Apparent critical current density(j_(Ac)^(a))of garnet all-solid-state lithium metal symmetric cells(ASSLSCs)is a fundamental parameter for designing all-solid-state lithium metal batteries.Nevertheless,how much the p...Apparent critical current density(j_(Ac)^(a))of garnet all-solid-state lithium metal symmetric cells(ASSLSCs)is a fundamental parameter for designing all-solid-state lithium metal batteries.Nevertheless,how much the possible maximum apparent current density that a given ASSLSC system can endure and how to reveal this potential still require study.Herein,a capacity perturbation strategy aiming to better measure the possible maximum j_(Ac)^(a)is proposed for the first time.With garnet-based plane-surface structure ASSLSCs as an exemplification,the j_(Ac)^(a)is quite small when the capacity is dramatically large.Under a perturbed capacity of 0.001 mA h cm^(-2),the j_(Ac)^(a)is determined to be as high as 2.35 mA cm^(-2)at room temperature.This investigation demonstrates that the capacity perturbation strategy is a feasible strategy for measuring the possible maximum j_(Ac)^(a)of Li/solid electrolyte interface,and hopefully provides good references to explore the critical current density of other types of electrochemical systems.展开更多
High concentration of population and other elements brought by high urbanization has pushed the future construction of urban public spaces to be both "compact" and "ecological". Theory and methodol...High concentration of population and other elements brought by high urbanization has pushed the future construction of urban public spaces to be both "compact" and "ecological". Theory and methodology of landscape urbanism provides a new perspective for the construction of public spaces in high-density urban environment. Based on the concept and basic standpoints of landscape urbanism, this paper elaborated its potential value in spatial connection, functional integration and vitality promotion, and also analyzed practical strategies of landscape urbanism from three perspectives of structure, fold and stage by combining with typical cases, so as to provide references for designing urban public spaces in high-density environment.展开更多
High-density development is becoming an inevitable tendency in Chinese urbanization. In this study,the application of natural ventilation in high-density urban development is discussed. Based on the domestic and forei...High-density development is becoming an inevitable tendency in Chinese urbanization. In this study,the application of natural ventilation in high-density urban development is discussed. Based on the domestic and foreign study on natural ventilation,indoor and outdoor natural ventilated strategies,and the application on natural ventilation in underground space development are analyzed. From the study,the relationship between passive and active ventilated technologies is interpreted into what is described to be synergistic,complementary and additive.展开更多
The severe environmental problems and the demand for energy urgently require electrocatalysis to replace Haber-Bosch for the nitrogen reduction reaction(NRR).The descriptors and important properties of single-atom and...The severe environmental problems and the demand for energy urgently require electrocatalysis to replace Haber-Bosch for the nitrogen reduction reaction(NRR).The descriptors and important properties of single-atom and homonuclear double-atom catalysts have been preliminarily explored,but the relationship between the inherent properties and catalytic activity of heteronuclear double-atom catalysts with better performance remains unclear.Therefore,it is very significant to explore the prediction expressions of catalytic activity of heteronuclear double-atom catalysts based on their inherent properties and find the rule for selecting catalytic centers.Herein,by summarizing the free energy for the key steps of NRR on 55 catalysts calculated through the first-principle,the expressions of predicting the free energy and the corresponding descriptors are deduced by the machine learning,and the strategy for selecting the appropriate catalytic center is proposed.The selection strategy for the central atom of heteronuclear double-atom catalysts is that the atomic number of central B atom should be between group VB and VIIIB,and the electron difference between central A atom and B atom should be large enough,and the selectivity of NRR or hydrogen evolution reaction(HER)could be calculated through the prediction formula.Moreover,five catalysts are screened to have low limiting potential and excellent selectivity,and are further analyzed by electron transfer.This work explores the relationship between the inherent properties of heteronuclear double-atom catalysts and the catalytic activity,and puts forward the rules for selecting the heteronuclear double-atom catalytic center,which has guiding significance for the experiment.展开更多
密度峰值聚类(clustering by fast search and find of density peaks,DPC)算法是一种基于密度的聚类算法,它可以发现任意形状和维度的类簇,是具有里程碑意义的聚类算法。然而,DPC算法的样本局部密度定义不适用于同时发现数据集的稠密...密度峰值聚类(clustering by fast search and find of density peaks,DPC)算法是一种基于密度的聚类算法,它可以发现任意形状和维度的类簇,是具有里程碑意义的聚类算法。然而,DPC算法的样本局部密度定义不适用于同时发现数据集的稠密簇和稀疏簇;此外,DPC算法的一步分配策略使得一旦有一个样本分配错误,将导致更多样本的错误分配,产生“多米诺骨牌效应”。针对这些问题,提出一种新的样本局部密度定义,采用局部标准差指数定义样本局部密度,克服DPC的密度定义缺陷;采用两步分配策略代替DPC的一步分配策略,克服DPC的“多米诺骨牌效应”,得到ESDTS-DPC算法。与DPC及其改进算法KNN-DPC、FKNN-DPC、DPC-CE和经典密度聚类算法DBSCAN的实验比较显示,提出的ESDTS-DPC算法具有更好的聚类准确性。展开更多
Electrocatalytic 5-hydroxymethylfurfural oxidation reaction(HMFOR)provides a promising strategy to convert biomass derivative to highvalue-added chemicals.Herein,a cascade strategy is proposed to construct Pd-NiCo_(2)...Electrocatalytic 5-hydroxymethylfurfural oxidation reaction(HMFOR)provides a promising strategy to convert biomass derivative to highvalue-added chemicals.Herein,a cascade strategy is proposed to construct Pd-NiCo_(2)O_(4)electrocatalyst by Pd loading on Ni-doped Co3O4 and for highly active and stable synergistic HMF oxidation.An elevated current density of 800 mA cm^(-2)can be achieved at 1.5 V,and both Faradaic efficiency and yield of 2,5-furandicarboxylic acid remained close to 100%over 10 consecutive electrolysis.Experimental and theoretical results unveil that the introduction of Pd atoms can modulate the local electronic structure of Ni/Co,which not only balances the competitive adsorption of HMF and OH-species,but also promote the active Ni^(3+)species formation,inducing high indirect oxidation activity.We have also discovered that Ni incorporation facilitates the Co2+pre-oxidation and electrophilic OH*generation to contribute direct oxidation process.This work provides a new approach to design advanced electrocatalyst for biomass upgrading.展开更多
Leaf economics spectrum(LES)describes the fundamental trade-offs between leaf structural,chemical,and physiological investments.Generally,structurally robust thick leaves with high leaf dry mass per unit area(LMA)exhi...Leaf economics spectrum(LES)describes the fundamental trade-offs between leaf structural,chemical,and physiological investments.Generally,structurally robust thick leaves with high leaf dry mass per unit area(LMA)exhibit lower photosynthetic capacity per dry mass(Amass).Paradoxically,“soft and thinleaved”mosses and spikemosses have very low Amass,but due to minute-size foliage elements,their LMA and its components,leaf thickness(LT)and density(LD),have not been systematically estimated.Here,we characterized LES and associated traits in cryptogams in unprecedented details,covering five evolutionarily different lineages.We found that mosses and spikemosses had the lowest LMA and LT values ever measured for terrestrial plants.Across a broad range of species from different lineages,Amass and LD were negatively correlated.In contrast,Amass was only related to LMA when LMA was greater than 14 g cm^(-2).In fact,low Amass reflected high LD and cell wall thickness in the studied cryptogams.We conclude that evolutionarily old plant lineages attained poorly differentiated,ultrathin mesophyll by increasing LD.Across plant lineages,LD,not LMA,is the trait that represents the trade-off between leaf robustness and physiology in the LES.展开更多
基金the financial support from the Natural Science Foundation for Distinguished Young Scholars of Hunan Province(2020JJ2047)the science and technology innovation Program of Hunan Province(2022RC3048)+2 种基金the Program of Huxiang Young Talents(2019RS2002)the Innovation-Driven Project of Central South University(2020CX027)the Fundamental Research Funds for the Central Universities of Central South University(2021zzts0125)。
文摘Apparent critical current density(j_(Ac)^(a))of garnet all-solid-state lithium metal symmetric cells(ASSLSCs)is a fundamental parameter for designing all-solid-state lithium metal batteries.Nevertheless,how much the possible maximum apparent current density that a given ASSLSC system can endure and how to reveal this potential still require study.Herein,a capacity perturbation strategy aiming to better measure the possible maximum j_(Ac)^(a)is proposed for the first time.With garnet-based plane-surface structure ASSLSCs as an exemplification,the j_(Ac)^(a)is quite small when the capacity is dramatically large.Under a perturbed capacity of 0.001 mA h cm^(-2),the j_(Ac)^(a)is determined to be as high as 2.35 mA cm^(-2)at room temperature.This investigation demonstrates that the capacity perturbation strategy is a feasible strategy for measuring the possible maximum j_(Ac)^(a)of Li/solid electrolyte interface,and hopefully provides good references to explore the critical current density of other types of electrochemical systems.
文摘High concentration of population and other elements brought by high urbanization has pushed the future construction of urban public spaces to be both "compact" and "ecological". Theory and methodology of landscape urbanism provides a new perspective for the construction of public spaces in high-density urban environment. Based on the concept and basic standpoints of landscape urbanism, this paper elaborated its potential value in spatial connection, functional integration and vitality promotion, and also analyzed practical strategies of landscape urbanism from three perspectives of structure, fold and stage by combining with typical cases, so as to provide references for designing urban public spaces in high-density environment.
基金Sponsored by the 12th Five-year National Science and Technology Support Program:Research on the Key Technologies of Efficiency Optimization of High-density Urban Space(Grant No.2012BAJ15B03)
文摘High-density development is becoming an inevitable tendency in Chinese urbanization. In this study,the application of natural ventilation in high-density urban development is discussed. Based on the domestic and foreign study on natural ventilation,indoor and outdoor natural ventilated strategies,and the application on natural ventilation in underground space development are analyzed. From the study,the relationship between passive and active ventilated technologies is interpreted into what is described to be synergistic,complementary and additive.
基金supports by the National Natural Science Foundation of China(NSFC,52271113)the Natural Science Foundation of Shaanxi Province,China(2020JM 218)+1 种基金the Fundamental Research Funds for the Central Universities(CHD300102311405)HPC platform,Xi’an Jiaotong University。
文摘The severe environmental problems and the demand for energy urgently require electrocatalysis to replace Haber-Bosch for the nitrogen reduction reaction(NRR).The descriptors and important properties of single-atom and homonuclear double-atom catalysts have been preliminarily explored,but the relationship between the inherent properties and catalytic activity of heteronuclear double-atom catalysts with better performance remains unclear.Therefore,it is very significant to explore the prediction expressions of catalytic activity of heteronuclear double-atom catalysts based on their inherent properties and find the rule for selecting catalytic centers.Herein,by summarizing the free energy for the key steps of NRR on 55 catalysts calculated through the first-principle,the expressions of predicting the free energy and the corresponding descriptors are deduced by the machine learning,and the strategy for selecting the appropriate catalytic center is proposed.The selection strategy for the central atom of heteronuclear double-atom catalysts is that the atomic number of central B atom should be between group VB and VIIIB,and the electron difference between central A atom and B atom should be large enough,and the selectivity of NRR or hydrogen evolution reaction(HER)could be calculated through the prediction formula.Moreover,five catalysts are screened to have low limiting potential and excellent selectivity,and are further analyzed by electron transfer.This work explores the relationship between the inherent properties of heteronuclear double-atom catalysts and the catalytic activity,and puts forward the rules for selecting the heteronuclear double-atom catalytic center,which has guiding significance for the experiment.
文摘密度峰值聚类(clustering by fast search and find of density peaks,DPC)算法是一种基于密度的聚类算法,它可以发现任意形状和维度的类簇,是具有里程碑意义的聚类算法。然而,DPC算法的样本局部密度定义不适用于同时发现数据集的稠密簇和稀疏簇;此外,DPC算法的一步分配策略使得一旦有一个样本分配错误,将导致更多样本的错误分配,产生“多米诺骨牌效应”。针对这些问题,提出一种新的样本局部密度定义,采用局部标准差指数定义样本局部密度,克服DPC的密度定义缺陷;采用两步分配策略代替DPC的一步分配策略,克服DPC的“多米诺骨牌效应”,得到ESDTS-DPC算法。与DPC及其改进算法KNN-DPC、FKNN-DPC、DPC-CE和经典密度聚类算法DBSCAN的实验比较显示,提出的ESDTS-DPC算法具有更好的聚类准确性。
基金financially supported by Key Research and Development Projects of Sichuan Province (2023YFG0222)“Tianfu Emei” Science and Technology Innovation Leader Program in Sichuan Province (2021)+3 种基金University of Electronic Science and Technology of China Talent Start-up Funds (A1098 5310 2360 1208)the Youth Innovation Promotion Association of CAS (2020458)National Natural Science Foundation of China (21464015, 21472235, 52122212, 12274391, 223210001)Beijing Natural Science Foundation (IS23045)
文摘Electrocatalytic 5-hydroxymethylfurfural oxidation reaction(HMFOR)provides a promising strategy to convert biomass derivative to highvalue-added chemicals.Herein,a cascade strategy is proposed to construct Pd-NiCo_(2)O_(4)electrocatalyst by Pd loading on Ni-doped Co3O4 and for highly active and stable synergistic HMF oxidation.An elevated current density of 800 mA cm^(-2)can be achieved at 1.5 V,and both Faradaic efficiency and yield of 2,5-furandicarboxylic acid remained close to 100%over 10 consecutive electrolysis.Experimental and theoretical results unveil that the introduction of Pd atoms can modulate the local electronic structure of Ni/Co,which not only balances the competitive adsorption of HMF and OH-species,but also promote the active Ni^(3+)species formation,inducing high indirect oxidation activity.We have also discovered that Ni incorporation facilitates the Co2+pre-oxidation and electrophilic OH*generation to contribute direct oxidation process.This work provides a new approach to design advanced electrocatalyst for biomass upgrading.
基金funded by the EU Regional Development Fund within the framework of the Centre of Excellence EcolChange(2014-2020.4.01.15-0002),the European Commission through the European Research Council(advanced grant 322603,SIPVOL+),the Estonian Research Council(personal grant PSG884)base funding nr 190200,the National Natural Science foundation of China(31711530648)+2 种基金the Personnel Startup Project of the Scientific Research and Development Foundation of Zhejiang A&F University(2021FR041)the study was partly purchased from funding by the EU Regional Development Fund(AnaEE Estonia,2014-2020.4.01.20-0285,and the project“Plant Biology Infrastructure-TAIM”,2014-2020.4.01.20-0282)the Estonian Research Council(“Plant Biology Infrastructure-TAIM”,TT5).
文摘Leaf economics spectrum(LES)describes the fundamental trade-offs between leaf structural,chemical,and physiological investments.Generally,structurally robust thick leaves with high leaf dry mass per unit area(LMA)exhibit lower photosynthetic capacity per dry mass(Amass).Paradoxically,“soft and thinleaved”mosses and spikemosses have very low Amass,but due to minute-size foliage elements,their LMA and its components,leaf thickness(LT)and density(LD),have not been systematically estimated.Here,we characterized LES and associated traits in cryptogams in unprecedented details,covering five evolutionarily different lineages.We found that mosses and spikemosses had the lowest LMA and LT values ever measured for terrestrial plants.Across a broad range of species from different lineages,Amass and LD were negatively correlated.In contrast,Amass was only related to LMA when LMA was greater than 14 g cm^(-2).In fact,low Amass reflected high LD and cell wall thickness in the studied cryptogams.We conclude that evolutionarily old plant lineages attained poorly differentiated,ultrathin mesophyll by increasing LD.Across plant lineages,LD,not LMA,is the trait that represents the trade-off between leaf robustness and physiology in the LES.
