In molecular modeling of electrical double layers(EDLs),the constant charge method(CCM)is prized for its computational efficiency but cannot maintain electrode equipotentiality like the more resourceintensive constant...In molecular modeling of electrical double layers(EDLs),the constant charge method(CCM)is prized for its computational efficiency but cannot maintain electrode equipotentiality like the more resourceintensive constant potential method(CPM),potentially leading to inaccuracies.In certain scenarios,CCM can yield results identical to CPM.However,there are no clear guidelines to determine when CCM is sufficient and when CPM is required.Here,we conduct a series of molecular simulations across various electrodes and electrolytes to present a comprehensive comparison between CCM and CPM under different charging modes.Results reveal that CCM approximates CPM effectively in capturing equilibrium EDL and current-driven dynamics in open electrode systems featuring ionic liquids or regular concentration aqueous electrolytes,while CPM is indispensable in scenarios involving organic and highly concentrated aqueous electrolytes,nanoconfinement effects,and voltage-driven dynamics.This work helps to select appropriate methods for modeling EDL systems,prioritizing accuracy while considering computationalefficiency.展开更多
Asymmetric behaviors of capacitance and charging dynamics in the cathode and anode are general for nanoporous supercapacitors.Understanding this behavior is essential for the optimal design of supercapacitors.Herein,w...Asymmetric behaviors of capacitance and charging dynamics in the cathode and anode are general for nanoporous supercapacitors.Understanding this behavior is essential for the optimal design of supercapacitors.Herein,we perform constant-potential molecular dynamics simulations to reveal asymmetric features of porous supercapacitors and their effects on capacitance and charging dynamics.Our simulations show that,counterintuitively,charging dynamics can be fast in pores providing slow ion diffusion and vice versa.Unlike electrodes with singlesize pores,multi-pore electrodes show overcharging and accelerated co-ion desorption,which can be attributed to the subtle interplay between the dynamics and charging mechanisms.We find that capacitance and charging dynamics correlate with how the ions respond to an applied cell voltage in the cathode and anode.We demonstrate that symmetrizing this response can help boost power density,which may find practical applications in supercapacitor optimization.展开更多
Background: Vegetation distribution maps are of great significance for nature protection and management. In diverse tropical forests, accurate spatial mapping of vegetation types is challenging;the high species divers...Background: Vegetation distribution maps are of great significance for nature protection and management. In diverse tropical forests, accurate spatial mapping of vegetation types is challenging;the high species diversity and abundance of rare species challenge classification concepts, while remote sensing signals may not vary systematically with species composition, complicating the technical capability for delineating vegetation types in the landscape.Methods: We used a combination of field-based compositional data and their relations to environmental variables to predict the distribution of forest types in the Wuzhishan National Natural Reserve(WNNR), Hainan Island,China, using multivariate regression trees(MRT). The MRT was based on arboreal vegetation composition in 132plots of 20 m×20 m with a regular spacing of 1 km. Apart from the MRT, non-metric multidimensional scaling(NMDS) was used to evaluate vegetation-environment relationships.Results: The MRT model worked best when using 14 key environmental variables including topography, climate,latitude and soil, although the difference with the simpler model including only topographical variables was small. The full model classified the 132 plots into 3 vegetation types, 6 formation groups, 20 formations and 65associations at different hierarchical syntaxonomic levels. This model was the basis for forest vegetation maps for the WNNR. MRT and NMDS showed that elevation was the main driving force for the distribution of vegetation types and formation groups. Climate, latitude, and soil(especially available P), together with topographic variables, all influenced the distribution of formations and associations.Conclusions: While elevation determines forest-type distributions, lower-level syntaxonomic forest classes respond to the topographic diversity typical for mountains. Apart from providing the first detailed forest vegetation map for any part of WNNR, we show how, in spite of limitations, MRT with existing environmental data can be a useful method for mapping diverse and remote tropical forests.展开更多
Water in room temperature ionic liquids(RTILs) could impose significant effects on their interfacial properties at a charged surface. Although the interfaces between RTILs and mica surfaces exhibit rich microstructure...Water in room temperature ionic liquids(RTILs) could impose significant effects on their interfacial properties at a charged surface. Although the interfaces between RTILs and mica surfaces exhibit rich microstructure, the influence of water content on such interfaces is little understood,in particular, considering the fact that RTILs are always associated with water due to their hygroscopicity. In this work, we studied how different types of RTILs and different amounts of water molecules affect the RTIL-mica interfaces, especially the water distribution at mica surfaces,using molecular dynamics(MD) simulation. MD results showed that(1) there is more water and a thicker water layer adsorbed on the mica surface as the water content increases, and correspondingly the average location of K^+ ions is farther from mica surface;(2) more water accumulated at the interface with the hydrophobic [Emim][TFSI] than in case of the hydrophilic [Emim][BF4] due to the respective RTIL hydrophobicity and ion size. A similar trend was also observed in the hydrogen bonds formed between water molecules. Moreover, the 2D number density map of adsorbed water revealed that the high-density areas of water seem to be related to K^+ ions and silicon/aluminum atoms on mica surface. These results are of great importance to understand the effects of hydrophobicity/hydrophicility of RTIL and water on the interfacial microstructure at electrified surfaces.展开更多
基金the funding support from the National Natural Science Foundation of China(T2325012 and 52161135104)the Program for HUST Academic Frontier Youth Team.
文摘In molecular modeling of electrical double layers(EDLs),the constant charge method(CCM)is prized for its computational efficiency but cannot maintain electrode equipotentiality like the more resourceintensive constant potential method(CPM),potentially leading to inaccuracies.In certain scenarios,CCM can yield results identical to CPM.However,there are no clear guidelines to determine when CCM is sufficient and when CPM is required.Here,we conduct a series of molecular simulations across various electrodes and electrolytes to present a comprehensive comparison between CCM and CPM under different charging modes.Results reveal that CCM approximates CPM effectively in capturing equilibrium EDL and current-driven dynamics in open electrode systems featuring ionic liquids or regular concentration aqueous electrolytes,while CPM is indispensable in scenarios involving organic and highly concentrated aqueous electrolytes,nanoconfinement effects,and voltage-driven dynamics.This work helps to select appropriate methods for modeling EDL systems,prioritizing accuracy while considering computationalefficiency.
基金funding support from the National Natural Science Foundation of China(51876072)the Hubei Provincial Natural Science Foundation of China(2019CFA002,2020CFA093)supported by the Program for HUST Academic Frontier Youth Team
文摘Asymmetric behaviors of capacitance and charging dynamics in the cathode and anode are general for nanoporous supercapacitors.Understanding this behavior is essential for the optimal design of supercapacitors.Herein,we perform constant-potential molecular dynamics simulations to reveal asymmetric features of porous supercapacitors and their effects on capacitance and charging dynamics.Our simulations show that,counterintuitively,charging dynamics can be fast in pores providing slow ion diffusion and vice versa.Unlike electrodes with singlesize pores,multi-pore electrodes show overcharging and accelerated co-ion desorption,which can be attributed to the subtle interplay between the dynamics and charging mechanisms.We find that capacitance and charging dynamics correlate with how the ions respond to an applied cell voltage in the cathode and anode.We demonstrate that symmetrizing this response can help boost power density,which may find practical applications in supercapacitor optimization.
基金financially supported by National Key R&D Program of China(2021YFD220040403 and 2021YFD220040304)the China Scholarship Council(202107565021).
文摘Background: Vegetation distribution maps are of great significance for nature protection and management. In diverse tropical forests, accurate spatial mapping of vegetation types is challenging;the high species diversity and abundance of rare species challenge classification concepts, while remote sensing signals may not vary systematically with species composition, complicating the technical capability for delineating vegetation types in the landscape.Methods: We used a combination of field-based compositional data and their relations to environmental variables to predict the distribution of forest types in the Wuzhishan National Natural Reserve(WNNR), Hainan Island,China, using multivariate regression trees(MRT). The MRT was based on arboreal vegetation composition in 132plots of 20 m×20 m with a regular spacing of 1 km. Apart from the MRT, non-metric multidimensional scaling(NMDS) was used to evaluate vegetation-environment relationships.Results: The MRT model worked best when using 14 key environmental variables including topography, climate,latitude and soil, although the difference with the simpler model including only topographical variables was small. The full model classified the 132 plots into 3 vegetation types, 6 formation groups, 20 formations and 65associations at different hierarchical syntaxonomic levels. This model was the basis for forest vegetation maps for the WNNR. MRT and NMDS showed that elevation was the main driving force for the distribution of vegetation types and formation groups. Climate, latitude, and soil(especially available P), together with topographic variables, all influenced the distribution of formations and associations.Conclusions: While elevation determines forest-type distributions, lower-level syntaxonomic forest classes respond to the topographic diversity typical for mountains. Apart from providing the first detailed forest vegetation map for any part of WNNR, we show how, in spite of limitations, MRT with existing environmental data can be a useful method for mapping diverse and remote tropical forests.
基金supported by the National Natural Science Foundation of China (51406060)Shenzhen Basic Research Project (JCYJ20170307171511292)the National Supercomputing Centers in Tianjin (Tianhe-1A) and Guangzhou (Tianhe Ⅱ)
文摘Water in room temperature ionic liquids(RTILs) could impose significant effects on their interfacial properties at a charged surface. Although the interfaces between RTILs and mica surfaces exhibit rich microstructure, the influence of water content on such interfaces is little understood,in particular, considering the fact that RTILs are always associated with water due to their hygroscopicity. In this work, we studied how different types of RTILs and different amounts of water molecules affect the RTIL-mica interfaces, especially the water distribution at mica surfaces,using molecular dynamics(MD) simulation. MD results showed that(1) there is more water and a thicker water layer adsorbed on the mica surface as the water content increases, and correspondingly the average location of K^+ ions is farther from mica surface;(2) more water accumulated at the interface with the hydrophobic [Emim][TFSI] than in case of the hydrophilic [Emim][BF4] due to the respective RTIL hydrophobicity and ion size. A similar trend was also observed in the hydrogen bonds formed between water molecules. Moreover, the 2D number density map of adsorbed water revealed that the high-density areas of water seem to be related to K^+ ions and silicon/aluminum atoms on mica surface. These results are of great importance to understand the effects of hydrophobicity/hydrophicility of RTIL and water on the interfacial microstructure at electrified surfaces.
