Lithium-ion batteries(LIBs)with the“double-high”characteristics of high energy density and high power density are in urgent demand for facilitating the development of advanced portable electronics.However,the lithiu...Lithium-ion batteries(LIBs)with the“double-high”characteristics of high energy density and high power density are in urgent demand for facilitating the development of advanced portable electronics.However,the lithium ion(Li+)-storage performance of the most commercialized lithium cobalt oxide(LiCoO_(2),LCO)cathodes is still far from satisfactory in terms of high-voltage and fast-charging capabilities for reaching the double-high target.Herein,we systematically summarize and discuss high-voltage and fast-charging LCO cathodes,covering in depth the key fundamental challenges,latest advancements in modification strategies,and future perspectives in this field.Comprehensive and elaborated discussions are first presented on key fundamental challenges related to structural degradation,interfacial instability,the inhomogeneity reactions,and sluggish interfacial kinetics.We provide an instructive summary of deep insights into promising modification strategies and underlying mechanisms,categorized into element doping(Li-site,cobalt-/oxygen-site,and multi-site doping)for improved Li+diffusivity and bulkstructure stability;surface coating(dielectrics,ionic/electronic conductors,and their combination)for surface stability and conductivity;nanosizing;combinations of these strategies;and other strategies(i.e.,optimization of the electrolyte,binder,tortuosity of electrodes,charging protocols,and prelithiation methods).Finally,forward-looking perspectives and promising directions are sketched out and insightfully elucidated,providing constructive suggestions and instructions for designing and realizing high-voltage and fast-charging LCO cathodes for next-generation double-high LIBs.展开更多
High-voltage and fast-charging LiCoO_(2)(LCO)is key to high-energy/power-density Li-ion batteries.However,unstable surface structure and unfavorable electronic/ionic conductivity severely hinder its high-voltage fast-...High-voltage and fast-charging LiCoO_(2)(LCO)is key to high-energy/power-density Li-ion batteries.However,unstable surface structure and unfavorable electronic/ionic conductivity severely hinder its high-voltage fast-charging cyclability.Here,we construct a Li/Na-B-Mg-Si-O-F-rich mixed ion/electron interface network on the 4.65 V LCO electrode to enhance its rate capability and long-term cycling stability.Specifically,the resulting artificial hybrid conductive network enhances the reversible conversion of Co^(3+)/^(4+)/O_(2)/nredox by the interfacial ion–electron cooperation and suppresses interface side reactions,inducing an ultrathin yet compact cathode electrolyte interphase.Simultaneously,the derived near-surface Na+/Mg2+/Si^(4+)-pillared local intercalation structure greatly promotes the Li^(+)diffusion around the 4.55 V phase transition and stabilizes the cathode interface.Finally,excellent 3 C(1 C=274 mA g1)fast charging performance is demonstrated with 73.8%capacity retention over 1000 cycles.Our findings shed new insights to the fundamental mechanism of interfacial ion/electron synergy in stabilizing and enhancing fast-charging cathode materials.展开更多
Controlled pedigrees and the multi-decade timescale of national crop plant breeding programs offer a unique experimental context for examining how selection affects plant genomes.More than 3000 wheat cultivars have be...Controlled pedigrees and the multi-decade timescale of national crop plant breeding programs offer a unique experimental context for examining how selection affects plant genomes.More than 3000 wheat cultivars have been registered,released,and documented since 1949 in China.In this study,a set of 145 elite cultivars selected from historical points of wheat breeding in China were re-sequenced.A total of 43.75 Tb of sequence data were generated with an average read depth of 17.94x for each cultivar,and more than 60.92 million SNPs and 2.54 million InDels were captured,based on the Chinese Spring RefSeq genome v1.0.Seventy years of breeder-driven selection led to dramatic changes in grain yield and related phenotypes,with distinct genomic regions and phenotypes tar-geted by different breeders across the decades.There are very clear instances illustrating how introduced Italian and otherforeign germplasm was integrated into Chinese wheat programs and reshaped the genomic landscape of local modern cultivars.Importantly,the resequencing data also highlighted significant asymmetric breeding selec-tion among the three sub-genomes:this was evident in both the collinear blocks for homeologous chromosomes and among sets of three homeologous genes.Accumulation of more newly assembled genes in newer cultivars implied the potential value of these genes in breeding.Conserved and extended sharing of linkage disequilibrium(LD)blocks was highlighted among pedigree-related cultivars,in which fewer haplotype differences were detected.Fixation or replacement of haplotypes from founder genotypes after generations of breeding was related to their breeding value.Based on the haplotype frequency changes in LD blocks of pedigree-related cultivars,we propose a strategy for evaluating the breeding value of any given line on the basis of the accumulation(pyramiding)of bene-ficial haplotypes.Collectively,our study demonstrates the influence of "founder genotypes" on the output of breeding efforts over many decades and also suggests that founder genotype perspectives are in fact more dy-namic when applied in the context of modern genomics-informed breeding.展开更多
Two-dimensional(2 D)heterostructural Ni2 P/rGO is successfully fabricated by in-situ phosphating selfassembled NiO/rGO composites and shows the enhanced electrochemical performances.In this design,the rGO sheets effec...Two-dimensional(2 D)heterostructural Ni2 P/rGO is successfully fabricated by in-situ phosphating selfassembled NiO/rGO composites and shows the enhanced electrochemical performances.In this design,the rGO sheets effectively reduce the lattice strain created during the phase transformation from NiO to Ni2 P,thereby maintaining ultrathin nanostructures of Ni2 P.The resulting Ni2 P/rGO layered heterostructure gives the composite plenty of pores or channels,good electrical conductivity and well-exposed active sites.Density functional theory(DFT)calculation further demonstrates that the Fermi energy level and electron localize of near Ni atoms in Ni2 P is higher than that of NiO,which endow Ni2 P with faster and more reversible redox reactivity in dynamic.Benefiting from their structural and compositional merits,the as-synthesized Ni2 P/rGO exhibits high specific discharge capacity and excellent rate performance.Furthermore,a hybrid supercapacitor built with Ni2 P/rGO and activated carbon shows a high specific energy of 38.6 Wh/kg at specific power of 375 W/kg.展开更多
基金supported by the National Key Research and Development Program of China(2022YFA1504100)the National Natural Science Foundation of China(22125903,51872283,and 22005298)+4 种基金Dalian Innovation Support Plan for High Level Talents(2019RT09)Dalian National Laboratory For Clean Energy(DNL),Chinese Academy of Sciences(CAS),DNL Cooperation Fund,CAS(DNL202016 and DNL202019)Dalian Institute of Chemical Physics(DICP I2020032)Exploratory Research Project of Yanchang Petroleum International Limited and DICP(yc-hw-2022ky-01)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2021002 and 2021009).
文摘Lithium-ion batteries(LIBs)with the“double-high”characteristics of high energy density and high power density are in urgent demand for facilitating the development of advanced portable electronics.However,the lithium ion(Li+)-storage performance of the most commercialized lithium cobalt oxide(LiCoO_(2),LCO)cathodes is still far from satisfactory in terms of high-voltage and fast-charging capabilities for reaching the double-high target.Herein,we systematically summarize and discuss high-voltage and fast-charging LCO cathodes,covering in depth the key fundamental challenges,latest advancements in modification strategies,and future perspectives in this field.Comprehensive and elaborated discussions are first presented on key fundamental challenges related to structural degradation,interfacial instability,the inhomogeneity reactions,and sluggish interfacial kinetics.We provide an instructive summary of deep insights into promising modification strategies and underlying mechanisms,categorized into element doping(Li-site,cobalt-/oxygen-site,and multi-site doping)for improved Li+diffusivity and bulkstructure stability;surface coating(dielectrics,ionic/electronic conductors,and their combination)for surface stability and conductivity;nanosizing;combinations of these strategies;and other strategies(i.e.,optimization of the electrolyte,binder,tortuosity of electrodes,charging protocols,and prelithiation methods).Finally,forward-looking perspectives and promising directions are sketched out and insightfully elucidated,providing constructive suggestions and instructions for designing and realizing high-voltage and fast-charging LCO cathodes for next-generation double-high LIBs.
基金supported by the National Natural Science Foundation of China(22125903,51872283,and 22005298)the National Key R&D Program of China(2022YFA1504100 and 2023YFB4005204)+3 种基金Dalian Innovation Support Plan for High Level Talents(2019RT09)Dalian Institute of Chemical Physics(DICP I2020032)The Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2021002,YLU-DNL Fund 2021009)Exploratory Research Project of Yanchang Petroleum International Limited and DICP(yc-hw-2022ky-01).
文摘High-voltage and fast-charging LiCoO_(2)(LCO)is key to high-energy/power-density Li-ion batteries.However,unstable surface structure and unfavorable electronic/ionic conductivity severely hinder its high-voltage fast-charging cyclability.Here,we construct a Li/Na-B-Mg-Si-O-F-rich mixed ion/electron interface network on the 4.65 V LCO electrode to enhance its rate capability and long-term cycling stability.Specifically,the resulting artificial hybrid conductive network enhances the reversible conversion of Co^(3+)/^(4+)/O_(2)/nredox by the interfacial ion–electron cooperation and suppresses interface side reactions,inducing an ultrathin yet compact cathode electrolyte interphase.Simultaneously,the derived near-surface Na+/Mg2+/Si^(4+)-pillared local intercalation structure greatly promotes the Li^(+)diffusion around the 4.55 V phase transition and stabilizes the cathode interface.Finally,excellent 3 C(1 C=274 mA g1)fast charging performance is demonstrated with 73.8%capacity retention over 1000 cycles.Our findings shed new insights to the fundamental mechanism of interfacial ion/electron synergy in stabilizing and enhancing fast-charging cathode materials.
基金the Key Research and Development Program of China(2016YFD0100302)the Central Public-interest Scientific Institution Basal Research Fund(Y2017PT39)the CAAS-Innovation Team Program(CAAS-XTCX2018020).
文摘Controlled pedigrees and the multi-decade timescale of national crop plant breeding programs offer a unique experimental context for examining how selection affects plant genomes.More than 3000 wheat cultivars have been registered,released,and documented since 1949 in China.In this study,a set of 145 elite cultivars selected from historical points of wheat breeding in China were re-sequenced.A total of 43.75 Tb of sequence data were generated with an average read depth of 17.94x for each cultivar,and more than 60.92 million SNPs and 2.54 million InDels were captured,based on the Chinese Spring RefSeq genome v1.0.Seventy years of breeder-driven selection led to dramatic changes in grain yield and related phenotypes,with distinct genomic regions and phenotypes tar-geted by different breeders across the decades.There are very clear instances illustrating how introduced Italian and otherforeign germplasm was integrated into Chinese wheat programs and reshaped the genomic landscape of local modern cultivars.Importantly,the resequencing data also highlighted significant asymmetric breeding selec-tion among the three sub-genomes:this was evident in both the collinear blocks for homeologous chromosomes and among sets of three homeologous genes.Accumulation of more newly assembled genes in newer cultivars implied the potential value of these genes in breeding.Conserved and extended sharing of linkage disequilibrium(LD)blocks was highlighted among pedigree-related cultivars,in which fewer haplotype differences were detected.Fixation or replacement of haplotypes from founder genotypes after generations of breeding was related to their breeding value.Based on the haplotype frequency changes in LD blocks of pedigree-related cultivars,we propose a strategy for evaluating the breeding value of any given line on the basis of the accumulation(pyramiding)of bene-ficial haplotypes.Collectively,our study demonstrates the influence of "founder genotypes" on the output of breeding efforts over many decades and also suggests that founder genotype perspectives are in fact more dy-namic when applied in the context of modern genomics-informed breeding.
基金supported by the DNL Cooperation Fund,CAS(No.DNL201915)National Science Foundation for Excellent Young Scholars of China(No.21922815)+1 种基金National Natural Science Foundation of China(No.21975275)Key Research and Development(R&D)Projects of Shanxi Province(No.201903D121007)。
文摘Two-dimensional(2 D)heterostructural Ni2 P/rGO is successfully fabricated by in-situ phosphating selfassembled NiO/rGO composites and shows the enhanced electrochemical performances.In this design,the rGO sheets effectively reduce the lattice strain created during the phase transformation from NiO to Ni2 P,thereby maintaining ultrathin nanostructures of Ni2 P.The resulting Ni2 P/rGO layered heterostructure gives the composite plenty of pores or channels,good electrical conductivity and well-exposed active sites.Density functional theory(DFT)calculation further demonstrates that the Fermi energy level and electron localize of near Ni atoms in Ni2 P is higher than that of NiO,which endow Ni2 P with faster and more reversible redox reactivity in dynamic.Benefiting from their structural and compositional merits,the as-synthesized Ni2 P/rGO exhibits high specific discharge capacity and excellent rate performance.Furthermore,a hybrid supercapacitor built with Ni2 P/rGO and activated carbon shows a high specific energy of 38.6 Wh/kg at specific power of 375 W/kg.
