Metal-air batteries face a great challenge in developing efficient and durable low-cost oxygen reduction reaction(ORR)electrocatalysts.Single-atom iron catalysts embedded into nitrogen doped carbon(Fe-N-C)have emerged...Metal-air batteries face a great challenge in developing efficient and durable low-cost oxygen reduction reaction(ORR)electrocatalysts.Single-atom iron catalysts embedded into nitrogen doped carbon(Fe-N-C)have emerged as attractive materials for potential replacement of Pt in ORR,but their catalytic performance was limited by the symmetrical electronic structure distribution around the single-atom Fe site.Here,we report our findings in significantly enhancing the ORR performance of Fe-N-C by moderate Fe_(2)O_(3) integration via the strong electronic interaction.Remarkably,the optimized catalyst(M-Fe_(2)O_(3)/Fe_(SA)@NC)exhibits excellent activity,durability and good tolerance to methanol,outperforming the benchmark Pt/C catalyst.When M-Fe_(2)O_(3)/Fe_(SA)@NC catalyst was used in a practical zinc-air battery assembly,peak power density of 155 mW cm^(-2)and specific capacity of 762 mA h g_(Zn)^(-1)were achieved and the battery assembly has shown superior cycling stability over a period of 200 h.More importantly,theoretical studies suggest that the introduction of Fe_(2)O_(3) can evoke the crystal field alteration and electron redistribution on single Fe atoms,which can break the symmetric charge distribution of Fe-N_(4) and thereby optimize the corresponding adsorption energy of intermediates to promote the O_(2)reduction.This study provides a new pathway to promote the catalytic performance of single-atom catalysts.展开更多
The development of bi-functional electrocatalyst with high catalytic activity and stable performance for both oxygen evolution/reduction reactions(OER/ORR)in aqueous alkaline solution is key to realize practical appli...The development of bi-functional electrocatalyst with high catalytic activity and stable performance for both oxygen evolution/reduction reactions(OER/ORR)in aqueous alkaline solution is key to realize practical application of zinc-air batteries(ZABs).In this study,we reported a new porous nano-micro-composite as a bifunctional electrocatalyst for ZABs,devised by the in situ growth of metal-organic framework(MOF)nanocrystals onto the micrometersized Ba0.5Sr0.5Co0.8Fe0.2O3(BSCF)perovskite oxide.Upon carbonization,MOF was converted to porous nitrogen-doped carbon nanocages and ultrafine cobalt oxides and CoN4 nanoparticles dispersing inside the carbon nanocages,which further anchored on the surface of BSCF oxide.We homogeneously dispersed BSCF perovskite particles in the surfactant;subsequently,ZIF-67 nanocrystals were grown onto the BSCF particles.In this way,leaching of metallic or organic species in MOFs and the aggregation of BSCF were effectively suppressed,thus maximizing the number of active sites for improving OER.The BSCF in turn acted as catalyst to promote the graphitization of carbon during pyrolysis,as well as to optimize the transition metal-tocarbon ratio,thus enhancing the ORR catalytic activity.A ZAB fabricated from such air electrode showed outstanding performance with a potential gap of only 0.83 V at 5 mA cm-2 for OER/ORR.Notably,no obvious performance degradation was observed for the continuous charge-discharge operation for 1800 cycles over an extended period of 300 h.展开更多
Supercapacitors(SCs)are emerging as efficient energy storage devices but still suffering from limited energy density compared with batteries.Electrolytes have been regarded as the key to determine the energy storage p...Supercapacitors(SCs)are emerging as efficient energy storage devices but still suffering from limited energy density compared with batteries.Electrolytes have been regarded as the key to determine the energy storage performance of SCs.However,none of the conventional electrolytes can fully meet the increasing requirements of SCs in terms of high ion conductivity,excellent stability,wide voltage window and operating temperature range,as well as environmentally friend concerns.To this end,hybrid electrolytes have sprung up in recent years,which are believed to be the candidate to solve these shortcomings.Herein,the state-of-the-art types of hybrid electrolytes for SCs,including the combination of aqueous and organic,aqueous and gel polymer,ionic liquids(ILs)and organic,and ILs and gel polymer hybrid electrolytes,are reviewed.The effects of different hybrid systems on the performance of SCs and the underlying mechanisms are among the focal points of the review,and prospects and possible directions are discussed as well to provide further insight into the future development of this field.展开更多
The study of atomically dispersed metal-nitrogen electrocatalysts is still limited in terms of understanding their catalytic mechanism because of the inability to precisely regulate the coordination number and type of...The study of atomically dispersed metal-nitrogen electrocatalysts is still limited in terms of understanding their catalytic mechanism because of the inability to precisely regulate the coordination number and type of N in combination with the metal elements.Inspired by the high catalytic activity and selectivity of natural enzymes,herein,we have designed and fabricated ultrathin carbon nanosheet-supported Mn single-atom catalysts(SACs)with a precise pyrrole-type Mn-N4(PT-MnN4)configuration using a bio-mimicking strategy.The PT-MnN4 SACs display outstanding oxygen reduction reaction(ORR)activity,with a half-wave potential(E_(1/2))of 0.88 V(vs.revisible hydrogen electrode[RHE])and extremely high stability in alkaline media.Moreover,superior ORR activities are also obtained,E_(1/2) of 0.73 V and 0.63 V in acid and neutral electrolytes,respectively,indicating the efficient pH-universal ORR performances.The assembled zinc-air battery using the PT-MnN4 SACs as air cathodes exhibits a high peak power density(175 mW cm^(−2))and long-term stability up to 150 h,implying its promising application in metal-air batteries.This study has paved the way toward the rational design and precise regulation of single-atom electrocatalysts.展开更多
With a rising energy demand and anabatic environmental crisis arising from the fast growth in human population and society economics,numerous efforts have been devoted to explore and design plentiful multifunctional m...With a rising energy demand and anabatic environmental crisis arising from the fast growth in human population and society economics,numerous efforts have been devoted to explore and design plentiful multifunctional materials for meeting highefficiency energy transfer processes,which happen in various developed energy conversion and storage systems.As a special kind of multi-metal oxides,perovskite with attractive physical and chemical properties,is becoming a rapidly rising star on the horizon of high-performance catalytic materials with substantial research behaviors worldwide.The porous nanostructure in targeted catalysts is favorable to the catalytic activity and thus improves the overall efficiency of these energy-related installations.In this review paper,recent advances made in the porous perovskite nanostructures for catalyzing several anodic or cathodic reactions in fuel cells and metal-air batteries are comprehensively summarized.Plenty of general preparation methods employed to attain porous perovskite-type oxides are provided,followed by a further discussion about the influence of various strategies on structures and catalytic properties of the porous perovskites.Furthermore,deep insights gathered in the future development of porous perovskite-based materials for energy conversion and storage technologies are also provided.展开更多
The rapid development of power generation from renewable energy,such as geothermal,wind,and tidal energy,arises the need for efficient and economic electrochemical energy storage systems for integrating electric power...The rapid development of power generation from renewable energy,such as geothermal,wind,and tidal energy,arises the need for efficient and economic electrochemical energy storage systems for integrating electric power smoothly into power grids.The lithium-ion battery has been successfully utilized for a variety of portable electronic devices but its application in large-scale energy storage has raised concerns about safety,availability of lithium resources,and its increasing price.Alternatively,sodium-ion battery(SIB)has been in acquisition predominantly,because of the abundant sodium resources over the earth’s crust at low cost.Developing high energy density electrode materials is one of the most intensive research topics.Oxides have been extensively investigated as the cathode and anode materials for high-performance and durable SIBs,owing to their various advantages including facile synthesis,versatile compositions,and easy structural tuning.In this review,we provide an in-time thorough summary of recent advances in oxide materials for cathodes and anodes for high energy density SIBs.The energy storage mechanism,challenges,categories,and optimizations of both electrodes are discussed.Existing research gaps and future perspectives are also outlined.This review is expected to accelerate the research for developing new pathways for tuning the properties of the oxide electrodes based on different sodium storage mechanisms.展开更多
Electrochemical nitrogen reduction reaction(ENRR) provides a promising strategy to achieve sustainable synthesis of ammonia. However, despite great efforts devoted to this research field, the problems such as low ener...Electrochemical nitrogen reduction reaction(ENRR) provides a promising strategy to achieve sustainable synthesis of ammonia. However, despite great efforts devoted to this research field, the problems such as low energy efficiency and weak selectivity still impede its practical implementation. Most of the research to date has been concentrated on creating sophisticated electrocatalysts, and adequate knowledge of electrolytes is still lacking. Herein, the recent progress in electrolytes for ENRR, including alkaline, neutral,acidic, water-in-salt, organic, ionic liquid, and mixed water-organic electrolytes, is thoroughly reviewed to obtain an in-depth understanding of their effects on electrocatalytic performance. Recently developed representative electrocatalysts in various types of electrolytes are also introduced, and future research priorities of different electrolytes are proposed to develop new and efficient ENRR systems.展开更多
Solid-state electrolytes(SSEs)are a solution to safety issues related to flammable organic electrolytes for Li batteries.Insufficient contact between the anode and SSE results in high interface resistance,thus causing...Solid-state electrolytes(SSEs)are a solution to safety issues related to flammable organic electrolytes for Li batteries.Insufficient contact between the anode and SSE results in high interface resistance,thus causing the batteries to exhibit high charging and discharging overpotentials.Recently,we reduced the overpotential of Li stripping and plating by introducing a high proportion of dual-conductive phases into a composite anode.The current study investigates the interface resistance and stability of a composite electrode modified with Zn and a lower proportion of dual-conductive phases.Zn-cation-adsorbed Prussian blue is synthesized as an intermediate component for a Zn-modified composite electrode(Li-FeZnNC).The Li-FeZnNC symmetric cell presents a lower interface resistance and overpotential compared with Li-FeNC(without Zn modification)and Li-symmetric cells.The Li-FeZnNC symmetric cell shows high electrochemical stability during Li stripping and plating at different current densities and high stability for 200 h.Full batteries with a Li-FeZnNC composite anode,garnet-type SSE,and LiFePO4 cathode show low charging and discharging overpotentials,a capacity of 152 mAh g−1,and high stability for 200 cycles.展开更多
Despite being widely used in people's daily life,the safety issue of lithium-ion batteries(LIBs)has become the major barrier for them to be applied in electrical vehicles(EVs)or large-scale energy storage.Typicall...Despite being widely used in people's daily life,the safety issue of lithium-ion batteries(LIBs)has become the major barrier for them to be applied in electrical vehicles(EVs)or large-scale energy storage.Typically,due to the use of liquid electrolytes containing flammable solvents which are easily oxidized by excessive and accumulated heat,the potential thermal runaway is a major safety concern for traditional LIBs.A strategy for a safer electrolyte design is controlling the flammability and volatility of the liquid electro-lytes,to effectively prevent thermal runaway,thus avoiding fire or other risks.Through this study,the mechanisms of thermal runa-way and the recent progress in electrolyte engineering toward LIBs were summarized,covering the major strategies including adding flame-retardants,the utilization of ionic liquid electrolytes and solid electrolytes.The characteristics,strengths and weaknesses of different strategies were discussed.New designing directions of safer electrolytes for the LIBs were also provided.展开更多
Supercapacitors(SCs)are rated as the foremost efficient devices bridging the production and consumption of renewable energy.To address the ever-increasing energy requirements,it is indispensable to further develop hig...Supercapacitors(SCs)are rated as the foremost efficient devices bridging the production and consumption of renewable energy.To address the ever-increasing energy requirements,it is indispensable to further develop high-performance SCs with merits of high energy-density,acceptable price and long-term stability.This review highlights the recent advances on halogen-based functionalized chemistry engineering in the state-of-the-art electrode system for high-performance SCs,primarily referring to the doping and decoration strategies of F,Cl,Br and I elements.Due to the discrepancy of electronegativity and atomic radius,the functionalization of each halogen element endows the substrate materials with different physicochemical properties,including energy bandgap structure,porosity distribution and surface affinity.The principle of halogen embedment into host materials by precisely controlling ionic adsorption and electronic structure is presented.And,the vital perspectives on the future challenges of halogen functionalization are also discussed.This work aims to deepen the understanding of halogen-based functionalized strategies to motivate further research for the development of high-performance SCs,and it also provides a prospect for exploring new material modification methods for electrochemical energy storage.展开更多
The pursuit of safer and high-performance lithium-ion batteries(LIBs)has triggered extensive research activities on solid-state batteries,while challenges related to the unstable electrode-elec-trolyte interface hinde...The pursuit of safer and high-performance lithium-ion batteries(LIBs)has triggered extensive research activities on solid-state batteries,while challenges related to the unstable electrode-elec-trolyte interface hinder their practical implementation.Polymer has been used extensively to improve the cathode-electrolyte interface in garnet-based all-solid-state LIBs(ASSLBs),while it introduces new concerns about thermal stability.In this study,we propose the incorporation of a multi-functional flame-retardant triphenyl phos-phate additive into poly(ethylene oxide),acting as a thin buffer layer between LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathode and garnet electro-lyte.Through electrochemical stability tests,cycling performance evaluations,interfacial thermal stability analysis and flammability tests,improved thermal stability(capacity retention of 98.5%after 100 cycles at 60℃,and 89.6%after 50 cycles at 80℃)and safety characteristics(safe and stable cycling up to 100℃)are demonstrated.Based on various materials characterizations,the mechanism for the improved thermal stability of the interface is proposed.The results highlight the potential of multi-functional flame-retardant additives to address the challenges associated with the electrode-electrolyte interface in ASSLBs at high temperature.Efficient thermal modification in ASSLBs operating at elevated temperatures is also essential for enabling large-scale energy storage with safety being the primary concern.展开更多
Supercapacitors(SCs) with high power density and long cycling span life are demanding energy storage devices that will be an attractive power solution to modern electronic and electrical applications. Numerous theoret...Supercapacitors(SCs) with high power density and long cycling span life are demanding energy storage devices that will be an attractive power solution to modern electronic and electrical applications. Numerous theoretical and experimental works have been devoted to exploring various possibilities to increase the functionality and the specific capacitance of electrodes for SCs. Non-carbon two-dimensional(2D)materials have been considered as encouraging electrode candidates for their chemical and physical advantages such as tunable surface chemistry, high electronic conductivity, large mechanical strength, more active sites, and dual non-faradaic and faradaic electrochemical performances. Besides, these 2D materials also play particular roles in constructing highway channels for fast ion diffusion. This concise review summarizes cutting-edge progress of some representative 2D non-carbon materials for the aqueous electrolyte-based SCs, including transition metal oxides(TMOs), transition metal hydroxides(TMHs), transition metal chalcogenides(TMCs), MXenes, metal-organic frameworks(MOFs) and some emerging materials. Different synthetic methods, effective structural designs and corresponding electrochemical performances are reviewed in detail. And we finally present a detailed discussion of the current intractable challenges and technical bottlenecks, and highlight future directions and opportunities for the development of next-generation high-performance energy storage devices.展开更多
过渡金属氧化态调控工程是一种很有前景的改善电极材料的氧化还原活性、增加活性位点的策略.本文提出了一种简单的三乙醇胺辅助自模板法,制备了一种由交错钴硫化物纳米片(Co_(x)S_(y)-T NSs)组装而成的独特的三维蜂窝状网络结构.有趣的...过渡金属氧化态调控工程是一种很有前景的改善电极材料的氧化还原活性、增加活性位点的策略.本文提出了一种简单的三乙醇胺辅助自模板法,制备了一种由交错钴硫化物纳米片(Co_(x)S_(y)-T NSs)组装而成的独特的三维蜂窝状网络结构.有趣的是,我们首次发现在该体系中,三乙醇胺可以有效地增加目标产物中的高价态Co^(3+)的比例.Co_(x)S_(y)-T NSs电极具有高含量的Co^(3+)和三维网络结构,使得其在5 A g^(-1)的电流密度下表现出351 mA h g^(-1)(2635 F g^(-1))的最大比容量和优异的循环稳定性.此外,由Co_(x)S_(y)-T NSs和活性炭(AC)电极组装的固态不对称超级电容器在0.81 kW kg^(-1)功率密度下展现出81.62 W h kg^(-1)的高能量密度和卓越的长周期循环稳定性,7000次循环后仍有96.2%的容量保持率.该结果证明同时调控高价态的金属物种并构筑三维网络结构是一种简单而有效的制备用于能源存储与转换的高活性电极材料的策略.展开更多
The development of low-cost and highly efficient bifunctional electrocatalysts toward oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is of critical importance for clean energy devices such as fuel cel...The development of low-cost and highly efficient bifunctional electrocatalysts toward oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is of critical importance for clean energy devices such as fuel cells and metal-air batteries.Herein,a sophisticated na nostructure composed of CoS,Co and MoC nanoparticles incorporated in N and S dual-doped porous carbon nanofibers(CoS/Co/MoC-N,SPCNFs)as a high-efficiency bifunctional electrocatalyst is designed and synthesized via an efficient multistep strategy.The as-prepared CoS/Co/MoC-N,S-PCNFs exhibit a positive half-wave potential(E1/2)of0.871 V for ORR and a low overpotential of 289 mV at 10 mA/cm^(2) for OER,outperforming the non-noble metal-based catalysts reported.Furthermore,the assembled Zn-air battery based on CoS/Co/MoC-N,SPCNFs delivers an excellent power density(169.1 mW/cm^(2)),a large specific capacity(819.3 mAh/g)and robust durability,demonstrating the great potential of the as-developed bifunctional electrocatalyst in practical applications.This work is expected to inspire the design of advanced bifunctional nonprecious metal-based electrocatalysts for energy storage.展开更多
In some applications,there are signals with piecewise structure to be recovered.In this paper,we propose a piecewise_ISS(P_ISS)method which aims to preserve the piecewise sparse structure(or the small-scaled entries)o...In some applications,there are signals with piecewise structure to be recovered.In this paper,we propose a piecewise_ISS(P_ISS)method which aims to preserve the piecewise sparse structure(or the small-scaled entries)of piecewise signals.In order to avoid selecting redundant false small-scaled elements,we also implement the piecewise_ISS algorithm in parallel and distributed manners equipped with a deletion rule.Numerical experiments indicate that compared with alSS,the P_ISS algorithm is more effective and robust for piecewise sparse recovery.展开更多
基金supported by the Australian Research Council Australian Laureate Fellowship(No.FL200100049)the support of Natural Science Foundation for Young Scholars of Jiangsu Province(No.BK20220879)+1 种基金National Natural Science Foundation for Young Scholars of China(No.22209072)Monash University for a PhD scholarship as part of the university support for establishment of the ARC Research Hub for Energy-efficient Separation(H170100009)。
文摘Metal-air batteries face a great challenge in developing efficient and durable low-cost oxygen reduction reaction(ORR)electrocatalysts.Single-atom iron catalysts embedded into nitrogen doped carbon(Fe-N-C)have emerged as attractive materials for potential replacement of Pt in ORR,but their catalytic performance was limited by the symmetrical electronic structure distribution around the single-atom Fe site.Here,we report our findings in significantly enhancing the ORR performance of Fe-N-C by moderate Fe_(2)O_(3) integration via the strong electronic interaction.Remarkably,the optimized catalyst(M-Fe_(2)O_(3)/Fe_(SA)@NC)exhibits excellent activity,durability and good tolerance to methanol,outperforming the benchmark Pt/C catalyst.When M-Fe_(2)O_(3)/Fe_(SA)@NC catalyst was used in a practical zinc-air battery assembly,peak power density of 155 mW cm^(-2)and specific capacity of 762 mA h g_(Zn)^(-1)were achieved and the battery assembly has shown superior cycling stability over a period of 200 h.More importantly,theoretical studies suggest that the introduction of Fe_(2)O_(3) can evoke the crystal field alteration and electron redistribution on single Fe atoms,which can break the symmetric charge distribution of Fe-N_(4) and thereby optimize the corresponding adsorption energy of intermediates to promote the O_(2)reduction.This study provides a new pathway to promote the catalytic performance of single-atom catalysts.
基金the support provided by the“Australian Government Research Training Program(RTP)Scholarship”at Curtin University,Perth,Australia。
文摘The development of bi-functional electrocatalyst with high catalytic activity and stable performance for both oxygen evolution/reduction reactions(OER/ORR)in aqueous alkaline solution is key to realize practical application of zinc-air batteries(ZABs).In this study,we reported a new porous nano-micro-composite as a bifunctional electrocatalyst for ZABs,devised by the in situ growth of metal-organic framework(MOF)nanocrystals onto the micrometersized Ba0.5Sr0.5Co0.8Fe0.2O3(BSCF)perovskite oxide.Upon carbonization,MOF was converted to porous nitrogen-doped carbon nanocages and ultrafine cobalt oxides and CoN4 nanoparticles dispersing inside the carbon nanocages,which further anchored on the surface of BSCF oxide.We homogeneously dispersed BSCF perovskite particles in the surfactant;subsequently,ZIF-67 nanocrystals were grown onto the BSCF particles.In this way,leaching of metallic or organic species in MOFs and the aggregation of BSCF were effectively suppressed,thus maximizing the number of active sites for improving OER.The BSCF in turn acted as catalyst to promote the graphitization of carbon during pyrolysis,as well as to optimize the transition metal-tocarbon ratio,thus enhancing the ORR catalytic activity.A ZAB fabricated from such air electrode showed outstanding performance with a potential gap of only 0.83 V at 5 mA cm-2 for OER/ORR.Notably,no obvious performance degradation was observed for the continuous charge-discharge operation for 1800 cycles over an extended period of 300 h.
基金financial support from the National Natural Science Foundation of China(21671173)Zhejiang Provincial Ten Thousand Talent Program(2017R52043)。
文摘Supercapacitors(SCs)are emerging as efficient energy storage devices but still suffering from limited energy density compared with batteries.Electrolytes have been regarded as the key to determine the energy storage performance of SCs.However,none of the conventional electrolytes can fully meet the increasing requirements of SCs in terms of high ion conductivity,excellent stability,wide voltage window and operating temperature range,as well as environmentally friend concerns.To this end,hybrid electrolytes have sprung up in recent years,which are believed to be the candidate to solve these shortcomings.Herein,the state-of-the-art types of hybrid electrolytes for SCs,including the combination of aqueous and organic,aqueous and gel polymer,ionic liquids(ILs)and organic,and ILs and gel polymer hybrid electrolytes,are reviewed.The effects of different hybrid systems on the performance of SCs and the underlying mechanisms are among the focal points of the review,and prospects and possible directions are discussed as well to provide further insight into the future development of this field.
基金support from the Independent Designing Scientific Research Project of Zhejiang Normal University(2020ZS03)the Zhejiang Provincial Ten Thousand Talent Program(2017R52043)+1 种基金support from the Zhejiang Province Basic Public Welfare Research Project(LGF19B070006)supported by the National Natural Science Foundation of China(No.21775138).
文摘The study of atomically dispersed metal-nitrogen electrocatalysts is still limited in terms of understanding their catalytic mechanism because of the inability to precisely regulate the coordination number and type of N in combination with the metal elements.Inspired by the high catalytic activity and selectivity of natural enzymes,herein,we have designed and fabricated ultrathin carbon nanosheet-supported Mn single-atom catalysts(SACs)with a precise pyrrole-type Mn-N4(PT-MnN4)configuration using a bio-mimicking strategy.The PT-MnN4 SACs display outstanding oxygen reduction reaction(ORR)activity,with a half-wave potential(E_(1/2))of 0.88 V(vs.revisible hydrogen electrode[RHE])and extremely high stability in alkaline media.Moreover,superior ORR activities are also obtained,E_(1/2) of 0.73 V and 0.63 V in acid and neutral electrolytes,respectively,indicating the efficient pH-universal ORR performances.The assembled zinc-air battery using the PT-MnN4 SACs as air cathodes exhibits a high peak power density(175 mW cm^(−2))and long-term stability up to 150 h,implying its promising application in metal-air batteries.This study has paved the way toward the rational design and precise regulation of single-atom electrocatalysts.
基金the funding support(Project Number.PolyU 152214/17E)from Research Grant Council,University Grants Committee,Hong Kong SARthe financial support from National Nature Science Foundation of China under contract No.21878158the National Key Research and Development Program of China under contract No.2018YFB0905402
文摘With a rising energy demand and anabatic environmental crisis arising from the fast growth in human population and society economics,numerous efforts have been devoted to explore and design plentiful multifunctional materials for meeting highefficiency energy transfer processes,which happen in various developed energy conversion and storage systems.As a special kind of multi-metal oxides,perovskite with attractive physical and chemical properties,is becoming a rapidly rising star on the horizon of high-performance catalytic materials with substantial research behaviors worldwide.The porous nanostructure in targeted catalysts is favorable to the catalytic activity and thus improves the overall efficiency of these energy-related installations.In this review paper,recent advances made in the porous perovskite nanostructures for catalyzing several anodic or cathodic reactions in fuel cells and metal-air batteries are comprehensively summarized.Plenty of general preparation methods employed to attain porous perovskite-type oxides are provided,followed by a further discussion about the influence of various strategies on structures and catalytic properties of the porous perovskites.Furthermore,deep insights gathered in the future development of porous perovskite-based materials for energy conversion and storage technologies are also provided.
基金This work was supported by the Australian Research Council Dis-covery Project,Grant No.DP200103332 and DP200103315。
文摘The rapid development of power generation from renewable energy,such as geothermal,wind,and tidal energy,arises the need for efficient and economic electrochemical energy storage systems for integrating electric power smoothly into power grids.The lithium-ion battery has been successfully utilized for a variety of portable electronic devices but its application in large-scale energy storage has raised concerns about safety,availability of lithium resources,and its increasing price.Alternatively,sodium-ion battery(SIB)has been in acquisition predominantly,because of the abundant sodium resources over the earth’s crust at low cost.Developing high energy density electrode materials is one of the most intensive research topics.Oxides have been extensively investigated as the cathode and anode materials for high-performance and durable SIBs,owing to their various advantages including facile synthesis,versatile compositions,and easy structural tuning.In this review,we provide an in-time thorough summary of recent advances in oxide materials for cathodes and anodes for high energy density SIBs.The energy storage mechanism,challenges,categories,and optimizations of both electrodes are discussed.Existing research gaps and future perspectives are also outlined.This review is expected to accelerate the research for developing new pathways for tuning the properties of the oxide electrodes based on different sodium storage mechanisms.
基金financially supported by the National Natural Science Foundation of China (No.22272150)the Major Program of Zhejiang Provincial Natural Science Foundation of China(Nos.LD22B030002 and LZ23B030002)+1 种基金the Zhejiang Provincial Ten Thousand Talent Program (No.2021R51009)the Key Science and Technology Project of Jinhua City (No.2020-1-044)。
文摘Electrochemical nitrogen reduction reaction(ENRR) provides a promising strategy to achieve sustainable synthesis of ammonia. However, despite great efforts devoted to this research field, the problems such as low energy efficiency and weak selectivity still impede its practical implementation. Most of the research to date has been concentrated on creating sophisticated electrocatalysts, and adequate knowledge of electrolytes is still lacking. Herein, the recent progress in electrolytes for ENRR, including alkaline, neutral,acidic, water-in-salt, organic, ionic liquid, and mixed water-organic electrolytes, is thoroughly reviewed to obtain an in-depth understanding of their effects on electrocatalytic performance. Recently developed representative electrocatalysts in various types of electrolytes are also introduced, and future research priorities of different electrolytes are proposed to develop new and efficient ENRR systems.
基金supported by the Australian Research Council Discovery Projects(grant nos.DP200103315,DP200103332,DP220103669,and DP230100685)Linkage Projects(grant no.LP220200920).
文摘Solid-state electrolytes(SSEs)are a solution to safety issues related to flammable organic electrolytes for Li batteries.Insufficient contact between the anode and SSE results in high interface resistance,thus causing the batteries to exhibit high charging and discharging overpotentials.Recently,we reduced the overpotential of Li stripping and plating by introducing a high proportion of dual-conductive phases into a composite anode.The current study investigates the interface resistance and stability of a composite electrode modified with Zn and a lower proportion of dual-conductive phases.Zn-cation-adsorbed Prussian blue is synthesized as an intermediate component for a Zn-modified composite electrode(Li-FeZnNC).The Li-FeZnNC symmetric cell presents a lower interface resistance and overpotential compared with Li-FeNC(without Zn modification)and Li-symmetric cells.The Li-FeZnNC symmetric cell shows high electrochemical stability during Li stripping and plating at different current densities and high stability for 200 h.Full batteries with a Li-FeZnNC composite anode,garnet-type SSE,and LiFePO4 cathode show low charging and discharging overpotentials,a capacity of 152 mAh g−1,and high stability for 200 cycles.
基金supported by the Australian Research Council discovery project,grant Nos.DP200103332,DP200103315.
文摘Despite being widely used in people's daily life,the safety issue of lithium-ion batteries(LIBs)has become the major barrier for them to be applied in electrical vehicles(EVs)or large-scale energy storage.Typically,due to the use of liquid electrolytes containing flammable solvents which are easily oxidized by excessive and accumulated heat,the potential thermal runaway is a major safety concern for traditional LIBs.A strategy for a safer electrolyte design is controlling the flammability and volatility of the liquid electro-lytes,to effectively prevent thermal runaway,thus avoiding fire or other risks.Through this study,the mechanisms of thermal runa-way and the recent progress in electrolyte engineering toward LIBs were summarized,covering the major strategies including adding flame-retardants,the utilization of ionic liquid electrolytes and solid electrolytes.The characteristics,strengths and weaknesses of different strategies were discussed.New designing directions of safer electrolytes for the LIBs were also provided.
基金financially supported by the Major Program of Zhejiang Provincial Natural Science Foundation of China(No.LD22B030002)Zhejiang Provincial Ten Thousand Talent Programthe Independent Designing Scientific Research Project of Zhejiang Normal University(No.2020ZS03)。
文摘Supercapacitors(SCs)are rated as the foremost efficient devices bridging the production and consumption of renewable energy.To address the ever-increasing energy requirements,it is indispensable to further develop high-performance SCs with merits of high energy-density,acceptable price and long-term stability.This review highlights the recent advances on halogen-based functionalized chemistry engineering in the state-of-the-art electrode system for high-performance SCs,primarily referring to the doping and decoration strategies of F,Cl,Br and I elements.Due to the discrepancy of electronegativity and atomic radius,the functionalization of each halogen element endows the substrate materials with different physicochemical properties,including energy bandgap structure,porosity distribution and surface affinity.The principle of halogen embedment into host materials by precisely controlling ionic adsorption and electronic structure is presented.And,the vital perspectives on the future challenges of halogen functionalization are also discussed.This work aims to deepen the understanding of halogen-based functionalized strategies to motivate further research for the development of high-performance SCs,and it also provides a prospect for exploring new material modification methods for electrochemical energy storage.
基金This work was supported by the Australian Research Council via Discovery Projects(Nos.DP200103315,DP200103332 and DP230100685)Linkage Projects(No.LP220200920).The authors acknowledge the Microscopy and Microanalysis Facility—John de Laeter Centre,Curtin University for the scientific and technical assistance of material characterizations.L.Zhao and C.Cao would like to acknowledge the PhD scholarship supported by BLACKSTONE Minerals Ltd.
文摘The pursuit of safer and high-performance lithium-ion batteries(LIBs)has triggered extensive research activities on solid-state batteries,while challenges related to the unstable electrode-elec-trolyte interface hinder their practical implementation.Polymer has been used extensively to improve the cathode-electrolyte interface in garnet-based all-solid-state LIBs(ASSLBs),while it introduces new concerns about thermal stability.In this study,we propose the incorporation of a multi-functional flame-retardant triphenyl phos-phate additive into poly(ethylene oxide),acting as a thin buffer layer between LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathode and garnet electro-lyte.Through electrochemical stability tests,cycling performance evaluations,interfacial thermal stability analysis and flammability tests,improved thermal stability(capacity retention of 98.5%after 100 cycles at 60℃,and 89.6%after 50 cycles at 80℃)and safety characteristics(safe and stable cycling up to 100℃)are demonstrated.Based on various materials characterizations,the mechanism for the improved thermal stability of the interface is proposed.The results highlight the potential of multi-functional flame-retardant additives to address the challenges associated with the electrode-electrolyte interface in ASSLBs at high temperature.Efficient thermal modification in ASSLBs operating at elevated temperatures is also essential for enabling large-scale energy storage with safety being the primary concern.
基金financial support from National Natural Science Foundation of China (No. 21671173)the Independent Designing Scientific Research Project of Zhejiang Normal University (No. 2020ZS03)Zhejiang Provincial Ten Thousand Talent Program (No. 2017R52043)。
文摘Supercapacitors(SCs) with high power density and long cycling span life are demanding energy storage devices that will be an attractive power solution to modern electronic and electrical applications. Numerous theoretical and experimental works have been devoted to exploring various possibilities to increase the functionality and the specific capacitance of electrodes for SCs. Non-carbon two-dimensional(2D)materials have been considered as encouraging electrode candidates for their chemical and physical advantages such as tunable surface chemistry, high electronic conductivity, large mechanical strength, more active sites, and dual non-faradaic and faradaic electrochemical performances. Besides, these 2D materials also play particular roles in constructing highway channels for fast ion diffusion. This concise review summarizes cutting-edge progress of some representative 2D non-carbon materials for the aqueous electrolyte-based SCs, including transition metal oxides(TMOs), transition metal hydroxides(TMHs), transition metal chalcogenides(TMCs), MXenes, metal-organic frameworks(MOFs) and some emerging materials. Different synthetic methods, effective structural designs and corresponding electrochemical performances are reviewed in detail. And we finally present a detailed discussion of the current intractable challenges and technical bottlenecks, and highlight future directions and opportunities for the development of next-generation high-performance energy storage devices.
基金the National Natural Science Foundation of China(21671173)Zhejiang Provincial Ten Thousand Talent Program(2017R52043)。
文摘过渡金属氧化态调控工程是一种很有前景的改善电极材料的氧化还原活性、增加活性位点的策略.本文提出了一种简单的三乙醇胺辅助自模板法,制备了一种由交错钴硫化物纳米片(Co_(x)S_(y)-T NSs)组装而成的独特的三维蜂窝状网络结构.有趣的是,我们首次发现在该体系中,三乙醇胺可以有效地增加目标产物中的高价态Co^(3+)的比例.Co_(x)S_(y)-T NSs电极具有高含量的Co^(3+)和三维网络结构,使得其在5 A g^(-1)的电流密度下表现出351 mA h g^(-1)(2635 F g^(-1))的最大比容量和优异的循环稳定性.此外,由Co_(x)S_(y)-T NSs和活性炭(AC)电极组装的固态不对称超级电容器在0.81 kW kg^(-1)功率密度下展现出81.62 W h kg^(-1)的高能量密度和卓越的长周期循环稳定性,7000次循环后仍有96.2%的容量保持率.该结果证明同时调控高价态的金属物种并构筑三维网络结构是一种简单而有效的制备用于能源存储与转换的高活性电极材料的策略.
基金the financial support from Natural Science Foundation of China(No.21671173)the Independent Designing Scientific Research Project of Zhejiang Normal University(No.2020ZS03)Zhejiang Provincial Ten Thousand Talent Program(No.2017R52043)。
文摘The development of low-cost and highly efficient bifunctional electrocatalysts toward oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is of critical importance for clean energy devices such as fuel cells and metal-air batteries.Herein,a sophisticated na nostructure composed of CoS,Co and MoC nanoparticles incorporated in N and S dual-doped porous carbon nanofibers(CoS/Co/MoC-N,SPCNFs)as a high-efficiency bifunctional electrocatalyst is designed and synthesized via an efficient multistep strategy.The as-prepared CoS/Co/MoC-N,S-PCNFs exhibit a positive half-wave potential(E1/2)of0.871 V for ORR and a low overpotential of 289 mV at 10 mA/cm^(2) for OER,outperforming the non-noble metal-based catalysts reported.Furthermore,the assembled Zn-air battery based on CoS/Co/MoC-N,SPCNFs delivers an excellent power density(169.1 mW/cm^(2)),a large specific capacity(819.3 mAh/g)and robust durability,demonstrating the great potential of the as-developed bifunctional electrocatalyst in practical applications.This work is expected to inspire the design of advanced bifunctional nonprecious metal-based electrocatalysts for energy storage.
基金National Natural Science Foundation of China(Nos.11871137,11471066,11290143)the Fundamental Research of Civil Aircraft(No.MJ-F-2012-04)。
文摘In some applications,there are signals with piecewise structure to be recovered.In this paper,we propose a piecewise_ISS(P_ISS)method which aims to preserve the piecewise sparse structure(or the small-scaled entries)of piecewise signals.In order to avoid selecting redundant false small-scaled elements,we also implement the piecewise_ISS algorithm in parallel and distributed manners equipped with a deletion rule.Numerical experiments indicate that compared with alSS,the P_ISS algorithm is more effective and robust for piecewise sparse recovery.
