The electrolyte integrated with lithium metal anodes is subjected to the issues of interfacial compatibility and stability,which strongly influence the performances of high-energy lithium metal batteries.Here,we repor...The electrolyte integrated with lithium metal anodes is subjected to the issues of interfacial compatibility and stability,which strongly influence the performances of high-energy lithium metal batteries.Here,we report a new electrolyte recipe viz.a moderately concentrated electrolyte comprising of 2.4 M lithium bis(fluorosulfonyl)imide(LiFSI)in a cosolvent mixture of fluorinated ethylene carbonate(FEC)and dimethyl carbonate(DMC)with relatively high ion conductivity.Owing to the preferential decomposition of LiFSI and FEC,an inorganic-rich interphase with abundant Li_(2)O and LiF nanocrystals is formed on lithium metal with improved robustness and ion transfer kinetics,enabling lithium plating/stripping with an extremely low overpotential of~8 mV and the average CE of 97%.When tested in Li||LiFePO_(4) cell,this electrolyte provides long-term cycling with a capacity retention of 98.3%after 1000 cycles at 1 C and an excellent rate performance of 20 C,as well as an areal capacity of 1.35 mA h cm^(-2)at the cathode areal loading of 9 mg cm^(-2).Moreover,the Li||LiFePO_(4) cell exhibits excellent wide-temperature performances(-40~60℃),including long-term cycling stability over 2600 cycles without visible capacity fading at 0℃,as well as extremely high average CEs of 99.6%and 99.8% over 400 cycles under-20℃ and 45℃.展开更多
Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides an attractive approach to carbon capture and utilization for the production high-value-added products.However,CO_(2)RR still suffers from poor select...Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides an attractive approach to carbon capture and utilization for the production high-value-added products.However,CO_(2)RR still suffers from poor selectivity and low current density due to its sluggish kinetics and multitudinous reaction pathways.Single-atom catalysts(SACs)demonstrate outstanding activity,excellent selectivity,and remarkable atom utilization efficiency,which give impetus to the search for electrocatalytic processes aiming at high selectivity.There appears significant activity in the development of efficient SACs for CO_(2)RR,while the density of the atomic sites remains a considerable barrier to be overcome.To construct high-metal-loading SACs,aggregation must be prevented,and thus novel strategies are required.The key to creating high-density atomically dispersed sites is designing enough anchoring sites,normally defects,to stabilize the highly mobile separated metal atoms.In this review,we summarized the advances in developing high-loading SACs through defect engineering,with a focus on the synthesis strategies to achieve high atomic site loading.Finally,the future opportunities and challenges for CO_(2)RR in the area of high-loading single-atom electrocatalysts are also discussed.展开更多
Lithium-ion batteries (LIB) have received substantial attention in the last 10 years,as they offer great promise as power sources that can lead to the electric vehicle (EV) revolution in the next 5 years.Since the cat...Lithium-ion batteries (LIB) have received substantial attention in the last 10 years,as they offer great promise as power sources that can lead to the electric vehicle (EV) revolution in the next 5 years.Since the cathode serves as a key component in LIB,its properties significantly affect the performance of the whole system.Recently,the cathode surface modification based on coating technique has been widely employed to enhance the electrochemical performances by improving the material conductivity,stabilising the physical structure of materials,as well as preventing the reactions between the electrode and electrolyte.In this work,we reviewed the present of a number of promising cathode materials for Li-ion batteries.After that,we summarized the very recent research progress focusing on the surface coating strategies,mainly including the coating materials,the coating technologies,as well as the corresponding working mechanisms for cathodes.At last,the challenges faced and future guidelines for optimizing cathode materials are discussed.In this study,we propose that the structure of cathode is a crucial factor during the selection of coating materials and technologies.展开更多
Commercial lithium-ion(Li-ion)batteries based on graphite anodes are meeting their bottlenecks that are limited energy densities.In order to satisfy the large market demands of smaller and lighter rechargeable batteri...Commercial lithium-ion(Li-ion)batteries based on graphite anodes are meeting their bottlenecks that are limited energy densities.In order to satisfy the large market demands of smaller and lighter rechargeable batteries,high-capacity metallic Li replacing low-specific-capacity graphite enables the higher energy density in next-generation rechargeable Li metal batteries(LMBs).However,Li metal anode has been suffering from dendritic problems,interfacial side reactions,volume change and low Coulombic efficiency.Therefore,performance enhancements of Li metal anodes are rather important to realize the high energy density characteristic of metallic Li.In this review,the annoying Li dendrite growth,unstable reaction interface and practical application issues of Li metal anodes are summarized and detailedly discussed to understand the current challenges concerning Li metal anodes.For overcoming such remaining challenges,the corresponding strategies and recent advances are covered and categorized.Finally,we discuss future opportunities and perspectives for developing high-performance Li metal anodes.展开更多
Lithium–sulfur(Li-S)batteries have been considered as promising candidates for large-scale high energy density devices due to the potentially high energy density,low cost,and more pronounced ecological compatibility....Lithium–sulfur(Li-S)batteries have been considered as promising candidates for large-scale high energy density devices due to the potentially high energy density,low cost,and more pronounced ecological compatibility.However,the complex Li-S conversion reactions,unsatisfactory battery performance,and unsafe metallic Li anode restrict the development of Li-S batteries to achieve commercialization.This review mainly focuses on three aspects which are the remaining challenges,recent advances,and applications in Li-S batteries.Firstly,this review portrays Li-S conversion chemistry involving the multi-step and multi-electron reaction mechanism,as well as the remaining challenges.Then,the scientific strategies and very recent advances of the cathode,electrolyte,lithium anode,and other constituent parts of Li-S batteries are detailly summed up,as well as their advantages and limitations.For the sake of promoting the Li-S batteries practicalization,next section is primarily concerned with problems,the corresponding solutions,and application scenarios of practical pouch cells.Finally,the important findings as guidelines and some future directions as trends for developing emerging Li-S batteries are briefly summarized.展开更多
Lithium(Li)metal is the most potential anode material for the next-generation high-energy rechargeable batteries.However,intrinsic surface unevenness and‘hostless’nature of Li metal induces infinite volume effect an...Lithium(Li)metal is the most potential anode material for the next-generation high-energy rechargeable batteries.However,intrinsic surface unevenness and‘hostless’nature of Li metal induces infinite volume effect and uncontrollable dendrite growth.Herein,we design the in-situ grown lithiophilic Ni_(2)P nanoarrays inside nickel foam(PNF).Uniform Ni_(2)P nanoarrays coating presents a very low nucleation overpotential,which induces the homogeneous Li deposition in the entire spaces of three-dimensional(3D)metal framework.Specifically,the lithiophilic Ni_(2)P nanoarrays possess characteristics of electrical conductivity and structural stability,which have almost no expansion and damage during repeating Li plating/stripping.Therefore,they chronically inhibit the growth of Li dendrites.This results in an outstanding Coulombic efficiency(CE)of 98% at 3 mA cm^(-2) and an ultra long cycling life over 2000 cycles with a low overpotential.Consequently,the PNF-Li||LiFePO_(4) battery maintains a capacity retention of 95.3% with a stable CE of 99.9% over 500 cycles at 2 C.展开更多
Objective:The degree of liver cirrhosis is one of the most important diagnostic and prognostic assessments in chronic liver disease.Among the etiologies of liver cirrhosis,hepatitis B virus(HBV)infection-induced liver...Objective:The degree of liver cirrhosis is one of the most important diagnostic and prognostic assessments in chronic liver disease.Among the etiologies of liver cirrhosis,hepatitis B virus(HBV)infection-induced liver damage is most common in Asia-Pacific regions,particularly in China.Many current conventionally used preoperative estimation of liver cirrhosis models.展开更多
Objective:Currently,liver resection is the most effective curative treatment for patients with resectable hepatocellular carcinoma(HCC).Severe post-hepatectomy liver failure(PHLF)is a serious complication for HCC pati...Objective:Currently,liver resection is the most effective curative treatment for patients with resectable hepatocellular carcinoma(HCC).Severe post-hepatectomy liver failure(PHLF)is a serious complication for HCC patients undergoing liver resection.Models have been used to predict severe PHLF in patients with HCC,such as the Child-Pugh score,model for end-stage liver disease(MELD)score.展开更多
The remarkable uplift of the Tibetan Plateau in the Neogene had great impacts on the climate and environment of East Asia and even the world.Therefore,establishment of the Neogene stratigraphic framework of the Tibeta...The remarkable uplift of the Tibetan Plateau in the Neogene had great impacts on the climate and environment of East Asia and even the world.Therefore,establishment of the Neogene stratigraphic framework of the Tibetan Plateau is of great significance to research in various fields of geosciences.Based on marine sediments,the international chronostratigraphic system of the Neogene is divided into six stages in the Miocene and two stages in the Pliocene.Since the beginning of the Cenozoic,the share of terrestrial strata on continents has increased rapidly.By the Neogene,it had far exceeded that of marine strata,and almost all deposits on the Tibetan Plateau and its surrounding areas were terrestrial strata.In China,the Miocene includes five stages and the Pliocene includes two stages.Except for the Tunggurian of the Miocene,which has a lower boundary at 15 Ma,the other stages have the same paleomagnetic definitions and time intervals as the corresponding international marine stages.Mammalian fossils play a very important role in the division and correlation of Cenozoic terrestrial strata,and rodent,carnivore,proboscidean,perissodactyl and artiodactyl fossils are especially important in Neogene terrestrial biostratigraphy.There are many basins with well-exposed strata and abundant mammalian fossils in the Tibetan Plateau.The lower boundary stratotype sections of the Neogene Xiejian and Bahean stages are located respectively in the Xining and Linxia basins,and there are precise paleomagnetic dates in coordination with mammalian fossils.The lower boundary stratotypes of other stages can also be effectively determined in the Tibetan Plateau.Many first appearing mammalian genera in East Asia also appeared in the Tibetan Plateau and its surrounding areas,especially in the Linxia Basin on the northeast margin and in the Siwaliks on the southwest margin.Among them,Prodeinotherium first appeared at the bottom of the Miocene in the Siwaliks,and the earliest Hipparion of the Old World first appeared at the bottom of the Bahean Stage in the Linxia Basin.Carbon and oxygen isotope analysis of enamel and paleosols of Cenozoic sediments and mammal fossils in the Tibetan Plateau and its surrounding areas have been used to reconstruct the climate,environment and vegetation development characteristics,and revealed that these changes were not only related to global change,but also had regional features.Evidence of the Late Miocene C4plant expansion event based on carbon isotope changes comes from the southern margin of the Tibetan Plateau,but in sharp contrast,δ13C indicates that there was still no clear or significant C4plant signal on the northern margin of the Tibetan Plateau until the end of the Neogene.Theδ18O analysis shows that there were several major climate change events in the Cenozoic,especially in the Late Miocene at about 7 Ma,when positive drift ofδ18O indicates that the northern and southern sides of the Tibetan Plateau were changing to drier environments.The strong uplift of the Tibetan Plateau in the Late Miocene strengthened the thermal contrast between sea and land,which strengthened monsoon circulation and led to the expansion of C4vegetation in South Asia.However,the East Asian summer monsoon,which can bring atmospheric precipitation and a climate suitable for C4plants to northern China,was not enough to affect the northern Tibetan Plateau.The Tibetan Plateau on the whole rose to an altitude of about 3000 m in the Miocene,becoming a barrier to mammalian migration;it reached its modern altitude of more than 4000 m in the Pliocene,thus forming a cryosphere environment,which led to the emergence of ancestral types of the Ice Age fauna.展开更多
Lithium metal batteries(LMBs)based on metallic Li exhibit high energy density to be competent for advanced energy storage applications.However,the unstable solid electrolyte interphase(SEI)layer due to continuous deco...Lithium metal batteries(LMBs)based on metallic Li exhibit high energy density to be competent for advanced energy storage applications.However,the unstable solid electrolyte interphase(SEI)layer due to continuous decomposition of electrolytes,and the attendant problem of Li dendrite growth frustrate their commercialization process.Herein,a hybrid SEI comprising abundant LiF,lithiophilic Li-Ge alloy,and Ge nanoparticles is constructed via a simple brush coating method.This fluorinated interface layer with embedded Ge-containing components isolates the Li anode from the corrosive electrolyte and facilitates homogenous Li nucleation as well as uniform growth.Consequently,the modified Li anode exhibits remarkable stability without notorious Li dendrites,delivering stable cycling lives of more than 1000 h for symmetric Li||Li cells and over 600 cycles for Li||Cu cells at 1 mA·cm^(−2).Moreover,the reinforced Li anodes endow multiple full-cell architectures with dramatically improved cyclability under different test conditions.This work provides rational guidance to design an artificial hybrid SEI layer and would stimulate more ideas to solve the dendrite issue and promote the further development of advanced LMBs.展开更多
Major historical events often trigger the rapid flourishing of a few lineages,which in turn shape established biodiversity patterns.How did this process occur and develop?This study provides a window into this issue.T...Major historical events often trigger the rapid flourishing of a few lineages,which in turn shape established biodiversity patterns.How did this process occur and develop?This study provides a window into this issue.The endemic East Asian carps(EEAC)dominated the ichthyofauna of East Asia and exhibited a high degree of adaptation to monsoonal river-lake ecosystems.A series of evidence,including ecogeography,phylogenetics,and macroevolution,suggests that the EEAC is a lineage that arose with the East Asian monsoon and thrived intimately with subsequent monsoon activities.We further deduce the evolution of the EEAC and find that a range of historical events in the monsoon setting(e.g.,marine transgression and regression and glacial-interglacial cycle)have further reshaped the distribution patterns of EEAC’s members.Comparative genomics analyses reveal that introgressions during the initial period of EEAC radiation and innovations in the regulation of the brain and nervous system may have aided their adaptation to river-lake ecosystems in a monsoon setting,which boosted radiation.Overall,this study strengthens knowledge of the evolutionary patterns of freshwater fishes in East Asia and provides a model case for understanding the impact of major historical events on the evolution of biota.展开更多
Holding particular biological resources,the Tibetan Plateau is a unique geologic-geographic-biotic interactively unite and hence play an important role in the global biodiversity domain.The Tibetan Plateau has undergo...Holding particular biological resources,the Tibetan Plateau is a unique geologic-geographic-biotic interactively unite and hence play an important role in the global biodiversity domain.The Tibetan Plateau has undergone vigorous environmental changes since the Cenozoic,and played roles switching from"a paradise of tropical animals and plants"to"the cradle of Ice Age mammalian fauna".Recent significant paleontological discoveries have refined a big picture of the evolutionary history of biodiversity on that plateau against the backdrop of major environmental changes,and paved the way for the assessment of its far-reaching impact upon the biota around the plateau and even in more remote regions.Here,based on the newly reported fossils from the Tibetan Plateau which include diverse animals and plants,we present a general review of the changing biodiversity on the Tibetan Plateau and its influence in a global scale.We define the Tibetan Plateau as a junction station of the history of modern biodiversity,whose performance can be categorized in the following three patterns:(1)Local origination of endemism;(2)Local origination and"Out of Tibet";(3)Intercontinental dispersal via Tibet.The first pattern is exemplified by the snow carps,the major component of the freshwater fish fauna on the plateau,whose temporal distribution pattern of the fossil schizothoracines approximately mirrors the spatial distribution pattern of their living counterparts.Through ascent with modification,their history reflects the biological responses to the stepwise uplift of the Tibetan Plateau.The second pattern is represented by the dispersal history of some mammals since the Pliocene and some plants.The ancestors of some Ice Age mammals,e.g.,the wholly rhino,Arctic fox,and argali sheep first originated and evolved in the uplifted and frozen Tibet during the Pliocene,and then migrated toward the Arctic regions or even the North American continent at beginning of the Ice Age;the ancestor of pantherines(big cats)first rose in Tibetan Plateau during the Pliocene,followed by the disperse of its descendants to other parts of Asia,Africa,North and South America to play as top predators of the local ecosystems.The early members of some plants,e.g.,Elaeagnaceae appeared in Tibet during the Late Eocene and then dispersed and were widely distributed to other regions.The last pattern is typified by the history of the tree of heaven(Ailanthus)and climbing perch.Ailanthus originated in the Indian subcontinent,then colonized into Tibet after the Indian-Asian plate collision,and dispersed therefrom to East Asia,Europe and even North America.The climbing perches among freshwater fishes probably rose in Southeast Asia during the Middle Eocene,dispersed to Tibet and then migrated into Africa via the docked India.These cases highlight the role of Tibet,which was involved in the continental collision,in the intercontinental biotic interchanges.The three evolutionary patterns above reflect both the history of biodiversity on the plateau and the biological and environmental effects of tectonic uplift.展开更多
The northward drift of the Indian Plate and its collision with Eurasia have profoundly impacted the evolutionary history of the terrestrial organisms, especially the ones along the Indian Ocean rim. Climbing perches(A...The northward drift of the Indian Plate and its collision with Eurasia have profoundly impacted the evolutionary history of the terrestrial organisms, especially the ones along the Indian Ocean rim. Climbing perches(Anabantidae) are primary freshwater fishes showing a disjunct south Asian-African distribution,but with an elusive paleobiogeographic history due to the lack of fossil evidence. Here, based on an updated time-calibrated anabantiform phylogeny integrating a number of relevant fossils, the divergence between Asian and African climbing perches is estimated to have occurred in the middle Eocene(ca.40 Ma, Ma: million years ago), a time when India had already joined with Eurasia. The key fossil lineage is ?Eoanabas, the oldest anabantid known so far, from the upper Oligocene of the Tibetan Plateau.Ancestral range reconstructions suggest a Southeast Asian origin in the early Eocene(ca. 48 Ma) and subsequent dispersals to Tibet and then India for this group. Thereby we propose their westbound dispersal to Africa via the biotic bridge between India and Africa. If so, climbing perch precursors had probably followed the paleobiogeographical route of snakehead fishes, which have a slightly older divergence between African and Asian taxa. As such, our study echoes some recent molecular analyses in rejecting the previously held ‘‘Gondwana continental drift vicariance" or late Mesozoic dispersal scenarios for the climbing perches, but provides a unique biogeographical model to highlight the role of the preuplift Tibet and the docked India in shaping the disjunct distribution of some air-breathing freshwater fishes around the Indian Ocean.展开更多
This paper describes a plant megafossil assemblage from the Pliocene strata of Xiangzi, Zanda Basin in the western Qinghai-Tibet Plateau. Twenty-one species belonging to 12 genera and 10 families were identified. Stud...This paper describes a plant megafossil assemblage from the Pliocene strata of Xiangzi, Zanda Basin in the western Qinghai-Tibet Plateau. Twenty-one species belonging to 12 genera and 10 families were identified. Studies show that the Pliocene vegetation in Zanda Basin was mostly deciduous shrub composed of Cotoneaster, Spiraea, Caragana, Hippophae,Rhododendron, Potentilla fruticosa, etc. Leaf sizes of these taxa were generally small. Paleoclimate reconstruction using Coexistence Analysis and CLAMP showed that this area had higher temperature and precipitation in the Pliocene than today, and distinct seasonal precipitation variability was established. The reconstructed paleoelevation of Zanda Basin in the Pliocene was similar to modern times. In the context of central Asian aridification, the gradual drought in the area beginning in the late Cenozoic caused vegetation to transition from shrub to desert, and the flora composition also changed.展开更多
Solid-state batteries have been considered as promising next-generation energy storage devices for potentially higher energy density and better safety compared with commercial lithium-ion batteries that are based on o...Solid-state batteries have been considered as promising next-generation energy storage devices for potentially higher energy density and better safety compared with commercial lithium-ion batteries that are based on organic liquid electrolytes.However,in terms of indispensable solid-state electrolytes,there are remaining issues to be solved before entering the market.Most solid-state electrolytes are air-sensitive,which causes a complex and expensive cell assembly and impressible interface.Therefore,the solid-state electrolytes are expected to be atmosphere-stable,which will undoubtedly bring significant benefits to solid-state battery manufacturing.This review covers air-stabilityrelated issues of different types of inorganic solid-state electrolytes and the corresponding strategies.First,we provide an overview of solid-state electrolytes and solid-state batteries,including their history and advantages/disadvantages.Then,different types of solid-state electrolytes are selected as examples to illustrate the unfavorable interactions in air and the corresponding adverse effects.Next,according to recent advances,we summarize the effective strategies of constructing different types of air-stable inorganic solid-state electrolytes.Finally,perspectives on designing accessible air-stable solid-state electrolytes are provided,aiming to achieve the assembly of high-performance solid-state batteries in the atmosphere.展开更多
Li-rich manganese-based cathode materials(LR) are considered as excellent cathode materials for a new generation of lithium-ion batteries causes their outstanding electrochemical performance, friendly price, and envir...Li-rich manganese-based cathode materials(LR) are considered as excellent cathode materials for a new generation of lithium-ion batteries causes their outstanding electrochemical performance, friendly price, and environmental friendliness. But defects such as rapid voltage decay and loss of lattice oxygen limit their applications. The electrochemical performance of LR has to be improved by means of modification. The previous single modification methods like element doping, surface coating, structure design, etc. can only optimize the electrochemical performance of LR from one aspect. Recently, multiple modifications,which can combine the advantages of multiple modifications, have been favored by researchers. Here, we comprehensively review the recent progress of multiple modification of LR based on the combination of different modification means. The review and summary of the multiple modification of LR will play a guiding role in its development in the future.展开更多
Sulphur(S)-template method based on conventional slurry-casting method has been developed to pro-duce porous silicon(Si)electrodes.The facile fabrication technology is suitable for current production line and expected...Sulphur(S)-template method based on conventional slurry-casting method has been developed to pro-duce porous silicon(Si)electrodes.The facile fabrication technology is suitable for current production line and expected to be widely applied to various electrode materials under large volume change during operation.Specifically,S particles as template agent are mixed with active material Si,carbon conductor and binder forming uniform slurry.After casting and drying,the electrodes are immersed in carbon disul-fide solution to remove S particles rapidly,generating pores in-situ at the original position of S particles.Electrochemical analysis shows that the pores inside electrodes are able to shorten lithium ion diffusion paths,reduce normal expansion rate and decrease formation of cracks in the Si electrode(2 mg_(Si)/cm^(2)),demonstrating a reversible capacity of 951 mAh/g at 0.5 A/g after 100 cycles(with a capacity retention of 99.5%)and a capacity of-826 mAh/g at 2 A/g.展开更多
基金the Innovation-Driven Project of Central South University(2019CX033)the National Natural Science Foundation of China(51904344 and 52172264)the Natural Science Foundation of Hunan Province of China(2021JJ10060 and 2022GK2033)。
文摘The electrolyte integrated with lithium metal anodes is subjected to the issues of interfacial compatibility and stability,which strongly influence the performances of high-energy lithium metal batteries.Here,we report a new electrolyte recipe viz.a moderately concentrated electrolyte comprising of 2.4 M lithium bis(fluorosulfonyl)imide(LiFSI)in a cosolvent mixture of fluorinated ethylene carbonate(FEC)and dimethyl carbonate(DMC)with relatively high ion conductivity.Owing to the preferential decomposition of LiFSI and FEC,an inorganic-rich interphase with abundant Li_(2)O and LiF nanocrystals is formed on lithium metal with improved robustness and ion transfer kinetics,enabling lithium plating/stripping with an extremely low overpotential of~8 mV and the average CE of 97%.When tested in Li||LiFePO_(4) cell,this electrolyte provides long-term cycling with a capacity retention of 98.3%after 1000 cycles at 1 C and an excellent rate performance of 20 C,as well as an areal capacity of 1.35 mA h cm^(-2)at the cathode areal loading of 9 mg cm^(-2).Moreover,the Li||LiFePO_(4) cell exhibits excellent wide-temperature performances(-40~60℃),including long-term cycling stability over 2600 cycles without visible capacity fading at 0℃,as well as extremely high average CEs of 99.6%and 99.8% over 400 cycles under-20℃ and 45℃.
基金This project was supported by the National Natural Science Foundation of China(U19A2017,22272206,51976143)Natural Science Foundation of Hunan Province(S2021JJMSXM3153).
文摘Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides an attractive approach to carbon capture and utilization for the production high-value-added products.However,CO_(2)RR still suffers from poor selectivity and low current density due to its sluggish kinetics and multitudinous reaction pathways.Single-atom catalysts(SACs)demonstrate outstanding activity,excellent selectivity,and remarkable atom utilization efficiency,which give impetus to the search for electrocatalytic processes aiming at high selectivity.There appears significant activity in the development of efficient SACs for CO_(2)RR,while the density of the atomic sites remains a considerable barrier to be overcome.To construct high-metal-loading SACs,aggregation must be prevented,and thus novel strategies are required.The key to creating high-density atomically dispersed sites is designing enough anchoring sites,normally defects,to stabilize the highly mobile separated metal atoms.In this review,we summarized the advances in developing high-loading SACs through defect engineering,with a focus on the synthesis strategies to achieve high atomic site loading.Finally,the future opportunities and challenges for CO_(2)RR in the area of high-loading single-atom electrocatalysts are also discussed.
基金the financial support from Research Training Program(RTP)funded by the Department of Education,Australian Government。
文摘Lithium-ion batteries (LIB) have received substantial attention in the last 10 years,as they offer great promise as power sources that can lead to the electric vehicle (EV) revolution in the next 5 years.Since the cathode serves as a key component in LIB,its properties significantly affect the performance of the whole system.Recently,the cathode surface modification based on coating technique has been widely employed to enhance the electrochemical performances by improving the material conductivity,stabilising the physical structure of materials,as well as preventing the reactions between the electrode and electrolyte.In this work,we reviewed the present of a number of promising cathode materials for Li-ion batteries.After that,we summarized the very recent research progress focusing on the surface coating strategies,mainly including the coating materials,the coating technologies,as well as the corresponding working mechanisms for cathodes.At last,the challenges faced and future guidelines for optimizing cathode materials are discussed.In this study,we propose that the structure of cathode is a crucial factor during the selection of coating materials and technologies.
基金financially supported by the Innovation-Driven Project of Central South University(No.2019CX033)the National Natural Science Foundation of China(No:51904344)+2 种基金the Natural Science Foundation of Guangdong Province(2019A1515012111)the Science&Technology Innovation Commission of Shenzhen(Grant No.20180123)the Shenzhen Science and Technology Program(KQTD20180412181422399)。
文摘Commercial lithium-ion(Li-ion)batteries based on graphite anodes are meeting their bottlenecks that are limited energy densities.In order to satisfy the large market demands of smaller and lighter rechargeable batteries,high-capacity metallic Li replacing low-specific-capacity graphite enables the higher energy density in next-generation rechargeable Li metal batteries(LMBs).However,Li metal anode has been suffering from dendritic problems,interfacial side reactions,volume change and low Coulombic efficiency.Therefore,performance enhancements of Li metal anodes are rather important to realize the high energy density characteristic of metallic Li.In this review,the annoying Li dendrite growth,unstable reaction interface and practical application issues of Li metal anodes are summarized and detailedly discussed to understand the current challenges concerning Li metal anodes.For overcoming such remaining challenges,the corresponding strategies and recent advances are covered and categorized.Finally,we discuss future opportunities and perspectives for developing high-performance Li metal anodes.
基金the Innovation-Driven Project of Central South University(No.2019CX033)the National Natural Science Foundation of China(No.51904344)。
文摘Lithium–sulfur(Li-S)batteries have been considered as promising candidates for large-scale high energy density devices due to the potentially high energy density,low cost,and more pronounced ecological compatibility.However,the complex Li-S conversion reactions,unsatisfactory battery performance,and unsafe metallic Li anode restrict the development of Li-S batteries to achieve commercialization.This review mainly focuses on three aspects which are the remaining challenges,recent advances,and applications in Li-S batteries.Firstly,this review portrays Li-S conversion chemistry involving the multi-step and multi-electron reaction mechanism,as well as the remaining challenges.Then,the scientific strategies and very recent advances of the cathode,electrolyte,lithium anode,and other constituent parts of Li-S batteries are detailly summed up,as well as their advantages and limitations.For the sake of promoting the Li-S batteries practicalization,next section is primarily concerned with problems,the corresponding solutions,and application scenarios of practical pouch cells.Finally,the important findings as guidelines and some future directions as trends for developing emerging Li-S batteries are briefly summarized.
基金financial supported by the National Natural Science Foundation of China(Grant Nos.51874361 and 51904343)the Science and technology program of Hunan Province(2019RS3002)。
文摘Lithium(Li)metal is the most potential anode material for the next-generation high-energy rechargeable batteries.However,intrinsic surface unevenness and‘hostless’nature of Li metal induces infinite volume effect and uncontrollable dendrite growth.Herein,we design the in-situ grown lithiophilic Ni_(2)P nanoarrays inside nickel foam(PNF).Uniform Ni_(2)P nanoarrays coating presents a very low nucleation overpotential,which induces the homogeneous Li deposition in the entire spaces of three-dimensional(3D)metal framework.Specifically,the lithiophilic Ni_(2)P nanoarrays possess characteristics of electrical conductivity and structural stability,which have almost no expansion and damage during repeating Li plating/stripping.Therefore,they chronically inhibit the growth of Li dendrites.This results in an outstanding Coulombic efficiency(CE)of 98% at 3 mA cm^(-2) and an ultra long cycling life over 2000 cycles with a low overpotential.Consequently,the PNF-Li||LiFePO_(4) battery maintains a capacity retention of 95.3% with a stable CE of 99.9% over 500 cycles at 2 C.
文摘Objective:The degree of liver cirrhosis is one of the most important diagnostic and prognostic assessments in chronic liver disease.Among the etiologies of liver cirrhosis,hepatitis B virus(HBV)infection-induced liver damage is most common in Asia-Pacific regions,particularly in China.Many current conventionally used preoperative estimation of liver cirrhosis models.
文摘Objective:Currently,liver resection is the most effective curative treatment for patients with resectable hepatocellular carcinoma(HCC).Severe post-hepatectomy liver failure(PHLF)is a serious complication for HCC patients undergoing liver resection.Models have been used to predict severe PHLF in patients with HCC,such as the Child-Pugh score,model for end-stage liver disease(MELD)score.
基金supported by the Second Comprehensive Scientific Expedition on the Tibetan Plateau(Grant No.2019QZKK0705)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant Nos.XDB26030000,XDA20070203)the National Natural Science Foundation of China(Grant Nos.41872005,41872006)。
文摘The remarkable uplift of the Tibetan Plateau in the Neogene had great impacts on the climate and environment of East Asia and even the world.Therefore,establishment of the Neogene stratigraphic framework of the Tibetan Plateau is of great significance to research in various fields of geosciences.Based on marine sediments,the international chronostratigraphic system of the Neogene is divided into six stages in the Miocene and two stages in the Pliocene.Since the beginning of the Cenozoic,the share of terrestrial strata on continents has increased rapidly.By the Neogene,it had far exceeded that of marine strata,and almost all deposits on the Tibetan Plateau and its surrounding areas were terrestrial strata.In China,the Miocene includes five stages and the Pliocene includes two stages.Except for the Tunggurian of the Miocene,which has a lower boundary at 15 Ma,the other stages have the same paleomagnetic definitions and time intervals as the corresponding international marine stages.Mammalian fossils play a very important role in the division and correlation of Cenozoic terrestrial strata,and rodent,carnivore,proboscidean,perissodactyl and artiodactyl fossils are especially important in Neogene terrestrial biostratigraphy.There are many basins with well-exposed strata and abundant mammalian fossils in the Tibetan Plateau.The lower boundary stratotype sections of the Neogene Xiejian and Bahean stages are located respectively in the Xining and Linxia basins,and there are precise paleomagnetic dates in coordination with mammalian fossils.The lower boundary stratotypes of other stages can also be effectively determined in the Tibetan Plateau.Many first appearing mammalian genera in East Asia also appeared in the Tibetan Plateau and its surrounding areas,especially in the Linxia Basin on the northeast margin and in the Siwaliks on the southwest margin.Among them,Prodeinotherium first appeared at the bottom of the Miocene in the Siwaliks,and the earliest Hipparion of the Old World first appeared at the bottom of the Bahean Stage in the Linxia Basin.Carbon and oxygen isotope analysis of enamel and paleosols of Cenozoic sediments and mammal fossils in the Tibetan Plateau and its surrounding areas have been used to reconstruct the climate,environment and vegetation development characteristics,and revealed that these changes were not only related to global change,but also had regional features.Evidence of the Late Miocene C4plant expansion event based on carbon isotope changes comes from the southern margin of the Tibetan Plateau,but in sharp contrast,δ13C indicates that there was still no clear or significant C4plant signal on the northern margin of the Tibetan Plateau until the end of the Neogene.Theδ18O analysis shows that there were several major climate change events in the Cenozoic,especially in the Late Miocene at about 7 Ma,when positive drift ofδ18O indicates that the northern and southern sides of the Tibetan Plateau were changing to drier environments.The strong uplift of the Tibetan Plateau in the Late Miocene strengthened the thermal contrast between sea and land,which strengthened monsoon circulation and led to the expansion of C4vegetation in South Asia.However,the East Asian summer monsoon,which can bring atmospheric precipitation and a climate suitable for C4plants to northern China,was not enough to affect the northern Tibetan Plateau.The Tibetan Plateau on the whole rose to an altitude of about 3000 m in the Miocene,becoming a barrier to mammalian migration;it reached its modern altitude of more than 4000 m in the Pliocene,thus forming a cryosphere environment,which led to the emergence of ancestral types of the Ice Age fauna.
基金the National Natural Science Foundation of China(Nos.51904344 and 52172264)the Natural Science Foundation of Hunan Province of China(Nos.2021JJ10060 and 2022GK2033).
文摘Lithium metal batteries(LMBs)based on metallic Li exhibit high energy density to be competent for advanced energy storage applications.However,the unstable solid electrolyte interphase(SEI)layer due to continuous decomposition of electrolytes,and the attendant problem of Li dendrite growth frustrate their commercialization process.Herein,a hybrid SEI comprising abundant LiF,lithiophilic Li-Ge alloy,and Ge nanoparticles is constructed via a simple brush coating method.This fluorinated interface layer with embedded Ge-containing components isolates the Li anode from the corrosive electrolyte and facilitates homogenous Li nucleation as well as uniform growth.Consequently,the modified Li anode exhibits remarkable stability without notorious Li dendrites,delivering stable cycling lives of more than 1000 h for symmetric Li||Li cells and over 600 cycles for Li||Cu cells at 1 mA·cm^(−2).Moreover,the reinforced Li anodes endow multiple full-cell architectures with dramatically improved cyclability under different test conditions.This work provides rational guidance to design an artificial hybrid SEI layer and would stimulate more ideas to solve the dendrite issue and promote the further development of advanced LMBs.
基金supported by the Strategic Priority Research Program of Chinese Academy of Sciences(XDB31000000)the National Natural Science Foundation of China(32100367,32122021,32170480,31972866)+5 种基金grants from the 1000 Talent Project of Shaanxi ProvinceChina Postdoctoral Science Foundation(2021M693342)Hubei Postdoctoral Innovation Post ProjectChinese Academy of Sciences(Youth Innovation Promotion Association,Chinese Academy of Sciences(http://www.yicas.cn)the Young Top-notch Talent Cultivation Program of Hubei Provincethe Wuhan Branch,Supercomputing Center,Chinese Academy of Sciences,China。
文摘Major historical events often trigger the rapid flourishing of a few lineages,which in turn shape established biodiversity patterns.How did this process occur and develop?This study provides a window into this issue.The endemic East Asian carps(EEAC)dominated the ichthyofauna of East Asia and exhibited a high degree of adaptation to monsoonal river-lake ecosystems.A series of evidence,including ecogeography,phylogenetics,and macroevolution,suggests that the EEAC is a lineage that arose with the East Asian monsoon and thrived intimately with subsequent monsoon activities.We further deduce the evolution of the EEAC and find that a range of historical events in the monsoon setting(e.g.,marine transgression and regression and glacial-interglacial cycle)have further reshaped the distribution patterns of EEAC’s members.Comparative genomics analyses reveal that introgressions during the initial period of EEAC radiation and innovations in the regulation of the brain and nervous system may have aided their adaptation to river-lake ecosystems in a monsoon setting,which boosted radiation.Overall,this study strengthens knowledge of the evolutionary patterns of freshwater fishes in East Asia and provides a model case for understanding the impact of major historical events on the evolution of biota.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant Nos.XDB26000000,XDA20070203,XDA20070301)the Second Comprehensive Scientific Expedition on the Tibetan Plateau(Grant No.QZK0705,2019)+3 种基金the National Natural Science Foundation of China(Grant Nos.41430102,41872006)the Frontier Science Key Research Project(Grant No.QYZDY-SSW-DQC022)the International Partnership Program(Grant No.GJHZ1885)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(Grant No.2017103)
文摘Holding particular biological resources,the Tibetan Plateau is a unique geologic-geographic-biotic interactively unite and hence play an important role in the global biodiversity domain.The Tibetan Plateau has undergone vigorous environmental changes since the Cenozoic,and played roles switching from"a paradise of tropical animals and plants"to"the cradle of Ice Age mammalian fauna".Recent significant paleontological discoveries have refined a big picture of the evolutionary history of biodiversity on that plateau against the backdrop of major environmental changes,and paved the way for the assessment of its far-reaching impact upon the biota around the plateau and even in more remote regions.Here,based on the newly reported fossils from the Tibetan Plateau which include diverse animals and plants,we present a general review of the changing biodiversity on the Tibetan Plateau and its influence in a global scale.We define the Tibetan Plateau as a junction station of the history of modern biodiversity,whose performance can be categorized in the following three patterns:(1)Local origination of endemism;(2)Local origination and"Out of Tibet";(3)Intercontinental dispersal via Tibet.The first pattern is exemplified by the snow carps,the major component of the freshwater fish fauna on the plateau,whose temporal distribution pattern of the fossil schizothoracines approximately mirrors the spatial distribution pattern of their living counterparts.Through ascent with modification,their history reflects the biological responses to the stepwise uplift of the Tibetan Plateau.The second pattern is represented by the dispersal history of some mammals since the Pliocene and some plants.The ancestors of some Ice Age mammals,e.g.,the wholly rhino,Arctic fox,and argali sheep first originated and evolved in the uplifted and frozen Tibet during the Pliocene,and then migrated toward the Arctic regions or even the North American continent at beginning of the Ice Age;the ancestor of pantherines(big cats)first rose in Tibetan Plateau during the Pliocene,followed by the disperse of its descendants to other parts of Asia,Africa,North and South America to play as top predators of the local ecosystems.The early members of some plants,e.g.,Elaeagnaceae appeared in Tibet during the Late Eocene and then dispersed and were widely distributed to other regions.The last pattern is typified by the history of the tree of heaven(Ailanthus)and climbing perch.Ailanthus originated in the Indian subcontinent,then colonized into Tibet after the Indian-Asian plate collision,and dispersed therefrom to East Asia,Europe and even North America.The climbing perches among freshwater fishes probably rose in Southeast Asia during the Middle Eocene,dispersed to Tibet and then migrated into Africa via the docked India.These cases highlight the role of Tibet,which was involved in the continental collision,in the intercontinental biotic interchanges.The three evolutionary patterns above reflect both the history of biodiversity on the plateau and the biological and environmental effects of tectonic uplift.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (CAS) (XDA20070203, XDB26000000, XDB310403, XDA20070301)the Second Tibetan Plateau Scientific Expedition Program, the National Natural Science Foundation of China (41872006)Youth Innovation Promotion Association, CAS (2017103, 2017439)
文摘The northward drift of the Indian Plate and its collision with Eurasia have profoundly impacted the evolutionary history of the terrestrial organisms, especially the ones along the Indian Ocean rim. Climbing perches(Anabantidae) are primary freshwater fishes showing a disjunct south Asian-African distribution,but with an elusive paleobiogeographic history due to the lack of fossil evidence. Here, based on an updated time-calibrated anabantiform phylogeny integrating a number of relevant fossils, the divergence between Asian and African climbing perches is estimated to have occurred in the middle Eocene(ca.40 Ma, Ma: million years ago), a time when India had already joined with Eurasia. The key fossil lineage is ?Eoanabas, the oldest anabantid known so far, from the upper Oligocene of the Tibetan Plateau.Ancestral range reconstructions suggest a Southeast Asian origin in the early Eocene(ca. 48 Ma) and subsequent dispersals to Tibet and then India for this group. Thereby we propose their westbound dispersal to Africa via the biotic bridge between India and Africa. If so, climbing perch precursors had probably followed the paleobiogeographical route of snakehead fishes, which have a slightly older divergence between African and Asian taxa. As such, our study echoes some recent molecular analyses in rejecting the previously held ‘‘Gondwana continental drift vicariance" or late Mesozoic dispersal scenarios for the climbing perches, but provides a unique biogeographical model to highlight the role of the preuplift Tibet and the docked India in shaping the disjunct distribution of some air-breathing freshwater fishes around the Indian Ocean.
基金supported by the Strategic Priority Research Program of CAS(Grant Nos.XDA2007030102,XDB26000000,XDA20070203)the Second Tibetan Plateau Scientific Expedition and Research(STEP)(Grant No.2019QZKK0705)+2 种基金the NSFC-NERC(the National Natural Science Foundation of China-Natural Environment Research Council of the United Kingdom)joint research program(Grant Nos.41661134049,NE/P013805/1)the Youth Innovation Promotion Association,CAS(Grant No.2017439)the Key Research Program of Frontier Sciences,CAS(Grant No.QYZDB-SSW-SMC016)
文摘This paper describes a plant megafossil assemblage from the Pliocene strata of Xiangzi, Zanda Basin in the western Qinghai-Tibet Plateau. Twenty-one species belonging to 12 genera and 10 families were identified. Studies show that the Pliocene vegetation in Zanda Basin was mostly deciduous shrub composed of Cotoneaster, Spiraea, Caragana, Hippophae,Rhododendron, Potentilla fruticosa, etc. Leaf sizes of these taxa were generally small. Paleoclimate reconstruction using Coexistence Analysis and CLAMP showed that this area had higher temperature and precipitation in the Pliocene than today, and distinct seasonal precipitation variability was established. The reconstructed paleoelevation of Zanda Basin in the Pliocene was similar to modern times. In the context of central Asian aridification, the gradual drought in the area beginning in the late Cenozoic caused vegetation to transition from shrub to desert, and the flora composition also changed.
基金supported by the Innovation-Driven Project of Central South University(No.2019CX033)the National Natural Science Foundation of China(Nos.51622210,51904344,51925207,U1910210 and 51872277)+1 种基金the National Synchrotron Radiation Laboratory(KY2060000173)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(grant nos.YLU-DNL Fund 2021002).
文摘Solid-state batteries have been considered as promising next-generation energy storage devices for potentially higher energy density and better safety compared with commercial lithium-ion batteries that are based on organic liquid electrolytes.However,in terms of indispensable solid-state electrolytes,there are remaining issues to be solved before entering the market.Most solid-state electrolytes are air-sensitive,which causes a complex and expensive cell assembly and impressible interface.Therefore,the solid-state electrolytes are expected to be atmosphere-stable,which will undoubtedly bring significant benefits to solid-state battery manufacturing.This review covers air-stabilityrelated issues of different types of inorganic solid-state electrolytes and the corresponding strategies.First,we provide an overview of solid-state electrolytes and solid-state batteries,including their history and advantages/disadvantages.Then,different types of solid-state electrolytes are selected as examples to illustrate the unfavorable interactions in air and the corresponding adverse effects.Next,according to recent advances,we summarize the effective strategies of constructing different types of air-stable inorganic solid-state electrolytes.Finally,perspectives on designing accessible air-stable solid-state electrolytes are provided,aiming to achieve the assembly of high-performance solid-state batteries in the atmosphere.
基金supported by the Natural Science Foundation of Hunan Province(Nos.2021JJ30823 and 2020JJ2048)National Natural Science Foundation of China(No.51974368)。
文摘Li-rich manganese-based cathode materials(LR) are considered as excellent cathode materials for a new generation of lithium-ion batteries causes their outstanding electrochemical performance, friendly price, and environmental friendliness. But defects such as rapid voltage decay and loss of lattice oxygen limit their applications. The electrochemical performance of LR has to be improved by means of modification. The previous single modification methods like element doping, surface coating, structure design, etc. can only optimize the electrochemical performance of LR from one aspect. Recently, multiple modifications,which can combine the advantages of multiple modifications, have been favored by researchers. Here, we comprehensively review the recent progress of multiple modification of LR based on the combination of different modification means. The review and summary of the multiple modification of LR will play a guiding role in its development in the future.
基金the National Natural Science Foundation of China(Nos.51904344,52172264)the Natural Science Foundation of Hunan Province of China(Nos.2021JJ10060,2022GK2033).
文摘Sulphur(S)-template method based on conventional slurry-casting method has been developed to pro-duce porous silicon(Si)electrodes.The facile fabrication technology is suitable for current production line and expected to be widely applied to various electrode materials under large volume change during operation.Specifically,S particles as template agent are mixed with active material Si,carbon conductor and binder forming uniform slurry.After casting and drying,the electrodes are immersed in carbon disul-fide solution to remove S particles rapidly,generating pores in-situ at the original position of S particles.Electrochemical analysis shows that the pores inside electrodes are able to shorten lithium ion diffusion paths,reduce normal expansion rate and decrease formation of cracks in the Si electrode(2 mg_(Si)/cm^(2)),demonstrating a reversible capacity of 951 mAh/g at 0.5 A/g after 100 cycles(with a capacity retention of 99.5%)and a capacity of-826 mAh/g at 2 A/g.