Anode-free solid-state lithium metal batteries(AF-SSLBs)have the potential to deliver higher energy density and improved safety beyond lithium-metal batteries.However,the unclear mechanism for the fast capacity decay ...Anode-free solid-state lithium metal batteries(AF-SSLBs)have the potential to deliver higher energy density and improved safety beyond lithium-metal batteries.However,the unclear mechanism for the fast capacity decay in AF-SSLBs,either determined by dead Li or solid electrolyte interface(SEI),limits the proposal of effective strategies to prolong cycling life.To clarify the underlying mechanism,herein,the evolution of SEI and dead Li is quantitatively analyzed by a solid-state nuclear magnetic resonance(ss-NMR)technology in a typical LiPF6-based polymer electrolyte.The results show that the initial capacity loss is attributed to the formation of SEI,while the dead Li dominates the following capacity loss and the growth rate is 0.141 mA h cm^(−2)cycle−1.To reduce the active Li loss,the combination of inorganic-rich SEI and self-healing electrostatic shield effect is proposed to improve the reversibility of Li deposition/dissolution behavior,which reduces the capacity loss rate for the initial SEI and following dead Li generation by 2.3 and 20.1 folds,respectively.As a result,the initial Coulombic efficiency(ICE)and stable CE increase by 15.1%and 15.3%in Li-Cu cells,which guides the rational design of high-performance AF-SSLBs.展开更多
Niobium pentoxide(Nb_(2)O_(5))is deemed one of the promising anode materials for lithium-ion batteries(LIBs)for its outstanding intrinsic fast Li-(de)intercalation kinetics.The specific capacity,however,is still limit...Niobium pentoxide(Nb_(2)O_(5))is deemed one of the promising anode materials for lithium-ion batteries(LIBs)for its outstanding intrinsic fast Li-(de)intercalation kinetics.The specific capacity,however,is still limited,because the(de)intercalation of excessive Li-ions brings the undesired stress to damage Nb_(2)O_(5) crystals.To increase the capacity of Nb_(2)O_(5) and alleviate the lattice distortion caused by stress,numerous homogeneous H-and M-phases junction interfaces were proposed to produce coercive stress within theNb_(2)O_(5)crystals.Such interfaces bring about rich oxygen vacancies with structural shrinkage tendency,which pre-generate coercive stress to resist the expansion stress caused by excessive Li-ions intercalation.Therefore,the synthesized Nb_(2)O_(5) achieves the highest lithium storage capacity of 315 mA h g−1 to date,and exhibits high-rate performance(118 mA h g^(-1) at 20 C)as well as excellent cycling stability(138 mA h g^(-1) at 10 C after 600 cycles).展开更多
Lithium-sulfur (Li-S) batteries have great potential as an electrochemical energy storage system because of the high theoretical energy density and acceptable cost of financial and environment.However,the shuttle effe...Lithium-sulfur (Li-S) batteries have great potential as an electrochemical energy storage system because of the high theoretical energy density and acceptable cost of financial and environment.However,the shuttle effect leads to severe capacity fading and low coulombic efficiency.Here,graphitic carbon nitride(g-C3N4) is designed and prepared via a feasible and simple method from trithiocyanuric acid (TTCA) to anchor the polysulfides and suppress the shuttle effect.The obtained g-C3N4 exhibits strong chemical interaction with polysulfides due to its high N-doping of 56.87 at%,which is beneficial to improve the cycling stability of Li-S batteries.Moreover,the novel porous framework and high specific surface area of g-C3N4 also provide fast ion transport and broad reaction interface of sulfur cathode,facilitating high capacity output and superior rate performance of Li-S batteries.As a result,Li-S batteries assembled with g-C3N4 can achieve high discharge capacity of 1200 mAh/g at 0.2 C and over 800 mAh/g is remained after 100 cycles with a coulombic efficiency more than 99.5%.When the C-rate rises to 5 C,the reversible capacity of Li-S batteries can still maintain at 607mAh/g.展开更多
Sodium ion batteries(SIBs)have been regarded as one of the alternatives to lithium ion batteries owing to their wide availability and significantly low cost of sodium sources.However,they face serious challenges of lo...Sodium ion batteries(SIBs)have been regarded as one of the alternatives to lithium ion batteries owing to their wide availability and significantly low cost of sodium sources.However,they face serious challenges of low energy&power density and short cycling lifespan owing to the heavy mass and large radius of Na^(+).Vanadium-based polyanionic compounds have advantageous characteristic of high operating voltage,high ionic conductivity and robust structural framework,which is conducive to their high energy&power density and long lifespan for SIBs.In this review,we will overview the latest V-based polyanionic compounds,along with the respective characteristic from the intrinsic crystal structure to performance presentation and improvement for SIBs.One of the most important aspect is to discover the essential problems existed in the present V-based polyanionic compounds for high-energy&power applications,and point out most suitable solutions from the crystal structure modulation,interface tailoring and electrode configuration design.Moreover,some scientific issues of V-based polyanionic compounds shall be also proposed and related future direction shall be provided.We believe that this review can serve as a motivation for further development of novel V-based polyanionic compounds and drive them toward high energy&power applications in the near future.展开更多
Aqueous rechargeable metal-ion batteries(ARMBs)hold intrinsic advantages of high safety,low cost and environmental benignity for large scale energy storage technologies.However,the research on aqueous Kion batteries(A...Aqueous rechargeable metal-ion batteries(ARMBs)hold intrinsic advantages of high safety,low cost and environmental benignity for large scale energy storage technologies.However,the research on aqueous Kion batteries(AKIBs)was hindered by limited materials.Herein,a novel AKIB was reported by employing environment-friendly 1,4,5,8-naphthalenetetracarboxylic dianhydride-derived polyimide(PNTCDA)as anode and Berlin green(FeHCF)as cathode.Both electrodes have high rate performance and excellent capacity retention during cycling.Kinetics researches verify the superior electrochemical property of PNTCDA in saturated KNO3 solution.In-situ XRD of FeHCF demonstrates the unique shift of peak position and negligible distortion of lattice during the insertion/extraction of K+.The AKIB exhibits an attractive energy density of 46.9 Wh/kg and a high capacity retention of 74%in 300 cycles.More importantly,the battery can reach a super-high power of 2079.1 W/kg with an energy density of 24.2 Wh/kg,ranking relatively high among the ARIMs.This system extends the use of polyimide and points a way of AKIBs for grid-scale energy storage.展开更多
Lithium metal-based secondary batteries are very promising for next generation power battery due to their high energy density.However,lithium anodes suffer from poor electrochemical reversibility in organic electrolyt...Lithium metal-based secondary batteries are very promising for next generation power battery due to their high energy density.However,lithium anodes suffer from poor electrochemical reversibility in organic electrolytes due to Li dendrites and instability of the solid electrolyte interphase.Recent research demonstrated that the problem can be alleviated via tetraethoxysilane(TEOS)treated lithium metal to form a silicon oxide layer on the lithium surface,however,its reaction mechanism is controversial.Herein,we deeply explore the reaction mechanism between TEOS and Li and propose:Fresh Li can directly react with TEOS even though no lithium hydroxide exists on the lithium surface,and the participation of water will accelerate the reaction process.Moreover,it was found that the silicon oxide layer can promote the uniform deposition of lithium ions by providing lithiophilic nucleation sites,thereby achieving a long cycle life of Li metal batteries.展开更多
Flow batteries with high energy density and long cycle life have been pursued to advance the progress of energy storage and grid application. Non-aqueous batteries with wide voltage windows represent a promising techn...Flow batteries with high energy density and long cycle life have been pursued to advance the progress of energy storage and grid application. Non-aqueous batteries with wide voltage windows represent a promising technology without the limitation of water electrolysis, but they suffer from low electrolyte concentration and unsatisfactory battery performance. Here, a non-aqueous lithium bromine rechargeable battery is proposed, which is based on Br;/Br;and Li;/Li as active redox pairs, with fast redox kinetics and good stability. The Li/Br battery combines the advantages of high output voltage（;.1 V）,electrolyte concentration（3.0 mol/L）, maximum power density（29.1 m W/cm;） and practical energy density（232.6 Wh/kg）. Additionally, the battery displays a columbic efficiency（CE） of 90.0%, a voltage efficiency（VE） of 88.0% and an energy efficiency（EE） of 80.0% at 1.0 m A/cm;after continuously running for more than 1000 cycles, which is by far the longest cycle life reported for non-aqueous flow batteries.展开更多
Silica-based anode is widely employed for high energy density Li-ion batteries owing to their high theoretical specific capacity(4200 m A h g-1).However,it is always accompanied by a huge volume expansion(300%)and shr...Silica-based anode is widely employed for high energy density Li-ion batteries owing to their high theoretical specific capacity(4200 m A h g-1).However,it is always accompanied by a huge volume expansion(300%)and shrinks during the lithiation/delithiation process,further leading to low cycle stability.Efforts to mitigate the adverse effects caused by volume expansion such as robust binder matrix,Coreshell structure,etc.,inevitably affect the electronic conductivity within the electrode.Herein,a high conductivity and elasticity Si anode(Ni-P-SBR(styrene-butadiene rubber)@Si)was designed and fabricated via the Ni-P-SBR composite-electroless-plating process.In this design,the Si particles are surrounded by SBR polymer and Ni particles,where the SBR can adapt to the volume change and Ni particles can provide the electrode with high electronic conductivity.Therefore,the Ni-P-SBR@Si delivers a high initial capacity of 3470 m A h g-1and presents capacity retention of 49.4%within 200 cycles at 600 m A g-1.Additionally,a high capacity of 1153 m A h g-1can be achieved at 2000 m A g-1and can be cycled stably under bending conditions.This strategy provides feasible ideas to solve the key issues that limit the practical application of Si anodes.展开更多
In-depth understanding of the electrolyte-dependent intercalation chemistry in batteries through direct operando/in situ characterizations is crucial for the development of the high-performance batteries.Herein,taking...In-depth understanding of the electrolyte-dependent intercalation chemistry in batteries through direct operando/in situ characterizations is crucial for the development of the high-performance batteries.Herein,taking the Al/graphite battery as a model system,the effect of electrolyte coordination structure on the intercalation processes has been investigated over the batteries with either 1-hexyl-3-methylimidazolium chloride(HMICl)-AlCl_(3) or 1-ethyl-3-methylimidazolium chloride(EMICl)-AlCl_(3) ionic liquid electrolyte using operando X-ray photoelectron spectroscopy(XPS)and X-ray diffraction.With a weaker anion-cation interaction in HMI-based electrolyte,the XPS-derived atomic ratio between cointercalated N and intercalated Al is 0.9,which is lower than 1.6 for EMI-based electrolyte.Attributed to the additional de-solvation process,the batteries with the HMI-based electrolyte show a lower ionic diffusion rate,capacity,and cycling performance,which agree with the operando characterization results.Our findings highlight the critical role of the electrolyte coordination structure on the(co-)intercalation chemistry.展开更多
Thermocatalytic CO_(2) hydrogenation with"green"H_(2) is one of the most promising carbon-negative technologies,wherein oxygen vacancy engineering serves as a novel strategy to boost the catalytic performanc...Thermocatalytic CO_(2) hydrogenation with"green"H_(2) is one of the most promising carbon-negative technologies,wherein oxygen vacancy engineering serves as a novel strategy to boost the catalytic performance of oxide-containing catalysts.To provide theoretical guidance and promote technical progress in this important field,the status and prospect of oxygen vacancy-boosted thermocatalytic CO_(2) hydrogenation have been thoroughly reviewed herein.Specifically,fundamentals including origin,construction,characterization,and function of oxygen vacancies will be systematically summarized and oxygen vacancy-boosted hydrogenation reactions including methanation,reverse water-gas shift(RWGS),methanol synthesis,and other hydrogenation processes will be comprehensively introduced.In addition,challenges and opportunities from the perspective of engineering strategies,promoting effects,and mediating mechanisms of oxygen vacancies will be succinctly proposed.Overall,this review is expected to gain more insights into the role of oxygen vacancies and shed new light on the design of efficient oxide-containing catalysts.展开更多
Sodium-ion batteries （SIBs） have attracted increasing attention in the past decades, because of high over-all abundance of precursors, their even geographical distribution, and low cost. Na3V2（PO4）3 （NVP）, atypi...Sodium-ion batteries （SIBs） have attracted increasing attention in the past decades, because of high over-all abundance of precursors, their even geographical distribution, and low cost. Na3V2（PO4）3 （NVP）, atypical sodium super ion conductor （NASlCON）-based electrode material, exhibits pronounced structuralstability, exceptionally high ion conductivity, rendering it a most promising electrode for sodium storage.However. the comparatively low electronic conductivity makes the theoretical capacity of NVP cannot befully accessible even at comparatively low rates, presenting a major drawback for further practical ap-plications, especially when high rate capability is especially important. Thus, many endeavors have beenconformed to increase the surface and intrinsic electrical conductivity of NVP by coating the active mate-rials with a conductive carbon layer, downsizing the NVP particles, combining the NVP particle with vari-ous carbon materials and ion doping strategy. In this review, to get a better understanding on the sodiumstorage in NVP, we firstly present 4 distinct crystal structures in the temperature range of-30℃-225℃ namely α-NVP, β-NVP, β′-NVP and γ-NVP. Moreover, we give an overview of recent approaches to en-hance the surface electrical conductivity and intrinsic electrical conductivity of NVP. Finally, some poten-tial applications of NVP such as in all-climate environment and PHEV, EV fields have been prospected.展开更多
The vanadium flow battery （VFB） has been considered as one of the most promising large-scale energy storage technologies in terms of its design flexibility, long cycle life, high efficiency and high safety. How- eve...The vanadium flow battery （VFB） has been considered as one of the most promising large-scale energy storage technologies in terms of its design flexibility, long cycle life, high efficiency and high safety. How- ever, the high cost prevents the VFB technology from broader market penetration. Improving the power density of the VFB is an effective solution to reduce its cost due to the reduced material consumption and stack size. Electrode, as one of the main components in the VFB, providing the reactions sites for redox couples, has an important effect on the voltage loss of the VFB associated with electrochemical polariza- tion, ohmic polarization and concentration polarization. Extensive research has been carried out on the electrode modification to reduce polarizations and hence improve the power density of the VFB. In this review, state-of-the-art of various modification methods on the VFB electrode materials is overviewed and summarized, and the future research directions helpful to reduce polarization loss are presented.展开更多
In recent years,more and more efforts are devoting to clean energy,renewable energies in particular to achieving net zero carbon dioxide emissions[1].However,renewable energies,like solar power and wind power,are gene...In recent years,more and more efforts are devoting to clean energy,renewable energies in particular to achieving net zero carbon dioxide emissions[1].However,renewable energies,like solar power and wind power,are generally intermittent and random,hindering their wide application[2,3].To address this problem,there is an urgent need in effective and reliable energy storage device.展开更多
Long duration energy storage(LDES)technologies are vital for wide utilization of renewable energy sources and increasing the penetration of these technologies within energy infrastructures.Herein,we propose a low-cost...Long duration energy storage(LDES)technologies are vital for wide utilization of renewable energy sources and increasing the penetration of these technologies within energy infrastructures.Herein,we propose a low-cost alkaline all-iron flow battery by coupling ferri/ferro-cyanide redox couple with ferric/ferrous-gluconate complexes redox couple.The designed all-iron flow battery demonstrates a coulombic efficiency of above 99%and an energy efficiency of~83%at a current density of80 m A cm^(-2),which can continuously run for more than 950 cycles.Most importantly,the battery demonstrates a coulombic efficiency of more than 99.0%and an energy efficiency of~83%for a long duration(~12,16 and 20 h per cycle)charge/discharge process.Benefiting from the low cost of iron electrolytes,the overall cost of the all-iron flow battery system can be reached as low as$76.11 per k Wh based on a10 h system with a power of 9.9 k W.This work provides a new option for next-generation cost-effective flow batteries for long duration large scale energy storage.展开更多
By utilizing hard template method to adjust the mesopore length, and alkali activation to generate micro pores, two hierarchical porous carbons (HPCs) were prepared. With controlling of their mesopore length and the a...By utilizing hard template method to adjust the mesopore length, and alkali activation to generate micro pores, two hierarchical porous carbons (HPCs) were prepared. With controlling of their mesopore length and the activation conditions, the complex system composed by HPCs and electrolyte was simplified and the effect of mesopore length on the performance of HPCs as electrodes in supercapacitors was investigated. It is found that with the mesopore length getting smaller, the ordered area gets smaller and the aggregation occurs, which is caused by the high surface energy of small grains. HPC with long pores (HPCL) exhibits a donut-like morphology with well-defined ordered mesopores and a regular orientation while in HPC with short pores (HPCS), short mesopores are only orderly distributed in small regions. Longer ordered channels form unobstructed ways for ions transport in the particles while shorter channels, only orderly distributed in small areas, results in blocked paths, which may hinder the electrolyte ions transport. Due to the unobstructed structure, HPCL exhibits good rate capability with a capacitance retention rate over 86% as current density increasing from 50 mA/g to 1000 mA/g. The specific capacitance of HPCL derived from the cyclic voltammetry test at 10 mV/s is up to 201.72 F/g, while the specific capacitance of HPCS is only 193.65 F/g. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.展开更多
For flow batteries(FBs), the current technologies are still expensive and have relatively low energy density, which limits their large-scale applications. Organic FBs(OFBs) which employ organic molecules as redox-acti...For flow batteries(FBs), the current technologies are still expensive and have relatively low energy density, which limits their large-scale applications. Organic FBs(OFBs) which employ organic molecules as redox-active materials have been considered as one of the promising technologies for achieving lowcost and high-performance. Herein, we present a critical overview of the progress on the OFBs, including the design principles of key components(redox-active molecules, membranes, and electrodes) and the latest achievement in both aqueous and nonaqueous systems. Finally, future directions in explorations of the high-performance OFB for electrochemical energy storage are also highlighted.展开更多
The effect of bismuth (Bi) for both VO2+/VO2+ and V3+/V2+ redox couples in vanadium flow batteries (VFBs) has been investigated by directly introducing Bi on the surface of carbon felt (CF). The results show that Bi h...The effect of bismuth (Bi) for both VO2+/VO2+ and V3+/V2+ redox couples in vanadium flow batteries (VFBs) has been investigated by directly introducing Bi on the surface of carbon felt (CF). The results show that Bi has no catalytic effect for VO2+/VO2(+) redox couple. During the first charge process, Bi is oxidized to Bi3+ (never return back to Bi metal in the subsequent cycles) due to the low standard redox potential of 0.308 V (vs. SHE) for Bi3+/Bi redox couple compared with VO2+/VO2+ redox couple and Bi3+ exhibit no (or neglectable) electro-catalytic activity. Additionally, the relationship between Bi loading and electrochemical activity for V3+/V2+ redox couple was studied in detail. 2 wt% Bi-modified carbon felt (2%-BiCF) exhibits the highest electrochemical activity. Using it as negative electrode, a high energy efficiency (EE) of 79.0% can be achieved at a high current density of 160 mA/cm(2), which is 5.5% higher than the pristine one. Moreover, the electrolyte utilization ratio is also increased by more than 30%. Even the cell operated at 140 mA/cm(2) for over 300 cycles, the EE can reach 80.9% without obvious fluctuation and attenuation, suggesting excellent catalytic activity and electrochemical stability in VFBs. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.展开更多
In the past few decades, supercapacitor(SC) has attracted great attention due to its significant advantages over traditional rechargeable battery systems, such as high power density, fast charge-discharge rate, long c...In the past few decades, supercapacitor(SC) has attracted great attention due to its significant advantages over traditional rechargeable battery systems, such as high power density, fast charge-discharge rate, long cycle life and environmental friendliness [1]. Up to now, supercapacitors have been widely used in backup power, electric vehicles, mobile power and so on [2,3].展开更多
The conversion of carbon dioxide to chemicals by the electrochemical reactions(ERC)is an efficient solution to the current energy crisis and excess CO_(2) emissions.It is still a great challenge and of significance to...The conversion of carbon dioxide to chemicals by the electrochemical reactions(ERC)is an efficient solution to the current energy crisis and excess CO_(2) emissions.It is still a great challenge and of significance to synthesize a highly selective,efficient,and non-noble metal electrocatalyst that facilitates the ERC reaction.A novel triton X-100(C_(14)H_(22)O(C_(2)H_(4)O)n)assisted electrodeposition method was developed to synthesize the ordered cone-structured tin(OCSn)electrocatalysts with controllable morphology and structure.The results suggest that Triton X-100 plays an important role in directing the structure of the Sn electrocatalysts during the electrodeposition process.The OCSn synthesized at 60 m A cm^(-2) achieves the best performances.It selectively catalyzes the ERC on the onset potential about 110 m V lower than Sn synthesized without Triton X-100.In 0.5 M Na HCO_(3),high faradaic efficiency(92%)for formate product on OCSn has been achieved.More prominently,the catalyst presents excellent stability,showing no performance deterioration during 30 h electrolysis.This work provides an efficient,green,and scalable synthesis method of the electrocatalyst for CO_(2) reduction to formate.展开更多
A membrane with high stability and ion conductivity in wide pH range is essential for energy storage devices.Here,we report a novel membrane with hierarchical core-shell structure,which demonstrates high stability and...A membrane with high stability and ion conductivity in wide pH range is essential for energy storage devices.Here,we report a novel membrane with hierarchical core-shell structure,which demonstrates high stability and ion conductivity,simultaneously under a wide pH range applications.Spectral characterizations and theoretical calculation indicate that the non-solvent induces the chain segment configuration and eventually leads to polymer-polymer phase separation,thus forming hierarchical porous core-shell structure.Benefiting from this structure,an acidic vanadium flow battery(VFB)with such a membrane shows excellent performance over 400 cycles with an energy efficiency(EE)of above 81%at current density of 120 mA cm^(-2) and an alkaline zinc-iron flow battery(AZIFB)delivers a cycling stability for more than 200 cycles at 160 mA cm^(-2),along with an EE of above 82%.This paper provides a cost-effective and simple way to fabricate membranes with high performance for variety of energyrelated devices.展开更多
基金supported by the CAS Project of Young Scientists in Basic Research(YSBR-058)the National Natural Science Foundation of China(22279135)+2 种基金the Outstanding Youth Foundation of Liaoning Province(2023JH3/10200019)the Dalian Science and Technology Innovation Fund(2023JJ11CG004)the Energy Revolution S&T Program of Yulin Innovation Institute of Clean Energy(YIICE E411010316)。
文摘Anode-free solid-state lithium metal batteries(AF-SSLBs)have the potential to deliver higher energy density and improved safety beyond lithium-metal batteries.However,the unclear mechanism for the fast capacity decay in AF-SSLBs,either determined by dead Li or solid electrolyte interface(SEI),limits the proposal of effective strategies to prolong cycling life.To clarify the underlying mechanism,herein,the evolution of SEI and dead Li is quantitatively analyzed by a solid-state nuclear magnetic resonance(ss-NMR)technology in a typical LiPF6-based polymer electrolyte.The results show that the initial capacity loss is attributed to the formation of SEI,while the dead Li dominates the following capacity loss and the growth rate is 0.141 mA h cm^(−2)cycle−1.To reduce the active Li loss,the combination of inorganic-rich SEI and self-healing electrostatic shield effect is proposed to improve the reversibility of Li deposition/dissolution behavior,which reduces the capacity loss rate for the initial SEI and following dead Li generation by 2.3 and 20.1 folds,respectively.As a result,the initial Coulombic efficiency(ICE)and stable CE increase by 15.1%and 15.3%in Li-Cu cells,which guides the rational design of high-performance AF-SSLBs.
基金supported by the National Natural Science Foundation of China(Nos.51673199,51972301,51677176)the Youth Innovation Promotion Association of CAS(2015148,Y201940)+2 种基金the Youth Innovation Foundation of DICP(ZZBS201615,ZZBS201708)the Dalian Outstanding Young Scientific Talent(2018RJ03)the National Key Research and Development Project(2019YFA0705600)。
文摘Niobium pentoxide(Nb_(2)O_(5))is deemed one of the promising anode materials for lithium-ion batteries(LIBs)for its outstanding intrinsic fast Li-(de)intercalation kinetics.The specific capacity,however,is still limited,because the(de)intercalation of excessive Li-ions brings the undesired stress to damage Nb_(2)O_(5) crystals.To increase the capacity of Nb_(2)O_(5) and alleviate the lattice distortion caused by stress,numerous homogeneous H-and M-phases junction interfaces were proposed to produce coercive stress within theNb_(2)O_(5)crystals.Such interfaces bring about rich oxygen vacancies with structural shrinkage tendency,which pre-generate coercive stress to resist the expansion stress caused by excessive Li-ions intercalation.Therefore,the synthesized Nb_(2)O_(5) achieves the highest lithium storage capacity of 315 mA h g−1 to date,and exhibits high-rate performance(118 mA h g^(-1) at 20 C)as well as excellent cycling stability(138 mA h g^(-1) at 10 C after 600 cycles).
基金the financial support from the National Natural Science Foundation of China(Nos.51673199 and 51677176)Youth Innovation Promotion Association of CAS(2015148)+1 种基金Innovation Foundation of DICP(ZZBS201615,ZZBS201708)Dalian Science and Technology Star Program(2016RQ026)。
文摘Lithium-sulfur (Li-S) batteries have great potential as an electrochemical energy storage system because of the high theoretical energy density and acceptable cost of financial and environment.However,the shuttle effect leads to severe capacity fading and low coulombic efficiency.Here,graphitic carbon nitride(g-C3N4) is designed and prepared via a feasible and simple method from trithiocyanuric acid (TTCA) to anchor the polysulfides and suppress the shuttle effect.The obtained g-C3N4 exhibits strong chemical interaction with polysulfides due to its high N-doping of 56.87 at%,which is beneficial to improve the cycling stability of Li-S batteries.Moreover,the novel porous framework and high specific surface area of g-C3N4 also provide fast ion transport and broad reaction interface of sulfur cathode,facilitating high capacity output and superior rate performance of Li-S batteries.As a result,Li-S batteries assembled with g-C3N4 can achieve high discharge capacity of 1200 mAh/g at 0.2 C and over 800 mAh/g is remained after 100 cycles with a coulombic efficiency more than 99.5%.When the C-rate rises to 5 C,the reversible capacity of Li-S batteries can still maintain at 607mAh/g.
基金financial support from the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA21070500)the DNL Cooperation Fund,CAS(DNL201914)。
文摘Sodium ion batteries(SIBs)have been regarded as one of the alternatives to lithium ion batteries owing to their wide availability and significantly low cost of sodium sources.However,they face serious challenges of low energy&power density and short cycling lifespan owing to the heavy mass and large radius of Na^(+).Vanadium-based polyanionic compounds have advantageous characteristic of high operating voltage,high ionic conductivity and robust structural framework,which is conducive to their high energy&power density and long lifespan for SIBs.In this review,we will overview the latest V-based polyanionic compounds,along with the respective characteristic from the intrinsic crystal structure to performance presentation and improvement for SIBs.One of the most important aspect is to discover the essential problems existed in the present V-based polyanionic compounds for high-energy&power applications,and point out most suitable solutions from the crystal structure modulation,interface tailoring and electrode configuration design.Moreover,some scientific issues of V-based polyanionic compounds shall be also proposed and related future direction shall be provided.We believe that this review can serve as a motivation for further development of novel V-based polyanionic compounds and drive them toward high energy&power applications in the near future.
文摘Aqueous rechargeable metal-ion batteries(ARMBs)hold intrinsic advantages of high safety,low cost and environmental benignity for large scale energy storage technologies.However,the research on aqueous Kion batteries(AKIBs)was hindered by limited materials.Herein,a novel AKIB was reported by employing environment-friendly 1,4,5,8-naphthalenetetracarboxylic dianhydride-derived polyimide(PNTCDA)as anode and Berlin green(FeHCF)as cathode.Both electrodes have high rate performance and excellent capacity retention during cycling.Kinetics researches verify the superior electrochemical property of PNTCDA in saturated KNO3 solution.In-situ XRD of FeHCF demonstrates the unique shift of peak position and negligible distortion of lattice during the insertion/extraction of K+.The AKIB exhibits an attractive energy density of 46.9 Wh/kg and a high capacity retention of 74%in 300 cycles.More importantly,the battery can reach a super-high power of 2079.1 W/kg with an energy density of 24.2 Wh/kg,ranking relatively high among the ARIMs.This system extends the use of polyimide and points a way of AKIBs for grid-scale energy storage.
基金the financial support from the National Natural Science Foundation of China(Nos.51673199,51972301,51677176)Youth Innovation Promotion Association of CAS(2015148)+2 种基金Youth Innovation Foundation of DICP(ZZBS201615,ZZBS201708)Dalian Outstanding Young Scientific Talent(2018RJ03)National Key Research and Development Project(2019YFA0705600)。
文摘Lithium metal-based secondary batteries are very promising for next generation power battery due to their high energy density.However,lithium anodes suffer from poor electrochemical reversibility in organic electrolytes due to Li dendrites and instability of the solid electrolyte interphase.Recent research demonstrated that the problem can be alleviated via tetraethoxysilane(TEOS)treated lithium metal to form a silicon oxide layer on the lithium surface,however,its reaction mechanism is controversial.Herein,we deeply explore the reaction mechanism between TEOS and Li and propose:Fresh Li can directly react with TEOS even though no lithium hydroxide exists on the lithium surface,and the participation of water will accelerate the reaction process.Moreover,it was found that the silicon oxide layer can promote the uniform deposition of lithium ions by providing lithiophilic nucleation sites,thereby achieving a long cycle life of Li metal batteries.
基金financial supported by the Natural Science Foundation of China(Grant No.21476224,21406219 and 51361135701)
文摘Flow batteries with high energy density and long cycle life have been pursued to advance the progress of energy storage and grid application. Non-aqueous batteries with wide voltage windows represent a promising technology without the limitation of water electrolysis, but they suffer from low electrolyte concentration and unsatisfactory battery performance. Here, a non-aqueous lithium bromine rechargeable battery is proposed, which is based on Br;/Br;and Li;/Li as active redox pairs, with fast redox kinetics and good stability. The Li/Br battery combines the advantages of high output voltage（;.1 V）,electrolyte concentration（3.0 mol/L）, maximum power density（29.1 m W/cm;） and practical energy density（232.6 Wh/kg）. Additionally, the battery displays a columbic efficiency（CE） of 90.0%, a voltage efficiency（VE） of 88.0% and an energy efficiency（EE） of 80.0% at 1.0 m A/cm;after continuously running for more than 1000 cycles, which is by far the longest cycle life reported for non-aqueous flow batteries.
基金financial support from the National Natural Science Foundation of China(No.51673199,51972301)the Youth Innovation Promotion Association of CAS(2015148)+2 种基金the Youth Innovation Foundation of DICP(ZZBS201615,ZZBS201708)the Dalian Outstanding Young Scientific Talent(2018RJ03)the National Key Research and Development Project(2019YFA0705600)。
文摘Silica-based anode is widely employed for high energy density Li-ion batteries owing to their high theoretical specific capacity(4200 m A h g-1).However,it is always accompanied by a huge volume expansion(300%)and shrinks during the lithiation/delithiation process,further leading to low cycle stability.Efforts to mitigate the adverse effects caused by volume expansion such as robust binder matrix,Coreshell structure,etc.,inevitably affect the electronic conductivity within the electrode.Herein,a high conductivity and elasticity Si anode(Ni-P-SBR(styrene-butadiene rubber)@Si)was designed and fabricated via the Ni-P-SBR composite-electroless-plating process.In this design,the Si particles are surrounded by SBR polymer and Ni particles,where the SBR can adapt to the volume change and Ni particles can provide the electrode with high electronic conductivity.Therefore,the Ni-P-SBR@Si delivers a high initial capacity of 3470 m A h g-1and presents capacity retention of 49.4%within 200 cycles at 600 m A g-1.Additionally,a high capacity of 1153 m A h g-1can be achieved at 2000 m A g-1and can be cycled stably under bending conditions.This strategy provides feasible ideas to solve the key issues that limit the practical application of Si anodes.
基金financially supported by the National Key R&D Program of China (2021YFA1502800)the National Natural Science Foundation of China (21825203,22288201,and 91945302)+1 种基金the Photon Science Center for Carbon Neutrality,Liao Ning Revitalization Talents Program (XLYC1902117)the Youth Innovation Fund of Dalian institute of Chemical Physics (DICP I202125)。
文摘In-depth understanding of the electrolyte-dependent intercalation chemistry in batteries through direct operando/in situ characterizations is crucial for the development of the high-performance batteries.Herein,taking the Al/graphite battery as a model system,the effect of electrolyte coordination structure on the intercalation processes has been investigated over the batteries with either 1-hexyl-3-methylimidazolium chloride(HMICl)-AlCl_(3) or 1-ethyl-3-methylimidazolium chloride(EMICl)-AlCl_(3) ionic liquid electrolyte using operando X-ray photoelectron spectroscopy(XPS)and X-ray diffraction.With a weaker anion-cation interaction in HMI-based electrolyte,the XPS-derived atomic ratio between cointercalated N and intercalated Al is 0.9,which is lower than 1.6 for EMI-based electrolyte.Attributed to the additional de-solvation process,the batteries with the HMI-based electrolyte show a lower ionic diffusion rate,capacity,and cycling performance,which agree with the operando characterization results.Our findings highlight the critical role of the electrolyte coordination structure on the(co-)intercalation chemistry.
基金financial supports from the National Natural Science Foundation of China(22378017,21776007)the National Key Research and Development Program of China(2022YFC2105604)are acknowledged。
文摘Thermocatalytic CO_(2) hydrogenation with"green"H_(2) is one of the most promising carbon-negative technologies,wherein oxygen vacancy engineering serves as a novel strategy to boost the catalytic performance of oxide-containing catalysts.To provide theoretical guidance and promote technical progress in this important field,the status and prospect of oxygen vacancy-boosted thermocatalytic CO_(2) hydrogenation have been thoroughly reviewed herein.Specifically,fundamentals including origin,construction,characterization,and function of oxygen vacancies will be systematically summarized and oxygen vacancy-boosted hydrogenation reactions including methanation,reverse water-gas shift(RWGS),methanol synthesis,and other hydrogenation processes will be comprehensively introduced.In addition,challenges and opportunities from the perspective of engineering strategies,promoting effects,and mediating mechanisms of oxygen vacancies will be succinctly proposed.Overall,this review is expected to gain more insights into the role of oxygen vacancies and shed new light on the design of efficient oxide-containing catalysts.
基金financial support from the National Natural Science Foundation of China (No.21501171,51403209,21406221,51177156/E0712)
文摘Sodium-ion batteries （SIBs） have attracted increasing attention in the past decades, because of high over-all abundance of precursors, their even geographical distribution, and low cost. Na3V2（PO4）3 （NVP）, atypical sodium super ion conductor （NASlCON）-based electrode material, exhibits pronounced structuralstability, exceptionally high ion conductivity, rendering it a most promising electrode for sodium storage.However. the comparatively low electronic conductivity makes the theoretical capacity of NVP cannot befully accessible even at comparatively low rates, presenting a major drawback for further practical ap-plications, especially when high rate capability is especially important. Thus, many endeavors have beenconformed to increase the surface and intrinsic electrical conductivity of NVP by coating the active mate-rials with a conductive carbon layer, downsizing the NVP particles, combining the NVP particle with vari-ous carbon materials and ion doping strategy. In this review, to get a better understanding on the sodiumstorage in NVP, we firstly present 4 distinct crystal structures in the temperature range of-30℃-225℃ namely α-NVP, β-NVP, β′-NVP and γ-NVP. Moreover, we give an overview of recent approaches to en-hance the surface electrical conductivity and intrinsic electrical conductivity of NVP. Finally, some poten-tial applications of NVP such as in all-climate environment and PHEV, EV fields have been prospected.
基金supported by the National Natural Science Foundation of China (Grant no. 21506210)the Outstanding Young Scientist Foundation, Chinese Academy of Sciences (CAS)State Grid Corporation of Science and Technology Projects (Research on key technology of bipolar plate material development and engineering for vanadium redox flow battery)
文摘The vanadium flow battery （VFB） has been considered as one of the most promising large-scale energy storage technologies in terms of its design flexibility, long cycle life, high efficiency and high safety. How- ever, the high cost prevents the VFB technology from broader market penetration. Improving the power density of the VFB is an effective solution to reduce its cost due to the reduced material consumption and stack size. Electrode, as one of the main components in the VFB, providing the reactions sites for redox couples, has an important effect on the voltage loss of the VFB associated with electrochemical polariza- tion, ohmic polarization and concentration polarization. Extensive research has been carried out on the electrode modification to reduce polarizations and hence improve the power density of the VFB. In this review, state-of-the-art of various modification methods on the VFB electrode materials is overviewed and summarized, and the future research directions helpful to reduce polarization loss are presented.
基金financially supported by the National Natural Science Foundation of China(Grant No.21935003 and 21908217)DICP I201928+1 种基金the China Postdoctoral Science Foundation(No.2019M651158)the CAS Engineering Laboratory for Electrochemical Energy Storage。
文摘In recent years,more and more efforts are devoting to clean energy,renewable energies in particular to achieving net zero carbon dioxide emissions[1].However,renewable energies,like solar power and wind power,are generally intermittent and random,hindering their wide application[2,3].To address this problem,there is an urgent need in effective and reliable energy storage device.
基金the financial support from National Natural Science Foundation of China(22078313,21908214 and 21925804)the Dalian High Level Talent Innovation support program(2020RD05)+2 种基金the Dalian Young Star of Science and Technology(2021RQ122)the Free exploring basic research project of Liaoning(2022JH6/100100005)the Youth Innovation Promotion Association CAS(2019182)。
文摘Long duration energy storage(LDES)technologies are vital for wide utilization of renewable energy sources and increasing the penetration of these technologies within energy infrastructures.Herein,we propose a low-cost alkaline all-iron flow battery by coupling ferri/ferro-cyanide redox couple with ferric/ferrous-gluconate complexes redox couple.The designed all-iron flow battery demonstrates a coulombic efficiency of above 99%and an energy efficiency of~83%at a current density of80 m A cm^(-2),which can continuously run for more than 950 cycles.Most importantly,the battery demonstrates a coulombic efficiency of more than 99.0%and an energy efficiency of~83%for a long duration(~12,16 and 20 h per cycle)charge/discharge process.Benefiting from the low cost of iron electrolytes,the overall cost of the all-iron flow battery system can be reached as low as$76.11 per k Wh based on a10 h system with a power of 9.9 k W.This work provides a new option for next-generation cost-effective flow batteries for long duration large scale energy storage.
基金financial support from the Natural Science Foundation of China(no.51177156/E0712)
文摘By utilizing hard template method to adjust the mesopore length, and alkali activation to generate micro pores, two hierarchical porous carbons (HPCs) were prepared. With controlling of their mesopore length and the activation conditions, the complex system composed by HPCs and electrolyte was simplified and the effect of mesopore length on the performance of HPCs as electrodes in supercapacitors was investigated. It is found that with the mesopore length getting smaller, the ordered area gets smaller and the aggregation occurs, which is caused by the high surface energy of small grains. HPC with long pores (HPCL) exhibits a donut-like morphology with well-defined ordered mesopores and a regular orientation while in HPC with short pores (HPCS), short mesopores are only orderly distributed in small regions. Longer ordered channels form unobstructed ways for ions transport in the particles while shorter channels, only orderly distributed in small areas, results in blocked paths, which may hinder the electrolyte ions transport. Due to the unobstructed structure, HPCL exhibits good rate capability with a capacitance retention rate over 86% as current density increasing from 50 mA/g to 1000 mA/g. The specific capacitance of HPCL derived from the cyclic voltammetry test at 10 mV/s is up to 201.72 F/g, while the specific capacitance of HPCS is only 193.65 F/g. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.
基金supported by the China Natural Science Foundation(U1808209)the CAS-DOE program,CAS(QYZDB-SSWJSC032)+1 种基金the Key R&D project of Dalian(2018YF17GX020)the DICP funding(ZZBS201707)。
文摘For flow batteries(FBs), the current technologies are still expensive and have relatively low energy density, which limits their large-scale applications. Organic FBs(OFBs) which employ organic molecules as redox-active materials have been considered as one of the promising technologies for achieving lowcost and high-performance. Herein, we present a critical overview of the progress on the OFBs, including the design principles of key components(redox-active molecules, membranes, and electrodes) and the latest achievement in both aqueous and nonaqueous systems. Finally, future directions in explorations of the high-performance OFB for electrochemical energy storage are also highlighted.
基金the financial support from the China Natural Science Foundation(Grant nos.51403209,21406221,21206158,21476224,21406219 and 51361135701)the Outstanding Young Scientist Foundation,Chinese Academy of Sciences(CAS)+2 种基金Supported by the Key Research Program of the Chinese Academy of Sciences(KG2D-EW-602-2)Science and Technology Service Network Initiative(KFJ-EW-STS-108)Dalian Municipal Outstanding Young Talent Foundation(2014J11JH131)
文摘The effect of bismuth (Bi) for both VO2+/VO2+ and V3+/V2+ redox couples in vanadium flow batteries (VFBs) has been investigated by directly introducing Bi on the surface of carbon felt (CF). The results show that Bi has no catalytic effect for VO2+/VO2(+) redox couple. During the first charge process, Bi is oxidized to Bi3+ (never return back to Bi metal in the subsequent cycles) due to the low standard redox potential of 0.308 V (vs. SHE) for Bi3+/Bi redox couple compared with VO2+/VO2+ redox couple and Bi3+ exhibit no (or neglectable) electro-catalytic activity. Additionally, the relationship between Bi loading and electrochemical activity for V3+/V2+ redox couple was studied in detail. 2 wt% Bi-modified carbon felt (2%-BiCF) exhibits the highest electrochemical activity. Using it as negative electrode, a high energy efficiency (EE) of 79.0% can be achieved at a high current density of 160 mA/cm(2), which is 5.5% higher than the pristine one. Moreover, the electrolyte utilization ratio is also increased by more than 30%. Even the cell operated at 140 mA/cm(2) for over 300 cycles, the EE can reach 80.9% without obvious fluctuation and attenuation, suggesting excellent catalytic activity and electrochemical stability in VFBs. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.
基金financially supported by the Shandong Provincial Natural Science Foundation, China (ZR2019PB018)National Natural Science Foundation, China (21506210)。
文摘In the past few decades, supercapacitor(SC) has attracted great attention due to its significant advantages over traditional rechargeable battery systems, such as high power density, fast charge-discharge rate, long cycle life and environmental friendliness [1]. Up to now, supercapacitors have been widely used in backup power, electric vehicles, mobile power and so on [2,3].
基金the financially support of the National Natural Science Foundation of China(No.21576255 and No.21577141)Dalian Science Fund for Distinguished Young Scholars(2018RJ09)。
文摘The conversion of carbon dioxide to chemicals by the electrochemical reactions(ERC)is an efficient solution to the current energy crisis and excess CO_(2) emissions.It is still a great challenge and of significance to synthesize a highly selective,efficient,and non-noble metal electrocatalyst that facilitates the ERC reaction.A novel triton X-100(C_(14)H_(22)O(C_(2)H_(4)O)n)assisted electrodeposition method was developed to synthesize the ordered cone-structured tin(OCSn)electrocatalysts with controllable morphology and structure.The results suggest that Triton X-100 plays an important role in directing the structure of the Sn electrocatalysts during the electrodeposition process.The OCSn synthesized at 60 m A cm^(-2) achieves the best performances.It selectively catalyzes the ERC on the onset potential about 110 m V lower than Sn synthesized without Triton X-100.In 0.5 M Na HCO_(3),high faradaic efficiency(92%)for formate product on OCSn has been achieved.More prominently,the catalyst presents excellent stability,showing no performance deterioration during 30 h electrolysis.This work provides an efficient,green,and scalable synthesis method of the electrocatalyst for CO_(2) reduction to formate.
基金the financial support from NSFC(21925804,U1808209 and 21908214)CAS Engineering Laboratory for Electrochemical Energy Storage,CAS,STS program.Major scientific and technological innovation project of Shandong(2018YFJH0106)+1 种基金the CAS(DNL201910)Youth Innovation Promotion Association CAS。
文摘A membrane with high stability and ion conductivity in wide pH range is essential for energy storage devices.Here,we report a novel membrane with hierarchical core-shell structure,which demonstrates high stability and ion conductivity,simultaneously under a wide pH range applications.Spectral characterizations and theoretical calculation indicate that the non-solvent induces the chain segment configuration and eventually leads to polymer-polymer phase separation,thus forming hierarchical porous core-shell structure.Benefiting from this structure,an acidic vanadium flow battery(VFB)with such a membrane shows excellent performance over 400 cycles with an energy efficiency(EE)of above 81%at current density of 120 mA cm^(-2) and an alkaline zinc-iron flow battery(AZIFB)delivers a cycling stability for more than 200 cycles at 160 mA cm^(-2),along with an EE of above 82%.This paper provides a cost-effective and simple way to fabricate membranes with high performance for variety of energyrelated devices.
