Layered LiCoO_(2)(LCO)acts as a dominant cathode material for lithium-ion batteries(LIBs)in 3C products because of its high compacted density and volumetric energy density.Although improving the high cutoff voltage is...Layered LiCoO_(2)(LCO)acts as a dominant cathode material for lithium-ion batteries(LIBs)in 3C products because of its high compacted density and volumetric energy density.Although improving the high cutoff voltage is an effective strategy to increase its capacity,such behavior would trigger rapid capacity decay due to the surface or/and structure degradation.Herein,we propose a bi-functional surface strategy involving constructing a robust spinel-like phase coating layer with great integrity and compatibility to LiCoO_(2) and modulating crystal lattice by anion and cation gradient co-doping at the subsurface.As a result,the modified LiCoO_(2)(AFM-LCO)shows a capacity retention of 80.9%after 500 cycles between 3.0and 4.6 V.The Al,F,Mg enriched spinel-like phase coating layer serves as a robust physical barrier to effectively inhibit the undesired side reactions between the electrolyte and the cathode.Meanwhile,the Al,F,Mg gradient co-doping significantly enhances the surficial structure stability,suppresses Co dissolution and oxygen release,providing a stable path for Li-ions mobility all through the long-term cycles.Thus,the surface bi-functional strategy is an effective method to synergistically improve the electrochemical performances of LCO at a high cut-off voltage of 4.6 V.展开更多
Ni-Fe bimetallic electrodes are currently recognized as a kind of benchmark transition metal-based oxygen evolution reaction(OER)electrocatalysts.Facile synthesis of Ni-Fe bimetallic electrode materials with excellent...Ni-Fe bimetallic electrodes are currently recognized as a kind of benchmark transition metal-based oxygen evolution reaction(OER)electrocatalysts.Facile synthesis of Ni-Fe bimetallic electrode materials with excellent catalytic activity and satisfied stability by a simple and low-cost route is still a big challenge.Herein,well-defined Ni-Fe nanoparticles in-situ developed on a planar Fe substrate(Ni-Fe NPs/Fe)is fabricated via a facile one-step galvanic replacement reaction(GRR)carried out in an Ethaline-based deep eutectic solvent(DES).The prepared Ni-Fe NPs/Fe exhibits outstanding OER performance,which needs an overpotential of only 319 mV to drive a current density of 10 mA cm^(-2),with a small Tafel slope of 41.2 mV dec^(-1) in 1.0 mol L^(-1) KOH,high mass activity(up to 319.78 A g^(-1) at an overpotential of 300 mV)and robust durability for 200 h.Impressively,the Ni-Fe bimetallic oxygen-evolution electrode obtained from the Ethaline-based DES is catalytically more active and durable than that of its counterpart derived from the 4.2 mol L^(-1) NaCl aqueous solution.The reason for this is mainly related to the different morphology and surface state of the Ni-Fe catalysts obtained from these different solvent environments,particularly for the differences in phy-chemical properties,active species formed and deposition kinetics,offered by the Ethaline-based DES.展开更多
Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple ...Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple pyrolysis of biomass always generates inadequate porosity with limited surface area.Moreover,biomass-derived carbon also suffers from poor wettability and single physical adsorption of ions,resulting in limited desalination performance.Herein,pore structure optimization and element co-doping are integrated on banana peels(BP)-derived carbon to construct hierarchically porous and B,N co-doped carbon with large ions-accessible surface area.A unique expansionactivation(EA)strategy is proposed to modulate the porosity and specific surface area of carbon.Furthermore,B,N co-doping could increase the ions-accessible sites with improved hydrophilicity,and promote ions adsorption.Benefitting from the synergistic effect of hierarchical porosity and B,N co-doping,the resultant electrode manifest enhanced CDI performance for NaCl with large desalination capacity(29.5 mg g^(-1)),high salt adsorption rate(6.2 mg g^(-1)min^(-1)),and versatile adsorption ability for other salts.Density functional theory reveals the enhanced deionization mechanism by pore and B,N co-doping.This work proposes a facile EA strategy for pore structure modulation of biomass-derived carbon,and demonstrates great potentials of integrating pore and heteroatoms-doping on constructing high-performance CDI electrode.展开更多
Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.Howev...Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.However,developing high-performance anode materials to improve sodium storage performa nce still remains a major challenge.Here,a facile one-pot method has been developed to fabricate a hybrid of MoSeTe nanosheets implanted within the N,F co-doped honeycomb carbon skeleton(MoSeTe/N,F@C).Experimental results demonstrate that the incorporation of large-sized Te atoms into MoSeTe nanosheets enlarges the layer spacing and creates abundant anion vacancies,which effectively facilitate the insertion/extraction of Na^(+) and provide numerous ion adsorption sites for rapid surface capacitive behavior.Additionally,the heteroatoms N,F co-doped honeycomb carbon skeleton with a highly conductive network can restrain the volume expansion and boost reaction kinetics within the electrode.As anticipated,the MoSeTe/N,F@C anode exhibits high reversible capacities along with exceptional cycle stability.When coupled with Na_(3)V_(2)(PO_(4))_(3)@C(NVPF@C) to form SIB full cells,the anode delivers a reversible specific capacity of 126 mA h g^(-1) after 100 cycles at 0.1 A g^(-1).Furthermore,when combined with AC to form SIHC full cells,the anode demonstrates excellent cycling stability with a reversible specific capacity of50 mA h g^(-1) keeping over 3700 cycles at 1.0 A g^(-1).In situ XRD,ex situ TEM characterization,and theoretical calculations(DFT) further confirm the reversibility of sodium storage in MoSeTe/N,F@C anode materials during electrochemical reactions,highlighting their potential for widespread practical application.This work provides new insights into the promising utilization of advanced transition metal dichalcogenides as anode materials for Na^(+)-based energy storage devices.展开更多
基金supported by the National Natural Science Foundation of China(22075170,52072233)the Beijing National Laboratory for Condensed Matter Physics。
文摘Layered LiCoO_(2)(LCO)acts as a dominant cathode material for lithium-ion batteries(LIBs)in 3C products because of its high compacted density and volumetric energy density.Although improving the high cutoff voltage is an effective strategy to increase its capacity,such behavior would trigger rapid capacity decay due to the surface or/and structure degradation.Herein,we propose a bi-functional surface strategy involving constructing a robust spinel-like phase coating layer with great integrity and compatibility to LiCoO_(2) and modulating crystal lattice by anion and cation gradient co-doping at the subsurface.As a result,the modified LiCoO_(2)(AFM-LCO)shows a capacity retention of 80.9%after 500 cycles between 3.0and 4.6 V.The Al,F,Mg enriched spinel-like phase coating layer serves as a robust physical barrier to effectively inhibit the undesired side reactions between the electrolyte and the cathode.Meanwhile,the Al,F,Mg gradient co-doping significantly enhances the surficial structure stability,suppresses Co dissolution and oxygen release,providing a stable path for Li-ions mobility all through the long-term cycles.Thus,the surface bi-functional strategy is an effective method to synergistically improve the electrochemical performances of LCO at a high cut-off voltage of 4.6 V.
基金support of the National Natural Science Foundation of China (21962008)Yunnan Province Excellent Youth Fund Project (202001AW070005)+1 种基金Candidate Talents Training Fund of Yunnan Province (2017PY269SQ,2018HB007)Yunnan Ten Thousand Talents Plan Young&Elite Talents Project (YNWR-QNBJ-2018-346)。
文摘Ni-Fe bimetallic electrodes are currently recognized as a kind of benchmark transition metal-based oxygen evolution reaction(OER)electrocatalysts.Facile synthesis of Ni-Fe bimetallic electrode materials with excellent catalytic activity and satisfied stability by a simple and low-cost route is still a big challenge.Herein,well-defined Ni-Fe nanoparticles in-situ developed on a planar Fe substrate(Ni-Fe NPs/Fe)is fabricated via a facile one-step galvanic replacement reaction(GRR)carried out in an Ethaline-based deep eutectic solvent(DES).The prepared Ni-Fe NPs/Fe exhibits outstanding OER performance,which needs an overpotential of only 319 mV to drive a current density of 10 mA cm^(-2),with a small Tafel slope of 41.2 mV dec^(-1) in 1.0 mol L^(-1) KOH,high mass activity(up to 319.78 A g^(-1) at an overpotential of 300 mV)and robust durability for 200 h.Impressively,the Ni-Fe bimetallic oxygen-evolution electrode obtained from the Ethaline-based DES is catalytically more active and durable than that of its counterpart derived from the 4.2 mol L^(-1) NaCl aqueous solution.The reason for this is mainly related to the different morphology and surface state of the Ni-Fe catalysts obtained from these different solvent environments,particularly for the differences in phy-chemical properties,active species formed and deposition kinetics,offered by the Ethaline-based DES.
基金We gratefully acknowledge financial supports from the National Natural Science Foundation of China(No.52202371,51905125,52102364)the Natural Science Foundation of Shandong Province(No.ZR2020QE066)+2 种基金Opening Project of State Key Laboratory of Advanced Technology for Float Glass(No.2020KF08)SDUT&Zibo City Integration Development Project(No.2021SNPT0045)the fellowship of China Postdoctoral Science Foundation(No.2020M672081).
文摘Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple pyrolysis of biomass always generates inadequate porosity with limited surface area.Moreover,biomass-derived carbon also suffers from poor wettability and single physical adsorption of ions,resulting in limited desalination performance.Herein,pore structure optimization and element co-doping are integrated on banana peels(BP)-derived carbon to construct hierarchically porous and B,N co-doped carbon with large ions-accessible surface area.A unique expansionactivation(EA)strategy is proposed to modulate the porosity and specific surface area of carbon.Furthermore,B,N co-doping could increase the ions-accessible sites with improved hydrophilicity,and promote ions adsorption.Benefitting from the synergistic effect of hierarchical porosity and B,N co-doping,the resultant electrode manifest enhanced CDI performance for NaCl with large desalination capacity(29.5 mg g^(-1)),high salt adsorption rate(6.2 mg g^(-1)min^(-1)),and versatile adsorption ability for other salts.Density functional theory reveals the enhanced deionization mechanism by pore and B,N co-doping.This work proposes a facile EA strategy for pore structure modulation of biomass-derived carbon,and demonstrates great potentials of integrating pore and heteroatoms-doping on constructing high-performance CDI electrode.
基金supported by the National Natural Science Foundation of China(No.52002320,and 51972267)the China Postdoctoral Science Foundation(No.2022M712574)+3 种基金the Science Foundation of Shaanxi Province(2022GD-TSLD-18,No.2023-JCZD-03)Natural Science Foundation of Shaanxi Province(No.2022GY-372,2021GY-153)Industrial Projects Foundation of Ankang Science and Technology Bureau(No.AK2020-GY02-2)the Platform Construction Projects and Technology Service Teams of Ankang University(No.2021AYPT12 and 2022TD07)。
文摘Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.However,developing high-performance anode materials to improve sodium storage performa nce still remains a major challenge.Here,a facile one-pot method has been developed to fabricate a hybrid of MoSeTe nanosheets implanted within the N,F co-doped honeycomb carbon skeleton(MoSeTe/N,F@C).Experimental results demonstrate that the incorporation of large-sized Te atoms into MoSeTe nanosheets enlarges the layer spacing and creates abundant anion vacancies,which effectively facilitate the insertion/extraction of Na^(+) and provide numerous ion adsorption sites for rapid surface capacitive behavior.Additionally,the heteroatoms N,F co-doped honeycomb carbon skeleton with a highly conductive network can restrain the volume expansion and boost reaction kinetics within the electrode.As anticipated,the MoSeTe/N,F@C anode exhibits high reversible capacities along with exceptional cycle stability.When coupled with Na_(3)V_(2)(PO_(4))_(3)@C(NVPF@C) to form SIB full cells,the anode delivers a reversible specific capacity of 126 mA h g^(-1) after 100 cycles at 0.1 A g^(-1).Furthermore,when combined with AC to form SIHC full cells,the anode demonstrates excellent cycling stability with a reversible specific capacity of50 mA h g^(-1) keeping over 3700 cycles at 1.0 A g^(-1).In situ XRD,ex situ TEM characterization,and theoretical calculations(DFT) further confirm the reversibility of sodium storage in MoSeTe/N,F@C anode materials during electrochemical reactions,highlighting their potential for widespread practical application.This work provides new insights into the promising utilization of advanced transition metal dichalcogenides as anode materials for Na^(+)-based energy storage devices.
