2D nanosheets such as graphene, silicene, phosphorene, metal dichalcogenides and MXenes are emerging and promising for lithium storage due to their ultrathin nature and corresponding chemical/physical properties. Howe...2D nanosheets such as graphene, silicene, phosphorene, metal dichalcogenides and MXenes are emerging and promising for lithium storage due to their ultrathin nature and corresponding chemical/physical properties. However, the serious restacking and aggregation of the 2D nanosheets are still hampering their applications. To circumvent the issues of 2D nanosheets, one efficient strategy is to construct 3D structures with hierarchical porous structures, good chemical/mechanical stabilities and tunable electrical conductivities. In this review, we firstly focus on the available synthetic approaches of 3D structures from 2D nanosheets, and then summarize the relationships between the microstructures of 3D structures built from 2D nanosheets and their electrochemical behaviors for lithium storage. On the basis of above results, some challenges are briefly discussed in the perspective of the development of various functional 3D structures.展开更多
In this work,a facile and effective strategy to prepare three-dimensional(3D)hierarchical flower-like Mg–Al layered double hydroxides(3D-LDH)was developed via a one-step double-drop coprecipitation method usingγ-Al ...In this work,a facile and effective strategy to prepare three-dimensional(3D)hierarchical flower-like Mg–Al layered double hydroxides(3D-LDH)was developed via a one-step double-drop coprecipitation method usingγ-Al 2O 3particles as a template.The characterization and experimental results showed that the calcined product,3D-LDO,features a large specific surface area of 204.2 m^(2)/g,abundant active sites,and excellent adsorption performance for Congo red(CR),methyl orange(MO),and methyl blue(MB).The maximum adsorption capacities of 3D-LDO for CR,MO,and MB were 1428.6,476.2,and 1666.7 mg/g,respectively;such performance is superior to that of most reported adsorbents.The adsorption mechanism of organic anionic dyes by 3D-LDO was extensively investigated and attributed to surface adsorption,the memory effect of 3D-LDO,and the unique 3D hierarchical flower-like structure of the adsorbent.Recycling performance tests revealed that3D-LDO has satisfactory reusability for the three organic anionic dyes.展开更多
The North China Plain(NCP)is troubled by severe haze pollution and the evolution of haze pollution is closely related to the atmospheric boundary layer(ABL).However,experimental and theoretical studies on the physical...The North China Plain(NCP)is troubled by severe haze pollution and the evolution of haze pollution is closely related to the atmospheric boundary layer(ABL).However,experimental and theoretical studies on the physical-chemical processes of the ABL in the NCP are lacking,with many scientific problems to be addressed.To solve these problems,the Comprehensive Observation on the Atmospheric boundary layer Three-dimensional Structure(COATS)during haze pollution was carried out in the NCP from 2016 to 2020.The COATS experiment adopted a"point-line-surface"spatial layout,obtaining both spatial-temporal profiles of the meteorological and environmental elements in the ABL and the turbulent transport data of fine particulate matter(PM_(2.5))in winter and summer.The research achievements are as follows.The spatial-temporal distribution characteristics of the ABL structure and PM_(2.5)concentrations in NCP were determined.The typical thermal structure of persistent heavy haze events and the pollutant removal mechanism by low-level jets were revealed.It was determined that the spatial structure of the ABL adjusted by the Taihang Mountains is responsible for the heterogeneous distribution of haze pollution in the NCP,and that mountain-induced vertical circulations can promote the formation of elevated pollution layers.The restraints of the atmospheric internal boundaries on horizontal diffusion of pollutants were emphasized.The contribution of the ABL to haze pollution in winter and summer was qualitatively compared and quantitatively estimated.The turbulent transport nature behind the relationship between the atmospheric boundary layer height(ABLH)and surface PM_(2.5)concentrations was analyzed.The concept of"aerosol accumulation layer"was defined,and the applicability of the material method in determining ABLH was clarified.A measurement system for obtaining the turbulent flux of PM_(2.5)concentrations was developed,and the turbulence characteristics of PM_(2.5)concentrations were demonstrated.The COATS experiment is of great theoretical significance for thoroughly understanding the physical mechanisms of the ABL during haze pollution and filling the knowledge gap on the impacts of the ABL three-dimensional structure on haze pollution.The results of this study are conducive to the improvement and development of ABL parameterization schemes and serve as a scientific basis for formulating regional pollution prevention and control measures.展开更多
NiFe composites have been regarded as promising candidates to replace commercial noble-based electrocatalysts for the oxygen evolution reaction(OER).However,their practical applications still suffer from poor conducti...NiFe composites have been regarded as promising candidates to replace commercial noble-based electrocatalysts for the oxygen evolution reaction(OER).However,their practical applications still suffer from poor conductivity,limited activity,durability.To address these issues,herein,by utilizing three-dimensional covalent organic framework(3D-COF)with porous confined structures and abundant coordinate N sites as the precursor,the partially oxidized Ni_(3)Fe nanoalloys wrapped by Ndoped carbon(N-C)layers are constructed via simple pyrolysis and subsequent oxidization.Benefiting from the 3D curved hierarchical structure,high-conductivity of Ni_(3)Fe and N-C layers,well-distributed active sites,the as-synthesized O-Ni_(3)Fe-NC catalyst demonstrates excellent activity and durability for catalyzing OER.Experimental and theoretical analyses disclose that both high-temperature oxidization and the OER process greatly promote the formation and exposure of the Ni(Fe)OOH active species as well as lower charge transfer resistance,inducing its optimized OER activity.The robust graphitized N-C layers with superior conductivity and their couplings with oxidized Ni_(3)Fe nanoalloys are beneficial for stabilizing catalytic centers,thereby imparting O-Ni_(3)Fe-N-C with such outstanding stability.This work not only provides a rational guidance for enriching and stabilizing high-activity catalytic sites towards OER but also offers more insights into the structural evolution of NiFe-based OER catalysts.展开更多
基金financially supported by the National Science Foundation of China(Nos.51572007 and 51622203),"Recruitment Program of Global Experts"
文摘2D nanosheets such as graphene, silicene, phosphorene, metal dichalcogenides and MXenes are emerging and promising for lithium storage due to their ultrathin nature and corresponding chemical/physical properties. However, the serious restacking and aggregation of the 2D nanosheets are still hampering their applications. To circumvent the issues of 2D nanosheets, one efficient strategy is to construct 3D structures with hierarchical porous structures, good chemical/mechanical stabilities and tunable electrical conductivities. In this review, we firstly focus on the available synthetic approaches of 3D structures from 2D nanosheets, and then summarize the relationships between the microstructures of 3D structures built from 2D nanosheets and their electrochemical behaviors for lithium storage. On the basis of above results, some challenges are briefly discussed in the perspective of the development of various functional 3D structures.
基金supported by the National Key R&D Program of China(No.2017YFB0602702-02)。
文摘In this work,a facile and effective strategy to prepare three-dimensional(3D)hierarchical flower-like Mg–Al layered double hydroxides(3D-LDH)was developed via a one-step double-drop coprecipitation method usingγ-Al 2O 3particles as a template.The characterization and experimental results showed that the calcined product,3D-LDO,features a large specific surface area of 204.2 m^(2)/g,abundant active sites,and excellent adsorption performance for Congo red(CR),methyl orange(MO),and methyl blue(MB).The maximum adsorption capacities of 3D-LDO for CR,MO,and MB were 1428.6,476.2,and 1666.7 mg/g,respectively;such performance is superior to that of most reported adsorbents.The adsorption mechanism of organic anionic dyes by 3D-LDO was extensively investigated and attributed to surface adsorption,the memory effect of 3D-LDO,and the unique 3D hierarchical flower-like structure of the adsorbent.Recycling performance tests revealed that3D-LDO has satisfactory reusability for the three organic anionic dyes.
基金supported by the National Natural Science Foundation of China(Grant Nos.42090031,42175092,92044301&91544216)the National Key R&D Program of China(Grant Nos.2016YFC0203306&2017YFC0209600)the National Research Program for Key Issues in Air Pollution Control(Grant Nos.DQGG0104&DQGG0106)。
文摘The North China Plain(NCP)is troubled by severe haze pollution and the evolution of haze pollution is closely related to the atmospheric boundary layer(ABL).However,experimental and theoretical studies on the physical-chemical processes of the ABL in the NCP are lacking,with many scientific problems to be addressed.To solve these problems,the Comprehensive Observation on the Atmospheric boundary layer Three-dimensional Structure(COATS)during haze pollution was carried out in the NCP from 2016 to 2020.The COATS experiment adopted a"point-line-surface"spatial layout,obtaining both spatial-temporal profiles of the meteorological and environmental elements in the ABL and the turbulent transport data of fine particulate matter(PM_(2.5))in winter and summer.The research achievements are as follows.The spatial-temporal distribution characteristics of the ABL structure and PM_(2.5)concentrations in NCP were determined.The typical thermal structure of persistent heavy haze events and the pollutant removal mechanism by low-level jets were revealed.It was determined that the spatial structure of the ABL adjusted by the Taihang Mountains is responsible for the heterogeneous distribution of haze pollution in the NCP,and that mountain-induced vertical circulations can promote the formation of elevated pollution layers.The restraints of the atmospheric internal boundaries on horizontal diffusion of pollutants were emphasized.The contribution of the ABL to haze pollution in winter and summer was qualitatively compared and quantitatively estimated.The turbulent transport nature behind the relationship between the atmospheric boundary layer height(ABLH)and surface PM_(2.5)concentrations was analyzed.The concept of"aerosol accumulation layer"was defined,and the applicability of the material method in determining ABLH was clarified.A measurement system for obtaining the turbulent flux of PM_(2.5)concentrations was developed,and the turbulence characteristics of PM_(2.5)concentrations were demonstrated.The COATS experiment is of great theoretical significance for thoroughly understanding the physical mechanisms of the ABL during haze pollution and filling the knowledge gap on the impacts of the ABL three-dimensional structure on haze pollution.The results of this study are conducive to the improvement and development of ABL parameterization schemes and serve as a scientific basis for formulating regional pollution prevention and control measures.
基金the National Natural Science Foundation of China(Nos.22075062 and 21871167)and the Volkswagen Foundation(Freigeist Fellowship)。
文摘NiFe composites have been regarded as promising candidates to replace commercial noble-based electrocatalysts for the oxygen evolution reaction(OER).However,their practical applications still suffer from poor conductivity,limited activity,durability.To address these issues,herein,by utilizing three-dimensional covalent organic framework(3D-COF)with porous confined structures and abundant coordinate N sites as the precursor,the partially oxidized Ni_(3)Fe nanoalloys wrapped by Ndoped carbon(N-C)layers are constructed via simple pyrolysis and subsequent oxidization.Benefiting from the 3D curved hierarchical structure,high-conductivity of Ni_(3)Fe and N-C layers,well-distributed active sites,the as-synthesized O-Ni_(3)Fe-NC catalyst demonstrates excellent activity and durability for catalyzing OER.Experimental and theoretical analyses disclose that both high-temperature oxidization and the OER process greatly promote the formation and exposure of the Ni(Fe)OOH active species as well as lower charge transfer resistance,inducing its optimized OER activity.The robust graphitized N-C layers with superior conductivity and their couplings with oxidized Ni_(3)Fe nanoalloys are beneficial for stabilizing catalytic centers,thereby imparting O-Ni_(3)Fe-N-C with such outstanding stability.This work not only provides a rational guidance for enriching and stabilizing high-activity catalytic sites towards OER but also offers more insights into the structural evolution of NiFe-based OER catalysts.