Rechargeable Mg batteries(RMBs)have become one of the best subsitutes for lithium-ion batteries due to the high volumetric capacity,abundant resources,and uniform plating behavior of Mg metal anode.However,the safety ...Rechargeable Mg batteries(RMBs)have become one of the best subsitutes for lithium-ion batteries due to the high volumetric capacity,abundant resources,and uniform plating behavior of Mg metal anode.However,the safety hazard induced by the formation of high-modulue Mg dendrites under a high current density(10 mA cm^(-1))was still revealed in recent years.It has forced researchers to re-examine the safety of RMBs.In this review,the intrinsic safety factors of key components in RMBs,such as uneven plating,pitting and flammability of Mg anode,heat release and crystalline water decomposition of cathode,strong corrosion,low oxidition stability and flammability of electrolytes,and soforth,are systematacially summarized.Their origins,formation mechanisms,and possible safety hazards are deeply discussed.To develop high-performance Mg anode,current strategies including designing artificial SEI,three-dimensional substrates,and Mg alloys are summarized.For practical electrolytes,the configurations of boron-centered anions and simple Mg salts and the functionalized solvent with high boiling point and low flammability are suggested to comprehensively design.In addition,the future study should more focus on the investigation on the thermal runaway and decomposition of cathode materials and separa-tors.This review aims to provide fundamental insights into the relationship between electrochemistry and safety,further promoting the sustainable development of RMBs.展开更多
Generally,the practical capacity of an electrode should include the weight of non-active components such as current collector,polymer binder,and conductive additives,which were as high as 70 wt%in current reported wor...Generally,the practical capacity of an electrode should include the weight of non-active components such as current collector,polymer binder,and conductive additives,which were as high as 70 wt%in current reported works,seriously limiting the practical capacity.This work pioneered the usage of ultralight reduced graphene fiber(rGF)fabrics as conductive scaffolds,aiming to reduce the weight of nonactive components and enhance the practical capacity.Ultrathin SnS2 nanosheets/rGF hybrids were prepared and used as binder-free electrodes of sodium-ion batteries(SIBs).The interfused graphene fibers endow the electrode a porous,continuous,and conductive network.The in situ phase transformation from SnO2 to SnS2 could preserve the strong interfacial interactions between SnS2 and graphene.Benefitting from these,the designed binder-free electrode delivers a high specific capacity of 500 mAh g?1 after 500 cycles at a current rate of 0.5 A g?1 with almost 100%Coulombic efficiency.Furthermore,the weight percentage of SnS2 in the whole electrode could reach up to 67.2 wt%,much higher than that of common electrode configurations using Cu foil,Al foil,or carbon cloth,significantly highlighting the ultralight characters and advantages of the rGF fabrics for using as binder-free electrodes of SIBs.展开更多
Lithium metal anode is the most potential anode material for the next generation high-energy rechargeable batteries owing to its highest specific capacity and lowest redox potential.Unfortunately,the uneven deposition...Lithium metal anode is the most potential anode material for the next generation high-energy rechargeable batteries owing to its highest specific capacity and lowest redox potential.Unfortunately,the uneven deposition of Li during plating/stripping and the formation of uncontrolled Li dendrites,which might cause poor battery performance and serious safety problems,are demonstrating to be a huge challenge for its practical application.Here,we show that a flexible and free-standing film hybriding with polypyrrole(PPy) nanotubes and reduced graphene oxide(rGO) can significantly regulate the Li nucleation and deposition,and further prohibit the formation of Li dendrites,owing to the large specific surface area,rich of nitrogen functional groups and porous structures.Finally,the high Coulombic efficiency and stable Li plating/stripping cycling performance with 98% for 230 cycles at 0.5 mA cm^(-2) and more than 900 hours stable lifespan are achieved.No Li dendrites form even at a Li deposition capacity as high as4.0 mA h cm^(-2).Besides,the designed PPy/rGO hybrid anode scaffold can also drive a superior battery performance in the lithium-metal full cell applications.展开更多
The rechargeable Mg-S batteries are attractive because of their resource abundances of Mg and S,high volumetric energy density,and less dendrite property of Mg anodes.However,the development is barred by the intrinsic...The rechargeable Mg-S batteries are attractive because of their resource abundances of Mg and S,high volumetric energy density,and less dendrite property of Mg anodes.However,the development is barred by the intrinsic low electronic conductivity of S and the discharge products as well as the lack of understanding the hidden electrochemical kinetics.Here,a Co_(3)S_(4)@MXene heterostructure is proposed as effective sulfur host for reversible Mg-S batteries.XPS results and density functional theory(DFT)calculation confirm that the chemical interaction between the decorated Co_(3)S_(4)nanocrystals host and polysulfide intermediates could well absorb and catalyze the polysulfides conversion,thus improve the electrochemical redox kinetics.Meanwhile,the MXene matrix could promote Mg ion diffusion dynamics greatly.As a result,the developed Mg-S batteries using the Co_(3)S_(4)@MXene-S as the cathode material could demonstrate high sulfur utilization with specific capacity of 1220 mAh g^(-1) and retain a capacity of 528 mAh g^(-1) after 100 cycles,together with a satisfactory rate performance even at 2 C.This work shed light on the advanced cathode design for reversible high energy Mg-S batteries.展开更多
Zinc-air batteries(ZnABs) with high theoretical capacity and environmental benignity are the most promising candidates for next-generation electronics. However, their large-scale applications are greatly hindered due ...Zinc-air batteries(ZnABs) with high theoretical capacity and environmental benignity are the most promising candidates for next-generation electronics. However, their large-scale applications are greatly hindered due to the lack of high-efficient and cost-effective electrocatalysts. Transition metal phosphides(TMPs) have been reported as promising electrocatalysts. Notably,(Ni_(1-x)Cr_(x))_(2) P(0≤x≤0.15) is an unstable electrocatalyst, which undergoes in-situ electrochemical oxidation during the initial oxygen evolution reaction(OER) and even in the activation cycles, and is eventually converted to Cr-NiOOH serving as the actual OER active sites with high efficiency. Density functional theory(DFT) simulations and experimental results elucidate that the OER performance could be significantly promoted by the synergistic effect of surface engineering and electronic modulations by Cr doping and in-situ phase transformation. The constructed rechargeable ZnABs could stably cycle for more than 208 h at 5 m A cm^(-2), while the voltage degradation is negligible. Furthermore, the developed catalytic materials could be assembled into flexible and all-solid-state Zn ABs to power wearable electronics with high performance.展开更多
Solid-state lithium-metal-batteries(SSLMBs)using garnet Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)as the solid electrolyte are expected to conquer the safety concerns of high energy Li batteries with organic liquid e...Solid-state lithium-metal-batteries(SSLMBs)using garnet Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)as the solid electrolyte are expected to conquer the safety concerns of high energy Li batteries with organic liquid electrolytes owing to its nonflammable nature and good mechanical strength.However,the poor interfacial contact between the Li anode and LLZTO greatly restrains the practical applications of the electrolyte,because large polarization,dendritic Li formation and penetration can occur at the interfaces.Here,an effective method is proposed to improve the wettability of the LLZTO toward lithium and reduce the interfacial resistance by engineering universal lithiophilic interfacial layers.Thanks to the in-situ formed lithiophilic and ionic conductive Co/Li_(2)O interlayers,the symmetric Li/CoO-LLZTO/Li batteries present much smaller overpotential,ultra-low areal specific resistance(ASR,12.3 X cm^(2)),high critical current density(CCD,1.1 mA cm^(-2)),and outstanding cycling performance(1696 h at a current density of 0.3 mA cm^(-2))at 25℃.Besides,the solid-state Li/CoO-LLZTO/LFP cells deliver an excellent electrochemical performance with a high coulombic efficiency of~100%and a long cycling time over 185 times.Surprisingly,the high-voltage(4.6 V)solid state Li/CoO-LLZTO/Li_(1.4)Mn_(0.6)Ni_(0.2)Co_(0.2)O_(2.4)(LMNC622)batteries can also realize an ultra-high specific capacity(232.5 mAh g-1)under 0.1 C at 25℃.This work paves an effective way for practical applications of the dendrite-free SSLMBs.展开更多
Marine microbial eukaryotes are important primary producers and play critical roles in key biogeochemical cycles.Recent advances in sequencing technology have focused attention on the extent of microbial biodiversity,...Marine microbial eukaryotes are important primary producers and play critical roles in key biogeochemical cycles.Recent advances in sequencing technology have focused attention on the extent of microbial biodiversity,revealing a huge,previously underestimated phylogenetic diversity with many new lineages.This technology has now become the most important tool to understand the ecological signifcance of this huge and novel diversity in polar oceans.In particular,high-throughput sequencing technologies have been successfully applied to enumerate and compare marine microbial diversity in polar environments.Here,a brief overview of polar microbial eukaryote diversity,as revealed by in-situ surveys of the high-throughput sequencing on 18S rRNA gene,is presented.Using these‘omic’approaches,further attention still needs to be focused on diferences between specifc locations and/or entire polar oceans and on bipolar comparisons of diversity and distribution.展开更多
Background:Distinct neuroanatomic subtypes have been identified in never-treated patients with schizophrenia based on cerebral structural abnormalities,but whether antipsychotic-treated patients would be stratified un...Background:Distinct neuroanatomic subtypes have been identified in never-treated patients with schizophrenia based on cerebral structural abnormalities,but whether antipsychotic-treated patients would be stratified under the guidance of such previously formed classification remains unclear.Objective:The present study aimed to investigate alterations of brain structures in antipsychotic-treated patients with schizophrenia based on a predefined morphological classification and their relationships with cognitive performance.Methods:Cortical thickness,surface area,and subcortical volume were extracted from 147 antipsychotictreated patients with schizophrenia using structural magnetic resonance imaging for classification.The Brief Assessment of Cognition in Schizophrenia(BACS)and Positive and Negative Syndrome Scale(PANSS)were used to assess cognition and symptoms.Results:Antipsychotic-treated patients were categorized into three subtypes with distinct patterns of brain morphological alterations.Subtypes 1 and 2 were characterized by widespread deficits in cortical thickness but relatively limited deficits in surface area.In contrast,subtype 3 demonstrated cortical thickening mainly in parietal-occipital regions and widespread deficits in surface area.All three subgroups demonstrated cognitive deficits compared with healthy controls.Significant associations between neuroanatomic and cognitive abnormalitieswere only observed in subtype 1,where cortical thinning in the left lingual gyruswas conversely related to symbol coding performance.Conclusions:Similar to drug-naıve patients,neuroanatomic heterogeneity exists in antipsychotic-treated patients,with disparate associations with cognition.These findings promote our understanding of relationships between neuroanatomic abnormalities and cognitive performance in the context of heterogeneity.Moreover,these results suggest that neurobiological heterogeneity needs to be considered in cognitive research in schizophrenia.展开更多
基金supported by the National Key R&D Program of China(No.2023YFB3809500)the National Natural Science Foundation of China(No.U23A20555,52202211)+1 种基金the Ninth Young Elite Scientists Sponsorship Program by CAST(2023QNRC001)the Chongqing Technology Innovation and Application Development Project(No.CSTB2022TIAD-KPX0028).
文摘Rechargeable Mg batteries(RMBs)have become one of the best subsitutes for lithium-ion batteries due to the high volumetric capacity,abundant resources,and uniform plating behavior of Mg metal anode.However,the safety hazard induced by the formation of high-modulue Mg dendrites under a high current density(10 mA cm^(-1))was still revealed in recent years.It has forced researchers to re-examine the safety of RMBs.In this review,the intrinsic safety factors of key components in RMBs,such as uneven plating,pitting and flammability of Mg anode,heat release and crystalline water decomposition of cathode,strong corrosion,low oxidition stability and flammability of electrolytes,and soforth,are systematacially summarized.Their origins,formation mechanisms,and possible safety hazards are deeply discussed.To develop high-performance Mg anode,current strategies including designing artificial SEI,three-dimensional substrates,and Mg alloys are summarized.For practical electrolytes,the configurations of boron-centered anions and simple Mg salts and the functionalized solvent with high boiling point and low flammability are suggested to comprehensively design.In addition,the future study should more focus on the investigation on the thermal runaway and decomposition of cathode materials and separa-tors.This review aims to provide fundamental insights into the relationship between electrochemistry and safety,further promoting the sustainable development of RMBs.
基金financially supported by the National Natural Science Foundation of China(Nos.21503025,21503178 and 21603019)Fundamental Research Funds for the Central Universities(Nos.0903005203377 and 106112016CDJZR325520)+3 种基金Key Program for International Science and Technology Cooperation Projects of Ministry of Science and Technology of China(No.2016YFE0125900)Venture and Innovation Support Program for Chongqing Overseas Returnees(cx2017060 and cx2017115)Chongqing Research Program of Basic Research and Frontier Technology(No.cstc2016jcyjA1059)Hundred Talents Program of Chongqing University.
文摘Generally,the practical capacity of an electrode should include the weight of non-active components such as current collector,polymer binder,and conductive additives,which were as high as 70 wt%in current reported works,seriously limiting the practical capacity.This work pioneered the usage of ultralight reduced graphene fiber(rGF)fabrics as conductive scaffolds,aiming to reduce the weight of nonactive components and enhance the practical capacity.Ultrathin SnS2 nanosheets/rGF hybrids were prepared and used as binder-free electrodes of sodium-ion batteries(SIBs).The interfused graphene fibers endow the electrode a porous,continuous,and conductive network.The in situ phase transformation from SnO2 to SnS2 could preserve the strong interfacial interactions between SnS2 and graphene.Benefitting from these,the designed binder-free electrode delivers a high specific capacity of 500 mAh g?1 after 500 cycles at a current rate of 0.5 A g?1 with almost 100%Coulombic efficiency.Furthermore,the weight percentage of SnS2 in the whole electrode could reach up to 67.2 wt%,much higher than that of common electrode configurations using Cu foil,Al foil,or carbon cloth,significantly highlighting the ultralight characters and advantages of the rGF fabrics for using as binder-free electrodes of SIBs.
基金supported by the National Natural Science Foundation of China(Nos.21603019,201503025)Key Program for International Science and Technology Cooperation Projects of Ministry of Science and Technology of China(No.2016YFE0125900)program for the Hundred Talents Program of Chongqing University。
文摘Lithium metal anode is the most potential anode material for the next generation high-energy rechargeable batteries owing to its highest specific capacity and lowest redox potential.Unfortunately,the uneven deposition of Li during plating/stripping and the formation of uncontrolled Li dendrites,which might cause poor battery performance and serious safety problems,are demonstrating to be a huge challenge for its practical application.Here,we show that a flexible and free-standing film hybriding with polypyrrole(PPy) nanotubes and reduced graphene oxide(rGO) can significantly regulate the Li nucleation and deposition,and further prohibit the formation of Li dendrites,owing to the large specific surface area,rich of nitrogen functional groups and porous structures.Finally,the high Coulombic efficiency and stable Li plating/stripping cycling performance with 98% for 230 cycles at 0.5 mA cm^(-2) and more than 900 hours stable lifespan are achieved.No Li dendrites form even at a Li deposition capacity as high as4.0 mA h cm^(-2).Besides,the designed PPy/rGO hybrid anode scaffold can also drive a superior battery performance in the lithium-metal full cell applications.
基金This work was financially supported by the National Natu-ral Science Foundation of China(No.21603019)the Opening Project of State Key Laboratory of High Performance Ce-ramics and Superfine Microstructure(SKL201807SIC)program for the Hundred Talents Program of Chongqing University.
文摘The rechargeable Mg-S batteries are attractive because of their resource abundances of Mg and S,high volumetric energy density,and less dendrite property of Mg anodes.However,the development is barred by the intrinsic low electronic conductivity of S and the discharge products as well as the lack of understanding the hidden electrochemical kinetics.Here,a Co_(3)S_(4)@MXene heterostructure is proposed as effective sulfur host for reversible Mg-S batteries.XPS results and density functional theory(DFT)calculation confirm that the chemical interaction between the decorated Co_(3)S_(4)nanocrystals host and polysulfide intermediates could well absorb and catalyze the polysulfides conversion,thus improve the electrochemical redox kinetics.Meanwhile,the MXene matrix could promote Mg ion diffusion dynamics greatly.As a result,the developed Mg-S batteries using the Co_(3)S_(4)@MXene-S as the cathode material could demonstrate high sulfur utilization with specific capacity of 1220 mAh g^(-1) and retain a capacity of 528 mAh g^(-1) after 100 cycles,together with a satisfactory rate performance even at 2 C.This work shed light on the advanced cathode design for reversible high energy Mg-S batteries.
基金supported by the National Natural Science Foundation of China (21603019 and 201503025)the National Key Research and Development Program of China (2016YFE0125900)the program for the Hundred Talents Program of Chongqing University。
文摘Zinc-air batteries(ZnABs) with high theoretical capacity and environmental benignity are the most promising candidates for next-generation electronics. However, their large-scale applications are greatly hindered due to the lack of high-efficient and cost-effective electrocatalysts. Transition metal phosphides(TMPs) have been reported as promising electrocatalysts. Notably,(Ni_(1-x)Cr_(x))_(2) P(0≤x≤0.15) is an unstable electrocatalyst, which undergoes in-situ electrochemical oxidation during the initial oxygen evolution reaction(OER) and even in the activation cycles, and is eventually converted to Cr-NiOOH serving as the actual OER active sites with high efficiency. Density functional theory(DFT) simulations and experimental results elucidate that the OER performance could be significantly promoted by the synergistic effect of surface engineering and electronic modulations by Cr doping and in-situ phase transformation. The constructed rechargeable ZnABs could stably cycle for more than 208 h at 5 m A cm^(-2), while the voltage degradation is negligible. Furthermore, the developed catalytic materials could be assembled into flexible and all-solid-state Zn ABs to power wearable electronics with high performance.
基金supported by the National Natural Science Foundation of China (21603019 and 201503025)Program for the Hundred Talents Program of Chongqing University。
文摘Solid-state lithium-metal-batteries(SSLMBs)using garnet Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)as the solid electrolyte are expected to conquer the safety concerns of high energy Li batteries with organic liquid electrolytes owing to its nonflammable nature and good mechanical strength.However,the poor interfacial contact between the Li anode and LLZTO greatly restrains the practical applications of the electrolyte,because large polarization,dendritic Li formation and penetration can occur at the interfaces.Here,an effective method is proposed to improve the wettability of the LLZTO toward lithium and reduce the interfacial resistance by engineering universal lithiophilic interfacial layers.Thanks to the in-situ formed lithiophilic and ionic conductive Co/Li_(2)O interlayers,the symmetric Li/CoO-LLZTO/Li batteries present much smaller overpotential,ultra-low areal specific resistance(ASR,12.3 X cm^(2)),high critical current density(CCD,1.1 mA cm^(-2)),and outstanding cycling performance(1696 h at a current density of 0.3 mA cm^(-2))at 25℃.Besides,the solid-state Li/CoO-LLZTO/LFP cells deliver an excellent electrochemical performance with a high coulombic efficiency of~100%and a long cycling time over 185 times.Surprisingly,the high-voltage(4.6 V)solid state Li/CoO-LLZTO/Li_(1.4)Mn_(0.6)Ni_(0.2)Co_(0.2)O_(2.4)(LMNC622)batteries can also realize an ultra-high specific capacity(232.5 mAh g-1)under 0.1 C at 25℃.This work paves an effective way for practical applications of the dendrite-free SSLMBs.
基金This work is supported by the Natural Science Foundation of China(no.41676178)the Marine S&T Fund of Shandong Province for Pilot National Laboratory for Marine Science and Technology(Qingdao),China(nos.2018SDKJ0104-4,2018SDKJ0406-6)+1 种基金the National Key Research and Development Program of China(no.2017YFA0603200)the Grant from Education Department of Shandong Province(S190007170001).
文摘Marine microbial eukaryotes are important primary producers and play critical roles in key biogeochemical cycles.Recent advances in sequencing technology have focused attention on the extent of microbial biodiversity,revealing a huge,previously underestimated phylogenetic diversity with many new lineages.This technology has now become the most important tool to understand the ecological signifcance of this huge and novel diversity in polar oceans.In particular,high-throughput sequencing technologies have been successfully applied to enumerate and compare marine microbial diversity in polar environments.Here,a brief overview of polar microbial eukaryote diversity,as revealed by in-situ surveys of the high-throughput sequencing on 18S rRNA gene,is presented.Using these‘omic’approaches,further attention still needs to be focused on diferences between specifc locations and/or entire polar oceans and on bipolar comparisons of diversity and distribution.
基金supported by the National Natural Science Foundation of China[Grant Nos.82120108014(to S.L.),82071908(to S.L.),81671664(to S.L.),81621003(to Q.G.),81820108018(to Q.G.),and 81901705(to Y.X.)]the US-China joint grant[Grant Nos NSFC81761128023(to Q.G.),R01MH112189-01(to Q.G.)]+4 种基金1.3.5 project for disciplines of excellence,West China Hospital,Sichuan University[Project Nos.ZYYC08001(to S.L.)and ZYJC18020(to S.L.)]Sichuan Science and Technology Program[Grant Nos.2021JDTD0002(to S.L.)and 2020YFS0116(to Y.X.)]China Postdoctoral Science Foundation[Grant No.2019M663513(to Y.X.)]the Postdoctoral Interdisciplinary Research Project of Sichuan University[Grant No.0040204153082(to Y.X.)]S.L.acknowledges support from Humboldt Foundation Research Awards and Chang Jiang Scholars(Program No.T2019069).
文摘Background:Distinct neuroanatomic subtypes have been identified in never-treated patients with schizophrenia based on cerebral structural abnormalities,but whether antipsychotic-treated patients would be stratified under the guidance of such previously formed classification remains unclear.Objective:The present study aimed to investigate alterations of brain structures in antipsychotic-treated patients with schizophrenia based on a predefined morphological classification and their relationships with cognitive performance.Methods:Cortical thickness,surface area,and subcortical volume were extracted from 147 antipsychotictreated patients with schizophrenia using structural magnetic resonance imaging for classification.The Brief Assessment of Cognition in Schizophrenia(BACS)and Positive and Negative Syndrome Scale(PANSS)were used to assess cognition and symptoms.Results:Antipsychotic-treated patients were categorized into three subtypes with distinct patterns of brain morphological alterations.Subtypes 1 and 2 were characterized by widespread deficits in cortical thickness but relatively limited deficits in surface area.In contrast,subtype 3 demonstrated cortical thickening mainly in parietal-occipital regions and widespread deficits in surface area.All three subgroups demonstrated cognitive deficits compared with healthy controls.Significant associations between neuroanatomic and cognitive abnormalitieswere only observed in subtype 1,where cortical thinning in the left lingual gyruswas conversely related to symbol coding performance.Conclusions:Similar to drug-naıve patients,neuroanatomic heterogeneity exists in antipsychotic-treated patients,with disparate associations with cognition.These findings promote our understanding of relationships between neuroanatomic abnormalities and cognitive performance in the context of heterogeneity.Moreover,these results suggest that neurobiological heterogeneity needs to be considered in cognitive research in schizophrenia.
