In spite of the tumor microenvironments responsive cancer therapy based on Fenton reaction(i.e.,chemodynamic therapy,CDT)has been attracted more attentions in recent years,the limited Fenton reaction efficiency is the...In spite of the tumor microenvironments responsive cancer therapy based on Fenton reaction(i.e.,chemodynamic therapy,CDT)has been attracted more attentions in recent years,the limited Fenton reaction efficiency is the important obstacle to further application in clinic.Herein,we synthesized novel FeO/MoS2 nanocomposites modified by bovine serum albumin(FeO/MoS2-BSA)with boosted Fenton reaction efficiency by the synergistic effect of co-catalyze and photothermal effect of MoS2 nanosheets triggered by the second near-infrared(NIR II)light.In the tumor microenvironments,the MoS2 nanosheets not only can accelerate the conversion of Fe3+ions to Fe2+ions by Mo4+ions on their surface to improve Fenton reaction efficiency,but also endow FeO/MoS2-BSA with good photothermal performances for photothermal-enhanced CDT and photothermal therapy(PTT).Consequently,benefiting from the synergetic-enhanced CDT/PTT,the tumors are eradicated completely in vivo.This work provides innovative synergistic strategy for constructing nanocomposites for highly efficient CDT.展开更多
The electrocatalytic activity of transition-metal-based compounds is closely related to the electronic configuration.However,optimizing the surface electron spin state of catalysts remains a challenge.Here,we develope...The electrocatalytic activity of transition-metal-based compounds is closely related to the electronic configuration.However,optimizing the surface electron spin state of catalysts remains a challenge.Here,we developed a spin-state and delocalized electron regulation method to optimize oxygen evolution reaction(OER)performance by in-situ growth of NiCo_(2)(OH)_(x) using Oswald ripening and coordinating etching process on MXene and plasma treatment.X-ray absorption spectroscopy,magnetic tests and electron paramagnetic resonance reveal that the coupling of NiCo_(2)(OH)_(x) and MXene can induce remarkable spin-state transition of Co^(3+)and transition metal ions electron delocalization,plasma treatment further optimizes the 3 d orbital structure and delocalized electron density.The unique Jahn-Teller phenomenon can be brought by the intermediate spin state(t2 _(g)^(5) e_(g)^(1))of Co^(3+),which benefits from the partial electron occupied egorbitals.This distinct electron configuration(t2_(g)^(5) e_(g)^(1))with unpaired electrons leads to orbital degeneracy,that the adsorption free energy of intermediate species and conductivity were further optimized.The optimized electrocatalyst exhibits excellent OER activity with an overpotential of 268 m V at 10 m A cm^(-2).DFT calculations show that plasma treatment can effectively regulate the d-band center of TMs to optimize the adsorption and improve the OER activity.This approach could guide the rational design and discovery of electrocatalysts with ideal electron configurations in the future.展开更多
Antimony-based anodes have attracted wide attention in potassium-ion batteries due to their high theoretical specific capacities(∼660 mA h g^(-1))and suitable voltage platforms.However,severe capacity fading caused b...Antimony-based anodes have attracted wide attention in potassium-ion batteries due to their high theoretical specific capacities(∼660 mA h g^(-1))and suitable voltage platforms.However,severe capacity fading caused by huge volume change and limited ion transportation hinders their practical applications.Recently,strategies for controlling the morphologies of Sb-based materials to improve the electrochemical performances have been proposed.Among these,the two-dimensional Sb(2D-Sb)materials present excellent properties due to shorted ion immigration paths and enhanced ion diffusion.Nevertheless,the synthetic methods are usually tedious,and even the mechanism of these strategies remains elusive,especially how to obtain large-scale 2D-Sb materials.Herein,a novel strategy to synthesize 2D-Sb material using a straightforward solvothermal method without the requirement of a complex nanostructure design is provided.This method leverages the selective adsorption of aldehyde groups in furfural to induce crystal growth,while concurrently reducing and coating a nitrogen-doped carbon layer.Compared to the reported methods,it is simpler,more efficient,and conducive to the production of composite nanosheets with uniform thickness(3–4 nm).The 2D-Sb@NC nanosheet anode delivers an extremely high capacity of 504.5 mA h g^(-1) at current densities of 100 mA g^(-1) and remains stable for more than 200 cycles.Through characterizations and molecular dynamic simulations,how potassium storage kinetics between 2D Sb-based materials and bulk Sb-based materials are explored,and detailed explanations are provided.These findings offer novel insights into the development of durable 2D alloy-based anodes for next-generation potassium-ion batteries.展开更多
KFeSO_(4)F(KFSF)is considered a potential cathode due to the large capacity and low cost.However,the inferior electronic conductivity leads to poor electrochemical performance.Defect engineering can facilitate the ele...KFeSO_(4)F(KFSF)is considered a potential cathode due to the large capacity and low cost.However,the inferior electronic conductivity leads to poor electrochemical performance.Defect engineering can facilitate the electron/ion transfer by tuning electronic structure,thus providing favorable electrochemical performance.Herein,through the regulation of surface defect engineering in reduced graphene oxide(rGO),the Fe–C bonds were formed between KFSF and rGO.The Fe–C bonds formed work in regulating the Fe-3d orbital as well as promoting the migration ability of K ions and increasing the electronic conductivity of KFSF.Thus,the KFSF@rGO delivers a high capacity of 119.6 mAh g^(-1).When matched with a graphite@pitch-derived S-doped carbon anode,the full cell delivers an energy density of 250.5 Wh kg^(-1) and a capacity retention of 81.5%after 400 cycles.This work offers a simple and valid method to develop high-performance cathodes by tuning defect sites.展开更多
Manganese oxides are regarded as one of the most promising cathode materials in rechargeable aqueous Zn-ion batteries(ZIBs)because of the low price and high security.However,the practical application of Mn2O3 in ZIBs ...Manganese oxides are regarded as one of the most promising cathode materials in rechargeable aqueous Zn-ion batteries(ZIBs)because of the low price and high security.However,the practical application of Mn2O3 in ZIBs is still plagued by the low specific capacity and poor rate capability.Herein,highly crystalline Mn2O3 materials with interconnected mesostructures and controllable pore sizes are obtained via a ligand-assisted self-assembly process and used as high-performance electrode materials for reversible aqueous ZIBs.The coordination degree between Mn2+and citric acid ligand plays a crucial role in the formation of the mesostructure,and the pore sizes can be easily tuned from 3.2 to 7.3 nm.Ascribed to the unique feature of nanoporous architectures,excellent zinc-storage performance can be achieved in ZIBs during charge/discharge processes.The Mn2O3 electrode exhibits high reversible capacity(233 mAh g−1 at 0.3 A g−1),superior rate capability(162 mAh g−1 retains at 3.08 A g−1)and remarkable cycling durability over 3000 cycles at a high current rate of 3.08 A g−1.Moreover,the corresponding electrode reaction mechanism is studied in depth according to a series of analytical methods.These results suggest that rational design of the nanoporous architecture for electrode materials can effectively improve the battery performance.展开更多
Kesterite Cu2ZnSn(S,Se)4(CZTSSe)solar cells have drawn worldwide attention for their promising photovoltaics performance and earth-abundant element composition,yet the record efficiency of this type of device is still...Kesterite Cu2ZnSn(S,Se)4(CZTSSe)solar cells have drawn worldwide attention for their promising photovoltaics performance and earth-abundant element composition,yet the record efficiency of this type of device is still far lower than its theoretical conversion efficiency.Undesirable band alignment and severe non-radiative recombination at CZTSSe/CdS heterojunction interfaces are the major causes limiting the current/voltage output and overall device performance.Herein,we propose a novel two-step CdS deposition strategy to improve the quality of CZTSSe/CdS heterojunction interface and thereby improve the performance of CZTSSe solar cell.The two-step strategy includes firstly pre-deposits CdS thin layer on CZTSSe absorber layer by chemical bath deposition(CBD),followed with a mild heat treatment to facilitate element inter-diffusion,and secondly deposits an appropriate thickness of CdS layer by CBD to cover the whole surface of pre-deposited CdS and CZTSSe layers.The solar energy conversion efficiency of CZTSSe solar cells with two-step deposited CdS layer approaches to 8.76%(with an active area of about 0.19 cm2),which shows an encouraging improvement of over 87.98%or 30.16%compared to the devices with traditional CBD-deposited CdS layer without and with the mild annealing process,respectively.The performance enhancement by the two-step CdS deposition is attributed to the formation of more favorable band alignment at CZTSSe/CdS interface as well as the effective decrease in interfacial recombination paths on the basis of material and device characterizations.The two-step CdS deposition strategy is simple but effective,and should have large room to improve the quality of CZTSSe/CdS heterojunction interface and further lift up the conversion efficiency of CZTSSe solar cells.展开更多
Ultra-high nickel cobalt-free lithium layered oxides are promising cathode material for lithium-ion batteries(LIBs)because of their relatively high capacity and low cost.Nevertheless,the high nickel content would indu...Ultra-high nickel cobalt-free lithium layered oxides are promising cathode material for lithium-ion batteries(LIBs)because of their relatively high capacity and low cost.Nevertheless,the high nickel content would induce bulk structure degradation and interfacial environment deterioration,and the absence of Co element reduces the lithium diffusion kinetics,severely limiting the performance liberation of this kind of cathodes.Herein,a multifunctional Ti/Zr dual cation co-doping strategy has been employed to improve the lithium storage performance of LiNi_(0.9)Mn_(0.1)O_(2)(NM91)cathode.On the one hand,the Ti/Zr co-doping weakens the Li^(+)/Ni^(2+)mixing through magnetic interactions due to the inexistence of unpaired electrons for Ti^(4+)and Zr^(4+),increasing the lithium diffusion rate and suppressing the harmful coexistence of H1 and H2 phases.On the other hand,they enhance the lattice oxygen stability because of the strong Ti-O and Zr-O bonds,inhibiting the undesired H3 phase transition and lattice oxygen loss,improving the bulk structure and cathode-electrolyte interface stability.As a result,the Ti/Zr co-doped NM91(NMTZ)exhibits a 91.2%capacity retention rate after 100 cycles,while that of NM91 is only82.9%.Also,the NMTZ displays better rate performance than NM91 with output capacities of 115 and93 mA h g^(-1)at a high current density of 5 C,respectively.Moreover,the designed NMTZ could enable the full battery to deliver an energy density up to 263 W h kg^(-1),making the ultra-high nickel cobaltfree lithium layered oxide cathode closer to practical applications.展开更多
Galvanic deposition method was used to prepare the Pd/Ni-Al2O3-GD catalyst for the combustion of methane under lean conditions. The new catalyst and compared catalysts （Pd/Al2O3-IW, Pd-Ni/Al2O3-IW, Pd/Ni-Al2O3-IW） p...Galvanic deposition method was used to prepare the Pd/Ni-Al2O3-GD catalyst for the combustion of methane under lean conditions. The new catalyst and compared catalysts （Pd/Al2O3-IW, Pd-Ni/Al2O3-IW, Pd/Ni-Al2O3-IW） prepared by incipient wetness impregnation were characterized by N2-physisorption, XRD and TEM to clarify particle size and size distribution of palladium species. Combined O2-TPD and XPS results with the catalytic data, it shows that the surface palladium species with low valence exhibits better combustion performance due to their stronger interaction with support. The results indicate that the galvanic deposition method is an effective route to prepare efficient catalyst for methane combustion, and it also provides useful information for improving the present commercial catalyst.展开更多
Despite of suitable band structures for harvesting solar light and driving water redox reactions,polymeric carbon nitride(PCN)has suffered from poor charge transfer ability and sluggish surface reaction kinetics,which...Despite of suitable band structures for harvesting solar light and driving water redox reactions,polymeric carbon nitride(PCN)has suffered from poor charge transfer ability and sluggish surface reaction kinetics,which limit its photocatalytic activity for water splitting.Herein,atomically dispersed Zn-coordinated three-dimensional(3D)sponge-like PCN(Zn-PCN)is synthesized through a novel intermediate coordination strategy.Advanced characterizations and theoretical calculations well evidence that Zn single atoms are coordinated and stabilized on PCN in the form of Zn-N_(6) configura-tion featured with an electron-deficient state.Such an electronic configuration has been demonstrated contributive to promoted electron excitation,accelerated charge separation and transfer as well as reduced water redox barriers.Further benefited from the abundant surface active sites derived from the 3D porous structure,Zn-PCN realizes visible-light photocatalysis for overall water splitting with H_(2) and O_(2) simultaneously evolved at a stoichiometric ratio of 2:1.This work brings new insights into the design of novel single-atom photocatalysts by deepening the understanding of electronic configurations and reactive sites favorable to excellent photocatalysis for water splitting and related solar energy conversion reactions.展开更多
Supercapacitors（SCs） have attracted much attention as one of the alternative energy devices due to their high power performance,long cycle life,and low maintenance cost.Graphene is considered as an innovative and pr...Supercapacitors（SCs） have attracted much attention as one of the alternative energy devices due to their high power performance,long cycle life,and low maintenance cost.Graphene is considered as an innovative and promising material due to its large theoretical specific surface area,high electrical conductivity,good mechanical properties and chemical stability.Herein,we report an effective strategy for elaborately constructing rationally functionalized self-standing graphene（SG） obtained from giant graphene oxide（GGO） paper followed by an ultrarapid thermal-processing.This treatment results in both the exfoliation of graphene sheets and the reduction of GGO by elimination of oxygencontaining groups.The as-prepared SG electrode materials without additive and conducting agent provide an excellent combination of the electrical double layer capacitor（EDLC） and pseudocapacitor（PC） functions and exhibit superior electrochemical performance,including high specific capacitance,good rate capability and excellent cycling stability when investigated in three-electrode electrochemical cells.展开更多
The solid electrolyte interphase(SEI)layer,formed on the electrode through electrolyte decomposition,has garnered significant attention over the past several decades.Numerous characterization studies have shown that t...The solid electrolyte interphase(SEI)layer,formed on the electrode through electrolyte decomposition,has garnered significant attention over the past several decades.Numerous characterization studies have shown that the SEI enhances the stability of both the electrolyte and electrode,particularly by mitigating the well-known cation-solvent co-intercalation in graphite electrodes in lithium-ion batteries.However,recent electrolyte exchange experiments have revealed that variations in electrolyte solvation structure and the resulting desolvation behaviors play a more dominant role than the SEI in influencing electrolyte and electrode stability,which in turn critically impacts battery performance.In addition to contributing to the ongoing debate,electrolyte exchange experiments have proven to be a valuable tool for analyzing failures in electrolytes,electrodes,and batteries.This review highlights the application of electrolyte exchange experiments across various metal-ion batteries,incorporating diverse combinations of electrolytes and electrodes.It examines the influence of electrolyte solvation structures and desolvation behaviors on the stability of both electrolytes and electrodes.The aim is to enhance the methodology of electrolyte exchange experiments to deepen the understanding of the molecular interactions among metal ions,anions,and solvents within the electrolyte.This approach complements existing insights into SEI effects,providing a more thorough and accurate framework for battery failure analysis.展开更多
基金This work was supported by the financial aid from the National Natural Science Foundation of China(Grant Nos.51502284,21834007,21521092,21590794,and 21673220)the Program of Science and Technology Development Plan of Jilin Province of China(No.20170101186JC)+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB20030300)the Youth Innovation Promotion Association of Chinese Academy of Sciences(2019232).
文摘In spite of the tumor microenvironments responsive cancer therapy based on Fenton reaction(i.e.,chemodynamic therapy,CDT)has been attracted more attentions in recent years,the limited Fenton reaction efficiency is the important obstacle to further application in clinic.Herein,we synthesized novel FeO/MoS2 nanocomposites modified by bovine serum albumin(FeO/MoS2-BSA)with boosted Fenton reaction efficiency by the synergistic effect of co-catalyze and photothermal effect of MoS2 nanosheets triggered by the second near-infrared(NIR II)light.In the tumor microenvironments,the MoS2 nanosheets not only can accelerate the conversion of Fe3+ions to Fe2+ions by Mo4+ions on their surface to improve Fenton reaction efficiency,but also endow FeO/MoS2-BSA with good photothermal performances for photothermal-enhanced CDT and photothermal therapy(PTT).Consequently,benefiting from the synergetic-enhanced CDT/PTT,the tumors are eradicated completely in vivo.This work provides innovative synergistic strategy for constructing nanocomposites for highly efficient CDT.
基金supported by the National Natural Science Foundation of China(21801090,21831003 and 21621001)the Jilin Scientific and Technological Development Program(20200802003GH)+2 种基金the Scientific Research Project in the Education Department of Jilin Province(JJKH20211044KJ)the Project on Experimental Technique of Jilin University(409020720202)supported by Users with the Excellence Program of Hefei Science Center CAS(2020HSC-UE002)。
文摘The electrocatalytic activity of transition-metal-based compounds is closely related to the electronic configuration.However,optimizing the surface electron spin state of catalysts remains a challenge.Here,we developed a spin-state and delocalized electron regulation method to optimize oxygen evolution reaction(OER)performance by in-situ growth of NiCo_(2)(OH)_(x) using Oswald ripening and coordinating etching process on MXene and plasma treatment.X-ray absorption spectroscopy,magnetic tests and electron paramagnetic resonance reveal that the coupling of NiCo_(2)(OH)_(x) and MXene can induce remarkable spin-state transition of Co^(3+)and transition metal ions electron delocalization,plasma treatment further optimizes the 3 d orbital structure and delocalized electron density.The unique Jahn-Teller phenomenon can be brought by the intermediate spin state(t2 _(g)^(5) e_(g)^(1))of Co^(3+),which benefits from the partial electron occupied egorbitals.This distinct electron configuration(t2_(g)^(5) e_(g)^(1))with unpaired electrons leads to orbital degeneracy,that the adsorption free energy of intermediate species and conductivity were further optimized.The optimized electrocatalyst exhibits excellent OER activity with an overpotential of 268 m V at 10 m A cm^(-2).DFT calculations show that plasma treatment can effectively regulate the d-band center of TMs to optimize the adsorption and improve the OER activity.This approach could guide the rational design and discovery of electrocatalysts with ideal electron configurations in the future.
基金financially supported by the Science and Technology Development Program of Jilin Province(YDZJ202101ZYTS185)the National Natural Science Foundation of China(21975250)。
文摘Antimony-based anodes have attracted wide attention in potassium-ion batteries due to their high theoretical specific capacities(∼660 mA h g^(-1))and suitable voltage platforms.However,severe capacity fading caused by huge volume change and limited ion transportation hinders their practical applications.Recently,strategies for controlling the morphologies of Sb-based materials to improve the electrochemical performances have been proposed.Among these,the two-dimensional Sb(2D-Sb)materials present excellent properties due to shorted ion immigration paths and enhanced ion diffusion.Nevertheless,the synthetic methods are usually tedious,and even the mechanism of these strategies remains elusive,especially how to obtain large-scale 2D-Sb materials.Herein,a novel strategy to synthesize 2D-Sb material using a straightforward solvothermal method without the requirement of a complex nanostructure design is provided.This method leverages the selective adsorption of aldehyde groups in furfural to induce crystal growth,while concurrently reducing and coating a nitrogen-doped carbon layer.Compared to the reported methods,it is simpler,more efficient,and conducive to the production of composite nanosheets with uniform thickness(3–4 nm).The 2D-Sb@NC nanosheet anode delivers an extremely high capacity of 504.5 mA h g^(-1) at current densities of 100 mA g^(-1) and remains stable for more than 200 cycles.Through characterizations and molecular dynamic simulations,how potassium storage kinetics between 2D Sb-based materials and bulk Sb-based materials are explored,and detailed explanations are provided.These findings offer novel insights into the development of durable 2D alloy-based anodes for next-generation potassium-ion batteries.
基金support from the National Key R&D Program of China(Grant No.2023YFE0202000)National Natural Science Foundation of China(Grant No.52102213)Science Technology Program of Jilin Province(Grant No.20230101128JC).
文摘KFeSO_(4)F(KFSF)is considered a potential cathode due to the large capacity and low cost.However,the inferior electronic conductivity leads to poor electrochemical performance.Defect engineering can facilitate the electron/ion transfer by tuning electronic structure,thus providing favorable electrochemical performance.Herein,through the regulation of surface defect engineering in reduced graphene oxide(rGO),the Fe–C bonds were formed between KFSF and rGO.The Fe–C bonds formed work in regulating the Fe-3d orbital as well as promoting the migration ability of K ions and increasing the electronic conductivity of KFSF.Thus,the KFSF@rGO delivers a high capacity of 119.6 mAh g^(-1).When matched with a graphite@pitch-derived S-doped carbon anode,the full cell delivers an energy density of 250.5 Wh kg^(-1) and a capacity retention of 81.5%after 400 cycles.This work offers a simple and valid method to develop high-performance cathodes by tuning defect sites.
基金the Young Thousand Talented Program and the National Natural Science Foundation of China (21671073 and 21621001)the “111” Project of the Ministry of Education of China (B17020)Program for JLU Science and Technology Innovative Research Team
文摘Manganese oxides are regarded as one of the most promising cathode materials in rechargeable aqueous Zn-ion batteries(ZIBs)because of the low price and high security.However,the practical application of Mn2O3 in ZIBs is still plagued by the low specific capacity and poor rate capability.Herein,highly crystalline Mn2O3 materials with interconnected mesostructures and controllable pore sizes are obtained via a ligand-assisted self-assembly process and used as high-performance electrode materials for reversible aqueous ZIBs.The coordination degree between Mn2+and citric acid ligand plays a crucial role in the formation of the mesostructure,and the pore sizes can be easily tuned from 3.2 to 7.3 nm.Ascribed to the unique feature of nanoporous architectures,excellent zinc-storage performance can be achieved in ZIBs during charge/discharge processes.The Mn2O3 electrode exhibits high reversible capacity(233 mAh g−1 at 0.3 A g−1),superior rate capability(162 mAh g−1 retains at 3.08 A g−1)and remarkable cycling durability over 3000 cycles at a high current rate of 3.08 A g−1.Moreover,the corresponding electrode reaction mechanism is studied in depth according to a series of analytical methods.These results suggest that rational design of the nanoporous architecture for electrode materials can effectively improve the battery performance.
基金supported by the National Natural Science Foundation of China(91833303,51872044,51372036,51202025 and 51602047)the Key Project of Chinese Ministry of Education(113020A)+3 种基金the 111 project(B13013)the Jilin Province Science and Technology Development Project(20180101175JC and 20140520096JH)the Fundamental Research Funds for the Central Universities(2412019FZ043)the Open Project of Key Laboratory for UV Emitting Materials and Technology of Ministry of Education(130028857).
文摘Kesterite Cu2ZnSn(S,Se)4(CZTSSe)solar cells have drawn worldwide attention for their promising photovoltaics performance and earth-abundant element composition,yet the record efficiency of this type of device is still far lower than its theoretical conversion efficiency.Undesirable band alignment and severe non-radiative recombination at CZTSSe/CdS heterojunction interfaces are the major causes limiting the current/voltage output and overall device performance.Herein,we propose a novel two-step CdS deposition strategy to improve the quality of CZTSSe/CdS heterojunction interface and thereby improve the performance of CZTSSe solar cell.The two-step strategy includes firstly pre-deposits CdS thin layer on CZTSSe absorber layer by chemical bath deposition(CBD),followed with a mild heat treatment to facilitate element inter-diffusion,and secondly deposits an appropriate thickness of CdS layer by CBD to cover the whole surface of pre-deposited CdS and CZTSSe layers.The solar energy conversion efficiency of CZTSSe solar cells with two-step deposited CdS layer approaches to 8.76%(with an active area of about 0.19 cm2),which shows an encouraging improvement of over 87.98%or 30.16%compared to the devices with traditional CBD-deposited CdS layer without and with the mild annealing process,respectively.The performance enhancement by the two-step CdS deposition is attributed to the formation of more favorable band alignment at CZTSSe/CdS interface as well as the effective decrease in interfacial recombination paths on the basis of material and device characterizations.The two-step CdS deposition strategy is simple but effective,and should have large room to improve the quality of CZTSSe/CdS heterojunction interface and further lift up the conversion efficiency of CZTSSe solar cells.
基金funded by the Key R&D Program of Jilin Province(20220201132GX)the Key R&D Program of Hubei Province(2022BAA084)the Open Funds of the State Key Laboratory of Rare Earth Resource Utilization(RERU2023008)。
文摘Ultra-high nickel cobalt-free lithium layered oxides are promising cathode material for lithium-ion batteries(LIBs)because of their relatively high capacity and low cost.Nevertheless,the high nickel content would induce bulk structure degradation and interfacial environment deterioration,and the absence of Co element reduces the lithium diffusion kinetics,severely limiting the performance liberation of this kind of cathodes.Herein,a multifunctional Ti/Zr dual cation co-doping strategy has been employed to improve the lithium storage performance of LiNi_(0.9)Mn_(0.1)O_(2)(NM91)cathode.On the one hand,the Ti/Zr co-doping weakens the Li^(+)/Ni^(2+)mixing through magnetic interactions due to the inexistence of unpaired electrons for Ti^(4+)and Zr^(4+),increasing the lithium diffusion rate and suppressing the harmful coexistence of H1 and H2 phases.On the other hand,they enhance the lattice oxygen stability because of the strong Ti-O and Zr-O bonds,inhibiting the undesired H3 phase transition and lattice oxygen loss,improving the bulk structure and cathode-electrolyte interface stability.As a result,the Ti/Zr co-doped NM91(NMTZ)exhibits a 91.2%capacity retention rate after 100 cycles,while that of NM91 is only82.9%.Also,the NMTZ displays better rate performance than NM91 with output capacities of 115 and93 mA h g^(-1)at a high current density of 5 C,respectively.Moreover,the designed NMTZ could enable the full battery to deliver an energy density up to 263 W h kg^(-1),making the ultra-high nickel cobaltfree lithium layered oxide cathode closer to practical applications.
基金supported by the National Natural Science Foundation of China (21273221)the National High Technology Research and Development Program of China (863 Program, 2011AA03A406)
文摘Galvanic deposition method was used to prepare the Pd/Ni-Al2O3-GD catalyst for the combustion of methane under lean conditions. The new catalyst and compared catalysts （Pd/Al2O3-IW, Pd-Ni/Al2O3-IW, Pd/Ni-Al2O3-IW） prepared by incipient wetness impregnation were characterized by N2-physisorption, XRD and TEM to clarify particle size and size distribution of palladium species. Combined O2-TPD and XPS results with the catalytic data, it shows that the surface palladium species with low valence exhibits better combustion performance due to their stronger interaction with support. The results indicate that the galvanic deposition method is an effective route to prepare efficient catalyst for methane combustion, and it also provides useful information for improving the present commercial catalyst.
基金This work was supported by the National Key Research and Development Program of China(2018YFB1502003)the National Natural Science Foundation of China(52225606,21875183,52172248)+2 种基金the“Fundamental Research Funds for the Central Universities”the Natural Science Basic Research Program of Shaanxi Province(2019JCW-10)“The Youth Innovation Team of Shaanxi Universities”.
文摘Despite of suitable band structures for harvesting solar light and driving water redox reactions,polymeric carbon nitride(PCN)has suffered from poor charge transfer ability and sluggish surface reaction kinetics,which limit its photocatalytic activity for water splitting.Herein,atomically dispersed Zn-coordinated three-dimensional(3D)sponge-like PCN(Zn-PCN)is synthesized through a novel intermediate coordination strategy.Advanced characterizations and theoretical calculations well evidence that Zn single atoms are coordinated and stabilized on PCN in the form of Zn-N_(6) configura-tion featured with an electron-deficient state.Such an electronic configuration has been demonstrated contributive to promoted electron excitation,accelerated charge separation and transfer as well as reduced water redox barriers.Further benefited from the abundant surface active sites derived from the 3D porous structure,Zn-PCN realizes visible-light photocatalysis for overall water splitting with H_(2) and O_(2) simultaneously evolved at a stoichiometric ratio of 2:1.This work brings new insights into the design of novel single-atom photocatalysts by deepening the understanding of electronic configurations and reactive sites favorable to excellent photocatalysis for water splitting and related solar energy conversion reactions.
基金supported by 100 Talents Programme of the Chinese Academy of SciencesNational Program on Key Basic Research Project of China(973 Program,Grant No.2012CB215500)+1 种基金Foundation for Innovative Research Groups of the National Natural Science Foundation of China(Grant No.20921002 and No.21101147)the Science and Technology Development Program of Jilin Province(Grant No.20100102 and 20116008)
文摘Supercapacitors（SCs） have attracted much attention as one of the alternative energy devices due to their high power performance,long cycle life,and low maintenance cost.Graphene is considered as an innovative and promising material due to its large theoretical specific surface area,high electrical conductivity,good mechanical properties and chemical stability.Herein,we report an effective strategy for elaborately constructing rationally functionalized self-standing graphene（SG） obtained from giant graphene oxide（GGO） paper followed by an ultrarapid thermal-processing.This treatment results in both the exfoliation of graphene sheets and the reduction of GGO by elimination of oxygencontaining groups.The as-prepared SG electrode materials without additive and conducting agent provide an excellent combination of the electrical double layer capacitor（EDLC） and pseudocapacitor（PC） functions and exhibit superior electrochemical performance,including high specific capacitance,good rate capability and excellent cycling stability when investigated in three-electrode electrochemical cells.
基金supported by the Jilin Provincial Scientific and Technological Development Program(YDZJ202401572ZYTS)the Overseas Expertise Introduction Project for Discipline Innovation of China(D18012)+1 种基金Education Department of Jilin Province(JJKH20240678KJ)the National Natural Science Foundation of China(22122904,22109155,22379136)。
文摘The solid electrolyte interphase(SEI)layer,formed on the electrode through electrolyte decomposition,has garnered significant attention over the past several decades.Numerous characterization studies have shown that the SEI enhances the stability of both the electrolyte and electrode,particularly by mitigating the well-known cation-solvent co-intercalation in graphite electrodes in lithium-ion batteries.However,recent electrolyte exchange experiments have revealed that variations in electrolyte solvation structure and the resulting desolvation behaviors play a more dominant role than the SEI in influencing electrolyte and electrode stability,which in turn critically impacts battery performance.In addition to contributing to the ongoing debate,electrolyte exchange experiments have proven to be a valuable tool for analyzing failures in electrolytes,electrodes,and batteries.This review highlights the application of electrolyte exchange experiments across various metal-ion batteries,incorporating diverse combinations of electrolytes and electrodes.It examines the influence of electrolyte solvation structures and desolvation behaviors on the stability of both electrolytes and electrodes.The aim is to enhance the methodology of electrolyte exchange experiments to deepen the understanding of the molecular interactions among metal ions,anions,and solvents within the electrolyte.This approach complements existing insights into SEI effects,providing a more thorough and accurate framework for battery failure analysis.
