In order to fundamentally solve the acidification problem of high sulfur-containing bauxite during storage, by simulating the environment of minerals storage in laboratory, the acidification mechanism and influencing ...In order to fundamentally solve the acidification problem of high sulfur-containing bauxite during storage, by simulating the environment of minerals storage in laboratory, the acidification mechanism and influencing factors of high sulfur-containing bauxite were studied and confirmed using the single variable method to control the atmosphere, water and other variables. The results show that the acidification is mostly caused by the oxidation of sulfur-containing bauxite, which is mainly the natural oxidation of Pyrite(Fe S2), then the alkaline minerals dissolute in the presence of water, leading to the acidification phenomenon, which is influenced by moisture and air flow. Finally, more acid-producing substances are formed, resulting in the acidification of high sulfur-containing bauxite. The acidification of high sulfur-containing bauxite results from the combined effect of the oxygen in the air and water, which can be significantly alleviated by controlling the diffusion of the oxygen in air.展开更多
The reverse flocculation method for removing pyritic sulfur from high sulfor coals has been conceptually beveloped and investigated. The tentative tests on China high sulfur coals have shown that this advanced physica...The reverse flocculation method for removing pyritic sulfur from high sulfor coals has been conceptually beveloped and investigated. The tentative tests on China high sulfur coals have shown that this advanced physical separation techaique can be very efficient in coal desulfurization, provided the process parameters are properly optimized. Under the circumsances of acquiring high coal recovery, the total sulfur rejection with four kinds of coal samples normally falls in tbe range 57% to 71 % by one-step reverse flocculation, and within the range 40% to 59% by one-step normal flocculation process.展开更多
Processing of Iranian high sulfur iron ore is problematic in minerals industry. The iron ores were studied by the means of polarizing microscopy, chemical analysis, X-ray diffraction. The study shows that the iron ore...Processing of Iranian high sulfur iron ore is problematic in minerals industry. The iron ores were studied by the means of polarizing microscopy, chemical analysis, X-ray diffraction. The study shows that the iron ores have high grade of iron, and complex structures. XRD showed that the iron ore consists of metallic minerals such as magnetite with a small amount of hematite and limonite and non-metallic minerals as serpentine, chlorite, and talc. The average particle size of magnetite crystals is 0.182 mm. The ore contains 1.62% sulfur as harmful impurity in form of pyrite mineral. Due to the isomorphism of magnesium and iron, magnetite mono crystal grade is lower than 68%, and difficult to be physically upgraded to a higher-grade iron concentrate using the available mineral processing technologies.展开更多
The state-selective cross section data are useful for understanding and modeling the x-ray emission in celestial observations.In the present work,using the cold target recoil ion momentum spectroscopy,for the first ti...The state-selective cross section data are useful for understanding and modeling the x-ray emission in celestial observations.In the present work,using the cold target recoil ion momentum spectroscopy,for the first time we investigated the state-selective single electron capture processes for S^(q+)–He and H_(2)(q=11–15)collision systems at an impact energy of q×20 keV and obtained the relative state-selective cross sections.The results indicate that only a few principal quantum states of the projectile energy level are populated in a single electron capture process.In particular,the increase of the projectile charge state leads to the population of the states with higher principal quantum numbers.It is also shown that the experimental averaged n-shell populations are reproduced well by the over-barrier model.The database is openly available in Science Data Bank at 10.57760/sciencedb.j00113.00091.展开更多
Lithium sulfur batteries(LSBs)are recognized as promising devices for developing next-generation energy storage systems.In addition,they are attractive rechargeable battery systems for replacing lithium-ion batteries(...Lithium sulfur batteries(LSBs)are recognized as promising devices for developing next-generation energy storage systems.In addition,they are attractive rechargeable battery systems for replacing lithium-ion batteries(LIBs)for commercial use owing to their higher theoretical energy density and lower cost compared to those of LIBs.However,LSBs are still beset with some persistent issues that prevent them from being used industrially,such as the unavoidable dissolution of lithium polysulfide intermediates during electrochemical reactions and large volume expansion(up to 80%)upon the formation of Li_(2)S,resulting in serious battery life and safety limitations.In the process of solving these problems,it is necessary to maintain a high sulfur content in the cathode materials to ensure that the LSBs have high energy densities and excellent cycle performance.In this review,the novel preparation methods and cathode materials used for preparing LSBs in recent years are reviewed considering the sulfur content and cycle performance.In addition,the problems and difficulties in practically applying cathode materials are described,and the development trend is discussed.展开更多
The practical application of lithium-sulfur(Li-S)batteries is greatly hindered by soluble polysulfides shuttling and sluggish sulfur redox kinetics.Rational design of multifunctional hybrid materials with superior ele...The practical application of lithium-sulfur(Li-S)batteries is greatly hindered by soluble polysulfides shuttling and sluggish sulfur redox kinetics.Rational design of multifunctional hybrid materials with superior electronic conductivity and high electrocatalytic activity,e.g.,heterostructures,is a promising strategy to solve the above obstacles.Herein,a binary metal sulfide MnS-MoS_(2) heterojunction electrocatalyst is first designed for the construction of high-sulfur-loaded and durable Li-S batteries.The MnS-MoS_(2) p-n heterojunction shows a unique structure of MoS_(2) nanosheets decorated with ample MnS nanodots,which contributes to the formation of a strong built-in electric field at the two-phase interface.The MnS-MoS_(2) hybrid host shows strong soluble polysulfide affinity,enhanced electronic conductivity,and exceptional catalytic effect on sulfur reduction.Benefiting from the synergistic effect,the as-derived S/MnS-MoS_(2) cathode delivers a superb rate capability(643 m A h g^(-1)at 6 C)and a durable cyclability(0.048%decay per cycle over 1000 cycles).More impressively,an areal capacity of 9.9 m A h cm^(-2)can be achieved even under an extremely high sulfur loading of 14.7 mg cm^(-2)and a low electrolyte to sulfur ratio of 2.9μL mg^(-1).This work provides an in-depth understanding of the interfacial catalytic effect of binary metal compound heterojunctions on sulfur reaction kinetics.展开更多
Achieving high loading of active sulfur yet rational regulating the shuttle effect of lithium polysulfide(LiPS)is of great significance in pursuit of high-performance lithium-sulfur(Li-S)battery.Herein,we develop a fr...Achieving high loading of active sulfur yet rational regulating the shuttle effect of lithium polysulfide(LiPS)is of great significance in pursuit of high-performance lithium-sulfur(Li-S)battery.Herein,we develop a free-standing graphene nitrogen(N),phosphorus(P)and fluorine(F)co-doped mesoporous carbon-sulfur(G-NPFMC-S)film,which was used as a binder-free cathode in Li-S battery.The developed mesoporous carbon(MC)achieved a high specific surface area of 921 m^(2)·g^(-1)with a uniform pore size distribution of 15 nm.The inserted graphene network inside G-NPFMC-S cathode can effectively improve its electrical conductivity and simultaneously restrict the shuttle of LiPS.A high sulfur loading of 86%was achieved due to the excellent porous structures of graphene-NPFMC(G-NPFMC)composite.When implemented as a freestanding cathode in Li-S battery,this G-NPFMC-S achieved a high specific capacity(1,356 mAh·g^(-1)),favorable rate capability,and long-term cycling stability up to 500 cycles with a minimum capacity fading rate of 0.025%per cycle,outperforming the corresponding performances of NPFMC-sulfur(NPFMC-S)and MC-sulfur(MC-S).These promising results can be ascribed to the featured structures that formed inside G-NPFMC-S film,as that highly porous NPFMC can provide sufficient storage space for the loading of sulfur,while,the N,P,F-doped carbonic interface and the inserted graphene network help hinder the shuttle of LiPS via chemical adsorption and physical barrier effect.This proposed unique structure can provide a bright prospect in that high mass loading of active sulfur and restriction the shuttle of LiPS can be simultaneously achieved for Li-S battery.展开更多
Lithium-sulfur(Li-S)battery is regarded as one of the most promising next-generation energy storage systems due to the ultra-high theoretical energy density of 2600 Wh kg^(-1).To address the insulation nature of sulfu...Lithium-sulfur(Li-S)battery is regarded as one of the most promising next-generation energy storage systems due to the ultra-high theoretical energy density of 2600 Wh kg^(-1).To address the insulation nature of sulfur,nanocarbon composition is essential to afford acceptable cycling capacity but inevitably sacrifices the actual energy density under working conditions.Therefore,rational structural design of the carbon/sulfur composite cathode is of great significance to realize satisfactory electrochemical performances with limited carbon content.Herein,the cathode carbon distribution is rationally regulated to construct high-sulfur-content and high-performance Li-S batteries.Concretely,a double-layer carbon(DLC)cathode is prepared by fabricating a surface carbon layer on the carbon/sulfur composite.The surface carbon layer not only provides more electrochemically active surfaces,but also blocks the polysulfide shuttle.Consequently,the DLC configuration with an increased sulfur content by nearly 10 wt%renders an initial areal capacity of 3.40 mAh cm^(-2) and capacity retention of 83.8%during 50 cycles,which is about two times than that of the low-sulfur-content cathode.The strategy of carbon distribution regulation affords an effective pathway to construct advanced high-sulfur-content cathodes for practical high-energy-density Li-S batteries.展开更多
The lithium-sulfur battery is the subject of much recent attention due to the high theoretical energy density,but practical applications are challenged by fast decay owing to polysulfide shuttle and electrode architec...The lithium-sulfur battery is the subject of much recent attention due to the high theoretical energy density,but practical applications are challenged by fast decay owing to polysulfide shuttle and electrode architecture degradation.A comprehensive study of the sulfur host microstructure design and the cell architecture construction based on the MXene phase(Ti3C2Tx nanosheets) is performed,aiming at realize stable cycling performance of Li-S battery with high sulfur areal loading.The interwoven KB@Ti3C2Tx composite formed by self-assembly of MXene and Ktej en black,not only provides superior conductivity and maintains the electrode integrality bearing the volume expansion/shrinkage when used as the sulfur host,but also functions as an interlayer on separator to further retard the polysulfide cross-diffusion that possibly escaped from the cathode.The KB@Ti3C2Tx interlayer is only 0.28 mg cm-2 in areal loading and 3 μm in thickness,which accounts a little contribution to the thick sulfur electrode;thus,the impacts on the energy density is minimal.By coupling the robust KB@Ti3C2Tx cathode and the effective KB@Ti3C2Tx modified separator,a stable Li-S battery with high sulfur areal loading(5.6 mg cm-2) and high areal capacity(6.4 mAh cm-2) at relatively lean electrolyte is achieved.展开更多
High-energy lithium-sulfur batteries(LSBs)have experienced relentless development over the past decade with discernible improvements in electrochemical performance.However,a scrutinization of the cell operation condit...High-energy lithium-sulfur batteries(LSBs)have experienced relentless development over the past decade with discernible improvements in electrochemical performance.However,a scrutinization of the cell operation conditions reveals a huge gap between the demands for practical batteries and those in the literature.Low sulfur loading,a high electrolyte/sulfur(E/S)ratio and excess anodes for lab-scale LSBs significantly offset their high-energy merit.To approach practical LSBs,high loading and lean electrolyte parameters are needed,which involve budding challenges of slow charge transfer,polysulfide precipitation and severe shuttle effects.To track these obstacles,the exploration of electrocatalysts to immobilize polysulfides and accelerate Li-S redox kinetics has been widely reported.Herein,this review aims to survey state-of-the-art catalytic materials for practical LSBs with emphasis on elucidating the correlation among catalyst design strategies,material structures and electrochemical performance.We also statistically evaluate the state-of-the-art catalyst-modified LSBs to identify the remaining discrepancy between the current advancements and the real-world requirements.In closing,we put forward our proposal for a catalytic material study to help realize practical LSBs.展开更多
High-energy density lithium-sulfur(Li-S) batteries have received intensive attention as promising energy storage system.Among diverse sulfur-based cathodes,sulfurized pyrolyzed poly(acrylonitrile)(S@pPAN)cathode deliv...High-energy density lithium-sulfur(Li-S) batteries have received intensive attention as promising energy storage system.Among diverse sulfur-based cathodes,sulfurized pyrolyzed poly(acrylonitrile)(S@pPAN)cathode delivered superior electrochemical performance.However,the sulfur content of S@pPAN is relatively low(<50 wt%),which significantly limits the energy density.Herein,a hydrogel SA-Cu binder was proposed with a crosslinking network constructed by Cu^(2+) ions.The introduction of Cu^(2+) ions enabled excellent electrochemical behaviors of S@pPAN cathode even with high sulfur content of 52.6 wt% via chemical interaction with sulfur and polysulfide.Moreover,a favorable cathode interphase was formed containing electrochemically active and conductive CuSx.S@pPAN/SA-Cu exhibited a high sulfur utilization of 85.3%,long cycling stability over 1000 cycles and remarkable capacity of 1200 mAh g_(s)^(-1) even at10 C.Furthermore,ascribed to the improved electrode structure,high-loading electrode(sulfur loading:4 mg cm^(-2)) displayed stable cycling with areal capacity of 5.26 mAh cm^(-2)(1315 mAh g_(s)^(-1)) after 40 cycles.This study provides new directions to prepare high-sulfur content and high-loading S@pPAN cathode for higher energy density.展开更多
Practical Li-sulfur batteries require the high sulfur loading cathode to meet the large-capacity power demand of electrical equipment.However,the sulfur content in cathode materials is usually unsatisfactory due to th...Practical Li-sulfur batteries require the high sulfur loading cathode to meet the large-capacity power demand of electrical equipment.However,the sulfur content in cathode materials is usually unsatisfactory due to the excessive use of carbon for improving the conductivity.Traditional cathode fabrication strategies can hardly realize both high sulfur content and homogeneous sulfur distribution without aggregation.Herein,we designed a cathode material with ultrahigh sulfur content of 88%(mass fraction)by uniformly distributing the water dispersible sulfur nanoparticles on three-dimensionally conductive graphene framework.The water processable fabrication can maximize the homogeneous contact between sulfur nanoparticles and graphene,improving the utilization of the interconnected conductive surface.The obtained cathode material showed a capacity of 500 mA·h/g after 500 cycles at 2.0 A/g with an areal loading of 2 mg/cm2.This strategy provides possibility for the mass production of high-performance electrode materials for high-capacity Li-S battery.展开更多
Lithium–sulfur(Li–S)batteries have been recognized as promising substitutes for current energy-storage technologies owing to their exceptional advantages in very high-energy density and excellent material sustainabi...Lithium–sulfur(Li–S)batteries have been recognized as promising substitutes for current energy-storage technologies owing to their exceptional advantages in very high-energy density and excellent material sustainability.The cathode with high sulfur areal loading is vital for the practical applications of Li–S batteries with very high energy density.However,the high sulfur loading in an electrode results in poor rate and cycling performances of batteries in most cases.Herein,we used diameters of 5.0(D5)and 13.0(D13)mm to probe the effect of electrodes with different sizes on the rate and cycling performances under a high sulfur loading(4.5 mg cm^-2).The cell with D5 sulfur cathode exhibits better rate and cycling performances comparing with a large(D13)cathode.Both the high concentration of lithium polysulfides and corrosion of lithium metal anode impede rapid kinetics of sulfur redox reactions,which results in inferior battery performance of the Li–S cell with large diameter cathode.This work highlights the importance of rational matching of the large sulfur cathode with a high areal sulfur loading,carbon modified separators,organic electrolyte,and Li metal anode in a pouch cell,wherein the sulfur redox kinetics and lithium metal protection should be carefully considered under the flooded lithium polysulfide conditions in a working Li–S battery.展开更多
Super-high sulfur coal resultes in serious coal-derived pollution but might have a particular genesis. Thus,a columnar section of an Early Permian Liangshan Formation coal seam. weight average sulfur content 5.80%,fro...Super-high sulfur coal resultes in serious coal-derived pollution but might have a particular genesis. Thus,a columnar section of an Early Permian Liangshan Formation coal seam. weight average sulfur content 5.80%,from Kaili,eastern Guizhou,was studied using the methods of coal petrology and geochemistry. The results show that the seam was apparently formed in seawater-effected peat bogs that developed in two distinct stages. During the first stage various layers were formed in a supratidal bog and have a composition characteristic of a bog with a gradually decreasing sea-water effect,decreasing water dynamics,and an increasingly reductive environment. Layers in the upper seam formed during a second stage in an intertidal bog. These layers are very high in total and inorganic sulfur,the ratios of or-ganic/inorganic sulfur and V/I drop,they are high in coal ash yield and have a high ash component index,considerable barkinite,oxidized and detrital macerals,have a porphyroclatic micro-structure and are rich in pyrite,all of which indi-cate the coal-forming environment had higher oxidation potential,strong and roiling water dynamics,and intermittent exposure to a sulfur rich environment.展开更多
Lithium-sulfur batteries(LSBs)are promising alternative energy storage devices to the commercial lithium-ion batteries.However,the LSBs have several limitations including the low electronic conductivity of sulfur(5...Lithium-sulfur batteries(LSBs)are promising alternative energy storage devices to the commercial lithium-ion batteries.However,the LSBs have several limitations including the low electronic conductivity of sulfur(5×10^-30S cm^-1),associated lithium polysulfides(PSs),and their migration from the cathode to the anode.In this study,a separator coated with a Ketjen black(KB)/Nafion composite was used in an LSB with a sulfur loading up to 7.88 mg cm^-2to mitigate the PS migration.A minimum specific capacity(Cs)loss of 0.06%was obtained at 0.2 C-rate at a high sulfur loading of 4.39 mg cm^-2.Furthermore,an initial areal capacity up to 6.70 mAh cm^-2 was obtained at a sulfur loading of 7.88 mg cm^-2.The low Cs loss and high areal capacity associated with the high sulfur loading are attributed to the large surface area of the KB and sulfonate group(SO3^-)of Nafion,respectively,which could physically and chemically trap the PSs.展开更多
Contents of the rare-earth elements (REE) in two coal seams from North Shanxi Province, China, were determined using the instrumental neutron activation method. Based on the REE distribution patterns, and correlation ...Contents of the rare-earth elements (REE) in two coal seams from North Shanxi Province, China, were determined using the instrumental neutron activation method. Based on the REE distribution patterns, and correlation analysis and cluster analysis, the main conclusions were drawn as follows. The REE contents are controlled mainly by the coal-forming environments, but might be affected by acidic solution leaching after peat sedimentation. The REE distribution patterns should be nearly the same in the sublayers of the same coal seam, and the occurrence of abnormal patterns might indicate the geological effect during post-sedimentation. The REE in coals are present mainly in the inorganic phase, and might be derived mainly from terrigenous detrital minerals. Some harmful elements, such as V, P, Mo, Cr, Cu, Mo, Th and Cd, might have cleaning potential during processing and dressing by washing because they are associated with REE.展开更多
基金Project(2013AA064102)supported by the National High Technology Research and Development Program of China
文摘In order to fundamentally solve the acidification problem of high sulfur-containing bauxite during storage, by simulating the environment of minerals storage in laboratory, the acidification mechanism and influencing factors of high sulfur-containing bauxite were studied and confirmed using the single variable method to control the atmosphere, water and other variables. The results show that the acidification is mostly caused by the oxidation of sulfur-containing bauxite, which is mainly the natural oxidation of Pyrite(Fe S2), then the alkaline minerals dissolute in the presence of water, leading to the acidification phenomenon, which is influenced by moisture and air flow. Finally, more acid-producing substances are formed, resulting in the acidification of high sulfur-containing bauxite. The acidification of high sulfur-containing bauxite results from the combined effect of the oxygen in the air and water, which can be significantly alleviated by controlling the diffusion of the oxygen in air.
文摘The reverse flocculation method for removing pyritic sulfur from high sulfor coals has been conceptually beveloped and investigated. The tentative tests on China high sulfur coals have shown that this advanced physical separation techaique can be very efficient in coal desulfurization, provided the process parameters are properly optimized. Under the circumsances of acquiring high coal recovery, the total sulfur rejection with four kinds of coal samples normally falls in tbe range 57% to 71 % by one-step reverse flocculation, and within the range 40% to 59% by one-step normal flocculation process.
文摘Processing of Iranian high sulfur iron ore is problematic in minerals industry. The iron ores were studied by the means of polarizing microscopy, chemical analysis, X-ray diffraction. The study shows that the iron ores have high grade of iron, and complex structures. XRD showed that the iron ore consists of metallic minerals such as magnetite with a small amount of hematite and limonite and non-metallic minerals as serpentine, chlorite, and talc. The average particle size of magnetite crystals is 0.182 mm. The ore contains 1.62% sulfur as harmful impurity in form of pyrite mineral. Due to the isomorphism of magnesium and iron, magnetite mono crystal grade is lower than 68%, and difficult to be physically upgraded to a higher-grade iron concentrate using the available mineral processing technologies.
基金Project supported by the National Key Research and Development Program of China(Grant No.2017YFA0402400)the National Natural Science Foundation of China(Grant Nos.11974358 and 11934004)+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB34020000)the Heavy Ion Research Facility in Lanzhou(HIRFL).
文摘The state-selective cross section data are useful for understanding and modeling the x-ray emission in celestial observations.In the present work,using the cold target recoil ion momentum spectroscopy,for the first time we investigated the state-selective single electron capture processes for S^(q+)–He and H_(2)(q=11–15)collision systems at an impact energy of q×20 keV and obtained the relative state-selective cross sections.The results indicate that only a few principal quantum states of the projectile energy level are populated in a single electron capture process.In particular,the increase of the projectile charge state leads to the population of the states with higher principal quantum numbers.It is also shown that the experimental averaged n-shell populations are reproduced well by the over-barrier model.The database is openly available in Science Data Bank at 10.57760/sciencedb.j00113.00091.
基金the National Natural Science Foundation of China(52103093)the Young Elite Scientists Sponsorship Program by China Association for Science and Technology(2021QNRC001)+2 种基金the Jiangxi Provincial Natural Science Foundation(20212BAB214048)Science and Technology Support Project of Shangrao(2020L009,2021J006)Science and Technological Project of Education Department of Jiangxi(GJJ211704)for funding their contributions to this paper。
文摘Lithium sulfur batteries(LSBs)are recognized as promising devices for developing next-generation energy storage systems.In addition,they are attractive rechargeable battery systems for replacing lithium-ion batteries(LIBs)for commercial use owing to their higher theoretical energy density and lower cost compared to those of LIBs.However,LSBs are still beset with some persistent issues that prevent them from being used industrially,such as the unavoidable dissolution of lithium polysulfide intermediates during electrochemical reactions and large volume expansion(up to 80%)upon the formation of Li_(2)S,resulting in serious battery life and safety limitations.In the process of solving these problems,it is necessary to maintain a high sulfur content in the cathode materials to ensure that the LSBs have high energy densities and excellent cycle performance.In this review,the novel preparation methods and cathode materials used for preparing LSBs in recent years are reviewed considering the sulfur content and cycle performance.In addition,the problems and difficulties in practically applying cathode materials are described,and the development trend is discussed.
基金financial support from the National Natural Science Foundation of China (NSFC,21875155,22032004)the support of the National Key Research and Development Program of China (2021YFA1201502)the support of the Nanqiang Young Top-notch Talent Fellowship in Xiamen University。
文摘The practical application of lithium-sulfur(Li-S)batteries is greatly hindered by soluble polysulfides shuttling and sluggish sulfur redox kinetics.Rational design of multifunctional hybrid materials with superior electronic conductivity and high electrocatalytic activity,e.g.,heterostructures,is a promising strategy to solve the above obstacles.Herein,a binary metal sulfide MnS-MoS_(2) heterojunction electrocatalyst is first designed for the construction of high-sulfur-loaded and durable Li-S batteries.The MnS-MoS_(2) p-n heterojunction shows a unique structure of MoS_(2) nanosheets decorated with ample MnS nanodots,which contributes to the formation of a strong built-in electric field at the two-phase interface.The MnS-MoS_(2) hybrid host shows strong soluble polysulfide affinity,enhanced electronic conductivity,and exceptional catalytic effect on sulfur reduction.Benefiting from the synergistic effect,the as-derived S/MnS-MoS_(2) cathode delivers a superb rate capability(643 m A h g^(-1)at 6 C)and a durable cyclability(0.048%decay per cycle over 1000 cycles).More impressively,an areal capacity of 9.9 m A h cm^(-2)can be achieved even under an extremely high sulfur loading of 14.7 mg cm^(-2)and a low electrolyte to sulfur ratio of 2.9μL mg^(-1).This work provides an in-depth understanding of the interfacial catalytic effect of binary metal compound heterojunctions on sulfur reaction kinetics.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.52270006 and 22209063)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(19KJA460004)the Priority Academic Program Development of Jiangsu Higher Education Institutions,and the Natural Science Foundation of Xuzhou City(KC21283).
文摘Achieving high loading of active sulfur yet rational regulating the shuttle effect of lithium polysulfide(LiPS)is of great significance in pursuit of high-performance lithium-sulfur(Li-S)battery.Herein,we develop a free-standing graphene nitrogen(N),phosphorus(P)and fluorine(F)co-doped mesoporous carbon-sulfur(G-NPFMC-S)film,which was used as a binder-free cathode in Li-S battery.The developed mesoporous carbon(MC)achieved a high specific surface area of 921 m^(2)·g^(-1)with a uniform pore size distribution of 15 nm.The inserted graphene network inside G-NPFMC-S cathode can effectively improve its electrical conductivity and simultaneously restrict the shuttle of LiPS.A high sulfur loading of 86%was achieved due to the excellent porous structures of graphene-NPFMC(G-NPFMC)composite.When implemented as a freestanding cathode in Li-S battery,this G-NPFMC-S achieved a high specific capacity(1,356 mAh·g^(-1)),favorable rate capability,and long-term cycling stability up to 500 cycles with a minimum capacity fading rate of 0.025%per cycle,outperforming the corresponding performances of NPFMC-sulfur(NPFMC-S)and MC-sulfur(MC-S).These promising results can be ascribed to the featured structures that formed inside G-NPFMC-S film,as that highly porous NPFMC can provide sufficient storage space for the loading of sulfur,while,the N,P,F-doped carbonic interface and the inserted graphene network help hinder the shuttle of LiPS via chemical adsorption and physical barrier effect.This proposed unique structure can provide a bright prospect in that high mass loading of active sulfur and restriction the shuttle of LiPS can be simultaneously achieved for Li-S battery.
基金supported by Scientific and Technological Key Project of Shanxi Province(20191102003)National Key Research and Development Program(2016YFA0202500)+1 种基金the National Natural Science Foundation of China(21776019)Beijing Natural Science Foundation(L182021)。
文摘Lithium-sulfur(Li-S)battery is regarded as one of the most promising next-generation energy storage systems due to the ultra-high theoretical energy density of 2600 Wh kg^(-1).To address the insulation nature of sulfur,nanocarbon composition is essential to afford acceptable cycling capacity but inevitably sacrifices the actual energy density under working conditions.Therefore,rational structural design of the carbon/sulfur composite cathode is of great significance to realize satisfactory electrochemical performances with limited carbon content.Herein,the cathode carbon distribution is rationally regulated to construct high-sulfur-content and high-performance Li-S batteries.Concretely,a double-layer carbon(DLC)cathode is prepared by fabricating a surface carbon layer on the carbon/sulfur composite.The surface carbon layer not only provides more electrochemically active surfaces,but also blocks the polysulfide shuttle.Consequently,the DLC configuration with an increased sulfur content by nearly 10 wt%renders an initial areal capacity of 3.40 mAh cm^(-2) and capacity retention of 83.8%during 50 cycles,which is about two times than that of the low-sulfur-content cathode.The strategy of carbon distribution regulation affords an effective pathway to construct advanced high-sulfur-content cathodes for practical high-energy-density Li-S batteries.
基金financially supported by National Key Research and Development Program(No.2019YFA0210600)the Major Technological Innovation Project of Hubei Science and Technology Department(No.2019AAA164)+1 种基金the National Natural Science Foundation of China(No.51972107)the Innovative Research Groups of Hunan Province(No.2019JJ10001)。
文摘The lithium-sulfur battery is the subject of much recent attention due to the high theoretical energy density,but practical applications are challenged by fast decay owing to polysulfide shuttle and electrode architecture degradation.A comprehensive study of the sulfur host microstructure design and the cell architecture construction based on the MXene phase(Ti3C2Tx nanosheets) is performed,aiming at realize stable cycling performance of Li-S battery with high sulfur areal loading.The interwoven KB@Ti3C2Tx composite formed by self-assembly of MXene and Ktej en black,not only provides superior conductivity and maintains the electrode integrality bearing the volume expansion/shrinkage when used as the sulfur host,but also functions as an interlayer on separator to further retard the polysulfide cross-diffusion that possibly escaped from the cathode.The KB@Ti3C2Tx interlayer is only 0.28 mg cm-2 in areal loading and 3 μm in thickness,which accounts a little contribution to the thick sulfur electrode;thus,the impacts on the energy density is minimal.By coupling the robust KB@Ti3C2Tx cathode and the effective KB@Ti3C2Tx modified separator,a stable Li-S battery with high sulfur areal loading(5.6 mg cm-2) and high areal capacity(6.4 mAh cm-2) at relatively lean electrolyte is achieved.
基金supported by grants from the Research Grants Council of the Hong Kong Special Administrative Region,China(Poly U25216121,Poly U15303219)the National Natural Science Foundation of China for Young Scholar(52102310)the Research Committee of the Hong Kong Polytechnic University(A-PB1 M,1-BBXK,1-CD4 M,and G-UAMV)。
文摘High-energy lithium-sulfur batteries(LSBs)have experienced relentless development over the past decade with discernible improvements in electrochemical performance.However,a scrutinization of the cell operation conditions reveals a huge gap between the demands for practical batteries and those in the literature.Low sulfur loading,a high electrolyte/sulfur(E/S)ratio and excess anodes for lab-scale LSBs significantly offset their high-energy merit.To approach practical LSBs,high loading and lean electrolyte parameters are needed,which involve budding challenges of slow charge transfer,polysulfide precipitation and severe shuttle effects.To track these obstacles,the exploration of electrocatalysts to immobilize polysulfides and accelerate Li-S redox kinetics has been widely reported.Herein,this review aims to survey state-of-the-art catalytic materials for practical LSBs with emphasis on elucidating the correlation among catalyst design strategies,material structures and electrochemical performance.We also statistically evaluate the state-of-the-art catalyst-modified LSBs to identify the remaining discrepancy between the current advancements and the real-world requirements.In closing,we put forward our proposal for a catalytic material study to help realize practical LSBs.
基金financially supported by the National Natural Science Foundation of China (U1705255 and 21975158)the Program of Shanghai Academic Research Leader (20XD1401900)the Key-Area Research and Development Program of Guangdong Province (2019B090908001)。
文摘High-energy density lithium-sulfur(Li-S) batteries have received intensive attention as promising energy storage system.Among diverse sulfur-based cathodes,sulfurized pyrolyzed poly(acrylonitrile)(S@pPAN)cathode delivered superior electrochemical performance.However,the sulfur content of S@pPAN is relatively low(<50 wt%),which significantly limits the energy density.Herein,a hydrogel SA-Cu binder was proposed with a crosslinking network constructed by Cu^(2+) ions.The introduction of Cu^(2+) ions enabled excellent electrochemical behaviors of S@pPAN cathode even with high sulfur content of 52.6 wt% via chemical interaction with sulfur and polysulfide.Moreover,a favorable cathode interphase was formed containing electrochemically active and conductive CuSx.S@pPAN/SA-Cu exhibited a high sulfur utilization of 85.3%,long cycling stability over 1000 cycles and remarkable capacity of 1200 mAh g_(s)^(-1) even at10 C.Furthermore,ascribed to the improved electrode structure,high-loading electrode(sulfur loading:4 mg cm^(-2)) displayed stable cycling with areal capacity of 5.26 mAh cm^(-2)(1315 mAh g_(s)^(-1)) after 40 cycles.This study provides new directions to prepare high-sulfur content and high-loading S@pPAN cathode for higher energy density.
基金This work was supported by the National Key Research and Development Program of China(No.2018YFE0124500)the Young Elite Scientists Sponsorship Program by Tianjin of China(No.TJSQNTJ-2020-11)the National Natural Science Foundation of China(Nos.51932005,U1710109).
文摘Practical Li-sulfur batteries require the high sulfur loading cathode to meet the large-capacity power demand of electrical equipment.However,the sulfur content in cathode materials is usually unsatisfactory due to the excessive use of carbon for improving the conductivity.Traditional cathode fabrication strategies can hardly realize both high sulfur content and homogeneous sulfur distribution without aggregation.Herein,we designed a cathode material with ultrahigh sulfur content of 88%(mass fraction)by uniformly distributing the water dispersible sulfur nanoparticles on three-dimensionally conductive graphene framework.The water processable fabrication can maximize the homogeneous contact between sulfur nanoparticles and graphene,improving the utilization of the interconnected conductive surface.The obtained cathode material showed a capacity of 500 mA·h/g after 500 cycles at 2.0 A/g with an areal loading of 2 mg/cm2.This strategy provides possibility for the mass production of high-performance electrode materials for high-capacity Li-S battery.
基金supported by the National Key Research and Development Program(2016YFA0202500 and 2016YFA0200102)the National Natural Science Foundation of China(21776019,21805162,51772069,and U1801257)+1 种基金China Postdoctoral Science Foundation(2018M630165)Beijing Key Research and Development Plan(Z181100004518001)
文摘Lithium–sulfur(Li–S)batteries have been recognized as promising substitutes for current energy-storage technologies owing to their exceptional advantages in very high-energy density and excellent material sustainability.The cathode with high sulfur areal loading is vital for the practical applications of Li–S batteries with very high energy density.However,the high sulfur loading in an electrode results in poor rate and cycling performances of batteries in most cases.Herein,we used diameters of 5.0(D5)and 13.0(D13)mm to probe the effect of electrodes with different sizes on the rate and cycling performances under a high sulfur loading(4.5 mg cm^-2).The cell with D5 sulfur cathode exhibits better rate and cycling performances comparing with a large(D13)cathode.Both the high concentration of lithium polysulfides and corrosion of lithium metal anode impede rapid kinetics of sulfur redox reactions,which results in inferior battery performance of the Li–S cell with large diameter cathode.This work highlights the importance of rational matching of the large sulfur cathode with a high areal sulfur loading,carbon modified separators,organic electrolyte,and Li metal anode in a pouch cell,wherein the sulfur redox kinetics and lithium metal protection should be carefully considered under the flooded lithium polysulfide conditions in a working Li–S battery.
基金Projects 40572095 supported by NSFC and 20060290503 by China Ministry of Education
文摘Super-high sulfur coal resultes in serious coal-derived pollution but might have a particular genesis. Thus,a columnar section of an Early Permian Liangshan Formation coal seam. weight average sulfur content 5.80%,from Kaili,eastern Guizhou,was studied using the methods of coal petrology and geochemistry. The results show that the seam was apparently formed in seawater-effected peat bogs that developed in two distinct stages. During the first stage various layers were formed in a supratidal bog and have a composition characteristic of a bog with a gradually decreasing sea-water effect,decreasing water dynamics,and an increasingly reductive environment. Layers in the upper seam formed during a second stage in an intertidal bog. These layers are very high in total and inorganic sulfur,the ratios of or-ganic/inorganic sulfur and V/I drop,they are high in coal ash yield and have a high ash component index,considerable barkinite,oxidized and detrital macerals,have a porphyroclatic micro-structure and are rich in pyrite,all of which indi-cate the coal-forming environment had higher oxidation potential,strong and roiling water dynamics,and intermittent exposure to a sulfur rich environment.
基金the Australian Government and University of Queensland for the research training program scholarship and research facilities used in this study.
文摘Lithium-sulfur batteries(LSBs)are promising alternative energy storage devices to the commercial lithium-ion batteries.However,the LSBs have several limitations including the low electronic conductivity of sulfur(5×10^-30S cm^-1),associated lithium polysulfides(PSs),and their migration from the cathode to the anode.In this study,a separator coated with a Ketjen black(KB)/Nafion composite was used in an LSB with a sulfur loading up to 7.88 mg cm^-2to mitigate the PS migration.A minimum specific capacity(Cs)loss of 0.06%was obtained at 0.2 C-rate at a high sulfur loading of 4.39 mg cm^-2.Furthermore,an initial areal capacity up to 6.70 mAh cm^-2 was obtained at a sulfur loading of 7.88 mg cm^-2.The low Cs loss and high areal capacity associated with the high sulfur loading are attributed to the large surface area of the KB and sulfonate group(SO3^-)of Nafion,respectively,which could physically and chemically trap the PSs.
文摘Contents of the rare-earth elements (REE) in two coal seams from North Shanxi Province, China, were determined using the instrumental neutron activation method. Based on the REE distribution patterns, and correlation analysis and cluster analysis, the main conclusions were drawn as follows. The REE contents are controlled mainly by the coal-forming environments, but might be affected by acidic solution leaching after peat sedimentation. The REE distribution patterns should be nearly the same in the sublayers of the same coal seam, and the occurrence of abnormal patterns might indicate the geological effect during post-sedimentation. The REE in coals are present mainly in the inorganic phase, and might be derived mainly from terrigenous detrital minerals. Some harmful elements, such as V, P, Mo, Cr, Cu, Mo, Th and Cd, might have cleaning potential during processing and dressing by washing because they are associated with REE.