Solid polymer electrolytes(SPEs)have become increasingly attractive in solid-state lithium-ion batteries(SSLIBs)in recent years because of their inherent properties of flexibility,processability,and interfacial compat...Solid polymer electrolytes(SPEs)have become increasingly attractive in solid-state lithium-ion batteries(SSLIBs)in recent years because of their inherent properties of flexibility,processability,and interfacial compatibility.However,the commercialization of SPEs remains challenging for flexible and high-energy-density LIBs.The incorporation of functional additives into SPEs could significantly improve the electrochemical and mechanical properties of SPEs and has created some historical milestones in boosting the development of SPEs.In this study,we review the roles of additives in SPEs,highlighting the working mechanisms and functionalities of the additives.The additives could afford significant advantages in boosting ionic conductivity,increasing ion transference number,improving high-voltage stability,enhancing mechanical strength,inhibiting lithium dendrite,and reducing flammability.Moreover,the application of functional additives in high-voltage cathodes,lithium-sulfur batteries,and flexible lithiumion batteries is summarized.Finally,future research perspectives are proposed to overcome the unresolved technical hurdles and critical issues in additives of SPEs,such as facile fabrication process,interfacial compatibility,investigation of the working mechanism,and special functionalities.展开更多
Carbon nitrides(including CN,C2N,C3N,C3N4,C4N,and C5N)are a unique family of nitrogen-rich carbon materials with multiple beneficial properties in crystalline structures,morphologies,and electronic configurations.In t...Carbon nitrides(including CN,C2N,C3N,C3N4,C4N,and C5N)are a unique family of nitrogen-rich carbon materials with multiple beneficial properties in crystalline structures,morphologies,and electronic configurations.In this review,we provide a comprehensive review on these materials properties,theoretical advantages,the synthesis and modification strategies of different carbon nitride-based materials(CNBMs)and their application in existing and emerging rechargeable battery systems,such as lithium-ion batteries,sodium and potassium-ion batteries,lithium sulfur batteries,lithium oxygen batteries,lithium metal batteries,zinc-ion batteries,and solid-state batteries.The central theme of this review is to apply the theoretical and computational design to guide the experimental synthesis of CNBMs for energy storage,i.e.,facilitate the application of first-principle studies and density functional theory for electrode material design,synthesis,and characterization of different CNBMs for the aforementioned rechargeable batteries.At last,we conclude with the challenges,and prospects of CNBMs,and propose future perspectives and strategies for further advancement of CNBMs for rechargeable batteries.展开更多
The authors regret that the wrong image of Fig.1 was uploaded in the paper.The correct one should be:We confirm the discrepancy is restricted to the image of Fig.1 only,the underlying data is correct and unchanged.The...The authors regret that the wrong image of Fig.1 was uploaded in the paper.The correct one should be:We confirm the discrepancy is restricted to the image of Fig.1 only,the underlying data is correct and unchanged.The authors would like to apologise for any inconvenience caused.展开更多
Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large...Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large volume change and active material loss in lithium-ion batteries during prolonged cycles. Herein, a hydrophilic polymer poly(methyl vinyl ether-alt-maleic acid) (PMVEMA) was explored as a dual-functional aqueous binder for the preparation of high-performance silicon anode and sulfur cathode. Benefiting from the dual functions of PMVEMA, i.e., the excellent dispersion ability and strong binding forces, the as-prepared electrodes exhibit improved capacity, rate capability and long-term cycling performance. In particular, the as-prepared Si electrode delivers a high initial discharge capacity of 1346.5 mAh g^(−1) at a high rate of 8.4 A/g and maintains 834.5 mAh g^(−1) after 300 cycles at 4.2 A/g, while the as-prepared S cathode exhibits enhanced cycling performance with high remaining discharge capacities of 663.4 mAh g^(−1) after 100 cycles at 0.2 C and 487.07 mAh g^(−1) after 300 cycles at 1 C, respectively. These encouraging results suggest that PMVEMA could be a universal binder to facilitate the green manufacture of both anode and cathode for high-capacity energy storage systems.展开更多
Bimetallic nanostructures have attracted great interest as efficient catalyst to enhance activity,selectivity and stability in catalytical conversion.Herein,we report a facile one‐pot carbothermal route to in‐situ c...Bimetallic nanostructures have attracted great interest as efficient catalyst to enhance activity,selectivity and stability in catalytical conversion.Herein,we report a facile one‐pot carbothermal route to in‐situ controllable synthesize heterogeneous bimetallic Ni3Fe NPs@C nanocatalyst.The X‐ray diffraction,transmission electron microscopy,X‐ray photoelectron spectroscopy and N2 adsorption‐description results reveal that the Ni3Fe alloy nanoparticles are evenly embedded in carbon matrix.The as‐prepared Ni3Fe NPs@C catalyst shows excellent selective hydrogenation catalytic performance toward the conversion of levulinic acid(LA)toγ‐valerolactone(GVL)via both direct hydrogenation(DH)and transfer hydrogenation(TH).In DH of LA,the bimetallic catalyst achieved a 93.8%LA conversion efficiency with a 95.5%GVL selectivity and 38.2 mmol g–1 h–1 GVL productivity(under 130°C,2MPa H2 within 2 h),which are 6 and 40 times in comparison with monometallic Ni NPs@C and Fe NPs@C catalysts,respectively.In addition,the identical catalyst displayed a full conversion of LA with almost 100%GVL selectivity and 167.1 mmol g–1 h–1 GVL productivity at 180°C within 0.5 h in TH of LA.Under optimal reaction conditions,the DH and TH catalytic performance of 500‐Ni3Fe NPs@C(3:1)catalyst for converting LA to GVL is comparable to the state‐of‐the‐art noble‐based catalysts.The demonstrated capability of bimetallic catalyst design approach to introduce dual‐catalytic functionality for DH and TH reactions could be adoptable for other catalysis processes.展开更多
Aqueous zinc-ion batteries(AZIBs)can be one of the most promising electrochemical energy storage devices for being non-flammable,low-cost,and sustainable.However,the challenges of AZIBs,including dendrite growth,hydro...Aqueous zinc-ion batteries(AZIBs)can be one of the most promising electrochemical energy storage devices for being non-flammable,low-cost,and sustainable.However,the challenges of AZIBs,including dendrite growth,hydrogen evolution,corrosion,and passivation of zinc anode during charging and discharging processes,must be overcome to achieve high cycling performance and stability in practical applications.In this work,we utilize a dual-func-tional organic additive cyclohexanedodecol(CHD)to firstly establish[Zn(H2O)5(CHD)]2+complex ion in an aqueous Zn electrolyte and secondly build a robust protection layer on the Zn surface to overcome these dilemmas.Systematic experiments and theoretical calculations are carried out to interpret the working mechanism of CHD.At a very low concentration of 0.1 mg mL^(−1) CHD,long-term reversible Zn plating/stripping could be achieved up to 2200 h at 2 mA cm^(−2),1000 h at 5 mA cm^(−2),and 650 h at 10 mA cm^(−2) at the fixed capacity of 1 mAh cm^(−2).When matched with V_(2)O_(5) cathode,the resultant AZIBs full cell with the CHD-modified electrolyte presents a high capacity of 175 mAh g^(−1) with the capacity retention of 92%after 2000 cycles under 2 A g^(−1).Such a performance could enable the commercialization of AZIBs for applications in grid energy storage and industrial energy storage.展开更多
It is challenging to create cation vacancies in electrode materials for enhancing the performance of rechargeable lithium ion batteries (LIBs). Herein, we utilized a strong alkaline etching method to successfully crea...It is challenging to create cation vacancies in electrode materials for enhancing the performance of rechargeable lithium ion batteries (LIBs). Herein, we utilized a strong alkaline etching method to successfully create Co vacancies at the interface of atomically thin Co_(3−x)O_(4)/graphene@CNT heterostructure for high-energy/power lithium storage. The creation of Co-vacancies in the sample was confirmed by high-resolution scanning transmission electron microscope (HRSTEM), X-ray photoelectron spectroscopy (XPS) and electron energy loss near-edge structures (ELNES). The obtained Co_(3−x)O_(4)/graphene@CNT delivers an ultra-high capacity of 1688.2 mAh g^(−1) at 0.2 C, excellent rate capability of 83.7% capacity retention at 1 C, and an ultralong life up to 1500 cycles with a reversible capacity of 1066.3 mAh g^(−1). Reaction kinetic study suggests a significant contribution from pseudocapacitive storage induced by the Co-vacancies at the Co_(3−x)O_(4)/graphene@CNT interface. Density functional theory confirms that the Co-vacancies could dramatically enhance the Li adsorption and provide an additional pathway with a lower energy barrier for Li diffusion, which results in an intercalation pseudocapacitive behavior and high-capacity/rate energy storage.展开更多
The high temperature mechanical properties(250 ℃) and microstructure of a die-forged Al-5.87 Zn-2.07 Mg-2.42 Cu alloy after T6 heat treatment were investigated. High temperature tensile tests show that as the tempera...The high temperature mechanical properties(250 ℃) and microstructure of a die-forged Al-5.87 Zn-2.07 Mg-2.42 Cu alloy after T6 heat treatment were investigated. High temperature tensile tests show that as the temperature increases from room temperature to 250 ℃, the ultimate tensile strength of the alloy decreases from 638 to 304 MPa, and the elongation rises from 13.6% to 20.4%. Transmission electron microscopy(TEM) and electron backscattered diffraction(EBSD) were applied for microstructure characterization, which indicates that the increase of tensile temperature can lead to the coarsening of precipitates, drop of dislocation density, and increase of dynamic recovery. After tensile testing at 250 ℃, a sub-grain structure composed of a high fraction of small-angle grain boundary is formed.展开更多
Extensive efforts have been devoted to the design of micro-, nano-, and/or molecular structures of sulfur hosts to address the challenges of lithium–sulfur(Li–S) batteries, yet comparatively little research has been...Extensive efforts have been devoted to the design of micro-, nano-, and/or molecular structures of sulfur hosts to address the challenges of lithium–sulfur(Li–S) batteries, yet comparatively little research has been carried out on the binders in Li–S batteries. Herein, we systematically review the polymer composite frameworks that confine the sulfur within the sulfur electrode, taking the roles of sulfur hosts and functions of binders into consideration. In particular, we investigate the binding mechanism between the binder and sulfur host(such as mechanical interlocking and interfacial interactions), the chemical interactions between the polymer binder and sulfur(such as covalent bonding, electrostatic bonding, etc.), as well as the beneficial functions that polymer binders can impart on Li–S cathodes, such as conductive binders, electrolyte intake, adhesion strength etc. This work could provide a more comprehensive strategy in designing sulfur electrodes for long-life, large-capacity and high-rate Li–S battery.展开更多
Low cost and green fabrication of high-performance electrocatalysts with earth-abundant resources for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are crucial for the large-scale application of rech...Low cost and green fabrication of high-performance electrocatalysts with earth-abundant resources for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are crucial for the large-scale application of rechargeable Zn-air batteries(ZABs).In this work,our density functional theory calculations on the electrocatalyst suggest that the rational construction of interfacial structure can induce local charge redistribution,improve the electronic conductivity and enhance the catalyst stability.In order to realize such a structure,we spatially immobilize heterogeneous CoS/CoO nanocrystals onto N-doped graphene to synthesize a bifunctional electrocatalyst(CoS/CoO@NGNs).The optimization of the composition,interfacial structure and conductivity of the electrocatalyst is conducted to achieve bifunctional catalytic activity and deliver outstanding efficiency and stability for both ORR and OER.The aqueous ZAB with the as-prepared CoS/CoO@NGNs cathode displays a high maximum power density of 137.8 mW cm^−2,a specific capacity of 723.9 mAh g^−1 and excellent cycling stability(continuous operating for 100 h)with a high round-trip efficiency.In addition,the assembled quasi-solid-state ZAB also exhibits outstanding mechanical flexibility besides high battery performances,showing great potential for applications in flexible and wearable electronic devices.展开更多
A non-noble-metal bifunctional catalyst with efficient and durable activity towards both the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER)is crucial to the development of rechargeable Zn-air bat...A non-noble-metal bifunctional catalyst with efficient and durable activity towards both the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER)is crucial to the development of rechargeable Zn-air batteries.Herein,a facile one-step hydrothermal method is reported for the synthesis of a high-performance bifunctional oxygen electrocatalyst,cobalt-doped Mn_(3)O_(4) nanocrystals supported on graphene nanosheets(Co–Mn_(3)O_(4)/G).Compare to pristine Mn_(3)O_(4),this Co–Mn_(3)O_(4)/G exhibits greatly enhanced electrocatalytic activity,delivering a halfwave potential of 0.866 V for the ORR and a low overpotential of 275 mV at 10 mA cm^(-2) for the OER.The zinc-air battery built with Co–Mn_(3)O_(4)/G shows a reduced charge–discharge voltage of 0.91 V at 10 mA cm^(-2),an power density of 115.24 mW cm^(-2) and excellent stability without any degradation after 945 cycles(315 h),outperforming the state-of-the-art Pt/C–Ir/C catalyst-based device.展开更多
Electrolyte engineering is considered as an effective strategy to establish stable solid electrolyte interface(SEI),and thus to suppress the growth of lithium dendrites.In a recent study reported in Advanced Functiona...Electrolyte engineering is considered as an effective strategy to establish stable solid electrolyte interface(SEI),and thus to suppress the growth of lithium dendrites.In a recent study reported in Advanced Functional Materials by Ma group,discovered that strong coordination force could be founded between 15-Crown-5 ether(15-C-5) and Li+,which facilitates the crown ether(15-C-1) to participate in the solvation structure of Li+ in the electrolyte for the same purpose.Such a novel strategy might impact the design of highperformance and safe lithium metal batteries(LMB s).展开更多
Catalytic hydrodeoxygenation(HDO)is one of the most promising strategies to transform oxygen-rich biomass derivatives into high value-added chemicals and fuels,but highly challenging due to the lack of highly efficien...Catalytic hydrodeoxygenation(HDO)is one of the most promising strategies to transform oxygen-rich biomass derivatives into high value-added chemicals and fuels,but highly challenging due to the lack of highly efficient nonprecious metal catalysts.Herein,we report for the first time of a facile synthetic approach to controllably fabricate well-defined Ni-Co alloy NPs confined on the tip of N-CNTs as HDO catalyst.The resultant Ni-Co alloy catalyst possesses outstanding HDO performance towards biomass-derived vanillin into 2-methoxy-4-methylphenol in water with 100%conversion efficiency and selectivity under mild reaction conditions,surpassing the reported high performance nonprecious HDO catalysts.Impressively,our experimental results also unveil that the Ni-Co alloy catalyst can be generically applied to catalyze HDO of vanillin derivatives and other aromatic aldehydes in water with 100%conversion efficiency and over 90%selectivity.Importantly,our DFT calculations and experimental results confirm that the achieved outstanding HDO catalytic performance is due to the greatly promoted selective adsorption and activation of C=O,and desorption of the activated hydrogen species by the synergism of the alloyed Ni-Co NPs.The findings of this work affords a new strategy to design and develop efficient transition metal-based catalysts for HDO reactions in water.展开更多
Porous materials have attracted great attention in energy and environment applications,such as metal organic frameworks(MOFs),metal aerogels,carbon aerogels,porous metal oxides.These materials could be also hybridized...Porous materials have attracted great attention in energy and environment applications,such as metal organic frameworks(MOFs),metal aerogels,carbon aerogels,porous metal oxides.These materials could be also hybridized with other materials into functional composites with superior properties.The high specific area of porous materials offer them the advantage as hosts to conduct catalytic and electrochemical reactions.On one hand,catalytic reactions include photocatalytic,p ho toe lectrocatalytic and electrocatalytic reactions over some gases.On the other hand,they can be used as electrodes in various batteries,such as alkaline metal ion batteries and electrochemical capacitors.So far,both catalysis and batteries are extremely attractive topics.There are also many obstacles to overcome in the exploration of these porous materials.The research related to porous materials for energy and environment applications is at extremely active stage,and this has motivated us to contribute with a roadmap on ’porous materials for energy and environment applications’.展开更多
Solar‐driven thermochemical water splitting represents one efficient route to the generation of H2as a clean and renewable fuel.Due to their outstanding catalytic abilities and promising solar fuel production capacit...Solar‐driven thermochemical water splitting represents one efficient route to the generation of H2as a clean and renewable fuel.Due to their outstanding catalytic abilities and promising solar fuel production capacities,perovskite‐type redox catalysts have attracted significant attention in this regard.In the present study,the perovskite series La1‐xCaxMn1‐yAlyO3(x,y=0.2,0.4,0.6,or0.8)was fabricated using a modified Pechini method and comprehensively investigated to determine the applicability of these materials to solar H2production via two‐step thermochemical water splitting.The thermochemical redox behaviors of these perovskites were optimized by doping at either the A(Ca)or B(Al)sites over a broad range of substitution values,from0.2to0.8.Through this doping,a highly efficient perovskite(La0.6Ca0.4Mn0.6Al0.4O3)was developed,which yielded a remarkable H2production rate of429μmol/g during two‐step thermochemical H2O splitting,going between1400and1000°C.Moreover,the performance of the optimized perovskite was found to be eight times higher than that of the benchmark catalyst CeO2under the same experimental conditions.Furthermore,these perovskites also showed impressive catalytic stability during two‐step thermochemical cycling tests.These newly developed La1‐xCaxMn1‐yAlyO3redox catalysts appear to have great potential for future practical applications in thermochemical solar fuel production.展开更多
Sustainable,conductive,and porous carbon materials are ideal for energy storage materials.In this study,honeycomb-like carbon materials(HCM)are synthesized via a“salty”thermal treatment of abundant and sustainable c...Sustainable,conductive,and porous carbon materials are ideal for energy storage materials.In this study,honeycomb-like carbon materials(HCM)are synthesized via a“salty”thermal treatment of abundant and sustainable coffee extract.Systematic materials characterization indicates that the as-prepared HCM consists of heteroatoms(N and O,etc.)doped ultra-thin carbon framework,possesses remarkable specific surface area,and excellent electrical conductivity.Such properties bestow HCM outstanding materials to be the blocking layer for Li-I2 battery,significantly eliminating the dissolution of I2 in the cathode region and stopping the I2 from shutting to anode compartment.Furthermore,our electrochemical investigation suggests that HCM could incur surface pseudo-capacitive iodine-ions charge storage and contribute additional energy storage capacity.As a result,the resultant Li-I2 battery achieves a robust and highly reversible capacity of 224.5 mAh·g−1 at the rate of 10 C.Even under a high rate of 50 C,the remarkable capacity of the as-prepared Li-I2 battery can still be maintained at 120.2 mAh·g−1 after 4000 cycles.展开更多
Silicon is a promising anode material for rechargeable Li-ion battery (LIB) due to its high energy density and relatively low operating voltage. However, silicon based electrodes suffer from rapid capacity degradation...Silicon is a promising anode material for rechargeable Li-ion battery (LIB) due to its high energy density and relatively low operating voltage. However, silicon based electrodes suffer from rapid capacity degradation during electrochemical cycling. The capacity decay is predominantly caused by (i) cracking due to large volume variations during lithium insertion/extraction and (ii) surface degradation due to excessive solid electrolyte interface (SEI) formation. In this work, we demonstrate that coating of a-Si thin film with a Li-active, nanoporous SiOx layer can result in exceptional electrochemical performance in Li-ion battery. The SiOx layer provides improved cracking resistance to the thin film and prevent the active material loss due to excessive SEI formation, benefiting the electrode cycling stability. Half-cell experiments using this anode material show an initial reversible capacity of 2173 mAh g^-1 with an excellent coulombic efficiency of 90.9%. Furthermore, the electrode shows remarkable capacity retention of ~97% after 100 cycles at C/2 charging rate. The proposed anode architecture is free from Liinactive binders and conductive additives and provides mechanical stability during the charge/discharge process.展开更多
Efficient bifunctional oxygen electrocatalysts for ORR and OER are fundamental to the development of high performance metal-air batteries.Herein,a facile cost-efficient two-step pyrolysis strategy for the fabrication ...Efficient bifunctional oxygen electrocatalysts for ORR and OER are fundamental to the development of high performance metal-air batteries.Herein,a facile cost-efficient two-step pyrolysis strategy for the fabrication of a bifunctional oxygen electrocatalyst has been proposed.The efficient non-preciousmetal-based electrocatalyst,Fe/Fe_(3)C@Fe-N_(x)-C consists of highly curved onion-like carbon shells that encapsulate Fe/Fe_(3)C nanoparticles,distributed on an extensively porous graphitic carbon aerogel.The obtained Fe/Fe_(3)C@Fe-N_(x)-C aerogel exhibited superb electrochemical activity,excellent durability,and high methanol tolerance.The experimental results indicated that the assembly of onion-like carbon shells with encapsulated Fe/Fe_(3)C yielded highly curved carbon surfaces with abundant Fe-Nxactive sites,a porous structure,and enhanced electrocatalytic activity towards ORR and OER,hence displaying promising potential for application as an air cathode in rechargeable Zn-air batteries.The constructed Zn-air battery possessed an exceptional peak power density of~147 mW cm^(-2),outstanding cycling stability(200 cycles,1 h per cycle),and a small voltage gap of 0.87 V.This study offers valuable insights regarding the construction of low-cost and highly active bifunctional oxygen electrocatalysts for efficient air batteries.展开更多
Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air ...Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air batteries and fuel cells.Here,we report a facile molten salt assisted two-step pyrolysis strategy to construct carbon nanosheets matrix with uniformly dispersed Fe_(3) N/Fe nanoparticles and abundant nitrogen-coordinated Fe single atom moieties(Fe@Fe_(SA)-N-C).Thermal exfoliation and etching effect of molten salt contribute to the formation of carbon nanosheets with high porosity,large surface area and abundant uniformly immobilized active sites.Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)image,X-ray absorption fine spectroscopy,and X-ray photoelectron spectroscopy indicate the generation of Fe(mainly Fe_(3) N/Fe)and Fe_(SA)-N-C moieties,which account for the catalytic activity for ORR.Further study on modulating the crystal structure and composition of Fe_(3) N/Fe nanoparticles reveals that proper chemical environment of Fe in Fe_(3) N/Fe notably optimizes the ORR activity.Consequently,the presence of abundant Fe_(SA)-N-C moieties,and potential synergies of Fe_(3) N/Fe nanoparticles and carbon shells,markedly promote the reaction kinetics.The as-developed Fe@Fe_(SA)-N-C-900 electrocatalyst displays superior ORR performance with a half-wave potential(E_(1/2))of 0.83 V versus reversible hydrogen electrode(RHE)and a diffusion limited current density of 5.6 mA cm^(-2).In addition,a rechargeable Zn-air battery device assembled by the Fe@Fe_(SA)-N-C-900 possesses remarkably stable performance with a small voltage gap without obvious voltage loss after500 h of operation.The facile synthesis strategy for the high-performance composites represents another viable avenue to stable and low-cost electrocatalysts for ORR catalysis.展开更多
Silicon(Si)has been investigated as a promising anode material because of its high theoretical capacity(4200 m Ah g^(-1)).However,silicon anode suffers from huge volume changes during repeated charge–discharge cycles...Silicon(Si)has been investigated as a promising anode material because of its high theoretical capacity(4200 m Ah g^(-1)).However,silicon anode suffers from huge volume changes during repeated charge–discharge cycles.In this work,inspired by a remarkable success of the glutinous rice mortar in the Great Wall with ca.2000-year history,amylopectin(AP),the key ingredient responsible for the strong bonding force,is extracted from glutinous rice and utilized as a flexible,aqueous,and resilient binder to address the most challenging drastic volume-expansion and pulverization issues of silicon anode.Additionally,the removal of toxic N-methyl-2-pyrrolidone(NMP)organic solvent makes the electrode fabrication process environmentally friendly and healthy.The as-prepared Si-AP electrode with 60 wt%of Si can uphold a high discharge capacity of 1517.9 m Ah g^(-1)at a rate of 0.1 C after 100 cycles.The cycling stability of the Si-AP has been remarkably improved in comparison with both traditional polyvinylidene fluoride(PVDF)and aqueous carboxymethylcellulose(CMC)binders.Moreover,when the content of silicon in the Si-AP electrode increases to 70 wt%,a high discharge capacity of 1463.1 m Ah g^(-1)can still be obtained after 50 cycles at 0.1°C.These preliminary results suggest that the sustainably available and environmentally benign amylopectin binders could be a promising choice for the construction of highly stable silicon anodes.展开更多
基金supported by the Australian Research Council(ARC)Discovery Projects(DP210103266 and DP1701048343)the Griffith University Ph.D.Scholarships.
文摘Solid polymer electrolytes(SPEs)have become increasingly attractive in solid-state lithium-ion batteries(SSLIBs)in recent years because of their inherent properties of flexibility,processability,and interfacial compatibility.However,the commercialization of SPEs remains challenging for flexible and high-energy-density LIBs.The incorporation of functional additives into SPEs could significantly improve the electrochemical and mechanical properties of SPEs and has created some historical milestones in boosting the development of SPEs.In this study,we review the roles of additives in SPEs,highlighting the working mechanisms and functionalities of the additives.The additives could afford significant advantages in boosting ionic conductivity,increasing ion transference number,improving high-voltage stability,enhancing mechanical strength,inhibiting lithium dendrite,and reducing flammability.Moreover,the application of functional additives in high-voltage cathodes,lithium-sulfur batteries,and flexible lithiumion batteries is summarized.Finally,future research perspectives are proposed to overcome the unresolved technical hurdles and critical issues in additives of SPEs,such as facile fabrication process,interfacial compatibility,investigation of the working mechanism,and special functionalities.
基金the Australia Research Council Discovery Projects(DP160102627 and DP1701048343)of AustraliaShenzhen Peacock Plan of China(KQTD2016112915051055)the 111 Project(D20015)of China Three Gorges University.
文摘Carbon nitrides(including CN,C2N,C3N,C3N4,C4N,and C5N)are a unique family of nitrogen-rich carbon materials with multiple beneficial properties in crystalline structures,morphologies,and electronic configurations.In this review,we provide a comprehensive review on these materials properties,theoretical advantages,the synthesis and modification strategies of different carbon nitride-based materials(CNBMs)and their application in existing and emerging rechargeable battery systems,such as lithium-ion batteries,sodium and potassium-ion batteries,lithium sulfur batteries,lithium oxygen batteries,lithium metal batteries,zinc-ion batteries,and solid-state batteries.The central theme of this review is to apply the theoretical and computational design to guide the experimental synthesis of CNBMs for energy storage,i.e.,facilitate the application of first-principle studies and density functional theory for electrode material design,synthesis,and characterization of different CNBMs for the aforementioned rechargeable batteries.At last,we conclude with the challenges,and prospects of CNBMs,and propose future perspectives and strategies for further advancement of CNBMs for rechargeable batteries.
文摘The authors regret that the wrong image of Fig.1 was uploaded in the paper.The correct one should be:We confirm the discrepancy is restricted to the image of Fig.1 only,the underlying data is correct and unchanged.The authors would like to apologise for any inconvenience caused.
基金This work was financially supported by the Australian Research Council(ARC)Discovery Projects(DP210103266 and DPI 701048343)the Griffith University Ph.D.Scholarships.
文摘Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large volume change and active material loss in lithium-ion batteries during prolonged cycles. Herein, a hydrophilic polymer poly(methyl vinyl ether-alt-maleic acid) (PMVEMA) was explored as a dual-functional aqueous binder for the preparation of high-performance silicon anode and sulfur cathode. Benefiting from the dual functions of PMVEMA, i.e., the excellent dispersion ability and strong binding forces, the as-prepared electrodes exhibit improved capacity, rate capability and long-term cycling performance. In particular, the as-prepared Si electrode delivers a high initial discharge capacity of 1346.5 mAh g^(−1) at a high rate of 8.4 A/g and maintains 834.5 mAh g^(−1) after 300 cycles at 4.2 A/g, while the as-prepared S cathode exhibits enhanced cycling performance with high remaining discharge capacities of 663.4 mAh g^(−1) after 100 cycles at 0.2 C and 487.07 mAh g^(−1) after 300 cycles at 1 C, respectively. These encouraging results suggest that PMVEMA could be a universal binder to facilitate the green manufacture of both anode and cathode for high-capacity energy storage systems.
文摘Bimetallic nanostructures have attracted great interest as efficient catalyst to enhance activity,selectivity and stability in catalytical conversion.Herein,we report a facile one‐pot carbothermal route to in‐situ controllable synthesize heterogeneous bimetallic Ni3Fe NPs@C nanocatalyst.The X‐ray diffraction,transmission electron microscopy,X‐ray photoelectron spectroscopy and N2 adsorption‐description results reveal that the Ni3Fe alloy nanoparticles are evenly embedded in carbon matrix.The as‐prepared Ni3Fe NPs@C catalyst shows excellent selective hydrogenation catalytic performance toward the conversion of levulinic acid(LA)toγ‐valerolactone(GVL)via both direct hydrogenation(DH)and transfer hydrogenation(TH).In DH of LA,the bimetallic catalyst achieved a 93.8%LA conversion efficiency with a 95.5%GVL selectivity and 38.2 mmol g–1 h–1 GVL productivity(under 130°C,2MPa H2 within 2 h),which are 6 and 40 times in comparison with monometallic Ni NPs@C and Fe NPs@C catalysts,respectively.In addition,the identical catalyst displayed a full conversion of LA with almost 100%GVL selectivity and 167.1 mmol g–1 h–1 GVL productivity at 180°C within 0.5 h in TH of LA.Under optimal reaction conditions,the DH and TH catalytic performance of 500‐Ni3Fe NPs@C(3:1)catalyst for converting LA to GVL is comparable to the state‐of‐the‐art noble‐based catalysts.The demonstrated capability of bimetallic catalyst design approach to introduce dual‐catalytic functionality for DH and TH reactions could be adoptable for other catalysis processes.
基金financial support from the Australia Research Council Discovery Projects(DP210103266)of Australiasupported by computational resources provided by the Australian Government through the National Computational Infrastructure(NCI)under the National Computational Merit Allocation Scheme and the Pawsey Supercomputing Centre with funding from the Australian Government and the Government of Western Australia。
文摘Aqueous zinc-ion batteries(AZIBs)can be one of the most promising electrochemical energy storage devices for being non-flammable,low-cost,and sustainable.However,the challenges of AZIBs,including dendrite growth,hydrogen evolution,corrosion,and passivation of zinc anode during charging and discharging processes,must be overcome to achieve high cycling performance and stability in practical applications.In this work,we utilize a dual-func-tional organic additive cyclohexanedodecol(CHD)to firstly establish[Zn(H2O)5(CHD)]2+complex ion in an aqueous Zn electrolyte and secondly build a robust protection layer on the Zn surface to overcome these dilemmas.Systematic experiments and theoretical calculations are carried out to interpret the working mechanism of CHD.At a very low concentration of 0.1 mg mL^(−1) CHD,long-term reversible Zn plating/stripping could be achieved up to 2200 h at 2 mA cm^(−2),1000 h at 5 mA cm^(−2),and 650 h at 10 mA cm^(−2) at the fixed capacity of 1 mAh cm^(−2).When matched with V_(2)O_(5) cathode,the resultant AZIBs full cell with the CHD-modified electrolyte presents a high capacity of 175 mAh g^(−1) with the capacity retention of 92%after 2000 cycles under 2 A g^(−1).Such a performance could enable the commercialization of AZIBs for applications in grid energy storage and industrial energy storage.
基金This work was financially supported by the Australian Research Council(ARC)Discovery Projects(DP210103266,DP200100965 and DP200100365)the ARC Discovery Early Career Researcher Award(DE210101102)the Griffith University Postdoctoral Fellowship Scheme(YUDOU 036 Research Internal).
文摘It is challenging to create cation vacancies in electrode materials for enhancing the performance of rechargeable lithium ion batteries (LIBs). Herein, we utilized a strong alkaline etching method to successfully create Co vacancies at the interface of atomically thin Co_(3−x)O_(4)/graphene@CNT heterostructure for high-energy/power lithium storage. The creation of Co-vacancies in the sample was confirmed by high-resolution scanning transmission electron microscope (HRSTEM), X-ray photoelectron spectroscopy (XPS) and electron energy loss near-edge structures (ELNES). The obtained Co_(3−x)O_(4)/graphene@CNT delivers an ultra-high capacity of 1688.2 mAh g^(−1) at 0.2 C, excellent rate capability of 83.7% capacity retention at 1 C, and an ultralong life up to 1500 cycles with a reversible capacity of 1066.3 mAh g^(−1). Reaction kinetic study suggests a significant contribution from pseudocapacitive storage induced by the Co-vacancies at the Co_(3−x)O_(4)/graphene@CNT interface. Density functional theory confirms that the Co-vacancies could dramatically enhance the Li adsorption and provide an additional pathway with a lower energy barrier for Li diffusion, which results in an intercalation pseudocapacitive behavior and high-capacity/rate energy storage.
基金Project(220636)supported by the Postdoctoral Science Foundation of the Central South University,ChinaProject(2016B090931004)supported by the Guangdong Province Science and Research Plan,ChinaProject(51601229)supported by the National Natural Science Foundation of China。
文摘The high temperature mechanical properties(250 ℃) and microstructure of a die-forged Al-5.87 Zn-2.07 Mg-2.42 Cu alloy after T6 heat treatment were investigated. High temperature tensile tests show that as the temperature increases from room temperature to 250 ℃, the ultimate tensile strength of the alloy decreases from 638 to 304 MPa, and the elongation rises from 13.6% to 20.4%. Transmission electron microscopy(TEM) and electron backscattered diffraction(EBSD) were applied for microstructure characterization, which indicates that the increase of tensile temperature can lead to the coarsening of precipitates, drop of dislocation density, and increase of dynamic recovery. After tensile testing at 250 ℃, a sub-grain structure composed of a high fraction of small-angle grain boundary is formed.
基金supported by the Australian Research Council Future FellowshipDiscovery Projects and Griffith University Ph.D. Scholarships
文摘Extensive efforts have been devoted to the design of micro-, nano-, and/or molecular structures of sulfur hosts to address the challenges of lithium–sulfur(Li–S) batteries, yet comparatively little research has been carried out on the binders in Li–S batteries. Herein, we systematically review the polymer composite frameworks that confine the sulfur within the sulfur electrode, taking the roles of sulfur hosts and functions of binders into consideration. In particular, we investigate the binding mechanism between the binder and sulfur host(such as mechanical interlocking and interfacial interactions), the chemical interactions between the polymer binder and sulfur(such as covalent bonding, electrostatic bonding, etc.), as well as the beneficial functions that polymer binders can impart on Li–S cathodes, such as conductive binders, electrolyte intake, adhesion strength etc. This work could provide a more comprehensive strategy in designing sulfur electrodes for long-life, large-capacity and high-rate Li–S battery.
基金the National Natural Science Foundation of China(Grant Numbers 21506081)the Provincial Natural Science Foundation of Jiangsu(Grant Numbers BK20191430)+2 种基金Six Talent Peaks Project of Jiangsu Province[Grant Numbers XNY-009]High-tech research key laboratory of Zhenjiang(Grant Numbers SS2018002)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions and the Research Foundation of Jiangsu University(Grant Numbers 17JDG007).
文摘Low cost and green fabrication of high-performance electrocatalysts with earth-abundant resources for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are crucial for the large-scale application of rechargeable Zn-air batteries(ZABs).In this work,our density functional theory calculations on the electrocatalyst suggest that the rational construction of interfacial structure can induce local charge redistribution,improve the electronic conductivity and enhance the catalyst stability.In order to realize such a structure,we spatially immobilize heterogeneous CoS/CoO nanocrystals onto N-doped graphene to synthesize a bifunctional electrocatalyst(CoS/CoO@NGNs).The optimization of the composition,interfacial structure and conductivity of the electrocatalyst is conducted to achieve bifunctional catalytic activity and deliver outstanding efficiency and stability for both ORR and OER.The aqueous ZAB with the as-prepared CoS/CoO@NGNs cathode displays a high maximum power density of 137.8 mW cm^−2,a specific capacity of 723.9 mAh g^−1 and excellent cycling stability(continuous operating for 100 h)with a high round-trip efficiency.In addition,the assembled quasi-solid-state ZAB also exhibits outstanding mechanical flexibility besides high battery performances,showing great potential for applications in flexible and wearable electronic devices.
基金financially supported by the Australian Research Council(ARC)Discovery Project and Griffith University Postdoctoral Fellowship.
文摘A non-noble-metal bifunctional catalyst with efficient and durable activity towards both the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER)is crucial to the development of rechargeable Zn-air batteries.Herein,a facile one-step hydrothermal method is reported for the synthesis of a high-performance bifunctional oxygen electrocatalyst,cobalt-doped Mn_(3)O_(4) nanocrystals supported on graphene nanosheets(Co–Mn_(3)O_(4)/G).Compare to pristine Mn_(3)O_(4),this Co–Mn_(3)O_(4)/G exhibits greatly enhanced electrocatalytic activity,delivering a halfwave potential of 0.866 V for the ORR and a low overpotential of 275 mV at 10 mA cm^(-2) for the OER.The zinc-air battery built with Co–Mn_(3)O_(4)/G shows a reduced charge–discharge voltage of 0.91 V at 10 mA cm^(-2),an power density of 115.24 mW cm^(-2) and excellent stability without any degradation after 945 cycles(315 h),outperforming the state-of-the-art Pt/C–Ir/C catalyst-based device.
文摘Electrolyte engineering is considered as an effective strategy to establish stable solid electrolyte interface(SEI),and thus to suppress the growth of lithium dendrites.In a recent study reported in Advanced Functional Materials by Ma group,discovered that strong coordination force could be founded between 15-Crown-5 ether(15-C-5) and Li+,which facilitates the crown ether(15-C-1) to participate in the solvation structure of Li+ in the electrolyte for the same purpose.Such a novel strategy might impact the design of highperformance and safe lithium metal batteries(LMB s).
文摘Catalytic hydrodeoxygenation(HDO)is one of the most promising strategies to transform oxygen-rich biomass derivatives into high value-added chemicals and fuels,but highly challenging due to the lack of highly efficient nonprecious metal catalysts.Herein,we report for the first time of a facile synthetic approach to controllably fabricate well-defined Ni-Co alloy NPs confined on the tip of N-CNTs as HDO catalyst.The resultant Ni-Co alloy catalyst possesses outstanding HDO performance towards biomass-derived vanillin into 2-methoxy-4-methylphenol in water with 100%conversion efficiency and selectivity under mild reaction conditions,surpassing the reported high performance nonprecious HDO catalysts.Impressively,our experimental results also unveil that the Ni-Co alloy catalyst can be generically applied to catalyze HDO of vanillin derivatives and other aromatic aldehydes in water with 100%conversion efficiency and over 90%selectivity.Importantly,our DFT calculations and experimental results confirm that the achieved outstanding HDO catalytic performance is due to the greatly promoted selective adsorption and activation of C=O,and desorption of the activated hydrogen species by the synergism of the alloyed Ni-Co NPs.The findings of this work affords a new strategy to design and develop efficient transition metal-based catalysts for HDO reactions in water.
基金financially support by an Australian Research Council (ARC) Discovery Project (No. DP200100965)a Griffith University Postdoctoral Fellowship
文摘Porous materials have attracted great attention in energy and environment applications,such as metal organic frameworks(MOFs),metal aerogels,carbon aerogels,porous metal oxides.These materials could be also hybridized with other materials into functional composites with superior properties.The high specific area of porous materials offer them the advantage as hosts to conduct catalytic and electrochemical reactions.On one hand,catalytic reactions include photocatalytic,p ho toe lectrocatalytic and electrocatalytic reactions over some gases.On the other hand,they can be used as electrodes in various batteries,such as alkaline metal ion batteries and electrochemical capacitors.So far,both catalysis and batteries are extremely attractive topics.There are also many obstacles to overcome in the exploration of these porous materials.The research related to porous materials for energy and environment applications is at extremely active stage,and this has motivated us to contribute with a roadmap on ’porous materials for energy and environment applications’.
基金supported by the Australian Research Council(FT120100913)the National Natural Science Foundation of China(51372248,51432009)~~
文摘Solar‐driven thermochemical water splitting represents one efficient route to the generation of H2as a clean and renewable fuel.Due to their outstanding catalytic abilities and promising solar fuel production capacities,perovskite‐type redox catalysts have attracted significant attention in this regard.In the present study,the perovskite series La1‐xCaxMn1‐yAlyO3(x,y=0.2,0.4,0.6,or0.8)was fabricated using a modified Pechini method and comprehensively investigated to determine the applicability of these materials to solar H2production via two‐step thermochemical water splitting.The thermochemical redox behaviors of these perovskites were optimized by doping at either the A(Ca)or B(Al)sites over a broad range of substitution values,from0.2to0.8.Through this doping,a highly efficient perovskite(La0.6Ca0.4Mn0.6Al0.4O3)was developed,which yielded a remarkable H2production rate of429μmol/g during two‐step thermochemical H2O splitting,going between1400and1000°C.Moreover,the performance of the optimized perovskite was found to be eight times higher than that of the benchmark catalyst CeO2under the same experimental conditions.Furthermore,these perovskites also showed impressive catalytic stability during two‐step thermochemical cycling tests.These newly developed La1‐xCaxMn1‐yAlyO3redox catalysts appear to have great potential for future practical applications in thermochemical solar fuel production.
基金This study was financially supported by the Australia Research Council Discovery Projects(DP170103721 andDP180102003)We also acknowledge the computational support from the Australian Government through the National Computational Infrastructure(NCI)under the National Computational Merit Allocation Scheme and the Pawsey Supercomputing Centre with funding from the Australian Government and the Government of Western Australia.
文摘Sustainable,conductive,and porous carbon materials are ideal for energy storage materials.In this study,honeycomb-like carbon materials(HCM)are synthesized via a“salty”thermal treatment of abundant and sustainable coffee extract.Systematic materials characterization indicates that the as-prepared HCM consists of heteroatoms(N and O,etc.)doped ultra-thin carbon framework,possesses remarkable specific surface area,and excellent electrical conductivity.Such properties bestow HCM outstanding materials to be the blocking layer for Li-I2 battery,significantly eliminating the dissolution of I2 in the cathode region and stopping the I2 from shutting to anode compartment.Furthermore,our electrochemical investigation suggests that HCM could incur surface pseudo-capacitive iodine-ions charge storage and contribute additional energy storage capacity.As a result,the resultant Li-I2 battery achieves a robust and highly reversible capacity of 224.5 mAh·g−1 at the rate of 10 C.Even under a high rate of 50 C,the remarkable capacity of the as-prepared Li-I2 battery can still be maintained at 120.2 mAh·g−1 after 4000 cycles.
基金financial support from ARC Discovery Projects (DP150101717 and DP180102003)
文摘Silicon is a promising anode material for rechargeable Li-ion battery (LIB) due to its high energy density and relatively low operating voltage. However, silicon based electrodes suffer from rapid capacity degradation during electrochemical cycling. The capacity decay is predominantly caused by (i) cracking due to large volume variations during lithium insertion/extraction and (ii) surface degradation due to excessive solid electrolyte interface (SEI) formation. In this work, we demonstrate that coating of a-Si thin film with a Li-active, nanoporous SiOx layer can result in exceptional electrochemical performance in Li-ion battery. The SiOx layer provides improved cracking resistance to the thin film and prevent the active material loss due to excessive SEI formation, benefiting the electrode cycling stability. Half-cell experiments using this anode material show an initial reversible capacity of 2173 mAh g^-1 with an excellent coulombic efficiency of 90.9%. Furthermore, the electrode shows remarkable capacity retention of ~97% after 100 cycles at C/2 charging rate. The proposed anode architecture is free from Liinactive binders and conductive additives and provides mechanical stability during the charge/discharge process.
基金supported financially by the National Natural Science Foundation of China,China(Grant No.51702180,51572136,91963113,21703116,51372127,51873096)The Scientific and Technical Development Project of Qingdao,China(Grant No.18-2-2-52-jch)+1 种基金The Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and TechnologyThe Natural Science Foundation of Hebei Province(B2019204009)。
文摘Efficient bifunctional oxygen electrocatalysts for ORR and OER are fundamental to the development of high performance metal-air batteries.Herein,a facile cost-efficient two-step pyrolysis strategy for the fabrication of a bifunctional oxygen electrocatalyst has been proposed.The efficient non-preciousmetal-based electrocatalyst,Fe/Fe_(3)C@Fe-N_(x)-C consists of highly curved onion-like carbon shells that encapsulate Fe/Fe_(3)C nanoparticles,distributed on an extensively porous graphitic carbon aerogel.The obtained Fe/Fe_(3)C@Fe-N_(x)-C aerogel exhibited superb electrochemical activity,excellent durability,and high methanol tolerance.The experimental results indicated that the assembly of onion-like carbon shells with encapsulated Fe/Fe_(3)C yielded highly curved carbon surfaces with abundant Fe-Nxactive sites,a porous structure,and enhanced electrocatalytic activity towards ORR and OER,hence displaying promising potential for application as an air cathode in rechargeable Zn-air batteries.The constructed Zn-air battery possessed an exceptional peak power density of~147 mW cm^(-2),outstanding cycling stability(200 cycles,1 h per cycle),and a small voltage gap of 0.87 V.This study offers valuable insights regarding the construction of low-cost and highly active bifunctional oxygen electrocatalysts for efficient air batteries.
基金supported financially by the National Natural Science Foundation of China,China(Grant No.51702180,51772162)the Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and Technologythe Scientific and Technical Development Project of Qingdao,China(Grant No.18-2-2-52-jch)。
文摘Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air batteries and fuel cells.Here,we report a facile molten salt assisted two-step pyrolysis strategy to construct carbon nanosheets matrix with uniformly dispersed Fe_(3) N/Fe nanoparticles and abundant nitrogen-coordinated Fe single atom moieties(Fe@Fe_(SA)-N-C).Thermal exfoliation and etching effect of molten salt contribute to the formation of carbon nanosheets with high porosity,large surface area and abundant uniformly immobilized active sites.Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)image,X-ray absorption fine spectroscopy,and X-ray photoelectron spectroscopy indicate the generation of Fe(mainly Fe_(3) N/Fe)and Fe_(SA)-N-C moieties,which account for the catalytic activity for ORR.Further study on modulating the crystal structure and composition of Fe_(3) N/Fe nanoparticles reveals that proper chemical environment of Fe in Fe_(3) N/Fe notably optimizes the ORR activity.Consequently,the presence of abundant Fe_(SA)-N-C moieties,and potential synergies of Fe_(3) N/Fe nanoparticles and carbon shells,markedly promote the reaction kinetics.The as-developed Fe@Fe_(SA)-N-C-900 electrocatalyst displays superior ORR performance with a half-wave potential(E_(1/2))of 0.83 V versus reversible hydrogen electrode(RHE)and a diffusion limited current density of 5.6 mA cm^(-2).In addition,a rechargeable Zn-air battery device assembled by the Fe@Fe_(SA)-N-C-900 possesses remarkably stable performance with a small voltage gap without obvious voltage loss after500 h of operation.The facile synthesis strategy for the high-performance composites represents another viable avenue to stable and low-cost electrocatalysts for ORR catalysis.
基金financial support from the Australia Research Council Discovery Projects(DP160102627 and DP1701048343)of Australiathe 111 Project(D20015)of China Three Gorges University
文摘Silicon(Si)has been investigated as a promising anode material because of its high theoretical capacity(4200 m Ah g^(-1)).However,silicon anode suffers from huge volume changes during repeated charge–discharge cycles.In this work,inspired by a remarkable success of the glutinous rice mortar in the Great Wall with ca.2000-year history,amylopectin(AP),the key ingredient responsible for the strong bonding force,is extracted from glutinous rice and utilized as a flexible,aqueous,and resilient binder to address the most challenging drastic volume-expansion and pulverization issues of silicon anode.Additionally,the removal of toxic N-methyl-2-pyrrolidone(NMP)organic solvent makes the electrode fabrication process environmentally friendly and healthy.The as-prepared Si-AP electrode with 60 wt%of Si can uphold a high discharge capacity of 1517.9 m Ah g^(-1)at a rate of 0.1 C after 100 cycles.The cycling stability of the Si-AP has been remarkably improved in comparison with both traditional polyvinylidene fluoride(PVDF)and aqueous carboxymethylcellulose(CMC)binders.Moreover,when the content of silicon in the Si-AP electrode increases to 70 wt%,a high discharge capacity of 1463.1 m Ah g^(-1)can still be obtained after 50 cycles at 0.1°C.These preliminary results suggest that the sustainably available and environmentally benign amylopectin binders could be a promising choice for the construction of highly stable silicon anodes.