In this study,diodo boron dipyrromethene(BODIPY)is employed a8 the energy donor and 3,4,9,10-perylene tetracarboxylic dianhydride(PDA)as the energy acceptor,enabling the synthesis of two new compounds:a BODIPY-perylen...In this study,diodo boron dipyrromethene(BODIPY)is employed a8 the energy donor and 3,4,9,10-perylene tetracarboxylic dianhydride(PDA)as the energy acceptor,enabling the synthesis of two new compounds:a BODIPY-perylene dyad named P1,and a triad named P2.To investigate the impact of the energy donor on the photophysical processes of the system,P1 comprises one diodo-BODIPY unit and one PDA unit,whereas P2 contains two diodo-BODIPY moieties and one PDA unit.Due to the good spectral complementarity between diiodo-BODIPY and PDA,these two compounds exhibit excellent light-harvesting capabilities in the 400-620 nm range.Steady-state fluorescence spectra demonstrate that when preferentially exciting the diodo-BODIPY moiety,it can effectively transfer energy to PDA;when selectively exciting the PDA moiety,quenching of PDA fluorescence is observed in both P1 and P2.Nanosecond transient absorption results show that both compounds can efficiently generate triplet excited states,which are located on the PDA part.The lifetimes of the triplet states for these two compounds are 103 and 89μs,respectively,significantly longer than that of diiodo-BODIPY.The results from the photooxidation experiments reveal that both P1 and P2 demonstrate good photostability and photooxidation capabilities,with P2 showing superior photooxidative efficiency.The photooxidation rate constant for P2 is 1.3 times that of P1,and its singlet oxygen quantum yield is 1.6 times that of P1.The results obtained here offer valuable insights for designing new photosensitizers.展开更多
The interest in curtailing environmental pollution issues through physical separation processes has inspired an extensive search for novel nanoporous materials with exceptional adsorption capabilities.Covalent triazin...The interest in curtailing environmental pollution issues through physical separation processes has inspired an extensive search for novel nanoporous materials with exceptional adsorption capabilities.Covalent triazine frameworks(CTFs),emerged as a class of crystalline covalent organic frameworks(COFs),have been widely examined for various separation applications,owing to their large porosity,high stability,and rich nitrogen(N)doping.The development of CTFs for efficient adsorption of mercury(Ⅱ)(Hg^(2+))is of great importance for the field,whereas it is rarely attempted,on account of limited synthetic strategies and unknown structural-property relations of conventional CTFs derived from ionothermal approaches.Herein,we report rational synthesis of a crystalline CTF with methylthio pendant arms for efficient removal of Hg^(2+)with an exceptional capacity of 751 mg·g^(-1),ranking at the top among previously-reported adsorbents.This work may open up new possibility in the synthesis of COFs for various separations.展开更多
Background,aim,and scope Solar radiation is the main source of energy for terrestrial ecosystems.Small changes in the absorption of solar radiation at the ground surface can have a significant impact on the climatic e...Background,aim,and scope Solar radiation is the main source of energy for terrestrial ecosystems.Small changes in the absorption of solar radiation at the ground surface can have a significant impact on the climatic environment.Natural and anthropogenic changes in ground cover are important factors affecting the absorption of solar radiation at the ground surface.This phenomenon is particularly pronounced in the mid and high latitudes.In order to quantify the inf luence of surface cover change on the absorption of solar radiation at the surface and to provide a scientific basis for changes in the climatic environment,this paper analyzed ground cover change,ground absorbed solar radiation change and the effect of ground cover change on ground absorbed solar radiation in the Three Northeastern Provinces of China from 2001 to 2018.Materials and methods In this study,the Three Northeastern Provinces of China were used as the study area.Firstly,satellite remote sensing data were used to obtain land cover data and albedo data for Aug.1st of each year in 2001,2005,2010,2015 and 2018.The albedo data were further used to calculate the absorbed solar radiation data at the ground surface.Next,the land cover data were used to count the area changes and shifts of different land classes over the five-year period.The land cover data were overlaid with the surface absorbed solar radiation data to obtain the mean and standard deviation of radiation absorption for different ground classes.The surface absorbed solar radiation data were subtracted to obtain the changes in surface absorbed solar radiation for 2001-2005,2005-2010,2010-2015 and 2015-2018.Ultimately,we used a combination of shifted changes in ground classes and changes in surface absorbed solar radiation data,with unchanged ground classes as a baseline and data such as slope orientation as an aid.We analyzed the effect of ground cover change on surface absorbed solar radiation at regional and pixel point scales.Results(1)The area of woodland and waters in the Three Northeastern Provinces of China increased and then decreased from 2001 to 2018,with an overall increase of 3.96%and 10.51%respectively.Cropland decreased and then increased,with a total decrease of 1.22%.Grassland continued to decrease,with an overall decrease of 19.36%.Building sites increased all the time,with a total increase of 11.08%.The main types of ground cover shifted were woodland,cropland and grassland.The main factors for the change in ground cover were China’s woodland protection policy and the saturation of the total woodland stock.(2)The five ground types absorb solar radiation in the order of waters>building sites>woodland>grassland>cropland.The surface absorption of solar radiation in the Songnen Plain,the Sanjiang Plain and the Songhua River Basin flowing through the Songnen Plain and the Sanjiang Plain varies significantly,by more than 25 W·m^(-2).(3)Changes in the ground cover type affected the absorption of solar radiation energy by the ground surface.There was a clear trend of interconversion between waters and cropland/grassland,cropland and woodland/grassland.In particular,the conversion of waters to both cropland and grassland radiation absorption values decreased significantly,while the opposite increased.The absolute difference between waters and cropland was a maximum of -156.66 W·m^(-2)in 2010-2015,and between waters and grassland was a maximum of 102.36 W·m^(-2) in 2005-2010.The radiative absorption values of woodland and grassland reclamation declined and conversely increased.The absolute difference between woodland and cropland was a maximum of-13.94 W·m^(-2) in 2010-2015 when woodland converted to cropland,and between grassland and cropland was a maximum of 22.36 W·m^(-2) in 2001-2005 when cropland converted to grassland,respectively.Discussion Ground cover changes in the Three Northeastern Provinces of China from 2001-2018 were inextricably linked to natural factors and the inf luence of Chinese national policies.The main inf luencing factors were China’s woodland protection policy,restoration of woodland fire sites,saturation of total woodland,optimization of cropland patterns,sanding of grassland,expansion of water conservancy projects,and urbanization expansion.There were differences in the radiation absorption characteristics of different ground cover types.This was due to the nature of the ground type itself and the regional environment.When ground cover types changed,their ability to absorb solar radiation also changed.The degree of change could be inf luenced by different ground types and different environmental factors.Different spatial scales can also produce variability.We need to consider the effects of ground cover change on the absorption of solar radiation at the surface in an integrated and comprehensive way.Conclusions The Three Northeastern Provinces of China had frequent changes in ground cover from 2001-2018,with the area of grassland decreased by almost 20%.These changes were due to natural environmental change and policies issued by China since the 21st century.The extent to which solar radiation was absorbed by different ground cover types was different,with grassland being the strongest and cropland the least.In the past few years,the Songnen Plain and Sanjiang Plain regions were the most significant changes in the absorption of solar radiation by the ground cover.The change in ground cover type led to a change in solar radiation absorption at the ground surface,with the conversion of waters to cropland or grassland and the conversion of cropland to woodland or grassland showing the greatest change in radiation absorption values,and vice versa.Of these,the absolute difference in the conversion of waters to cropland amounts to-156.66 W·m^(-2) in 2010-2015.The variation in the absorption of solar radiation at the ground surface was related to the characteristics of the ground class itself,but was also limited by the regional environment.Recommendations and perspectives This study showed that surface cover change can affect the absorption of solar radiation at the surface to varying degrees.The unchanged land classes were used as a comparative analysis in this paper,and it was clear from the paper that some of the unchanged land classes showed significant changes in radiation absorption that should be of interest in future studies.展开更多
基金supported by the Research Project for Outstanding Young People in Universities of Anhui Province(No.2023AH030099)the China Postdoctoral Science Foundation(No.2023M733378)+3 种基金the National Natural Science Foundation of China(No.21702042,No.22305059,No.22103010)the National University Students'Innovation and Entrepreneurship Training Program(No.202311059024)the Anhui Provincial Natural Science Foundation(No.2308085QB59)the Anhui Provincial Excellent Scientific Research and Innovation Team(No.2022AH010096).
文摘In this study,diodo boron dipyrromethene(BODIPY)is employed a8 the energy donor and 3,4,9,10-perylene tetracarboxylic dianhydride(PDA)as the energy acceptor,enabling the synthesis of two new compounds:a BODIPY-perylene dyad named P1,and a triad named P2.To investigate the impact of the energy donor on the photophysical processes of the system,P1 comprises one diodo-BODIPY unit and one PDA unit,whereas P2 contains two diodo-BODIPY moieties and one PDA unit.Due to the good spectral complementarity between diiodo-BODIPY and PDA,these two compounds exhibit excellent light-harvesting capabilities in the 400-620 nm range.Steady-state fluorescence spectra demonstrate that when preferentially exciting the diodo-BODIPY moiety,it can effectively transfer energy to PDA;when selectively exciting the PDA moiety,quenching of PDA fluorescence is observed in both P1 and P2.Nanosecond transient absorption results show that both compounds can efficiently generate triplet excited states,which are located on the PDA part.The lifetimes of the triplet states for these two compounds are 103 and 89μs,respectively,significantly longer than that of diiodo-BODIPY.The results from the photooxidation experiments reveal that both P1 and P2 demonstrate good photostability and photooxidation capabilities,with P2 showing superior photooxidative efficiency.The photooxidation rate constant for P2 is 1.3 times that of P1,and its singlet oxygen quantum yield is 1.6 times that of P1.The results obtained here offer valuable insights for designing new photosensitizers.
基金The National Natural Science Foundation of China(22078349,22005319,52170109)Self-deployment Program from Lanzhou Institute of Chemical Physics(E30159SQ).
文摘The interest in curtailing environmental pollution issues through physical separation processes has inspired an extensive search for novel nanoporous materials with exceptional adsorption capabilities.Covalent triazine frameworks(CTFs),emerged as a class of crystalline covalent organic frameworks(COFs),have been widely examined for various separation applications,owing to their large porosity,high stability,and rich nitrogen(N)doping.The development of CTFs for efficient adsorption of mercury(Ⅱ)(Hg^(2+))is of great importance for the field,whereas it is rarely attempted,on account of limited synthetic strategies and unknown structural-property relations of conventional CTFs derived from ionothermal approaches.Herein,we report rational synthesis of a crystalline CTF with methylthio pendant arms for efficient removal of Hg^(2+)with an exceptional capacity of 751 mg·g^(-1),ranking at the top among previously-reported adsorbents.This work may open up new possibility in the synthesis of COFs for various separations.
文摘Background,aim,and scope Solar radiation is the main source of energy for terrestrial ecosystems.Small changes in the absorption of solar radiation at the ground surface can have a significant impact on the climatic environment.Natural and anthropogenic changes in ground cover are important factors affecting the absorption of solar radiation at the ground surface.This phenomenon is particularly pronounced in the mid and high latitudes.In order to quantify the inf luence of surface cover change on the absorption of solar radiation at the surface and to provide a scientific basis for changes in the climatic environment,this paper analyzed ground cover change,ground absorbed solar radiation change and the effect of ground cover change on ground absorbed solar radiation in the Three Northeastern Provinces of China from 2001 to 2018.Materials and methods In this study,the Three Northeastern Provinces of China were used as the study area.Firstly,satellite remote sensing data were used to obtain land cover data and albedo data for Aug.1st of each year in 2001,2005,2010,2015 and 2018.The albedo data were further used to calculate the absorbed solar radiation data at the ground surface.Next,the land cover data were used to count the area changes and shifts of different land classes over the five-year period.The land cover data were overlaid with the surface absorbed solar radiation data to obtain the mean and standard deviation of radiation absorption for different ground classes.The surface absorbed solar radiation data were subtracted to obtain the changes in surface absorbed solar radiation for 2001-2005,2005-2010,2010-2015 and 2015-2018.Ultimately,we used a combination of shifted changes in ground classes and changes in surface absorbed solar radiation data,with unchanged ground classes as a baseline and data such as slope orientation as an aid.We analyzed the effect of ground cover change on surface absorbed solar radiation at regional and pixel point scales.Results(1)The area of woodland and waters in the Three Northeastern Provinces of China increased and then decreased from 2001 to 2018,with an overall increase of 3.96%and 10.51%respectively.Cropland decreased and then increased,with a total decrease of 1.22%.Grassland continued to decrease,with an overall decrease of 19.36%.Building sites increased all the time,with a total increase of 11.08%.The main types of ground cover shifted were woodland,cropland and grassland.The main factors for the change in ground cover were China’s woodland protection policy and the saturation of the total woodland stock.(2)The five ground types absorb solar radiation in the order of waters>building sites>woodland>grassland>cropland.The surface absorption of solar radiation in the Songnen Plain,the Sanjiang Plain and the Songhua River Basin flowing through the Songnen Plain and the Sanjiang Plain varies significantly,by more than 25 W·m^(-2).(3)Changes in the ground cover type affected the absorption of solar radiation energy by the ground surface.There was a clear trend of interconversion between waters and cropland/grassland,cropland and woodland/grassland.In particular,the conversion of waters to both cropland and grassland radiation absorption values decreased significantly,while the opposite increased.The absolute difference between waters and cropland was a maximum of -156.66 W·m^(-2)in 2010-2015,and between waters and grassland was a maximum of 102.36 W·m^(-2) in 2005-2010.The radiative absorption values of woodland and grassland reclamation declined and conversely increased.The absolute difference between woodland and cropland was a maximum of-13.94 W·m^(-2) in 2010-2015 when woodland converted to cropland,and between grassland and cropland was a maximum of 22.36 W·m^(-2) in 2001-2005 when cropland converted to grassland,respectively.Discussion Ground cover changes in the Three Northeastern Provinces of China from 2001-2018 were inextricably linked to natural factors and the inf luence of Chinese national policies.The main inf luencing factors were China’s woodland protection policy,restoration of woodland fire sites,saturation of total woodland,optimization of cropland patterns,sanding of grassland,expansion of water conservancy projects,and urbanization expansion.There were differences in the radiation absorption characteristics of different ground cover types.This was due to the nature of the ground type itself and the regional environment.When ground cover types changed,their ability to absorb solar radiation also changed.The degree of change could be inf luenced by different ground types and different environmental factors.Different spatial scales can also produce variability.We need to consider the effects of ground cover change on the absorption of solar radiation at the surface in an integrated and comprehensive way.Conclusions The Three Northeastern Provinces of China had frequent changes in ground cover from 2001-2018,with the area of grassland decreased by almost 20%.These changes were due to natural environmental change and policies issued by China since the 21st century.The extent to which solar radiation was absorbed by different ground cover types was different,with grassland being the strongest and cropland the least.In the past few years,the Songnen Plain and Sanjiang Plain regions were the most significant changes in the absorption of solar radiation by the ground cover.The change in ground cover type led to a change in solar radiation absorption at the ground surface,with the conversion of waters to cropland or grassland and the conversion of cropland to woodland or grassland showing the greatest change in radiation absorption values,and vice versa.Of these,the absolute difference in the conversion of waters to cropland amounts to-156.66 W·m^(-2) in 2010-2015.The variation in the absorption of solar radiation at the ground surface was related to the characteristics of the ground class itself,but was also limited by the regional environment.Recommendations and perspectives This study showed that surface cover change can affect the absorption of solar radiation at the surface to varying degrees.The unchanged land classes were used as a comparative analysis in this paper,and it was clear from the paper that some of the unchanged land classes showed significant changes in radiation absorption that should be of interest in future studies.
