Rechargeable batteries currently hold the largest share of the electrochemical energy storage market,and they play a major role in the sustainable energy transition and industrial decarbonization to respond to global ...Rechargeable batteries currently hold the largest share of the electrochemical energy storage market,and they play a major role in the sustainable energy transition and industrial decarbonization to respond to global climate change.Due to the increased popularity of consumer electronics and electric vehicles,lithium-ion batteries have quickly become the most successful rechargeable batteries in the past three decades,yet growing demands in diversified application scenarios call for new types of rechargeable batteries.Tremendous efforts are made to developing the next-generation post-Li-ion rechargeable batteries,which include,but are not limited to solid-state batteries,lithium–sulfur batteries,sodium-/potassium-ion batteries,organic batteries,magnesium-/zinc-ion batteries,aqueous batteries and flow batteries.Despite the great achievements,challenges persist in precise understandings about the electrochemical reaction and charge transfer process,and optimal design of key materials and interfaces in a battery.This roadmap tends to provide an overview about the current research progress,key challenges and future prospects of various types of rechargeable batteries.New computational methods for materials development,and characterization techniques will also be discussed as they play an important role in battery research.展开更多
Rechargeable lithium-oxygen(Li-O2)batteries have appeal to enormous attention because they demonstrate higher energy density than the state-of-the-art Li-ion batteries.Whereas,their practical application is impeded by...Rechargeable lithium-oxygen(Li-O2)batteries have appeal to enormous attention because they demonstrate higher energy density than the state-of-the-art Li-ion batteries.Whereas,their practical application is impeded by several challenging problems,such as the low energy round trip efficiencies and the insufficient cycle life,due to the cathode passivation caused by the accumulation of discharge products.Developing efficient catalyst for oxygen reduction and evolution reactions is effective to reduce the overpotentials in Li-O2cells.In our work,we report a Co3O4modified Ag/g-C3N4nanocomposite as a bifunctional cathode catalyst for Li-O2cells.The g-C3N4substrate prevents the accumulation of Ag and Co3O4nanoparticles and the presence of Ag NPs improves the surface area of g-C3N4and electronic conductivity,significantly improving the oxygen reduction/evolution capabilities of Co3O4.Due to a synergetic effect,the Ag/g-C3N4/Co3O4nanocomposite demonstrates a higher catalytic activity than each individual constituent of Co3O4or Ag/g-C3N4for the ORR/OER on as catalysts in Li-O2cells.As a result,the Ag/gC3N4/Co3O4composite shows impressive electrochemical performance in a Li-O2battery,including high discharge capacity,small gap between charge and discharge potential,and high cycling stability.展开更多
Gel polymer electrolytes(GPEs)are one of the promising candidates for high-energy-density quasi-solid-state lithium metal batteries(QSSLMBs),for their high ionic conductivity and excellent interfacial compatibility.Th...Gel polymer electrolytes(GPEs)are one of the promising candidates for high-energy-density quasi-solid-state lithium metal batteries(QSSLMBs),for their high ionic conductivity and excellent interfacial compatibility.The comprehension of dynamic evolution and structure-reactivity correlation at the GPE/Li interface becomes significant.Here,in situ electrochemical atomic force microscopy(EC-AFM)provides insights into the LiNO_(3)-regulated micromechanism of the Li plating/stripping processes upon cycles in GPE-based LMBs at nanoscale.The additive LiNO_(3)induces the formation of amorphous nitride SEI film and facilitates Li^(+) ion diffusion.It stabilizes a compatible interface and regulates the Li nucleation/growth at steady kinetics.The deposited Li is in the shape of chunks and tightly compact.The Li dissolution shows favorable reversibility,which guarantees the cycling performance of LMBs.In situ AFM monitoring provides a deep understanding into the dynamic evolution of Li deposition/dissolution and the interphasial properties of tunable SEI film,regulating the rational design of electrolyte and optimizing interfacial establishment for GPE-based QSSLMBs.展开更多
Micrometre-sized electrode materials have distinct advantages for battery applications in terms of energy density,processability,safety and cost.For the silicon monoxide anode that undergoes electrochemical alloying r...Micrometre-sized electrode materials have distinct advantages for battery applications in terms of energy density,processability,safety and cost.For the silicon monoxide anode that undergoes electrochemical alloying reaction with Li,the Li(de)intercalation by micron-sized active particles usually accompanies with a large volume variation,which pulverizes the particle structure and leads to rapidly faded storage performance.In this work,we proposed to stabilize the electrochemistry vs.Li of the micron-SiO_(x) anode by forming a rigid-flexible bi-layer coati ng on the particle surface.The coati ng consists of pyrolysis carbon as the inner layer and polydopamine as the outer layer.While the inner layer guarantees high structural rigidity at particle surface and provides efficient pathway for electron conduction,the outer layer shows high flexibility for maintaining the integrity of micrometre-sized particles against drastic volume variation,and together they facilitate formation of stable solid electrolyte interface on the SiO_(x) particles.A composite an ode prepared by mixing the coated micron-SiOx with graphite delivered improved Li storage performance,and promised a high-capacity,long-life LiFePO_(4)/SiO_(x)-graphite pouch cell.Our strategy provides a general and feasible solution for building high-energy rechargeable batteries from micrometre-sized electrode materials with significant volume variation.展开更多
Lithium-sulfur(Li-S) batteries have shown promises for the next-generation, high-energy electrochemical storage, yet are hindered by rapid performance decay due to the polysulfide shuttle in the cathode and safety con...Lithium-sulfur(Li-S) batteries have shown promises for the next-generation, high-energy electrochemical storage, yet are hindered by rapid performance decay due to the polysulfide shuttle in the cathode and safety concerns about potential thermal runaway. To address the above challenges, herein, we show a flame-retardant cathode binder that simultaneously improves the electrochemical stability and safety of batteries. The combination of soft and hard segments in the polymer framework of binders allows high flexibility and mechanical strength for adapting to the drastic volume change during the Li(de)intercalation of the S cathode. The binder contains a large number of polar groups, which show the high affinity to polysulfides so that they help to anchor active S species at the cathode. These polar groups also help to regulate and facilitate the Li-ion transport, promoting the kinetics of polysulfide conversion reaction. The binder contains abundant phosphine oxide groups, which, in the case of battery's thermal runaway, decompose and release PO· radicals to quench the combustion reactions and stop the fire. Consequently, Li-S batteries using the new cathode binder show the improved electrochemical performance, including a low-capacity decay of 0.046% per cycle for 800 cycles at 1 C and favorable rate capabilities of up to 3 C. This work offers new insights on the practical realization of high-energy rechargeable batteries with stable storage electrochemistry and high safety.展开更多
Aqueous rechargeable Li/Na-ion batteries have shown promise for sustainable large-scale energy storage due to their safety,low cost,and environmental benignity.However,practical applications of aqueous batteries are p...Aqueous rechargeable Li/Na-ion batteries have shown promise for sustainable large-scale energy storage due to their safety,low cost,and environmental benignity.However,practical applications of aqueous batteries are plagued by water's intrinsically narrow electrochemical stability window,which results in low energy density.In this perspective article,we review several strategies to broaden the electrochemical window of aqueous electrolytes and realize high-energy aqueous batteries.Specifically,we highlight our recent findings on stabilizing aqueous Li storage electrochemistry using a deuterium dioxide-based aqueous electrolyte,which shows significant hydrogen isotope effects that trigger a wider electrochemical window and inhibit detrimental parasitic processes.展开更多
Silicon has attracted much attention as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and rich resource abundance. However, the practical battery use of Si is challen...Silicon has attracted much attention as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and rich resource abundance. However, the practical battery use of Si is challenged by its low conductivity and drastic volume variation during the Li uptake/release process. Tremendous efforts have been made on shrinking the particle size of Si into nanoscale so that the volume variation could be accommodated. However, the bare nano-Si material would still pulverize upon (de)lithiation. Moreover, it shows an excessive surface area to invite unlimited growth of solid electrolyte interface that hinders the transportation of charge carriers, and an increased interparticle resistance. As a result, the Si nanoparticles gradually lose their electrical contact during the cycling process, which accounts for poor thermodynamic stability and sluggish kinetics of the anode reaction versus Li. To address these problems and improve the Li storage performance of nano-Si anode, proper structural design should be applied on the Si anode. In this perspective, we will briefly review some strategies for improving the electrochemistry versus Li of nano-Si materials and their derivatives, and show opinions on the optimal design of nanostructured Si anode for advanced LIBs.展开更多
Photocatalytic CO2 reduction on metal-oxide-based catalysts is promising for solving the energy and environmental crises faced by mankind. The oxygen vacancy （Vo） on metal oxides is expected to be a key factor affec...Photocatalytic CO2 reduction on metal-oxide-based catalysts is promising for solving the energy and environmental crises faced by mankind. The oxygen vacancy （Vo） on metal oxides is expected to be a key factor affecting the efficiency of photocatalytic CO2 reduction on metal-oxide-based catalysts. Yet, to date, the question of how an Vo influences photocatalytic CO2 reduction is still unanswered. Herein, we report that, on Vo-rich gallium oxide coated with Pt nanoparticles （Vo-rich Pt/Ga203）, CO2 is photocatalytically reduced to CO, with a highly enhanced CO evolution rate （21.0umol.h-1） compared to those on Vo-poor Pt/Ga2O3 （3.9 gmol-h-1） and Pt/TiO2（P25） （6.7 gmol.h-1）. We demonstrate that the Vo leads to improved CO2 adsorption and separation of the photoinduced charges on Pt/Ga203, thus enhancing the photocatalytic activity of Pt/Ga203. Rational fabrication of an Vo is thereby an attractive strategy for developing efficient catalysts for photocatalytic CO2 reduction.展开更多
Sodium-ion batteries have the potential to be an alternative to lithium-ion batteries especially for applications such as large-scale grid energy storage. The development of suitable cathode materials is crucial to th...Sodium-ion batteries have the potential to be an alternative to lithium-ion batteries especially for applications such as large-scale grid energy storage. The development of suitable cathode materials is crucial to the commercialization of sodium-ion batteries.Sodium-based layered-type transition metal oxides are promising candidates as cathode materials as they offer decent energy density and are easy to be synthesized. Unfortunately, most layered oxides suffer from poor air-stability, which greatly increases the cost of manufacturing and handling. The air-sensitivity severely limits the development and commercial application of sodium-ion batteries. A review that summarizes the latest understanding and solutions of air-sensitivity is desired. In this review,the background and fundamentals of sodium-based layered-type cathode materials are presented, followed by a discussion on the latest research on air-sensitivity of these materials. The mechanism is complex and involves multiple chemical and physical reactions. Various strategies are shown to alleviate some of the corresponding problems and promote the feasible application of sodium-ion batteries, followed by an outlook on current and future research directions of air-stable cathode materials. It is believed that this review will provide insights for researchers to develop practically relevant materials for sodium-ion batteries.展开更多
Conventional lithium-ion batteries(LIBs)with graphite anodes are approaching their theoretical limitations in energy density.Replacing the conventional graphite anodes with high-capacity Si-based anodes represents one...Conventional lithium-ion batteries(LIBs)with graphite anodes are approaching their theoretical limitations in energy density.Replacing the conventional graphite anodes with high-capacity Si-based anodes represents one of the most promising strategies to greatly boost the energy density of LIBs.However,the inherent huge volume expansion of Si-based materials after lithiation and the resulting series of intractable problems,such as unstable solid electrolyte interphase layer,cracking of electrode,and especially the rapid capacity degradation of cells,severely restrict the practical application of Sibased anodes.Over the past decade,numerous reports have demonstrated that polymer binders play a critical role in alleviating the volume expansion and maintaining the integrity and stable cycling of Si-based anodes.In this review,the state-of-the-art designing of polymer binders for Si-based anodes have been systematically summarized based on their structures,including the linear,branched,crosslinked,and conjugated conductive polymer binders.Especially,the comprehensive designing of multifunctional polymer binders,by a combination of multiple structures,interactions,crosslinking chemistries,ionic or electronic conductivities,soft and hard segments,and so forth,would be promising to promote the practical application of Si-based anodes.Finally,a perspective on the rational design of practical polymer binders for the large-scale application of Si-based anodes is presented.展开更多
Lithium-ion batteries （LIBs） are currently recognized as one of the most popular power sources available. To construct advanced LIBs exhibiting long-term endurance, great attention has been paid to enhancing their p...Lithium-ion batteries （LIBs） are currently recognized as one of the most popular power sources available. To construct advanced LIBs exhibiting long-term endurance, great attention has been paid to enhancing their poor cycle stabilities. As the performance of LIBs is dependent on the electrode materials employed, the most promising approach to improve their life span is the design of novel electrode materials. We herein describe the rational design of a three-dimensional （3D） porous MnO/C-N nanoarchitecture as an anode material for long cycle life LIBs based on their preparation from inexpensive, renewable, and abundant rapeseed pollen （R-pollen） via a facile immersion-annealing route. Remarkably, the as-prepared MnO/C-N with its optimized 3D nanostructure exhibited a high specific capacity （756.5 mAh·g^-1 at a rate of 100 mA·g^-1）, long life span （specific discharge capacity of 513.0 mAh·g^-1, -95.16% of the initial reversible capacity, after 400 cycles at 300 mA·g^-1）, and good rate capability. This material therefore represents a promising alternative candidate for the high-performance anode of next-generation LIBs.展开更多
Chalcogen elements,such as sulfur(S),selenium(Se),tellurium(Te)and the interchalcogen compounds,have been studied extensively as cathode materials for the next-generation rechargeable lithium/sodium(Li/Na)batteries.Th...Chalcogen elements,such as sulfur(S),selenium(Se),tellurium(Te)and the interchalcogen compounds,have been studied extensively as cathode materials for the next-generation rechargeable lithium/sodium(Li/Na)batteries.The high energy output of the Li/Na-chalcogen battery originates from the two-electron conversion reaction between chalcogen cathode and alkali metal anode,through which both electrodes are able to deliver high theoretical capacities.The reaction also leads to parasitic reactions that deteriorate the chemical environment in the battery,and different cathode-anode combinations show their own features.In this article,we intend to discuss the fundamental conversion electrochemistry between chalcogen elements and alkali metals and its potential influence,either positive or negative,on the performance of batteries.The strategies to improve the conversion electrochemistry of chalcogen cathode are also reviewed to offer insights into the reasonable design of rechargeable Li/Nachalcogen batteries.展开更多
The demand to increase energy density of rechargeable batteries for portable electronic devices and electric vehicles and to reduce the cost for grid-scale energy storage necessitates the exploration of new chemistrie...The demand to increase energy density of rechargeable batteries for portable electronic devices and electric vehicles and to reduce the cost for grid-scale energy storage necessitates the exploration of new chemistries of electrode materials for rechargeable batteries.The open framework-structure of Prussian-blue materials has recently been demonstrated as a promising cathode host for a variety of monovalent and multivalent cations with the tunable working voltage and discharge capacities.Recent progress toward the application of Prussian-blue cathode materials for rechargeable batteries is reviewed,with special emphasis on charge-storage mechanisms of different insertion species,factors influencing electrochemical performances,and possible approaches to overcome their intrinsic limitations.展开更多
Lithium metal has been widely studied as one of the most promising anode materials for realizing the next-generation high-energy-density rechargeable batteries.However,its practical use in rechargeable batteries has b...Lithium metal has been widely studied as one of the most promising anode materials for realizing the next-generation high-energy-density rechargeable batteries.However,its practical use in rechargeable batteries has been hindered by hazardous dendrite growth and huge volume variations during Li plating/stripping.Herein,we reported a borondoped three-dimensional(3D)layered MXene(Ti_(3)C_(2)T_(x))as the host of Li metal anode.The material was synthesized via a facile one-pot hydrothermal process.With uniform B-doping,the prepared 3D multilayered MXene sheets provided more sites for nucleation of Li metal,so that the deposited Li metal anode showed favorable cycling stability and a high Coulombic efficiency.With the use of the same host material,a hybrid lithium-metal battery with 3D Li anode coupling with LiFePO4 cathode showed long cycle life and favorable electrochemical stability.This work shed lights on reasonable structural and compositional design of host materials that enables high-performance Li-metal anode toward practical realization of highenergy rechargeable batteries。展开更多
Rechargeable batteries based on solid-state electrolytes are of great interest and importance for the next-generation energy storage due to their high energy output and improved safety.For building the solid-state bat...Rechargeable batteries based on solid-state electrolytes are of great interest and importance for the next-generation energy storage due to their high energy output and improved safety.For building the solid-state batteries,Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)represents a promising candidate as it features high chemical stability against air exposure and a high Na^(+)conductivity.NZSP pellets were usually calcined at a high temperature,and the high volatility of Na and P elements easily led to the formation of impurity phase.In this work,the effects of calcination temperature and stoichiometry on the phase purity and ionic conductivity of the NZSP electrolyte were studied.At an elevated sintering temperature,the NZSP electrolyte showed a high ionic conductivity owing to decreased porosity,and the highest ionic conductivity at 30℃was observed to be 2.75×10^(-5)S·cm^(-1)with an activation energy of 0.41 eV.For the stoichiometry,the introduction of 5 mol%excessive P results in formation of more Na_(3)PO_(4) and glass-like phase at the grain boundary,which caused the blurred grain boundary and reduced grain barrier,and effectively suppressed Na dendrite growth,then accounted for improved cycling performance of a Na‖Na symmetric cell.Our work provided insights on reasonable design and preparation of NZSP electrolyte towards practical realization of solid-state Na-metal batteries.展开更多
基金supported by the National Key R&D Program of China(Grant No.2019YFA0705703)CAS Project for Young Scientists in Basic Research(Grant No.YSBR-058)+1 种基金the National Natural Science Foundation of China(Grant Nos.21975266,52172252 and 22209188)the Beijing Natural Science Foundation(Grant No.JQ22005)。
基金supported by the CAS Project for Young Scientists in Basic Research(YSBR-058)the Basic Science Center Project of National Natural Science Foundation of China(52388201)+57 种基金the Beijing Natural Science Foundation(JQ22005)financially supported by the National Key R&D Program of China(2022YFB2404400)the National Natural Science Foundation of China(92263206,21875007,21975006,21974007,and U19A2018)the Youth Beijing Scholars program(PXM2021_014204_000023)the Beijing Natural Science Foundation(2222001 and KZ202010005007)supported by the National Key R&D Program of China(2021YFB2400200)the Youth Innovation Promotion Association CAS(2023040)the National Natural Science Foundation of China(22279148 and 21905286)the Beijing Natural Science Foundation(Z220021)supported by Beijing Municipal Natural Science Foundation(Z200011)National Key Research and Development Program(2021YFB2500300,2021YFB2400300)National Natural Science Foundation of China(22308190,22109084,22108151,22075029,and 22061132002)Key Research and Development Program of Yunnan Province(202103AA080019)the S&T Program of Hebei Province(22344402D)China Postdoctoral Science Foundation(2022TQ0165)Tsinghua-Jiangyin Innovation Special Fund(TJISF)Tsinghua-Toyota Joint Research Fundthe Institute of Strategic Research,Huawei Technologies Co.,LtdOrdos-Tsinghua Innovative&Collaborative Research Program in Carbon Neutralitythe Shuimu Tsinghua Scholar Program of Tsinghua Universityfinancially supported by the National Key R&D Program of China(2021YFB2400300)National Natural Science Foundation of China(22179083)Program of Shanghai Academic Research Leader(20XD1401900)Key-Area Research and Development Program of Guangdong Province(2019B090908001)financially supported by the National Key R&D Program of China(2020YFE0204500)the National Natural Science Foundation of China(52071311,52271140)Jilin Province Science and Technology Development Plan Funding Project(20220201112GX)Changchun Science and Technology Development Plan Funding Project(21ZY06)Youth Innovation Promotion Association CAS(2020230,2021223)supported by the National Natural Science Foundation of China(51971124,52171217,52202284 and 52250710680)the State Key Laboratory of Electrical Insulation and Power Equipment,Xi’an Jiaotong University(EIPE22208)Zhejiang Natural Science Foundation(LZ21E010001,LQ23E020002)Wenzhou Natural Science Foundation(G20220019,G20220021,ZG2022032,G2023027)Science and Technology Project of State Grid Corporation of China(5419-202158503A-0-5-ZN)Wenzhou Key Scientific and Technological Innovation Research Projects(ZG2023053)Cooperation between industry and education project of Ministry of Education(220601318235513)supported by the Australian Research Council(DP210101486 and FL210100050)supported by the National Natural Science Foundation of China(22179135,22109168,52072195,and 21975271)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA22010603,XDA22010600)Taishan Scholars Program for Young Expert of Shandong Province(tsqn202103145)Shandong Energy Institute(SEI I202108 and SEI I202127)the China Postdoctoral Science Foundation(BX20200344,2020M682251)supported by the National Key R&D Program of China(2022YFB2402200)the National Natural Science Foundation of China(22121005,22020102002,and 21835004)the Frontiers Science Center for New Organic Matter of Nankai University(63181206)the Haihe Laboratory of Sustainable Chemical Transformationssupported by National Key Research and Development Program of China(2022YFB2404500)Shenzhen Outstanding Talents Training Fundsupported by the National Key R&D Program of China(2019YFA0705104)GRF under the project number City U 11305218supported from National Natural Science Foundation of China(22078313,21925804)Free exploring basic research project of Liaoning(2022JH6/100100005)Youth Innovation Promotion Association CAS(2019182)supported from the Research Center for industries of the Future(RCIF)at Westlake Universitythe start-up fund from Westlake Universitysupported by the National Key R&D Program of China(2020YFB2007400)the National Natural Science Foundation of China(22075317)the Strategic Priority Research Program(B)(XDB07030200)of Chinese Academy of Sciences。
文摘Rechargeable batteries currently hold the largest share of the electrochemical energy storage market,and they play a major role in the sustainable energy transition and industrial decarbonization to respond to global climate change.Due to the increased popularity of consumer electronics and electric vehicles,lithium-ion batteries have quickly become the most successful rechargeable batteries in the past three decades,yet growing demands in diversified application scenarios call for new types of rechargeable batteries.Tremendous efforts are made to developing the next-generation post-Li-ion rechargeable batteries,which include,but are not limited to solid-state batteries,lithium–sulfur batteries,sodium-/potassium-ion batteries,organic batteries,magnesium-/zinc-ion batteries,aqueous batteries and flow batteries.Despite the great achievements,challenges persist in precise understandings about the electrochemical reaction and charge transfer process,and optimal design of key materials and interfaces in a battery.This roadmap tends to provide an overview about the current research progress,key challenges and future prospects of various types of rechargeable batteries.New computational methods for materials development,and characterization techniques will also be discussed as they play an important role in battery research.
基金the financial support from National Natural Science Foundation of China(Grant no.51472070,51872071)China Postdoctoral Science Foundation(Grant no.172731)。
文摘Rechargeable lithium-oxygen(Li-O2)batteries have appeal to enormous attention because they demonstrate higher energy density than the state-of-the-art Li-ion batteries.Whereas,their practical application is impeded by several challenging problems,such as the low energy round trip efficiencies and the insufficient cycle life,due to the cathode passivation caused by the accumulation of discharge products.Developing efficient catalyst for oxygen reduction and evolution reactions is effective to reduce the overpotentials in Li-O2cells.In our work,we report a Co3O4modified Ag/g-C3N4nanocomposite as a bifunctional cathode catalyst for Li-O2cells.The g-C3N4substrate prevents the accumulation of Ag and Co3O4nanoparticles and the presence of Ag NPs improves the surface area of g-C3N4and electronic conductivity,significantly improving the oxygen reduction/evolution capabilities of Co3O4.Due to a synergetic effect,the Ag/g-C3N4/Co3O4nanocomposite demonstrates a higher catalytic activity than each individual constituent of Co3O4or Ag/g-C3N4for the ORR/OER on as catalysts in Li-O2cells.As a result,the Ag/gC3N4/Co3O4composite shows impressive electrochemical performance in a Li-O2battery,including high discharge capacity,small gap between charge and discharge potential,and high cycling stability.
基金financially supported by the National Key R&D Program of China(Grant No.2016YFA0202500)the National Natural Science Fund for Excellent Young Scholars(Grant No.21722508)。
文摘Gel polymer electrolytes(GPEs)are one of the promising candidates for high-energy-density quasi-solid-state lithium metal batteries(QSSLMBs),for their high ionic conductivity and excellent interfacial compatibility.The comprehension of dynamic evolution and structure-reactivity correlation at the GPE/Li interface becomes significant.Here,in situ electrochemical atomic force microscopy(EC-AFM)provides insights into the LiNO_(3)-regulated micromechanism of the Li plating/stripping processes upon cycles in GPE-based LMBs at nanoscale.The additive LiNO_(3)induces the formation of amorphous nitride SEI film and facilitates Li^(+) ion diffusion.It stabilizes a compatible interface and regulates the Li nucleation/growth at steady kinetics.The deposited Li is in the shape of chunks and tightly compact.The Li dissolution shows favorable reversibility,which guarantees the cycling performance of LMBs.In situ AFM monitoring provides a deep understanding into the dynamic evolution of Li deposition/dissolution and the interphasial properties of tunable SEI film,regulating the rational design of electrolyte and optimizing interfacial establishment for GPE-based QSSLMBs.
基金supported by the Innovation Team for R&D and Industrialization of High Energy Density Si-based Power batteries (2018607219003)the Basic Science Center Project of National Natural Science Foundation of China (51788104)+2 种基金the National Key R&D Program of China (2019YFA0705600)the “Transformational Technologies for Clean Energy and Demonstration”Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21070300).
文摘Micrometre-sized electrode materials have distinct advantages for battery applications in terms of energy density,processability,safety and cost.For the silicon monoxide anode that undergoes electrochemical alloying reaction with Li,the Li(de)intercalation by micron-sized active particles usually accompanies with a large volume variation,which pulverizes the particle structure and leads to rapidly faded storage performance.In this work,we proposed to stabilize the electrochemistry vs.Li of the micron-SiO_(x) anode by forming a rigid-flexible bi-layer coati ng on the particle surface.The coati ng consists of pyrolysis carbon as the inner layer and polydopamine as the outer layer.While the inner layer guarantees high structural rigidity at particle surface and provides efficient pathway for electron conduction,the outer layer shows high flexibility for maintaining the integrity of micrometre-sized particles against drastic volume variation,and together they facilitate formation of stable solid electrolyte interface on the SiO_(x) particles.A composite an ode prepared by mixing the coated micron-SiOx with graphite delivered improved Li storage performance,and promised a high-capacity,long-life LiFePO_(4)/SiO_(x)-graphite pouch cell.Our strategy provides a general and feasible solution for building high-energy rechargeable batteries from micrometre-sized electrode materials with significant volume variation.
基金financially supported by the National Key R&D Program of China(2019YFA0705703)Natural Science Foundation of Hubei Province(2021CFB082)+4 种基金Scientific Research Foundation of Wuhan Institute of Technology(K2021042)the Open Key Fund Project of State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology,2022-KF-10)National Natural Science Foundation of China(22275142,U22B6011)China Postdoctoral Science Foundation(2021M703268)the Junior Fellow Program of Beijing National Laboratory for Molecular Sciences(2021BMS20062)。
文摘Lithium-sulfur(Li-S) batteries have shown promises for the next-generation, high-energy electrochemical storage, yet are hindered by rapid performance decay due to the polysulfide shuttle in the cathode and safety concerns about potential thermal runaway. To address the above challenges, herein, we show a flame-retardant cathode binder that simultaneously improves the electrochemical stability and safety of batteries. The combination of soft and hard segments in the polymer framework of binders allows high flexibility and mechanical strength for adapting to the drastic volume change during the Li(de)intercalation of the S cathode. The binder contains a large number of polar groups, which show the high affinity to polysulfides so that they help to anchor active S species at the cathode. These polar groups also help to regulate and facilitate the Li-ion transport, promoting the kinetics of polysulfide conversion reaction. The binder contains abundant phosphine oxide groups, which, in the case of battery's thermal runaway, decompose and release PO· radicals to quench the combustion reactions and stop the fire. Consequently, Li-S batteries using the new cathode binder show the improved electrochemical performance, including a low-capacity decay of 0.046% per cycle for 800 cycles at 1 C and favorable rate capabilities of up to 3 C. This work offers new insights on the practical realization of high-energy rechargeable batteries with stable storage electrochemistry and high safety.
基金This work was supported by the National Key R&D Program of China(Grant No 2019YFA0705602)the Basic Science Center Project of National Natural Science Foundation of China(Grant No.51788104)+2 种基金the CAS Project for Young Scientists in Basic Research(Grant YSBR-058)the National Natural Science Foundation of China(Grant Nos.21975266,52172252 and 22209188)the Beijing Natural Science Foundation(Grant No.JQ22005).
文摘Aqueous rechargeable Li/Na-ion batteries have shown promise for sustainable large-scale energy storage due to their safety,low cost,and environmental benignity.However,practical applications of aqueous batteries are plagued by water's intrinsically narrow electrochemical stability window,which results in low energy density.In this perspective article,we review several strategies to broaden the electrochemical window of aqueous electrolytes and realize high-energy aqueous batteries.Specifically,we highlight our recent findings on stabilizing aqueous Li storage electrochemistry using a deuterium dioxide-based aqueous electrolyte,which shows significant hydrogen isotope effects that trigger a wider electrochemical window and inhibit detrimental parasitic processes.
基金the financial support of this work by the National Natural Science Foundation of China (No.21773078)the Fundamental Research Funds for the Central Universities of China (Nos.2662015PY163 and 2662017JC025).
文摘Silicon has attracted much attention as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and rich resource abundance. However, the practical battery use of Si is challenged by its low conductivity and drastic volume variation during the Li uptake/release process. Tremendous efforts have been made on shrinking the particle size of Si into nanoscale so that the volume variation could be accommodated. However, the bare nano-Si material would still pulverize upon (de)lithiation. Moreover, it shows an excessive surface area to invite unlimited growth of solid electrolyte interface that hinders the transportation of charge carriers, and an increased interparticle resistance. As a result, the Si nanoparticles gradually lose their electrical contact during the cycling process, which accounts for poor thermodynamic stability and sluggish kinetics of the anode reaction versus Li. To address these problems and improve the Li storage performance of nano-Si anode, proper structural design should be applied on the Si anode. In this perspective, we will briefly review some strategies for improving the electrochemistry versus Li of nano-Si materials and their derivatives, and show opinions on the optimal design of nanostructured Si anode for advanced LIBs.
文摘Photocatalytic CO2 reduction on metal-oxide-based catalysts is promising for solving the energy and environmental crises faced by mankind. The oxygen vacancy （Vo） on metal oxides is expected to be a key factor affecting the efficiency of photocatalytic CO2 reduction on metal-oxide-based catalysts. Yet, to date, the question of how an Vo influences photocatalytic CO2 reduction is still unanswered. Herein, we report that, on Vo-rich gallium oxide coated with Pt nanoparticles （Vo-rich Pt/Ga203）, CO2 is photocatalytically reduced to CO, with a highly enhanced CO evolution rate （21.0umol.h-1） compared to those on Vo-poor Pt/Ga2O3 （3.9 gmol-h-1） and Pt/TiO2（P25） （6.7 gmol.h-1）. We demonstrate that the Vo leads to improved CO2 adsorption and separation of the photoinduced charges on Pt/Ga203, thus enhancing the photocatalytic activity of Pt/Ga203. Rational fabrication of an Vo is thereby an attractive strategy for developing efficient catalysts for photocatalytic CO2 reduction.
基金supported by the National Natural Science Foundation of China (22179021)the Basic Science Center Project of National Natural Science Foundation of China (51788104)+1 种基金the Natural Science Foundation of Fujian Province (2019J01284)21C Innovation Laboratory Contemporary Amperex Technology Ltd (21C-OP-202011)。
文摘Sodium-ion batteries have the potential to be an alternative to lithium-ion batteries especially for applications such as large-scale grid energy storage. The development of suitable cathode materials is crucial to the commercialization of sodium-ion batteries.Sodium-based layered-type transition metal oxides are promising candidates as cathode materials as they offer decent energy density and are easy to be synthesized. Unfortunately, most layered oxides suffer from poor air-stability, which greatly increases the cost of manufacturing and handling. The air-sensitivity severely limits the development and commercial application of sodium-ion batteries. A review that summarizes the latest understanding and solutions of air-sensitivity is desired. In this review,the background and fundamentals of sodium-based layered-type cathode materials are presented, followed by a discussion on the latest research on air-sensitivity of these materials. The mechanism is complex and involves multiple chemical and physical reactions. Various strategies are shown to alleviate some of the corresponding problems and promote the feasible application of sodium-ion batteries, followed by an outlook on current and future research directions of air-stable cathode materials. It is believed that this review will provide insights for researchers to develop practically relevant materials for sodium-ion batteries.
基金Beijing National Laboratory for Molecular Sciences,Grant/Award Number:2019BMS20022National Natural Science Foundation of China,Grant/Award Number:22005314+3 种基金Strategic Priority Research Program of the Chinese Academy of Sciences,Grant/Award Number:XDA21070300The China Postdoctoral Science Foundation,Grant/Award Number:2019M660805The National Key R&D Program of China,Grant/Award Number:2019YFA0705600The Special Financial Grant from the China Postdoctoral Science Foundation,Grant/Award Number:2020T130658。
文摘Conventional lithium-ion batteries(LIBs)with graphite anodes are approaching their theoretical limitations in energy density.Replacing the conventional graphite anodes with high-capacity Si-based anodes represents one of the most promising strategies to greatly boost the energy density of LIBs.However,the inherent huge volume expansion of Si-based materials after lithiation and the resulting series of intractable problems,such as unstable solid electrolyte interphase layer,cracking of electrode,and especially the rapid capacity degradation of cells,severely restrict the practical application of Sibased anodes.Over the past decade,numerous reports have demonstrated that polymer binders play a critical role in alleviating the volume expansion and maintaining the integrity and stable cycling of Si-based anodes.In this review,the state-of-the-art designing of polymer binders for Si-based anodes have been systematically summarized based on their structures,including the linear,branched,crosslinked,and conjugated conductive polymer binders.Especially,the comprehensive designing of multifunctional polymer binders,by a combination of multiple structures,interactions,crosslinking chemistries,ionic or electronic conductivities,soft and hard segments,and so forth,would be promising to promote the practical application of Si-based anodes.Finally,a perspective on the rational design of practical polymer binders for the large-scale application of Si-based anodes is presented.
基金Acknowledgements This work is supported by the National Natural Science Foundation of China （Nos. 21431006 and 21503207）, the Foundation for Innovative Research Groups of the National Natural Science Foundation of China （No. 21521001）, the National Basic Research Program of China （Nos. 2014CB931800, 2013CB933900）, and Scientific Research Grant of Hefei Science Center of Chinese Academy of Sciences （Nos. 2015HSC-UE007 and 2015SRG-HSC038）, the China Postdoctoral Science Foundation （Nos. 2015T80662 and 2014M550346）, and the Fundamental Research Funds for the Central Universities （No. WK2060190047）. The authors also thank the help provided by Dr. Yue Lin and Prof. Yan-Wei Ding in Instruments＇ Center for Physical Science at the University of Science and Technology of China.
文摘Lithium-ion batteries （LIBs） are currently recognized as one of the most popular power sources available. To construct advanced LIBs exhibiting long-term endurance, great attention has been paid to enhancing their poor cycle stabilities. As the performance of LIBs is dependent on the electrode materials employed, the most promising approach to improve their life span is the design of novel electrode materials. We herein describe the rational design of a three-dimensional （3D） porous MnO/C-N nanoarchitecture as an anode material for long cycle life LIBs based on their preparation from inexpensive, renewable, and abundant rapeseed pollen （R-pollen） via a facile immersion-annealing route. Remarkably, the as-prepared MnO/C-N with its optimized 3D nanostructure exhibited a high specific capacity （756.5 mAh·g^-1 at a rate of 100 mA·g^-1）, long life span （specific discharge capacity of 513.0 mAh·g^-1, -95.16% of the initial reversible capacity, after 400 cycles at 300 mA·g^-1）, and good rate capability. This material therefore represents a promising alternative candidate for the high-performance anode of next-generation LIBs.
基金supported by the National Key R&D Program of China(2019YFA0705700)the National Natural Science Foundation of China(21975266,21805062)+1 种基金the Beijing National Laboratory for Molecular Sciences(BNLMS-CXXM-201906)support from the Start-up Funds from the Chinese Academy of Sciences。
文摘Chalcogen elements,such as sulfur(S),selenium(Se),tellurium(Te)and the interchalcogen compounds,have been studied extensively as cathode materials for the next-generation rechargeable lithium/sodium(Li/Na)batteries.The high energy output of the Li/Na-chalcogen battery originates from the two-electron conversion reaction between chalcogen cathode and alkali metal anode,through which both electrodes are able to deliver high theoretical capacities.The reaction also leads to parasitic reactions that deteriorate the chemical environment in the battery,and different cathode-anode combinations show their own features.In this article,we intend to discuss the fundamental conversion electrochemistry between chalcogen elements and alkali metals and its potential influence,either positive or negative,on the performance of batteries.The strategies to improve the conversion electrochemistry of chalcogen cathode are also reviewed to offer insights into the reasonable design of rechargeable Li/Nachalcogen batteries.
基金Experimental Center of Advanced Materials in Beijing Institute of TechnologyNational Key R&D Program of China,Grant/Award Number:2019YFA0705602+2 种基金National Natural Science Foundation of China,Grant/Award Numbers:51772029,51972029Shandong Huana New Energy Technology Co.,Ltd.Teli Young Scholars of Beijing Institute of Technology。
文摘The demand to increase energy density of rechargeable batteries for portable electronic devices and electric vehicles and to reduce the cost for grid-scale energy storage necessitates the exploration of new chemistries of electrode materials for rechargeable batteries.The open framework-structure of Prussian-blue materials has recently been demonstrated as a promising cathode host for a variety of monovalent and multivalent cations with the tunable working voltage and discharge capacities.Recent progress toward the application of Prussian-blue cathode materials for rechargeable batteries is reviewed,with special emphasis on charge-storage mechanisms of different insertion species,factors influencing electrochemical performances,and possible approaches to overcome their intrinsic limitations.
基金financially supported by the National Key R&D Program of China (No. 2019YFA0705602)the National Natural Science Foundation of China (Nos. 21975266 and 22075299)+3 种基金the Natural Science Foundation of Hebei Province (Nos. B2020205019, B2021205019, B2019205249 and B2021205029)the School Fund of Hebei Normal University (No. L2017B03)the Science and Technology Project of State Grid Corporation of China (No. 5400-202099510A-0-0-00)the Start-up Funds of the CAS and the BMS Senior Fellow of Beijing National Laboratory for Molecular Sciences (No. 2020BMS20032)
文摘Lithium metal has been widely studied as one of the most promising anode materials for realizing the next-generation high-energy-density rechargeable batteries.However,its practical use in rechargeable batteries has been hindered by hazardous dendrite growth and huge volume variations during Li plating/stripping.Herein,we reported a borondoped three-dimensional(3D)layered MXene(Ti_(3)C_(2)T_(x))as the host of Li metal anode.The material was synthesized via a facile one-pot hydrothermal process.With uniform B-doping,the prepared 3D multilayered MXene sheets provided more sites for nucleation of Li metal,so that the deposited Li metal anode showed favorable cycling stability and a high Coulombic efficiency.With the use of the same host material,a hybrid lithium-metal battery with 3D Li anode coupling with LiFePO4 cathode showed long cycle life and favorable electrochemical stability.This work shed lights on reasonable structural and compositional design of host materials that enables high-performance Li-metal anode toward practical realization of highenergy rechargeable batteries。
基金financially supported by the National Natural Science Foundation of China(Nos.51902238 and 52172234)the Fundamental Research Funds for the Central Universities(Nos.2020IVA069,2020IVB043 and 2021IVA020B)
文摘Rechargeable batteries based on solid-state electrolytes are of great interest and importance for the next-generation energy storage due to their high energy output and improved safety.For building the solid-state batteries,Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)represents a promising candidate as it features high chemical stability against air exposure and a high Na^(+)conductivity.NZSP pellets were usually calcined at a high temperature,and the high volatility of Na and P elements easily led to the formation of impurity phase.In this work,the effects of calcination temperature and stoichiometry on the phase purity and ionic conductivity of the NZSP electrolyte were studied.At an elevated sintering temperature,the NZSP electrolyte showed a high ionic conductivity owing to decreased porosity,and the highest ionic conductivity at 30℃was observed to be 2.75×10^(-5)S·cm^(-1)with an activation energy of 0.41 eV.For the stoichiometry,the introduction of 5 mol%excessive P results in formation of more Na_(3)PO_(4) and glass-like phase at the grain boundary,which caused the blurred grain boundary and reduced grain barrier,and effectively suppressed Na dendrite growth,then accounted for improved cycling performance of a Na‖Na symmetric cell.Our work provided insights on reasonable design and preparation of NZSP electrolyte towards practical realization of solid-state Na-metal batteries.
