The practical application of high-energy-density lithium-sulfur(Li-S)batteries have been highly praised for energy storage devices,while are largely hindered by the“shuttling effect”.Herein,core-shell carbon spheres...The practical application of high-energy-density lithium-sulfur(Li-S)batteries have been highly praised for energy storage devices,while are largely hindered by the“shuttling effect”.Herein,core-shell carbon spheres composed of interlinked porous core and lamellar shell were designed to restrain the polysulfide shuttling.The microporous structure with pore size of around 1 nm effectively trap lithium polysulfides.Furthermore,the interconnected porous core shortens the ion transfer distance and the lamellar carbon shell endows the carbon spheres with fast electron conduction,finally facilitating polysulfide conversion kinetics.Therefore,the Li-S batteries with the carbon spheres as the interlayer show high discharge specific capacity of 1002 m Ah/g at 2 C with 574 m Ah/g remaining after 600 cycles,and high areal capacity of 5.48 m Ah/cm^(2) with sulfur loading of 4.67 mg/cm^(2) at 0.1 C.The corresponding pouch cells also exhibit stable cycling stability with an initial discharge specific capacity of 1082 m Ah/g at 0.1 C.展开更多
The electroreduction of carbon dioxide to multi-carbon products(C_(2+))represents an effective pathway for achieving carbon cycling and high-density renewable energy storage.However,its practical implementation is cha...The electroreduction of carbon dioxide to multi-carbon products(C_(2+))represents an effective pathway for achieving carbon cycling and high-density renewable energy storage.However,its practical implementation is challenged by excessively high C-C coupling reaction energy barriers and competitive hydrogen evolution reaction(HER).Modifications to the local microenvironment play a decisive role in the three-phase interface reaction of CO_(2)electrocatalytic reduction.Therefore,this study employed an Al_(2)O_(3)-modified copper catalyst(AlO_(3)/Cu)to modulate the local reaction microenvironment,thereby promoting C_(2+)formation.Notably,the optimized Al_(2)O_(3)/Cu catalyst achieved a remarkable C_(2+)Faraday efficiency(FE)of 71.3%at-1.33 V vs.RHE(reversible hydrogen electrode;all potentials herein are referenced to RHE)in a neutral electrolyte using a flow cell,significantly outperforming unmodified Cu catalysts.This catalyst also demonstrated excellent catalytic stability,exceeding 56 h.Theoretical calculations and in situ spectroscopic characterization confirmed that introduced Al_(2)O_(3)species kinetically facilitate water dissociation and proton consumption,which is crucial for maintaining a transient localized high-pH environment under operating conditions.This alkaline microenvironment not only suppresses the HER but also stabilizes the critical Cu^(2+)/Cu^(+)active sites against over-reduction,while simultaneously lowering the energy barrier of C-C coupling reactions.This work underscores the critical role of dynamically modulating the localized chemical environment in neutral electrolytes for CO_(2)reduction reactions(CO_(2)RR),offering novel insights for designing such microenvironments.展开更多
Solid polymer electrolytes(SPEs)are promising substitutes for current flammable liquid electrolytes to achieve high-safety and high-energy-density lithium metal batteries.Polyethylene oxide(PEO)based solid polymer ele...Solid polymer electrolytes(SPEs)are promising substitutes for current flammable liquid electrolytes to achieve high-safety and high-energy-density lithium metal batteries.Polyethylene oxide(PEO)based solid polymer electrolytes have attracted increasing attention because of their excellent flexibility,manufacturability,light weight,and low-cost processing,while they often suffer from low ionic con-ductivity at room temperature,low lithium transference number and unsatisfactory interfacial resis-tance,which largely restrain their practical application.Herein,two-dimensional holey silica nanosheets(2D-HSN)as the fillers,together with LiNO_(3)as the electrolyte additive,are introduced in a PEO/poly(-vinylidene fiuoride-co-hexafluoropropylene)(PVDF-HFP)blended polymer matrix to obtain a SPE.The incorporation of HSN filler creates supplementary channels for lithium ion migration and lowers the crystallinity of the polymer,thereby facilitating the movement of lithium ions.The HSN-based SPE demonstrates higher ionic conductivity up to 3.7 x 10-4 S cm-1 at 30℃,larger Li+transference number close to 0.34,and more stable lithium plating/stripping than that without the fillers,and HSN can promote the formation of more stable solid electrolyte interphase(SEI)layer.The as-assembled LiFePO4||Li batteries deliver a high specific capacity of 159 mA h g-1 with the capacity retention of 95.5%after 200 cycles at 30℃,as well as superior rate performance and cycling stability compared to that using the blank SPE.展开更多
Pyraclostrobin,a quinone outside inhibitor(QoI)fungicide,has been registered to control apple tree Valsa canker(AVC)caused by Valsa mali in China.However,there is no data available regarding the resistance risk of V.m...Pyraclostrobin,a quinone outside inhibitor(QoI)fungicide,has been registered to control apple tree Valsa canker(AVC)caused by Valsa mali in China.However,there is no data available regarding the resistance risk of V.mali to pyraclostrobin.In this study,the sensitivities of 120 V.mali isolates to pyraclostrobin were detected.The isolates were collected from apple orchards with no application of pyraclostrob at six provinces in China during 2013–2015,and showed similar sensitivity to pyraclostrobin.The EC_(50) values of these 120 V.mali isolates to pyraclostrobin ranged from 0.0014 to 0.0240μg/mL,indicating an excellent inhibitory efficacy of pyraclostrobin to the pathogen.The EC_(50) values were distributed as a unimodal curve with a mean value of 0.0091μg/mL,and the mean EC_(50) displayed correlation with geographic location.Meanwhile,three pyraclostrobin-resistant mutants(PR mutants)of V.mali were obtained using fungicide adaption method,with a resistance factor(RF)of 41.0,56.8 and 22.0,respectively.The mutants showed a stable resistance to pyraclostrobin after 10 transfers on pyraclostrobin-free medium.Comparing with the corresponding parental isolates,the hyphal growth,mycelial dry weight and pathogenicity of PR mutants were significantly reduced,but the number of propagules showed no significant difference.More importantly,no cross-resistance of PR mutants to pyraclostrobin,tebuconazole,difenoconazole,imazalil and thiophanate-methyl was detected.In conclusion,V.mali showed a moderate risk to pyraclostrobin,and pyraclostrobin could be used as an alternative fungicide to control AVC in the field in China.展开更多
基金financially supported by National Natural Science Foundation of China(Nos.51972070 and 52062004)Guizhou Provincial High Level Innovative Talents Project(No.QKHPTRC-GCC[2022]013-1)+2 种基金Innovation Team for Advanced Electrochemical Energy Storage Devices and Key Materials of Guizhou Provincial Higher Education Institutions(No.Qian Jiao Ji[2023]054)Guizhou Provincial Science and Technology Projects(No.QKHJC[2020]1Z042)Cultivation Project of Guizhou University(No.GDPY[2019]01)。
文摘The practical application of high-energy-density lithium-sulfur(Li-S)batteries have been highly praised for energy storage devices,while are largely hindered by the“shuttling effect”.Herein,core-shell carbon spheres composed of interlinked porous core and lamellar shell were designed to restrain the polysulfide shuttling.The microporous structure with pore size of around 1 nm effectively trap lithium polysulfides.Furthermore,the interconnected porous core shortens the ion transfer distance and the lamellar carbon shell endows the carbon spheres with fast electron conduction,finally facilitating polysulfide conversion kinetics.Therefore,the Li-S batteries with the carbon spheres as the interlayer show high discharge specific capacity of 1002 m Ah/g at 2 C with 574 m Ah/g remaining after 600 cycles,and high areal capacity of 5.48 m Ah/cm^(2) with sulfur loading of 4.67 mg/cm^(2) at 0.1 C.The corresponding pouch cells also exhibit stable cycling stability with an initial discharge specific capacity of 1082 m Ah/g at 0.1 C.
基金National Natural Science Foundation of China(52074320)Joint Fund for Enterprise Innovation and Development of NSFC(U24B2037)。
文摘The electroreduction of carbon dioxide to multi-carbon products(C_(2+))represents an effective pathway for achieving carbon cycling and high-density renewable energy storage.However,its practical implementation is challenged by excessively high C-C coupling reaction energy barriers and competitive hydrogen evolution reaction(HER).Modifications to the local microenvironment play a decisive role in the three-phase interface reaction of CO_(2)electrocatalytic reduction.Therefore,this study employed an Al_(2)O_(3)-modified copper catalyst(AlO_(3)/Cu)to modulate the local reaction microenvironment,thereby promoting C_(2+)formation.Notably,the optimized Al_(2)O_(3)/Cu catalyst achieved a remarkable C_(2+)Faraday efficiency(FE)of 71.3%at-1.33 V vs.RHE(reversible hydrogen electrode;all potentials herein are referenced to RHE)in a neutral electrolyte using a flow cell,significantly outperforming unmodified Cu catalysts.This catalyst also demonstrated excellent catalytic stability,exceeding 56 h.Theoretical calculations and in situ spectroscopic characterization confirmed that introduced Al_(2)O_(3)species kinetically facilitate water dissociation and proton consumption,which is crucial for maintaining a transient localized high-pH environment under operating conditions.This alkaline microenvironment not only suppresses the HER but also stabilizes the critical Cu^(2+)/Cu^(+)active sites against over-reduction,while simultaneously lowering the energy barrier of C-C coupling reactions.This work underscores the critical role of dynamically modulating the localized chemical environment in neutral electrolytes for CO_(2)reduction reactions(CO_(2)RR),offering novel insights for designing such microenvironments.
基金supported by National Natural Science Foundation of China(grant Nos.52062004 and 51972070)Guizhou Provincial High Level Innovative Talents Project(grant No.QKHPTRC-GCC[2022]013-1)+1 种基金Guizhou Provincial Science and Technology Projects(grant Nos.QKHJC[2020]1Z042,QKHJC[2020]1Y230 and QKHZC[2021]YB317)Cultivation Project of Guizhou University(grant No.GDPY[2019]01).
文摘Solid polymer electrolytes(SPEs)are promising substitutes for current flammable liquid electrolytes to achieve high-safety and high-energy-density lithium metal batteries.Polyethylene oxide(PEO)based solid polymer electrolytes have attracted increasing attention because of their excellent flexibility,manufacturability,light weight,and low-cost processing,while they often suffer from low ionic con-ductivity at room temperature,low lithium transference number and unsatisfactory interfacial resis-tance,which largely restrain their practical application.Herein,two-dimensional holey silica nanosheets(2D-HSN)as the fillers,together with LiNO_(3)as the electrolyte additive,are introduced in a PEO/poly(-vinylidene fiuoride-co-hexafluoropropylene)(PVDF-HFP)blended polymer matrix to obtain a SPE.The incorporation of HSN filler creates supplementary channels for lithium ion migration and lowers the crystallinity of the polymer,thereby facilitating the movement of lithium ions.The HSN-based SPE demonstrates higher ionic conductivity up to 3.7 x 10-4 S cm-1 at 30℃,larger Li+transference number close to 0.34,and more stable lithium plating/stripping than that without the fillers,and HSN can promote the formation of more stable solid electrolyte interphase(SEI)layer.The as-assembled LiFePO4||Li batteries deliver a high specific capacity of 159 mA h g-1 with the capacity retention of 95.5%after 200 cycles at 30℃,as well as superior rate performance and cycling stability compared to that using the blank SPE.
基金supported by the National Key R&D Program of China(2016YFD0201100).
文摘Pyraclostrobin,a quinone outside inhibitor(QoI)fungicide,has been registered to control apple tree Valsa canker(AVC)caused by Valsa mali in China.However,there is no data available regarding the resistance risk of V.mali to pyraclostrobin.In this study,the sensitivities of 120 V.mali isolates to pyraclostrobin were detected.The isolates were collected from apple orchards with no application of pyraclostrob at six provinces in China during 2013–2015,and showed similar sensitivity to pyraclostrobin.The EC_(50) values of these 120 V.mali isolates to pyraclostrobin ranged from 0.0014 to 0.0240μg/mL,indicating an excellent inhibitory efficacy of pyraclostrobin to the pathogen.The EC_(50) values were distributed as a unimodal curve with a mean value of 0.0091μg/mL,and the mean EC_(50) displayed correlation with geographic location.Meanwhile,three pyraclostrobin-resistant mutants(PR mutants)of V.mali were obtained using fungicide adaption method,with a resistance factor(RF)of 41.0,56.8 and 22.0,respectively.The mutants showed a stable resistance to pyraclostrobin after 10 transfers on pyraclostrobin-free medium.Comparing with the corresponding parental isolates,the hyphal growth,mycelial dry weight and pathogenicity of PR mutants were significantly reduced,but the number of propagules showed no significant difference.More importantly,no cross-resistance of PR mutants to pyraclostrobin,tebuconazole,difenoconazole,imazalil and thiophanate-methyl was detected.In conclusion,V.mali showed a moderate risk to pyraclostrobin,and pyraclostrobin could be used as an alternative fungicide to control AVC in the field in China.
