Despite the significant progress in the fabrication of advanced electrode materials,complex control strategies and tedious processing are often involved for most targeted materials to tailor their compositions,morphol...Despite the significant progress in the fabrication of advanced electrode materials,complex control strategies and tedious processing are often involved for most targeted materials to tailor their compositions,morphologies,and chemistries.Inspired by the unique geometric structures of natural biomacromolecules together with their high affinities for metal species,we propose the use of skin collagen fibers for the template crafting of a novel multicore-shell Fe2N-carbon framework anode configuration,composed of hierarchical N-doped carbon nanofiber bundles firmly embedded with Fe2N nanoparticles(Fe2N@N-CFBs).In the resultant heterostructure,the Fe2N nanoparticles firmly confined inside the carbon shells are spatially isolated but electronically well connected by the long-range carbon nanofiber framework.This not only provides direct and continuous conductive pathways to facilitate electron/ion transport,but also helps cushion the volume expansion of the encapsulated Fe2N to preserve the electrode microstructure.Considering its unique structural characteristics,Fe2N@N-CFBs as an advanced anode material exhibits remarkable electrochemical performances for lithium-and potassium-ion batteries.Moreover,this bio-derived structural strategy can pave the way for novel low-cost and high-efficiency syntheses of metal-nitride/carbon nanofiber heterostructures for potential applications in energy-related fields and beyond.展开更多
The ever-growing demands for green and sustainable power sources for ap-plications in grid-scale energy storage and portable/wearable devices have enabled the continual development of advanced aqueous electrochemical ...The ever-growing demands for green and sustainable power sources for ap-plications in grid-scale energy storage and portable/wearable devices have enabled the continual development of advanced aqueous electrochemical energy storage(EES)systems.Aqueous batteries and supercapacitors made of iron-based anodes are one of the most promising options due to the remark-able electrochemical features and natural abundance,pretty low cost and good environmental friendliness of ferruginous species.Though impressive ad-vances in developing the state-of-the-art ferruginous anodes and designing various full-cell aqueous devices have been made,there still remain key issues and challenges on the way to practical applications,which urgently need discussing to put forwards possible solutions.In this review,rather than focusing on the detailed methods to optimize the iron anode,electrolyte,and device performance,we first give a comprehensive review on the charge storage mechanisms for ferruginous anodes in different electrolyte systems,as well as the newly developed iron-based aqueous EES devices.The deep in-sights,involving the inherent failure mechanisms and corresponding modification/optimization strategies toward iron anodes for the development of high-performance aqueous EES devices,will then be discussed.The advances in applying iron-based aqueous EES devices for emerging fields such as flexible/wearable electronics and functionalized building materials will be further outlined.Last,future research trends and perspectives for maximizing the potential of current iron anodes and devices as well as exploiting brand-new iron-based aqueous EES systems are put forward.展开更多
Sodium-ion batteries are promising candidates for large-scale grid storage systems and other applications.Their foremost advantage derives from superior environmental credentials,enhanced safety as well as lower raw m...Sodium-ion batteries are promising candidates for large-scale grid storage systems and other applications.Their foremost advantage derives from superior environmental credentials,enhanced safety as well as lower raw material costs than lithium-ion batteries.It is still challenging to explore desirable anode material.In this study,FeSe_(2)@CoSe_(2)/FeSe_(2),with a yolk-shell structure was prepared by ion exchange and selenisation.The FeSe_(2)@CoSe_(2)/FeSe_(2)prepared as anode material for sodiumion batteries exhibits excellent rate capability due to the synergistic effect of bimetallic selenides and the interfacial effect of the heterostructure.Moreover,it delivers high performance(510 mAh g^(-1)at 0.2 A g^(-1)),superior rate capa-bility(90%retention at 5 A g^(-1)),and good long-time cycling stability(78%capacity retention after 1800 cycles at a high current density of 2 A g^(-1)).The optimized sodiumion full cell with FeSe_(2)@CoSe_(2)/FeSe_(2)as the anode and Na 3 V 2(PO 4)3 as the cathode still demonstrates excellent performance.Namely,a ca-pacity of 272 mAh g^(-1)(at 1 A g^(-1))within the operating voltage from 1 to 3.8 V can be obtained.This work illustrates the potential of bimetallic selenides with heterostructures for performance enhancement of sodium-ion batteries.展开更多
Highly efficient and stable iron electrodes are of great significant to the development of iron-air battery(IAB).In this paper,iron nanoparticle-encapsulated C–N composite(NanoFe@CN)was synthesized by pyrolysis using...Highly efficient and stable iron electrodes are of great significant to the development of iron-air battery(IAB).In this paper,iron nanoparticle-encapsulated C–N composite(NanoFe@CN)was synthesized by pyrolysis using polyaniline as the C–N source.Electrochemical performance of the NanoFe@CN in different electrolytes(alkaline,neutral,and quasi-neutral)was investigated via cyclic voltammetry(CV).The IAB was assembled with NanoFe@CN as the anode and IrO_(2)+Pt/C as the cathode.The effects of different discharging/charging current densities and electrolytes on the battery performance were also studied.Neutral K_(2)SO_(4)electrolyte can effectively suppress the passivation of iron electrode,and the battery showed a good cycling stability during 180 charging/discharging cycles.Compared to the pure nano-iron(NanoFe)battery,the NanoFe@CN battery has a more stable cycling stability either in KOH or NH_(4)Cl+KCl electrolyte.展开更多
A strong interface coupling is of vital importance to develop metal oxide/carbon nanocomposite anodes for next-generation lithium ion batteries.Herein,a rational N-doped carb on riveting strategy is designed to boost ...A strong interface coupling is of vital importance to develop metal oxide/carbon nanocomposite anodes for next-generation lithium ion batteries.Herein,a rational N-doped carb on riveting strategy is designed to boost the lithium storage performance of Fe3O4/N-doped carbon tubular structures.Poly pyrrole(PPy)has been used as the precursor for N-doped carbon.N-doped carbon-riveted Fe3O4/N-doped carbon(N-C@Fe3O4@N-C)nanocomposites were obtained by pyrolysis of PPy-coated FeOOH@PPy nanotubes in Ar atmosphere.When tested as an anode for LIBs,the N-C@Fe3O4@N-C displays a high reversible discharge capacity of 675.8 mA h g-1 after 100 cycles at a current density of 100 mA g-1 and very good rate capability(470 mA h g_1 at 2 A g-1),which significantly surpasses the performance of Fe3O4@N-C.TEM analysis reveals that after battery cycling the FeOx particles detached from the carbon fibers for Fe3O4@N-C,while for N-C@Fe3O4@N-C the FeOx particles were still trapped in the carbon matrix,thus preserving good electrical contact.Consequently,the superior performance of N-C@Fe3C)4@N-C is attributed to the synergistic effect between Fe3O4 and N-doped carbon combined with the unique structure properties of the nanocomposites.The strategy reported in this work is expected to be applicable for designing other electrode materials for LIBs.展开更多
In this study,glucose and NH4F were utilized as sources of carbon and fluorine,respectively,for the synthesis of LiMn_(0.6)Fe_(0.4)PO_(4)(LMFP)nanoscales.These nanoscales were subsequently modified with varying levels...In this study,glucose and NH4F were utilized as sources of carbon and fluorine,respectively,for the synthesis of LiMn_(0.6)Fe_(0.4)PO_(4)(LMFP)nanoscales.These nanoscales were subsequently modified with varying levels of fluorine-doped carbon through co-precipitation and mechanical ball milling processes.The LMFP,incorporating carbon and varying levels of fluoride ions,exhibit higher specific discharge capacities at 0.2 Cand electrochemical characteristics compared to the original LMFP coated solely with carbon.The inclusion of fluorine-doped carbon in the composite material creates numerous pathways for expeditious electron transfer.Moreover,the partial formation of metal fluoride at the interface between the surface of LMFP and the layer of carbon coating doped with fluorine enhances the reduction in the charge-transfer resistance.The modified ferromanganese phosphate cathode material reveals an outstanding discharge capacity displaying a reversible discharge specific capacity value of 131.73 mA h g^(−1)at 10C and 154.6 mA h g^(−1)at 0.2C,due to its unique structure.展开更多
Design of electrode materials for stable and efficient electrocatalytic oxidation of As(Ⅲ)in arsenic-contaminated groundwater poses a great challenge due to the rapid deactivation of catalysts resulting from the high...Design of electrode materials for stable and efficient electrocatalytic oxidation of As(Ⅲ)in arsenic-contaminated groundwater poses a great challenge due to the rapid deactivation of catalysts resulting from the high oxygen evolution potential(OEP)and considerable barrier to generating reactive oxygen species(ROS).Herein,an innovative TNAs/SnO_(2)/PEDOT/Fe(Ⅲ)-RuO_(2) multilayer electrode was synthesized by utilizing a PEDOT-coated SnO_(2) interlayer as a supportive framework to combine Fe-doped amorphous RuO_(2) catalytic layer with TiO_(2) nanotube array substrate.Such electrode exhibited high activity and sta-bility for the oxidation of As(Ⅲ)to As(V)due to the large surface area provided by the TiO_(2) nanotube arrays and the SnO_(2)/PEDOT interlayer for facilitating the growth of the catalytic layer.The electrochem-ically active surface area of the electrode reached as high as 31.7 mF/cm^(2).Impressively,the doping of Fe into RuO_(2) layer led to a remarkable increase in the OEP value to 3.12 V,which boosted the indirect oxidation process mediated by ROS at a lower potential to achieve the As(Ⅲ)oxidation ratio of 98.5%.DFT calculations revealed that the Fe-doped amorphous RuO_(2) weakened the adsorption strength of·OH and.SO4-intermediates and lowered the energy barrier for generating ROS.Combined with ESR results,the formation of·OH and·SC4-with strong oxidizing properties was fully verified,providing further evi-dence for the involvement of ROS as the main mediator of the oxidation mechanism of As(Ⅲ).This work may provide valuable perspectives into the design of catalytic layer structures and heteroatom doping modifications for composite-coated electrodes.展开更多
Germanium-based oxide has been found to be a promising high-capacity anode material for lithium-ion batteries （LIBs）. However, it exhibits poor electrochemical performance because of the drastic volume change during...Germanium-based oxide has been found to be a promising high-capacity anode material for lithium-ion batteries （LIBs）. However, it exhibits poor electrochemical performance because of the drastic volume change during cycling. Herein, we designed porous Ge-Fe bimetal oxide nanowires （Ge-Fe-Ox-700 NWs） by a large-scale and facile solvothermal reaction. When used as the anode material for LIBs, these Ge-Fe-Ox-700 NWs exhibited superior electrochemical performance （- 1,120 mAh·g^-1 at a current density of 100 mA·g^-1） and good cycling performance （- 750 mAh·g^-1 after 50 cycles at a current density of 100 mA·g^-1）. The improved performance is due to the small NW diameter, which allows for better accommodation of the drastic volume changes and zero-dimensional nanoparticles, which shorten the diffusion length of ions and electrons.展开更多
基金financial support from the National Natural Science Foundation of China(21878192,51502180)the Fundamental Research Funds for the Central Universities(2016SCU04A18)+1 种基金the 1000 Talents Program of Sichuan Province,the Sichuan Province Science and Technology Support Program(2014GZ0093)the Australian Research Council(DP160102627).
文摘Despite the significant progress in the fabrication of advanced electrode materials,complex control strategies and tedious processing are often involved for most targeted materials to tailor their compositions,morphologies,and chemistries.Inspired by the unique geometric structures of natural biomacromolecules together with their high affinities for metal species,we propose the use of skin collagen fibers for the template crafting of a novel multicore-shell Fe2N-carbon framework anode configuration,composed of hierarchical N-doped carbon nanofiber bundles firmly embedded with Fe2N nanoparticles(Fe2N@N-CFBs).In the resultant heterostructure,the Fe2N nanoparticles firmly confined inside the carbon shells are spatially isolated but electronically well connected by the long-range carbon nanofiber framework.This not only provides direct and continuous conductive pathways to facilitate electron/ion transport,but also helps cushion the volume expansion of the encapsulated Fe2N to preserve the electrode microstructure.Considering its unique structural characteristics,Fe2N@N-CFBs as an advanced anode material exhibits remarkable electrochemical performances for lithium-and potassium-ion batteries.Moreover,this bio-derived structural strategy can pave the way for novel low-cost and high-efficiency syntheses of metal-nitride/carbon nanofiber heterostructures for potential applications in energy-related fields and beyond.
基金This study was supported by grants from the National Natural Science Foundation of China(Grant Nos.51802269,51972257,and 52172229)the National Key R&D Program of China(Grant No.2016YFA0202602)the Fundamental Research Funds for the Central Universities(WUT:2021IVA115).
文摘The ever-growing demands for green and sustainable power sources for ap-plications in grid-scale energy storage and portable/wearable devices have enabled the continual development of advanced aqueous electrochemical energy storage(EES)systems.Aqueous batteries and supercapacitors made of iron-based anodes are one of the most promising options due to the remark-able electrochemical features and natural abundance,pretty low cost and good environmental friendliness of ferruginous species.Though impressive ad-vances in developing the state-of-the-art ferruginous anodes and designing various full-cell aqueous devices have been made,there still remain key issues and challenges on the way to practical applications,which urgently need discussing to put forwards possible solutions.In this review,rather than focusing on the detailed methods to optimize the iron anode,electrolyte,and device performance,we first give a comprehensive review on the charge storage mechanisms for ferruginous anodes in different electrolyte systems,as well as the newly developed iron-based aqueous EES devices.The deep in-sights,involving the inherent failure mechanisms and corresponding modification/optimization strategies toward iron anodes for the development of high-performance aqueous EES devices,will then be discussed.The advances in applying iron-based aqueous EES devices for emerging fields such as flexible/wearable electronics and functionalized building materials will be further outlined.Last,future research trends and perspectives for maximizing the potential of current iron anodes and devices as well as exploiting brand-new iron-based aqueous EES systems are put forward.
基金supported by the National Natural Science Foundation of China(Nos.21801200 and 22075217)the Open Project of Hunan Key Laboratory of Applied Environmental Photocatalysis(No.2114504)the Natural Science Foundation of Hubei Province of China(No.2022CFA001).
文摘Sodium-ion batteries are promising candidates for large-scale grid storage systems and other applications.Their foremost advantage derives from superior environmental credentials,enhanced safety as well as lower raw material costs than lithium-ion batteries.It is still challenging to explore desirable anode material.In this study,FeSe_(2)@CoSe_(2)/FeSe_(2),with a yolk-shell structure was prepared by ion exchange and selenisation.The FeSe_(2)@CoSe_(2)/FeSe_(2)prepared as anode material for sodiumion batteries exhibits excellent rate capability due to the synergistic effect of bimetallic selenides and the interfacial effect of the heterostructure.Moreover,it delivers high performance(510 mAh g^(-1)at 0.2 A g^(-1)),superior rate capa-bility(90%retention at 5 A g^(-1)),and good long-time cycling stability(78%capacity retention after 1800 cycles at a high current density of 2 A g^(-1)).The optimized sodiumion full cell with FeSe_(2)@CoSe_(2)/FeSe_(2)as the anode and Na 3 V 2(PO 4)3 as the cathode still demonstrates excellent performance.Namely,a ca-pacity of 272 mAh g^(-1)(at 1 A g^(-1))within the operating voltage from 1 to 3.8 V can be obtained.This work illustrates the potential of bimetallic selenides with heterostructures for performance enhancement of sodium-ion batteries.
基金supported by the National Natural Science Foundation of China(Grant Nos.22379042 and 21875062)the Research and Development Planning Projects in Key Areas of Hunan Province(Grant No.2019GK2034).
文摘Highly efficient and stable iron electrodes are of great significant to the development of iron-air battery(IAB).In this paper,iron nanoparticle-encapsulated C–N composite(NanoFe@CN)was synthesized by pyrolysis using polyaniline as the C–N source.Electrochemical performance of the NanoFe@CN in different electrolytes(alkaline,neutral,and quasi-neutral)was investigated via cyclic voltammetry(CV).The IAB was assembled with NanoFe@CN as the anode and IrO_(2)+Pt/C as the cathode.The effects of different discharging/charging current densities and electrolytes on the battery performance were also studied.Neutral K_(2)SO_(4)electrolyte can effectively suppress the passivation of iron electrode,and the battery showed a good cycling stability during 180 charging/discharging cycles.Compared to the pure nano-iron(NanoFe)battery,the NanoFe@CN battery has a more stable cycling stability either in KOH or NH_(4)Cl+KCl electrolyte.
基金financially supported by the National Natural Science Foundation of China (Nos. 21601098 and 51602167)Shandong Provincial Science Foundation (ZR2016EMB07 and ZR2017JL021)+1 种基金Key Research and Development Program (2018GGX102033)Qingdao Applied Fundamental Research Project (16-5-1-92-jch and 17-1-1-81-jch)
文摘A strong interface coupling is of vital importance to develop metal oxide/carbon nanocomposite anodes for next-generation lithium ion batteries.Herein,a rational N-doped carb on riveting strategy is designed to boost the lithium storage performance of Fe3O4/N-doped carbon tubular structures.Poly pyrrole(PPy)has been used as the precursor for N-doped carbon.N-doped carbon-riveted Fe3O4/N-doped carbon(N-C@Fe3O4@N-C)nanocomposites were obtained by pyrolysis of PPy-coated FeOOH@PPy nanotubes in Ar atmosphere.When tested as an anode for LIBs,the N-C@Fe3O4@N-C displays a high reversible discharge capacity of 675.8 mA h g-1 after 100 cycles at a current density of 100 mA g-1 and very good rate capability(470 mA h g_1 at 2 A g-1),which significantly surpasses the performance of Fe3O4@N-C.TEM analysis reveals that after battery cycling the FeOx particles detached from the carbon fibers for Fe3O4@N-C,while for N-C@Fe3O4@N-C the FeOx particles were still trapped in the carbon matrix,thus preserving good electrical contact.Consequently,the superior performance of N-C@Fe3C)4@N-C is attributed to the synergistic effect between Fe3O4 and N-doped carbon combined with the unique structure properties of the nanocomposites.The strategy reported in this work is expected to be applicable for designing other electrode materials for LIBs.
基金Major Science and Technology Projects of Yunnan Province(grant No.202202AG050003).
文摘In this study,glucose and NH4F were utilized as sources of carbon and fluorine,respectively,for the synthesis of LiMn_(0.6)Fe_(0.4)PO_(4)(LMFP)nanoscales.These nanoscales were subsequently modified with varying levels of fluorine-doped carbon through co-precipitation and mechanical ball milling processes.The LMFP,incorporating carbon and varying levels of fluoride ions,exhibit higher specific discharge capacities at 0.2 Cand electrochemical characteristics compared to the original LMFP coated solely with carbon.The inclusion of fluorine-doped carbon in the composite material creates numerous pathways for expeditious electron transfer.Moreover,the partial formation of metal fluoride at the interface between the surface of LMFP and the layer of carbon coating doped with fluorine enhances the reduction in the charge-transfer resistance.The modified ferromanganese phosphate cathode material reveals an outstanding discharge capacity displaying a reversible discharge specific capacity value of 131.73 mA h g^(−1)at 10C and 154.6 mA h g^(−1)at 0.2C,due to its unique structure.
基金National Natural Science Foundation of China(No.21978182)。
文摘Design of electrode materials for stable and efficient electrocatalytic oxidation of As(Ⅲ)in arsenic-contaminated groundwater poses a great challenge due to the rapid deactivation of catalysts resulting from the high oxygen evolution potential(OEP)and considerable barrier to generating reactive oxygen species(ROS).Herein,an innovative TNAs/SnO_(2)/PEDOT/Fe(Ⅲ)-RuO_(2) multilayer electrode was synthesized by utilizing a PEDOT-coated SnO_(2) interlayer as a supportive framework to combine Fe-doped amorphous RuO_(2) catalytic layer with TiO_(2) nanotube array substrate.Such electrode exhibited high activity and sta-bility for the oxidation of As(Ⅲ)to As(V)due to the large surface area provided by the TiO_(2) nanotube arrays and the SnO_(2)/PEDOT interlayer for facilitating the growth of the catalytic layer.The electrochem-ically active surface area of the electrode reached as high as 31.7 mF/cm^(2).Impressively,the doping of Fe into RuO_(2) layer led to a remarkable increase in the OEP value to 3.12 V,which boosted the indirect oxidation process mediated by ROS at a lower potential to achieve the As(Ⅲ)oxidation ratio of 98.5%.DFT calculations revealed that the Fe-doped amorphous RuO_(2) weakened the adsorption strength of·OH and.SO4-intermediates and lowered the energy barrier for generating ROS.Combined with ESR results,the formation of·OH and·SC4-with strong oxidizing properties was fully verified,providing further evi-dence for the involvement of ROS as the main mediator of the oxidation mechanism of As(Ⅲ).This work may provide valuable perspectives into the design of catalytic layer structures and heteroatom doping modifications for composite-coated electrodes.
基金This work was finandally supported by the National Natural Science Foundation of China （Nos. 21171015, 21373195, 51522212 and 51421002）, the ＂Recruitment Program of Global Experts＂, the program for New Century Excellent Talents in University （No. NCET- 12-0515）, the Fundamental Research Funds for the Central Universities （No. WK340000004）, and the Collaborative Innovation Center of Suzhou Nano Science and Technology.
文摘Germanium-based oxide has been found to be a promising high-capacity anode material for lithium-ion batteries （LIBs）. However, it exhibits poor electrochemical performance because of the drastic volume change during cycling. Herein, we designed porous Ge-Fe bimetal oxide nanowires （Ge-Fe-Ox-700 NWs） by a large-scale and facile solvothermal reaction. When used as the anode material for LIBs, these Ge-Fe-Ox-700 NWs exhibited superior electrochemical performance （- 1,120 mAh·g^-1 at a current density of 100 mA·g^-1） and good cycling performance （- 750 mAh·g^-1 after 50 cycles at a current density of 100 mA·g^-1）. The improved performance is due to the small NW diameter, which allows for better accommodation of the drastic volume changes and zero-dimensional nanoparticles, which shorten the diffusion length of ions and electrons.
