded as an appealing strategy for renewable energy storage.Recently,bismuth(Bi)electrocatalysts have attracted much attention due to their excellent formate selectivity.However,many...CO_(2)electroreduction has been regarded as an appealing strategy for renewable energy storage.Recently,bismuth(Bi)electrocatalysts have attracted much attention due to their excellent formate selectivity.However,many reported Bi electrocatalysts suffer from low current densities,which are insufficient for industrial applications.To reach the goal of high current CO_(2)reduction to formate,we fabricate Bi nanosheets(NS)with high activity through edge/terrace control and defect engineering strategy.Bi NS with preferential exposure sites are obtained by topotactic transformation,and the processes are clearly monitored by in-situ Raman and ex-situ X-ray diffraction(XRD).Bi NS-1 with a high fraction of edge sites and defect sites exhibits excellent performance,and the current density is up to ca.870 mA·cm^(−2)in the flow cell,far above the industrially applicable level(100 mA·cm^(−2)),with a formate Faradaic efficiency greater than 90%.In-situ Fourier transform infrared(FT-IR)spectra detect*OCHO,and theoretical calculations reveal that the formation energy of*OCHO on edges is lower than that on terraces,while the defects on edges further reduce the free energy changes(ΔG).The differential charge density spatial distributions reveal that the presence of defects on edges causes charge enrichment around the C–H bond,benefiting the stabilization of the*OCHO intermediate,thus remarkably lowering theΔG.展开更多
The photoreversible color switching system(PCSS)is attracting increasing attention for use in alleviating energy crisis and environmental problems.We report a robust PCSS in which lattice matching enables bottom-up or...The photoreversible color switching system(PCSS)is attracting increasing attention for use in alleviating energy crisis and environmental problems.We report a robust PCSS in which lattice matching enables bottom-up oriented assembly between metal-organic frameworks(MOFs)and inorganic nanocrystals(INCs),two distinct entities that differ drastically in structure and function.Specifically,cubic-phase Prussian blue(PB)of a framework backbone is spontaneously attached to rutile TiO_(2)nanowires in a defined orientation triggered by the lattice matching between the(001)plane of TiO_(2)and the(222)plane of PB.Ultraviolet light irradiation accelerates the photoelectron transport within the oriented TiO_(2)/PB system and enables fast photo switching.The derived TiO_(2)/PB paper can be ranked as one of the best light-printing papers in literature because of its high resolution(∼µm)and capability to be repeatedly written for>100 times without significant loss of contrast.The ultrathin TiO_(2)nanowires are rich in oxygen and Ti vacancies,which allow visible-and sunlight-light printing.Density functional theory calculations suggest that the[Fe(CN)_(6)]^(4−) ligand from the PB attaches preferentially to the(110)surface of TiO_(2)to give the ordered TiO_(2)/PB assembly.The findings demonstrate the strong versatility of particles-mediated assembly in advanced materials design.展开更多
Li metal anodes have attracted tremendous attention in the last decade because of their high theoretical capacities and low electrochemical potentials.However,until now,there has only been limited success in improving...Li metal anodes have attracted tremendous attention in the last decade because of their high theoretical capacities and low electrochemical potentials.However,until now,there has only been limited success in improving the interfacial and structural stabilities and in realizing the highly controllable and large-scale fabrication of this emerging material;these limitations have posed great obstacles to further performing fundamental and applied studies in Li metal anodes.In this review,we focus on summarizing the existing challenges of Li metal anodes based on the leap from coin cells to pouch cells and on outlining typical methods for designing Li metal anodes on demand;we controllably engineer their surface protection layers and structure sizes by encapsulating structured Li metal inside a variety of synthetic protection layers.We aim to provide a comprehensive understanding and serve as a strategic guide for designing and fabricating practicable Li metal anodes for use in pouch batteries.Challenges and opportunities regarding this burgeoning field are critically evaluated at the end of this review.展开更多
Fusarium head blight (FHB) is one of the most destructive diseases in global wheat production. In order to count the FHB-infected wheat ears under field conditions, this study proposed an algorithm for diseased wheat ...Fusarium head blight (FHB) is one of the most destructive diseases in global wheat production. In order to count the FHB-infected wheat ears under field conditions, this study proposed an algorithm for diseased wheat ear detection based on improved YOLOv5s (Tr-YOLOv5s). The Swin Transformer was used to replace the CSPDarknet backbone network to enhance the extraction of characteristic information of the population wheat ears of FHB in the field background. The convolutional block attention module (CBAM) attention mechanism was added to improve the detection effect of target wheat ears, subsequently improving the overall accuracy of the model. The original loss function complete intersection over union (CIoU) was replaced by Scylla intersection over union (SIoU) loss to accelerate the model convergence and decrease the loss value. The results showed that the mean average precision (mAP) of the Tr-YOLOv5s model reached 90.64%, making a 4.63% improvement compared to the original YOLOv5s model. The improved model could quickly detect and count wheat FHB ear in the field environment, which laid a foundation for the subsequent automatic disease identification and grading of wheat FHB under field conditions.展开更多
Purpose In the JUNO,the LS serves as the medium for detecting neutrinos.When purifying the LS using HPN,it is essential to ensure low background levels of radioactive krypton and argon in the HPN Methods Using the low...Purpose In the JUNO,the LS serves as the medium for detecting neutrinos.When purifying the LS using HPN,it is essential to ensure low background levels of radioactive krypton and argon in the HPN Methods Using the low-temperature physical adsorption properties of activated carbon to adsorb and separate radioactive gases such as radon,krypton,and argon from nitrogen in a liquid nitrogen environment.Results Our results indicated that the Kr concentration in the HPN purified by HP activated carbon is 6.84μBq/m,and the Ar concentration is 3.6μBq/m for overground HPN,while the Kr concentration is 31.4μBq/m for underground HPN.The^(85)Kr concentration in the nitrogen purified by coconut shell activated carbon is 0.46μBq/m.Conclusions After adsorption with activated carbon,the content of^(39)Kr and Ar in HPN is lower than the 50μBq/m required by JUNO.This work validates that the^(85)Kr and^(39)Ar concentrations in HPN is fit the JUNO requirement.展开更多
基金financially supported by the General Research Fund(CityU 11315622 and CityU 11310123)National Natural Science Foundation(NSFC 52372229 and NSFC 52172241)+3 种基金Green Tech Fund(GTF202220105)Guangdong Basic and Applied Basic Research Foundation(2024A1515011008)City University of Hong Kong(No.9020002)the Shenzhen Research Institute of City University of Hong Kong.
文摘The development of flexible zinc-ion batteries(ZIBs)faces a threeway trade-off among the ionic conductivity,Zn^(2+)mobility,and the electrochemical stability of hydrogel electrolytes.To address this challenge,we designed a cationic hydrogel named PAPTMA to holistically improve the reversibility of ZIBs.The long cationic branch chains in the polymeric matrix construct express pathways for rapid Zn^(2+)transport through an ionic repulsion mechanism,achieving simultaneously high Zn^(2+)transference number(0.79)and high ionic conductivity(28.7 mS cm−1).Additionally,the reactivity of water in the PAPTMA hydrogels is significantly inhibited,thus possessing a strong resistance to parasitic reactions.Mechanical characterization further reveals the superior tensile and adhesion strength of PAPTMA.Leveraging these properties,symmetric batteries employing PAPTMA hydrogel deliver exceeding 6000 h of reversible cycling at 1 mA cm^(−2) and maintain stable operation for 1000 h with a discharge of depth of 71%.When applied in 4×4 cm2 pouch cells with MnO_(2) as the cathode material,the device demonstrates remarkable operational stability and mechanical robustness through 150 cycles.This work presents an eclectic strategy for designing advanced hydrogels that combine high ionic conductivity,enhanced Zn^(2+)mobility,and strong resistance to parasitic reactions,paving the way for long-lasting flexible ZIBs.
基金the National Natural Science Foundation of China(21771018,21875004)Beijing University of Chemical Technology(start-up grant buctrc201901,BUCT,China)Technology Innovation Project of New Energy Vehicles Industry and Pulead Technology Industry Co.Ltd。
文摘Lithium metal attracts growing attention as an ideal anode candidate for next generation lithium battery systems owing to its high capacity,low density,and low working potential.However,the volume expansion of the bulk and dendrite growth on the surface of lithium anode limits its practical application.Herein,we fabricate a composite lithium host featuring both multiple scaled structure and lithiophilic property to address obstacles at both aspects of bulk and surface simultaneously.In which,the multiple scaled structure provides void space to accommodate lithium volume change while zinc and cobalt oxides sites derived from Zeolitic Imidazolate Frameworks can react with lithium and form a stable solid electrolyte interphase,leading to a stable cycling of lithium symmetrical cell for more than 500 cycles with voltage hysteresis of only 88 mV at 2 mAcm^-2 and 5 mAh cm^-2.Moreover,full cells paired with LiFePO4 cathode can realize 500 cycles with 99.2%capacity retention,showing great potential for practical applications.The excellent electrochemical performance of the composite lithium anode proves the effectiveness of our anode design with multiple scaled structure and lithiophilic feature,which can be also expanded to other metal anodes for batteries.
文摘The photocatalytic production of syngas using a noble-metal-free catalytic system is a promising approach for renewable energy and environmental sustainability.In this study,we demonstrate an efficient catalytic system formed by integrating Co single sites,which act as the active sites,in covalent triazine frameworks(CTFs),which act as the photoabsorber,for the photocatalytic production of syngas from CO2 in aqueous solution.The enhanced light absorption of the CTFs,which contain intramolecular heterojunctions,in conjunction with 0.8 mmol L^‒1 of the Co complex enables excellent syngas production with a yield of 3303μmol g‒1(CO:H2=1.4:1)in 10 h,which is about three times greater than that achieved using CTF without a heterojunction.In the photocatalytic reaction,the coordinated single Co centers accept the photogenerated electrons from the CTF,and serve as active sites for CO2 conversion through an adsorption-activation-reaction mechanism.Theoretical calculations further reveal that the intramolecular heterojunctions highly promote photogenerated charge separation,thus boosting photocatalytic syngas production.This work reveals the promising potential of CTFs for single-metal-site-based photocatalysis.
基金Project supported by the National Natural Science Foundation of China (51972061,22109025,22171045,52072076)。
文摘The Er3+doped double perovskite Ba_(2)CaWO_(6) crystal is a promising ratiometric thermometer based on the fluorescence intensity ratio(FIR) of transitions from ^(2)H_(11/2) and ^(4)S_(3/2) to the lowered ^(4)I_(15/2) level.However,the Ca^(2+) vacancy defect caused by the charge difference between rare-earth ions and the substituted alkaline-earth ions gives rise to the non-radiative probability and limits the thermal sensitivity.Here,the up-conversion luminescence and thermometric performance of Er^(3+),Yb^(3+) dopedBa_(2)CaWO_(6) are tuned by tri-doping with alkaline ions.The Ca^(2+) vacancy defect can be eliminated by the introduction of Na^(+),which occupies the Ca^(2+) site when it is doped into Ba_(2)CaWO_(6) with Er^(3+) and Yb^(3+).On the contrary,the doping of Cs^(+) into Ba_(2)CaWO_(6) with Er^(3+) and Yb^(3+) enhances the defect concentration because it occupies the site of Ba^(2+).Thus,the tri-doping of Na^(+) reduces the non-radiative probability and enhances the quantum efficiency of Er^(3+),leading to the improvement of the thermometric sensitivity of Ba_(2)CaWO_(6).As a result,we get an excellent thermometric Ba_(2)CaWO_(6):8%Yb^(3+),3.5%Er^(3+),6%Na^(+) powder with a luminescence lifetime of 515 μs and maximum thermal sensitivity(S_(r)) of 1.45%/K,which is more than three times higher than that of the BCWO:Er^(3+) powder.
基金financially supported by PULEAD Technology Industry Co.,Ltd.,the Strategic Priority Research Program of Chinese Academy of Sciences (No. XDB36000000)the National Key Research and Development Program of China (No. 2016YFA0200904)+3 种基金the National Natural Science Foundation of China (Nos. 21771018and 21875004)the Natural Science Foundation of Beijing (No.2192018)National Natural Science Foundation of China-Regional Innovation Joint Exploration Fund (No. U19A2019)Beijing University of Chemical Technology (Start-up grant No. buctrc201901,BUCT, China)。
文摘Metal skeletons,such as Nickel Foam(NF) has attracted worldwide interests as stable host for lithium metal anode because of its high stability,large specific surface area and high conductivity.However,most metal skeletons have lithophobic surface and uneven current distribution that result in sporadic lithium nucleation and uncontrolled dendrites growth.Herein,we describe a sequential immersing strategy to generate interwoven Nickel(Ⅱ)-dimethylglyoxime(Ni-DMG) nanowires at NF to obtain composite skeleton(NDNF),which can be used as an stable host for Li metal storage.The Ni-DMG has proved effective to realize uniform lithium nucleation and dendrite-free lithium deposition.Combing with the three dimensional(3 D) hierarchical porous structure,the composite host shows a significantly improved coulombic efficiency(CE) than pristine commercial nickel foam.Moreover,the corresponding Li‖Li symmetrical cells can run more than 700 h with low voltage hysteresis 22 mV at 1.0 mA/cm^(2),and Li@NDNF‖LiFePO;full-cell exhibits a high capacity retention of 82.03% at 1.0 C during 630 cycles.These results proved the effectiveness of metal-organic complexes in governing Li metal growth and can be employed as a new strategy for dendrite-free Li metal anode and safe Li metal batteries(LMBs).
基金supported by the National Key R&D Program of China[Nos.2018YFB1304902,2016YFA0300804,2016YFA0300903]the National Natural Science Foundation of China[Nos.51672007,11974023,11904372,11704389,U1813211]+3 种基金the Key-Area Research and Development Program of Guang Dong Province[Nos.2018B030327001,2018B010109009]the‘‘2011 Program”Peking-Tsinghua-IOP Collaborative Innovation Center of Quantum Matterthe Beijing Institute of Technology Research Fund Program for Young Scholarsthe Beijing Institute of Technology laboratory research project[No.2019BITSYA03]。
文摘The two-dimensional (2D) structure of layered transition metal dichalcogenides (TMDs) provides unusual physical properties [1,2]and chemical reactivity [3,4], which can be influenced by defects such as dislocations [5,6]. For example, dislocations can act as nucleation sites for the onset of deformation when subjected to stress [7].
基金supported primarily by National Natural Science Foundation of China(Nos.22109025,51972061)National Key Research and Development Program of China(No.2020YFA0710303)Natural Science Foundation of Fujian Province,China(No.2021J05121)。
文摘Side reactions and dendrite growth triggered by the unstable interface and inhomogeneous deposition have become the biggest obstacle to the commercialization for lithium metal batteries.In this study,a highly-chlorinated organic-inorganic hybrid interfacial protective layer is developed by rationally tuning the interfacial passivation and robustness to achieve the convenient and efficient Li metal anode.The polyvinyl chloride(PVC)can effectively resist water and oxygen,which is confirmed by density functional theory.The organic-dominant solid electrolyte interphases(SEI)with lithium chloride are investigated by the X-ray photoelectron spectroscopy(XPS)with little mineralization of oxide,such as Li_(2)O and Li_(2)CO_(3).With such artificial SEI,a uniform and dense lithium deposition morphology are formed and an ultra-long stable cycle of over 500 h are achieved even at an ultra-high current density of 10 m A/cm^(2).Moreover,the simple and convenient protected anode also exhibits excellent battery stability when paired with the LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)and LiFePO_(4)(LFP)cathode,showing great potential for the commercial application of lithium metal batteries.
基金supported primarily by the National Natural Science Foundation of China(No.22109025)National Key Research and Development Program of China(No.2020YFA0710303)Natural Science Foundation of Fujian Province,China(No.2021J05121)。
文摘The development of lithium-metal batteries(LMBs)is seriously restricted by the out-of-control dendrites growth and infinite volume expansion.Herein,a pervasive organic-inorganic layer construction strategy is reported for the composite lithium metal anode with congener-derived organic-inorganic solid electrolyte interphase(SEI).In this strategy,the organic-inorganic Ag@polydopamine(Ag@PDA)layer is coated on the arbitrary substrates by a simple two-step method.The thin and stable congener-derived SEI is insitu formed with fewer inorganic components and more organic components during charging/discharging.The polydopamine with sufficient adhesion groups and lithiophilic Ag layer realize near-zero nucleation overpotential during lithium deposition.The low interface resistance and stable lithium deposition are achieved.Moreover,the practical areal and volumetric capacities of the composite anode with three-dimensional copper(3DCu)as the substrate are 10 mAh/cm^(2)and 1538 mAh/cm^3(vs.the mass of anode).The symmetrical cell shows very low polarization voltage(10 mV)and more than 2500 h cycles life at 1 mA/cm^(2)(1 mAh/cm^(2)).The LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)-based full cells show improved capacity retention(82%)after 100 cycles at 0.5 C.The modified lithiophilic anode with congener-derived interphase provides a promising strategy to realize the next-generation dendrite-free LMBs.
基金supported primarily by the National Key Research and Development Program of China(2020YFA0710303)National Natural Science Foundation of China(No.22109025)Natural Science Foundation of Fujian Province,China(2021J05121).
文摘Lithium-metal batteries with high energy/power densities have significant applications in electronics,electric vehicles,and stationary power plants.However,the unstable lithium-metal-anode/electrolyte interface has induced insufficient cycle life and safety issues.To improve the cycle life and safety,understanding the formation of the solid electrolyte interphase(SEI)and growth of lithium dendrites near the anode/electrolyte interface,regulating the electrodeposition/electrostripping processes of Li^(+),and developing multiple approaches for protecting the lithium-metal surface and SEI layer are crucial and necessary.This paper comprehensively reviews the research progress in SEI and lithium dendrite growth in terms of their classical electrochemical lithium plating/stripping processes,interface interaction/nucleation processes,anode geometric evolution,fundamental electrolyte reduction mechanisms,and effects on battery performance.Some important aspects,such as charge transfer,the local current distribution,solvation,desolvation,ion diffusion through the interface,inhibition of dendrites by the SEI,additives,models for dendrite formation,heterogeneous nucleation,asymmetric processes during stripping/plating,the host matrix,and in situ nucleation characterization,are also analyzed based on experimental observations and theoretical calculations.Several technical challenges in improving SEI properties and reducing lithium dendrite growth are analyzed.Furthermore,possible future research directions for overcoming the challenges are also proposed to facilitate further research and development toward practical applications.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.22105133 and 22101191)China Postdoctoral Science Foundation(Nos.BX20190222,2019M663490,and 2021M692261)+1 种基金the Fundamental Research Funds for the Central Universities(Nos.20826041E4211,20826041E4258,20826041E4212,2021SCU12150 and 2021SCU12151)the China Scholarship Council,and Sichuan Science and Technology Program(No.2021YJ0405).
文摘CO_(2)electroreduction has been regarded as an appealing strategy for renewable energy storage.Recently,bismuth(Bi)electrocatalysts have attracted much attention due to their excellent formate selectivity.However,many reported Bi electrocatalysts suffer from low current densities,which are insufficient for industrial applications.To reach the goal of high current CO_(2)reduction to formate,we fabricate Bi nanosheets(NS)with high activity through edge/terrace control and defect engineering strategy.Bi NS with preferential exposure sites are obtained by topotactic transformation,and the processes are clearly monitored by in-situ Raman and ex-situ X-ray diffraction(XRD).Bi NS-1 with a high fraction of edge sites and defect sites exhibits excellent performance,and the current density is up to ca.870 mA·cm^(−2)in the flow cell,far above the industrially applicable level(100 mA·cm^(−2)),with a formate Faradaic efficiency greater than 90%.In-situ Fourier transform infrared(FT-IR)spectra detect*OCHO,and theoretical calculations reveal that the formation energy of*OCHO on edges is lower than that on terraces,while the defects on edges further reduce the free energy changes(ΔG).The differential charge density spatial distributions reveal that the presence of defects on edges causes charge enrichment around the C–H bond,benefiting the stabilization of the*OCHO intermediate,thus remarkably lowering theΔG.
基金supported by the National Key Research and Development Program of China(2020YFA0710303)the National Natural Science Foundation of China(52002072,U1905215,52072076)the Natural Science Foundation of Fujian Province(2021J01589,2023J05082)。
基金supported by the National Key Research and Development Program of China(2020YFA0710303)the National Natural Science Foundation of China(U1905215,51772053,52072076)。
文摘The photoreversible color switching system(PCSS)is attracting increasing attention for use in alleviating energy crisis and environmental problems.We report a robust PCSS in which lattice matching enables bottom-up oriented assembly between metal-organic frameworks(MOFs)and inorganic nanocrystals(INCs),two distinct entities that differ drastically in structure and function.Specifically,cubic-phase Prussian blue(PB)of a framework backbone is spontaneously attached to rutile TiO_(2)nanowires in a defined orientation triggered by the lattice matching between the(001)plane of TiO_(2)and the(222)plane of PB.Ultraviolet light irradiation accelerates the photoelectron transport within the oriented TiO_(2)/PB system and enables fast photo switching.The derived TiO_(2)/PB paper can be ranked as one of the best light-printing papers in literature because of its high resolution(∼µm)and capability to be repeatedly written for>100 times without significant loss of contrast.The ultrathin TiO_(2)nanowires are rich in oxygen and Ti vacancies,which allow visible-and sunlight-light printing.Density functional theory calculations suggest that the[Fe(CN)_(6)]^(4−) ligand from the PB attaches preferentially to the(110)surface of TiO_(2)to give the ordered TiO_(2)/PB assembly.The findings demonstrate the strong versatility of particles-mediated assembly in advanced materials design.
基金supported by the National Natural Science Foundation of China(Nos.52071227,22109025)the Key Scientific Research Project in Shanxi Province(Grant No.201805D121003)+5 种基金the Special Found Projects for Central Government Guidance to Local Science and Technology Developmentthe Science and Technology Major Projects of Shanxi Province(20191102004)the Fundamental Research Program of Shanxi Province(202103021222006)the Natural Science Foundation of Shanxi Province(2019D111102)the Research Project Supported by Shanxi Scholarship Council of China(HGKY2019085)the Natural Science Foundation of Fujian Province,China(2021J05121).
文摘Li metal anodes have attracted tremendous attention in the last decade because of their high theoretical capacities and low electrochemical potentials.However,until now,there has only been limited success in improving the interfacial and structural stabilities and in realizing the highly controllable and large-scale fabrication of this emerging material;these limitations have posed great obstacles to further performing fundamental and applied studies in Li metal anodes.In this review,we focus on summarizing the existing challenges of Li metal anodes based on the leap from coin cells to pouch cells and on outlining typical methods for designing Li metal anodes on demand;we controllably engineer their surface protection layers and structure sizes by encapsulating structured Li metal inside a variety of synthetic protection layers.We aim to provide a comprehensive understanding and serve as a strategic guide for designing and fabricating practicable Li metal anodes for use in pouch batteries.Challenges and opportunities regarding this burgeoning field are critically evaluated at the end of this review.
基金Bai for their strong support for this work. This study was supported by the Natural Science Foundation of Henan Province (NO. 222301420113, 232102520006)Major Science and Technology Special Project of Henan Province (NO. 221100210600)+2 种基金Henan Province key research and development project (NO. 231111110100)Key Scientific and Technological Project of Henan Province (NO. 242102111193)the Natural Science Foundation of China(NO. 31501225, 42101362).
文摘Fusarium head blight (FHB) is one of the most destructive diseases in global wheat production. In order to count the FHB-infected wheat ears under field conditions, this study proposed an algorithm for diseased wheat ear detection based on improved YOLOv5s (Tr-YOLOv5s). The Swin Transformer was used to replace the CSPDarknet backbone network to enhance the extraction of characteristic information of the population wheat ears of FHB in the field background. The convolutional block attention module (CBAM) attention mechanism was added to improve the detection effect of target wheat ears, subsequently improving the overall accuracy of the model. The original loss function complete intersection over union (CIoU) was replaced by Scylla intersection over union (SIoU) loss to accelerate the model convergence and decrease the loss value. The results showed that the mean average precision (mAP) of the Tr-YOLOv5s model reached 90.64%, making a 4.63% improvement compared to the original YOLOv5s model. The improved model could quickly detect and count wheat FHB ear in the field environment, which laid a foundation for the subsequent automatic disease identification and grading of wheat FHB under field conditions.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA10010500).
文摘Purpose In the JUNO,the LS serves as the medium for detecting neutrinos.When purifying the LS using HPN,it is essential to ensure low background levels of radioactive krypton and argon in the HPN Methods Using the low-temperature physical adsorption properties of activated carbon to adsorb and separate radioactive gases such as radon,krypton,and argon from nitrogen in a liquid nitrogen environment.Results Our results indicated that the Kr concentration in the HPN purified by HP activated carbon is 6.84μBq/m,and the Ar concentration is 3.6μBq/m for overground HPN,while the Kr concentration is 31.4μBq/m for underground HPN.The^(85)Kr concentration in the nitrogen purified by coconut shell activated carbon is 0.46μBq/m.Conclusions After adsorption with activated carbon,the content of^(39)Kr and Ar in HPN is lower than the 50μBq/m required by JUNO.This work validates that the^(85)Kr and^(39)Ar concentrations in HPN is fit the JUNO requirement.
