Compared with organic electrolytes,aqueous electrolytes exhibit significantly higher ionic conductivity and possess inherent safety features,showcasing unique advantages in supercapacitors.However,challenges remain fo...Compared with organic electrolytes,aqueous electrolytes exhibit significantly higher ionic conductivity and possess inherent safety features,showcasing unique advantages in supercapacitors.However,challenges remain for low-salt aqueous electrolytes operating at high voltage and low temperature.Herein,we report a low-salt(0.87 m,m means mol kg^(-1))'salt in dimethyl sulfoxide/water'hybrid electrolyte with non-flammability via hybridizing aqueous electrolyte with an organic co-solvent of dimethyl sulfoxide(hydrogen bond acceptor).As a result,the 0.87 m hybrid electrolyte exhibits enhanced electrochemical stability,a freezing temperature below-50℃,and an outstanding ionic conductivity of 0.52mS cm~(-1)at-50℃.Dimethyl sulfoxide can anchor water molecules through intermolecular hydrogen bond interaction,effectively reinforcing the stability of water in the hybrid electrolyte.Furthermore,the interaction between dimethyl sulfoxide and water molecules diminishes the involvement of water in the generation of ordered ice crystals,finally facilitating the low-temperature performance of the hybrid electrolyte.When paired with the 0.87 m'salt in dimethyl sulfoxide/water'hybrid electrolyte,the symmetric supercapacitor presents a 2.0 V high operating voltage at 25℃,and can operate stably at-50℃.Importantly,the suppressed electrochemical reaction of water at-50℃further leads to the symmetric supercapacitor operated at a higher voltage of 2.6 V.This modification strategy opens an effective avenue to develop low-salt electrolytes for high-voltage and low-temperature aqueous supercapacitors.展开更多
Sediment-laden sea ice plays an important role in Arctic sediment transport and biogeochemical cycles,as well as the shortwave radiation budget and melt onset of ice surface.However,at present,there is a lack of effic...Sediment-laden sea ice plays an important role in Arctic sediment transport and biogeochemical cycles,as well as the shortwave radiation budget and melt onset of ice surface.However,at present,there is a lack of efficient observation approach from both space and in situ for the coverage of Arctic sediment-laden sea ice.Thus,both spatial distribution and long-term changes in area fraction of such ice floes are still unclear.This study proposes a new classification method to extract Arctic sediment-laden sea ice on the basic of the difference in spectral characteristics between sediment-laden sea ice and clean sea ice in the visible band using the MOD09A1 data with the resolution of 500 m,and obtains its area fraction over the pan Arctic Ocean during 2000−2021.Compared with Landsat-8 true color verification images with a resolution of 30 m,the overall accuracy of our classification method is 92.3%,and the Kappa coefficient is 0.84.The impact of clouds on the results of recognition and spatiotemporal changes of sediment-laden sea ice is relatively small from June to July,compared to that in May or August.Spatially,sediment-laden sea ice mostly appears over the marginal seas of the Arctic Ocean,especially the continental shelf of Chukchi Sea and the Siberian seas.Associated with the retreat of Arctic sea ice extent,the total area of sediment-laden sea ice in June-July also shows a significant decreasing trend of 8.99×10^(4) km^(2) per year.The occurrence of sediment-laden sea ice over the Arctic Ocean in June-July leads to the reduce of surface albedo over the ice-covered ocean by 14.1%.This study will help thoroughly understanding of the role of sediment-laden sea ice in the evolution of Arctic climate system and marine ecological environment,as well as the heat budget and mass balance of sea ice itself.展开更多
Supercapacitors are one of the most promising energy storage devices in the fields of vehicle transportation,flexible electronic devices,aerospace,etc.However,the existed self-discharge that is the spontaneous voltage...Supercapacitors are one of the most promising energy storage devices in the fields of vehicle transportation,flexible electronic devices,aerospace,etc.However,the existed self-discharge that is the spontaneous voltage decay after supercapacitors are fully charged,brings about the wide gap between experimental studies and practical utilization of supercapacitors.Although eliminating the selfdischarge completely is not reachable,suppressing the self-discharge rate to the lowest point is possible and feasible.So far,the significant endeavors have been devoted to achieve this goal.Herein,we summary and discuss the possible mechanisms for the self-discharge and the underlying influence factors.Moreover,the strategies to suppress the self-discharge are systemically summed up by three independent but unified aspects:modifying the electrode,modulating the electrolyte and tuning the separator.Finally,the major challenges to suppress the self-discharge of supercapacitors are concluded and the promising strategies are also pointed out and discussed.This review is presented with the view of serving as a guideline to suppress the self-discharge of supercapacitors and to across-the-board facilitate their widespread application.展开更多
For electric double layer supercapacitors,carbon materials originating from the purely physical energystorage mechanism limit the improvement in the capabilities of charge storage.To solve this problem,doping heteroat...For electric double layer supercapacitors,carbon materials originating from the purely physical energystorage mechanism limit the improvement in the capabilities of charge storage.To solve this problem,doping heteroatoms into carbon skeleton is a promising&charming strategy for enhancing electrochemical performance by providing the extra pseudocapacitance.However,the self-discharge behavior of such heteroatom-doped supercapacitors has been a challenging issue for a long time.Here,the porous carbon nanosheets with a tunable total content of heteroatoms are chosen as a demo to systemically decouple the correlation between the total content of heteroatoms and the specific capacitance as well as the self-discharge behavior.The capacitance changes in a range of 164–331 F g^(-1)@1 A g^(-1)with the increased total contents of doped heteroatom,strongly dependent on and sensitive to the total content of heteroatoms.The voltage retention rate and capacitance retention rate for the porous carbon nanosheets with a tunable total content of heteroatoms completely present a quick decline tendency as the increase in the content of heteroatoms,changing from 58%to 34%and 74%to 39%,respectively,indicative of a linear negative relationship.More importantly,the self-discharge mechanisms are elaborately explored and follow the combination of activation-and diffusion-controlled Faradic reactions.This work illustrates the diverse impacts of the doped heteroatoms on the electrochemical performance of supercapacitors,covering specific capacitance and self-discharge behavior,and highlights the importance of balancing the contents of doped heteroatoms in energy storage fields.展开更多
It is highly desirable for the promising sodium storage possessing high rate and long stable capability,which are mainly hindered by the unstable yet conventional solvent-derived organic-rich solid electrolyte interph...It is highly desirable for the promising sodium storage possessing high rate and long stable capability,which are mainly hindered by the unstable yet conventional solvent-derived organic-rich solid electrolyte interphases.Herein,an electrolyte solvation chemistry is elaborately manipulated to produce an enhanced anion-derived and inorganic components-dominated solid electrolyte interphases by introducing a low permittivity(4.33)bis(2,2,2-trifluoroethyl)ether diluent into the sodium bis(trifluoromethylsulfonyl)imidedimethoxyethane-based high concentration electrolyte to obtain a localized high concentration electrolyte.The bis(2,2,2-trifluoroethyl)ether breaks the balance of original cation solvation structure and tends to interact with Na^(+)-coordinated dimethoxyethane solvent rather than Na^(+)in high concentration electrolyte,leaving an enhanced Coulombic interaction between Na^(+)and(FSO_(2))_(2)N^(-),and more(FSO_(2))_(2)N^(-)can enter the Na^(+)solvation shell,forming a further increased number of Na^(+)-(FSO_(2))_(2)N^(-)-dimethoxyethane clusters(from 82.0%for high concentration electrolyte to 94.3%for localized high concentration electrolyte)at a low salt dosage.The preferential reduction of this(FSO_(2))_(2)N^(-)-enriched clusters rather than the dimethoxyethane-dominated Na^(+)solvation structure produces an enhanced anion-derived and inorganic components-dominated solid electrolyte interphases.The reversible charge storage process of Na is decoupled by operando Raman along with a shift of D and G peaks.Benefiting from the enhanced anion-derived electrode-electrolyte interface,the commercial hard carbon anode in localized high concentration electrolyte shows a well rate capability(5 A g^(−1),70 mAh g^(−1)),cycle performance and stability(85%of initial capacity after 700 cycles)in comparison to that of high concentration electrolyte(68%)and low concentration electrolyte(only 5%after 400 cycles),indicative of uniqueness and superiorities towards stable Na storage.展开更多
Amorphous carbon derived from biomass unusually combines the merits of large specific surface area and abundant micropores,offering massive anchoring points for ion adsorption in electrolyte.Nevertheless,the short-ran...Amorphous carbon derived from biomass unusually combines the merits of large specific surface area and abundant micropores,offering massive anchoring points for ion adsorption in electrolyte.Nevertheless,the short-range ordered structure in amorphous carbon hinders the fast electron transfer.Conversely,graphitic carbon with long-range ordered structure is beneficial for electron transfer.Thus,a low-cost strategy is required to marry hierarchical porous structure with long-range ordered structure,resulting in a long/short-range interconnected porous carbon and then leading to fast ion and electron transfer.Herein,we modified the solid-phase conversion process of biomass by employing the features of liquid-phase carbonization for petroleum asphalt.With the assistance of asphalt,the large specific surface area(>2,000 m^(2)·g^(-1)),high ratio of mesopores(ca.60%)together with long-range ordered structure are in-situ created in as-made porous carbon.Thanks to the well configured structure in small scale,the as-made co-converted carbon can be operated in high-viscosity EMIMBF4 electrolyte with a superior capacitance(315 F·g^(-1)@1 A·g^(-1)).Besides,the as-assembled symmetric supercapacitor can deliver a super-high specific energy of 174 Wh·kg^(-1)@2.0 kW·kg^(-1).This work provides a new version for designing highly porous biomass-derived carbon with long/short-range alternating structure at molecular level.展开更多
基金partly supported by the National Key R&D Program of China(2022YFB4101602)the National Natural Science Foundation of China(22078052)the Fundamental Research Funds for the Central Universities(DUT22ZD207)。
文摘Compared with organic electrolytes,aqueous electrolytes exhibit significantly higher ionic conductivity and possess inherent safety features,showcasing unique advantages in supercapacitors.However,challenges remain for low-salt aqueous electrolytes operating at high voltage and low temperature.Herein,we report a low-salt(0.87 m,m means mol kg^(-1))'salt in dimethyl sulfoxide/water'hybrid electrolyte with non-flammability via hybridizing aqueous electrolyte with an organic co-solvent of dimethyl sulfoxide(hydrogen bond acceptor).As a result,the 0.87 m hybrid electrolyte exhibits enhanced electrochemical stability,a freezing temperature below-50℃,and an outstanding ionic conductivity of 0.52mS cm~(-1)at-50℃.Dimethyl sulfoxide can anchor water molecules through intermolecular hydrogen bond interaction,effectively reinforcing the stability of water in the hybrid electrolyte.Furthermore,the interaction between dimethyl sulfoxide and water molecules diminishes the involvement of water in the generation of ordered ice crystals,finally facilitating the low-temperature performance of the hybrid electrolyte.When paired with the 0.87 m'salt in dimethyl sulfoxide/water'hybrid electrolyte,the symmetric supercapacitor presents a 2.0 V high operating voltage at 25℃,and can operate stably at-50℃.Importantly,the suppressed electrochemical reaction of water at-50℃further leads to the symmetric supercapacitor operated at a higher voltage of 2.6 V.This modification strategy opens an effective avenue to develop low-salt electrolytes for high-voltage and low-temperature aqueous supercapacitors.
基金The National Key Research and Development Program of China under contract No.2021YFC2803304the National Natural Science Foundation of China under contract No.42325604+2 种基金the Program of Shanghai Academic/Technology Research Leader under contract No.22XD1403600the Fundamental Research Funds for the Central Universities under contract No.2042024kf0037the Fund of Key Laboratory for Polar Science,Ministry of Natural Resources,Polar Research Institute of China,under contract No.KP202004.
文摘Sediment-laden sea ice plays an important role in Arctic sediment transport and biogeochemical cycles,as well as the shortwave radiation budget and melt onset of ice surface.However,at present,there is a lack of efficient observation approach from both space and in situ for the coverage of Arctic sediment-laden sea ice.Thus,both spatial distribution and long-term changes in area fraction of such ice floes are still unclear.This study proposes a new classification method to extract Arctic sediment-laden sea ice on the basic of the difference in spectral characteristics between sediment-laden sea ice and clean sea ice in the visible band using the MOD09A1 data with the resolution of 500 m,and obtains its area fraction over the pan Arctic Ocean during 2000−2021.Compared with Landsat-8 true color verification images with a resolution of 30 m,the overall accuracy of our classification method is 92.3%,and the Kappa coefficient is 0.84.The impact of clouds on the results of recognition and spatiotemporal changes of sediment-laden sea ice is relatively small from June to July,compared to that in May or August.Spatially,sediment-laden sea ice mostly appears over the marginal seas of the Arctic Ocean,especially the continental shelf of Chukchi Sea and the Siberian seas.Associated with the retreat of Arctic sea ice extent,the total area of sediment-laden sea ice in June-July also shows a significant decreasing trend of 8.99×10^(4) km^(2) per year.The occurrence of sediment-laden sea ice over the Arctic Ocean in June-July leads to the reduce of surface albedo over the ice-covered ocean by 14.1%.This study will help thoroughly understanding of the role of sediment-laden sea ice in the evolution of Arctic climate system and marine ecological environment,as well as the heat budget and mass balance of sea ice itself.
基金partly supported by the National Natural Science Foundation of China(NSFC,No.51872035)the Talent Program of Rejuvenation of the Liaoning(No.XLYC1807002)+1 种基金the Fundamental Research Funds for the Central Universities(DUT19LAB20)the National Key Research Development Program of China(2016YFB0101201)。
文摘Supercapacitors are one of the most promising energy storage devices in the fields of vehicle transportation,flexible electronic devices,aerospace,etc.However,the existed self-discharge that is the spontaneous voltage decay after supercapacitors are fully charged,brings about the wide gap between experimental studies and practical utilization of supercapacitors.Although eliminating the selfdischarge completely is not reachable,suppressing the self-discharge rate to the lowest point is possible and feasible.So far,the significant endeavors have been devoted to achieve this goal.Herein,we summary and discuss the possible mechanisms for the self-discharge and the underlying influence factors.Moreover,the strategies to suppress the self-discharge are systemically summed up by three independent but unified aspects:modifying the electrode,modulating the electrolyte and tuning the separator.Finally,the major challenges to suppress the self-discharge of supercapacitors are concluded and the promising strategies are also pointed out and discussed.This review is presented with the view of serving as a guideline to suppress the self-discharge of supercapacitors and to across-the-board facilitate their widespread application.
基金partly supported by the National Natural Science Foundation of China(51872035,22078052)the Innovation Program of Dalian City of Liaoning Province(2019RJ03)the Shandong Provincial Natural Science Foundation(ZR2020ZD08)。
文摘For electric double layer supercapacitors,carbon materials originating from the purely physical energystorage mechanism limit the improvement in the capabilities of charge storage.To solve this problem,doping heteroatoms into carbon skeleton is a promising&charming strategy for enhancing electrochemical performance by providing the extra pseudocapacitance.However,the self-discharge behavior of such heteroatom-doped supercapacitors has been a challenging issue for a long time.Here,the porous carbon nanosheets with a tunable total content of heteroatoms are chosen as a demo to systemically decouple the correlation between the total content of heteroatoms and the specific capacitance as well as the self-discharge behavior.The capacitance changes in a range of 164–331 F g^(-1)@1 A g^(-1)with the increased total contents of doped heteroatom,strongly dependent on and sensitive to the total content of heteroatoms.The voltage retention rate and capacitance retention rate for the porous carbon nanosheets with a tunable total content of heteroatoms completely present a quick decline tendency as the increase in the content of heteroatoms,changing from 58%to 34%and 74%to 39%,respectively,indicative of a linear negative relationship.More importantly,the self-discharge mechanisms are elaborately explored and follow the combination of activation-and diffusion-controlled Faradic reactions.This work illustrates the diverse impacts of the doped heteroatoms on the electrochemical performance of supercapacitors,covering specific capacitance and self-discharge behavior,and highlights the importance of balancing the contents of doped heteroatoms in energy storage fields.
基金partly supported by the Innovation Program of Dalian City of Liaoning Province(no.2019RJ03)National Natural Science Foundation of China(NSFC,no.51872035,22078052)
文摘It is highly desirable for the promising sodium storage possessing high rate and long stable capability,which are mainly hindered by the unstable yet conventional solvent-derived organic-rich solid electrolyte interphases.Herein,an electrolyte solvation chemistry is elaborately manipulated to produce an enhanced anion-derived and inorganic components-dominated solid electrolyte interphases by introducing a low permittivity(4.33)bis(2,2,2-trifluoroethyl)ether diluent into the sodium bis(trifluoromethylsulfonyl)imidedimethoxyethane-based high concentration electrolyte to obtain a localized high concentration electrolyte.The bis(2,2,2-trifluoroethyl)ether breaks the balance of original cation solvation structure and tends to interact with Na^(+)-coordinated dimethoxyethane solvent rather than Na^(+)in high concentration electrolyte,leaving an enhanced Coulombic interaction between Na^(+)and(FSO_(2))_(2)N^(-),and more(FSO_(2))_(2)N^(-)can enter the Na^(+)solvation shell,forming a further increased number of Na^(+)-(FSO_(2))_(2)N^(-)-dimethoxyethane clusters(from 82.0%for high concentration electrolyte to 94.3%for localized high concentration electrolyte)at a low salt dosage.The preferential reduction of this(FSO_(2))_(2)N^(-)-enriched clusters rather than the dimethoxyethane-dominated Na^(+)solvation structure produces an enhanced anion-derived and inorganic components-dominated solid electrolyte interphases.The reversible charge storage process of Na is decoupled by operando Raman along with a shift of D and G peaks.Benefiting from the enhanced anion-derived electrode-electrolyte interface,the commercial hard carbon anode in localized high concentration electrolyte shows a well rate capability(5 A g^(−1),70 mAh g^(−1)),cycle performance and stability(85%of initial capacity after 700 cycles)in comparison to that of high concentration electrolyte(68%)and low concentration electrolyte(only 5%after 400 cycles),indicative of uniqueness and superiorities towards stable Na storage.
基金supported by the National Natural Science Foundation of China(Nos.51872035 and 22078052)the Talent Program of Rejuvenation of Liaoning(No.XLYC1807002)the Innovation Program of Dalian City(No.2019RJ03).
文摘Amorphous carbon derived from biomass unusually combines the merits of large specific surface area and abundant micropores,offering massive anchoring points for ion adsorption in electrolyte.Nevertheless,the short-range ordered structure in amorphous carbon hinders the fast electron transfer.Conversely,graphitic carbon with long-range ordered structure is beneficial for electron transfer.Thus,a low-cost strategy is required to marry hierarchical porous structure with long-range ordered structure,resulting in a long/short-range interconnected porous carbon and then leading to fast ion and electron transfer.Herein,we modified the solid-phase conversion process of biomass by employing the features of liquid-phase carbonization for petroleum asphalt.With the assistance of asphalt,the large specific surface area(>2,000 m^(2)·g^(-1)),high ratio of mesopores(ca.60%)together with long-range ordered structure are in-situ created in as-made porous carbon.Thanks to the well configured structure in small scale,the as-made co-converted carbon can be operated in high-viscosity EMIMBF4 electrolyte with a superior capacitance(315 F·g^(-1)@1 A·g^(-1)).Besides,the as-assembled symmetric supercapacitor can deliver a super-high specific energy of 174 Wh·kg^(-1)@2.0 kW·kg^(-1).This work provides a new version for designing highly porous biomass-derived carbon with long/short-range alternating structure at molecular level.