High-energy density lithium-sulfur(Li-S) batteries have received intensive attention as promising energy storage system.Among diverse sulfur-based cathodes,sulfurized pyrolyzed poly(acrylonitrile)(S@pPAN)cathode deliv...High-energy density lithium-sulfur(Li-S) batteries have received intensive attention as promising energy storage system.Among diverse sulfur-based cathodes,sulfurized pyrolyzed poly(acrylonitrile)(S@pPAN)cathode delivered superior electrochemical performance.However,the sulfur content of S@pPAN is relatively low(<50 wt%),which significantly limits the energy density.Herein,a hydrogel SA-Cu binder was proposed with a crosslinking network constructed by Cu^(2+) ions.The introduction of Cu^(2+) ions enabled excellent electrochemical behaviors of S@pPAN cathode even with high sulfur content of 52.6 wt% via chemical interaction with sulfur and polysulfide.Moreover,a favorable cathode interphase was formed containing electrochemically active and conductive CuSx.S@pPAN/SA-Cu exhibited a high sulfur utilization of 85.3%,long cycling stability over 1000 cycles and remarkable capacity of 1200 mAh g_(s)^(-1) even at10 C.Furthermore,ascribed to the improved electrode structure,high-loading electrode(sulfur loading:4 mg cm^(-2)) displayed stable cycling with areal capacity of 5.26 mAh cm^(-2)(1315 mAh g_(s)^(-1)) after 40 cycles.This study provides new directions to prepare high-sulfur content and high-loading S@pPAN cathode for higher energy density.展开更多
S@pPAN has become promising cathode materials in rechargeable batteries due to its high compressed density,low E/S ratio,no polysulfide dissolution,no self-discharge,and stable cycling.However,it is a big challenge to...S@pPAN has become promising cathode materials in rechargeable batteries due to its high compressed density,low E/S ratio,no polysulfide dissolution,no self-discharge,and stable cycling.However,it is a big challenge to enhance its sulfur content which determines its practical specific capacity.Herein,we prepare crosslinked PAN as precursor,leading to effective enhancement of sulfur content up to 55 wt%and a reversible specific capacity of 838 mAh g _(composites)^(-1) at 0.2C.Because of the microporous structure and high specific area,crosslinked PAN provides more space to accommodate sulfur molecule and improve the interfacial reaction of S@pPAN as well.This work provides a promising direction to design S@pPAN for lithium sulfur batteries with high energy density.展开更多
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
Sulfurized polyacrylonitrile(S@pPAN)composite provides a conductive pathway for sulfur active material at the molecular level and has already become one of the most promising cathode materials in lithium-sulfur batter...Sulfurized polyacrylonitrile(S@pPAN)composite provides a conductive pathway for sulfur active material at the molecular level and has already become one of the most promising cathode materials in lithium-sulfur batteries because of its outstanding electrochemical performances via novel solid-solid conversion mechanism.Although there are a great number of researches on the S@pPAN composite material,the accurate structure of S@pPAN and its redox reaction mechanism during the charge-discharge process still have not been determined.The previous research and inferences about the structure of S@pPAN and its electrochemical reaction mechanism were summarized in this review,providing a reference for the future study of lithiumsulfur batteries.展开更多
Lithium metal batteries are regarded as promising alternative next-generation energy storage systems.However,the unstable anode interphase results in dendrite growth and irreversible lithium consumption with low Coulo...Lithium metal batteries are regarded as promising alternative next-generation energy storage systems.However,the unstable anode interphase results in dendrite growth and irreversible lithium consumption with low Coulombic efficiency(CE).Herein,we rationally design a Li^(+)coordination structure via electrolyte solvation chemistry.Nitrate anions are aggregated in the solvation sheath,even at low concentration in a solvent with moderate solvation ability,which promotes Li^(+)desolvation and constructs a nitrate anion-tuned interphase.Meanwhile,a high-donor-number solvent is introduced as an additive to strongly coordinate with Li^(+),which accelerates the ion-transfer kinetics and rate performance.This not only results in micro-sized lithium deposition and a high CE of 99.5%over 3500 h,but also enables superior anode stability even under 50%depth plating/stripping and with a lean electrolyte of 3 g Ah^(-1)at 50℃.A lithium-sulfur battery exhibits a prolonged lifespan of 2000 cycles with an average CE of 100%.A full battery using 1x excess lithium exhibits a high capacity near 1600 mAh g S^(-1)for 100 cycles without capacity loss.Moreover,a 0.55 Ah pouch cell delivers a reversible energy density of 423 Wh kg^(-1)based on these electrodes and electrolyte.展开更多
基金financially supported by the National Natural Science Foundation of China (U1705255 and 21975158)the Program of Shanghai Academic Research Leader (20XD1401900)the Key-Area Research and Development Program of Guangdong Province (2019B090908001)。
文摘High-energy density lithium-sulfur(Li-S) batteries have received intensive attention as promising energy storage system.Among diverse sulfur-based cathodes,sulfurized pyrolyzed poly(acrylonitrile)(S@pPAN)cathode delivered superior electrochemical performance.However,the sulfur content of S@pPAN is relatively low(<50 wt%),which significantly limits the energy density.Herein,a hydrogel SA-Cu binder was proposed with a crosslinking network constructed by Cu^(2+) ions.The introduction of Cu^(2+) ions enabled excellent electrochemical behaviors of S@pPAN cathode even with high sulfur content of 52.6 wt% via chemical interaction with sulfur and polysulfide.Moreover,a favorable cathode interphase was formed containing electrochemically active and conductive CuSx.S@pPAN/SA-Cu exhibited a high sulfur utilization of 85.3%,long cycling stability over 1000 cycles and remarkable capacity of 1200 mAh g_(s)^(-1) even at10 C.Furthermore,ascribed to the improved electrode structure,high-loading electrode(sulfur loading:4 mg cm^(-2)) displayed stable cycling with areal capacity of 5.26 mAh cm^(-2)(1315 mAh g_(s)^(-1)) after 40 cycles.This study provides new directions to prepare high-sulfur content and high-loading S@pPAN cathode for higher energy density.
基金financially supported by the National Natural Science Foundation of China (U1705255, 21975158)the Program of Shanghai Academic Research Leader (20XD1401900)the Key-Area Research and Development Program of Guangdong Province (2019B090908001)。
文摘S@pPAN has become promising cathode materials in rechargeable batteries due to its high compressed density,low E/S ratio,no polysulfide dissolution,no self-discharge,and stable cycling.However,it is a big challenge to enhance its sulfur content which determines its practical specific capacity.Herein,we prepare crosslinked PAN as precursor,leading to effective enhancement of sulfur content up to 55 wt%and a reversible specific capacity of 838 mAh g _(composites)^(-1) at 0.2C.Because of the microporous structure and high specific area,crosslinked PAN provides more space to accommodate sulfur molecule and improve the interfacial reaction of S@pPAN as well.This work provides a promising direction to design S@pPAN for lithium sulfur batteries with high energy density.
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supported by the National Key Research and Development(R&D)Program of China(No.2021YFB2400300)the National Natural Science Foundation of China(No.22179083)+1 种基金Program of Shanghai Academic Research Leader(No.20XD1401900)Key-Area Research and Development Program of Guangdong Province(No.2019B090908001).
文摘Sulfurized polyacrylonitrile(S@pPAN)composite provides a conductive pathway for sulfur active material at the molecular level and has already become one of the most promising cathode materials in lithium-sulfur batteries because of its outstanding electrochemical performances via novel solid-solid conversion mechanism.Although there are a great number of researches on the S@pPAN composite material,the accurate structure of S@pPAN and its redox reaction mechanism during the charge-discharge process still have not been determined.The previous research and inferences about the structure of S@pPAN and its electrochemical reaction mechanism were summarized in this review,providing a reference for the future study of lithiumsulfur batteries.
基金supported by the National Key R&D Program of China(2021YFB2400300)National Natural Science Foundation of China(22179083)+1 种基金Program of Shanghai Academic Research Leader(20XD1401900)Key-Area Research and Development Program of Guangdong Province(2019B090908001).
文摘Lithium metal batteries are regarded as promising alternative next-generation energy storage systems.However,the unstable anode interphase results in dendrite growth and irreversible lithium consumption with low Coulombic efficiency(CE).Herein,we rationally design a Li^(+)coordination structure via electrolyte solvation chemistry.Nitrate anions are aggregated in the solvation sheath,even at low concentration in a solvent with moderate solvation ability,which promotes Li^(+)desolvation and constructs a nitrate anion-tuned interphase.Meanwhile,a high-donor-number solvent is introduced as an additive to strongly coordinate with Li^(+),which accelerates the ion-transfer kinetics and rate performance.This not only results in micro-sized lithium deposition and a high CE of 99.5%over 3500 h,but also enables superior anode stability even under 50%depth plating/stripping and with a lean electrolyte of 3 g Ah^(-1)at 50℃.A lithium-sulfur battery exhibits a prolonged lifespan of 2000 cycles with an average CE of 100%.A full battery using 1x excess lithium exhibits a high capacity near 1600 mAh g S^(-1)for 100 cycles without capacity loss.Moreover,a 0.55 Ah pouch cell delivers a reversible energy density of 423 Wh kg^(-1)based on these electrodes and electrolyte.
