The stability and uniformity of solid electrolyte interphase(SEI)are critical for clarifying the origin of capacity fade and safety issues for lithium metal anodes(LMA).However,understanding the interplay of SEI heter...The stability and uniformity of solid electrolyte interphase(SEI)are critical for clarifying the origin of capacity fade and safety issues for lithium metal anodes(LMA).However,understanding the interplay of SEI heterogeneity and Li electrodeposition is limited by the coupling of complex electrochemistry and mechanics processes.Herein,the correlation between the SEI failure behavior and Li deposition morphology is investigated through a quantitative electrochemical-mechanical model.The local deformation and stress of SEI during Li electrodeposition identify that the heterogeneous interface between different components first fails.Compared with the well-known mechanical strength,component uniformity plays the most important role in the initial SEI failure and uneven Li deposition,and a relative component uniformity(p>0.01)represents a proper balance to ensure the stability of the naturally heterogeneous SEI.Furthermore,the component regulation of SEI via the designed electrolyte experimentally demonstrates that improving component uniformity benefits SEI stability and the uniform Li electrodeposition for LMA,thereby increasing the capacity by~20%after 300 cycles.These fundamental understandings and proposed strategy can be not only used to guide the SEI optimization via the electrolyte regulation,but also extended to the rational designs of artificial SEI for high-performance LMA.展开更多
Arid and semiarid ecosystems, or dryland, are important to global biogeochemical cycles. Dryland's community structure and vegetation dynamics as well as biogeochemical cycles are sensitive to changes in climate and ...Arid and semiarid ecosystems, or dryland, are important to global biogeochemical cycles. Dryland's community structure and vegetation dynamics as well as biogeochemical cycles are sensitive to changes in climate and atmospheric composition. Vegetation dynamic models has been applied in global change studies, but the com- plex interactions among the carbon (C), water, and nitrogen (N) cycles have not been adequately addressed in the current models. In this study, a process-based vegetation dynamic model was developed to study the responses of dryland ecosystems to environmental changes, emphasizing on the interactions among the C, water, and N proc- esses. To address the interactions between the C and water processes, it not only considers the effects of annual precipitation on vegetation distribution and soil moisture on organic matter (SOM) decomposition, but also explicitly models root competition for water and the water compensation processes. To address the interactions between C and N processes, it models the soil inorganic mater processes, such as N mineralization/immobilization, denitrifica- tion/nitrification, and N leaching, as well as the root competition for soil N. The model was parameterized for major plant functional types and evaluated against field observations.展开更多
Recent studies on alkaline soils of arid areas suggest a possible contribution of abiotic exchange to soil CO2 flux(Fc).However,both the overall contribution of abiotic CO2 exchange and its drivers remain unknown.He...Recent studies on alkaline soils of arid areas suggest a possible contribution of abiotic exchange to soil CO2 flux(Fc).However,both the overall contribution of abiotic CO2 exchange and its drivers remain unknown.Here we analyzed the environmental variables suggested as possible drivers by previous studies and constructed a function of these variables to model the contribution of abiotic exchange to Fc in alkaline soils of arid areas.An automated flux system was employed to measure Fc in the Manas River Basin of Xinjiang Uygur autonomous region,China.Soil pH,soil temperature at 0–5 cm(Ts),soil volumetric water content at 0–5 cm(θs)and air temperature at10 cm above the soil surface(Tas)were simultaneously analyzed.Results highlight reduced sensitivity of Fc to Ts and good prediction of Fc by the model Fc=R10Q10(Tas–10)/10+r7q7(pH–7)+λTas+μθs+e which represents Fc as a sum of biotic and abiotic components.This presents an approximate method to quantify the contribution of soil abiotic CO2 exchange to Fc in alkaline soils of arid areas.展开更多
The continuous and sustainable photo-activity on micro-or nano-carriers has always been a key stepping stone in the industrialization of photo-catalysis,photo-synthesis,and photo-degradation.Herein,we report a new ser...The continuous and sustainable photo-activity on micro-or nano-carriers has always been a key stepping stone in the industrialization of photo-catalysis,photo-synthesis,and photo-degradation.Herein,we report a new series of positively charged hollow microspheres carrying porphyrin moieties.Such hollow spheres are formed through crosslinking of well-ordered porous thin laminates,initiated by co-assembly of regular monomers and those decorated with porphyrin moieties.On the surface of an individual sphere,densely distributed positive sites attract anionic reactants.The superficial porphyrin decomposes the accumulated reactants under 1 Sun.After degradation and release of products,the photoactive sites are thereby renewed.We demonstrate that polymer network(1:10)exhibited superior sustainable photocatalytic performance with complete degradation of methyl orange(MO)in 40 min with no observable performance deterioration after six cycles.The established close loop of adsorption-reaction-release cycle makes possible many efficient and continuous photo-catalytic processes.展开更多
基金supported by the National Natural Science Foundation of China(52175317,U22B2069)the Fundamental Research Funds for the Central Universities(YCJJ202202004)+3 种基金the National Natural Science Foundation of China(52105325)the NSFC Projects of International Cooperation and Exchanges(52020105012)the Guangzhou Science and Technology Program(202201010405)the Key-Area Research and Development Program of Huizhou City(2022BQ010001)。
文摘The stability and uniformity of solid electrolyte interphase(SEI)are critical for clarifying the origin of capacity fade and safety issues for lithium metal anodes(LMA).However,understanding the interplay of SEI heterogeneity and Li electrodeposition is limited by the coupling of complex electrochemistry and mechanics processes.Herein,the correlation between the SEI failure behavior and Li deposition morphology is investigated through a quantitative electrochemical-mechanical model.The local deformation and stress of SEI during Li electrodeposition identify that the heterogeneous interface between different components first fails.Compared with the well-known mechanical strength,component uniformity plays the most important role in the initial SEI failure and uneven Li deposition,and a relative component uniformity(p>0.01)represents a proper balance to ensure the stability of the naturally heterogeneous SEI.Furthermore,the component regulation of SEI via the designed electrolyte experimentally demonstrates that improving component uniformity benefits SEI stability and the uniform Li electrodeposition for LMA,thereby increasing the capacity by~20%after 300 cycles.These fundamental understandings and proposed strategy can be not only used to guide the SEI optimization via the electrolyte regulation,but also extended to the rational designs of artificial SEI for high-performance LMA.
基金supported by the International Science & Technology Cooperation Program of China (2010DFA92720-10)the "Hundred Talents Program" of the Chinese Academy of Sciences (Y174131001)supported by the National Basic Research Program of China (2009CB825105)
文摘Arid and semiarid ecosystems, or dryland, are important to global biogeochemical cycles. Dryland's community structure and vegetation dynamics as well as biogeochemical cycles are sensitive to changes in climate and atmospheric composition. Vegetation dynamic models has been applied in global change studies, but the com- plex interactions among the carbon (C), water, and nitrogen (N) cycles have not been adequately addressed in the current models. In this study, a process-based vegetation dynamic model was developed to study the responses of dryland ecosystems to environmental changes, emphasizing on the interactions among the C, water, and N proc- esses. To address the interactions between the C and water processes, it not only considers the effects of annual precipitation on vegetation distribution and soil moisture on organic matter (SOM) decomposition, but also explicitly models root competition for water and the water compensation processes. To address the interactions between C and N processes, it models the soil inorganic mater processes, such as N mineralization/immobilization, denitrifica- tion/nitrification, and N leaching, as well as the root competition for soil N. The model was parameterized for major plant functional types and evaluated against field observations.
基金supported by the National Basic Research Program of China(2009CB825105)
文摘Recent studies on alkaline soils of arid areas suggest a possible contribution of abiotic exchange to soil CO2 flux(Fc).However,both the overall contribution of abiotic CO2 exchange and its drivers remain unknown.Here we analyzed the environmental variables suggested as possible drivers by previous studies and constructed a function of these variables to model the contribution of abiotic exchange to Fc in alkaline soils of arid areas.An automated flux system was employed to measure Fc in the Manas River Basin of Xinjiang Uygur autonomous region,China.Soil pH,soil temperature at 0–5 cm(Ts),soil volumetric water content at 0–5 cm(θs)and air temperature at10 cm above the soil surface(Tas)were simultaneously analyzed.Results highlight reduced sensitivity of Fc to Ts and good prediction of Fc by the model Fc=R10Q10(Tas–10)/10+r7q7(pH–7)+λTas+μθs+e which represents Fc as a sum of biotic and abiotic components.This presents an approximate method to quantify the contribution of soil abiotic CO2 exchange to Fc in alkaline soils of arid areas.
基金supported by the National Natural Science Foundation of China(Nos.22172045,U23A20122,21905076,21905077)the Key Science Foundation Project of Henan Province(No.232300421146)the Key Scientific Research Project of Colleges and Universities in Henan Province(No.22B150001).
文摘The continuous and sustainable photo-activity on micro-or nano-carriers has always been a key stepping stone in the industrialization of photo-catalysis,photo-synthesis,and photo-degradation.Herein,we report a new series of positively charged hollow microspheres carrying porphyrin moieties.Such hollow spheres are formed through crosslinking of well-ordered porous thin laminates,initiated by co-assembly of regular monomers and those decorated with porphyrin moieties.On the surface of an individual sphere,densely distributed positive sites attract anionic reactants.The superficial porphyrin decomposes the accumulated reactants under 1 Sun.After degradation and release of products,the photoactive sites are thereby renewed.We demonstrate that polymer network(1:10)exhibited superior sustainable photocatalytic performance with complete degradation of methyl orange(MO)in 40 min with no observable performance deterioration after six cycles.The established close loop of adsorption-reaction-release cycle makes possible many efficient and continuous photo-catalytic processes.