We constructed two types of copper-doped metal-organic framework(MOF),i.e.,Cu@UiO-66-NH2 and Cu-UiO-66-NH2.In the former,Cu2+ions are impregnated in the pore space of the amine-functionalized,Zr-based UiO-66-NH2;while...We constructed two types of copper-doped metal-organic framework(MOF),i.e.,Cu@UiO-66-NH2 and Cu-UiO-66-NH2.In the former,Cu2+ions are impregnated in the pore space of the amine-functionalized,Zr-based UiO-66-NH2;while in the latter,Cu^2+ions are incorporated to form a bimetal-center MOF,with Zr^4+being partially replaced by Cu2+in the Zr-O oxo-clusters.Ultrafast spectroscopy revealed that the photoinduced relaxation kinetics associated with the ligand-to-cluster charge-transfer state is promoted for both Cudoped MOFs relative to undoped one,but in a sequence of Cu-UiO-66-NH2>Cu@UiO-66-NH2>UiO-66-NH2.Such a sequence turned to be in line with the trend observed in the visible-light photocatalytic hydrogen evolution activity tests on the three MOFs.These findings highlighted the subtle effect of copper-doping location in this Zr-based MOF system,further suggesting that rational engineering of the specific metal-doping location in alike MOF systems to promote the photoinduced charge separation and hence suppress the detrimental charge recombination therein is beneficial for achieving improved performances in MOF-based photocatalysis.展开更多
Understanding the dynamic responses of hard rocks is crucial during deep mining and tunneling activities and when constructing nuclear waste repositories. However, the response of deep massive rocks with openings of d...Understanding the dynamic responses of hard rocks is crucial during deep mining and tunneling activities and when constructing nuclear waste repositories. However, the response of deep massive rocks with openings of different shapes and orientations to dynamic loading is not well understood. Therefore, this study investigates the dynamic responses of hard rocks of deep underground excavation activities. Split Hopkins Pressure Bar (SHPB) tests on granite with holes of different shapes (rectangle, circle, vertical ellipse (elliptical short (ES) axis parallel to the impact load direction), and horizontal ellipse (elliptical long (EL) axis parallel to the impact load direction)) were carried out. The influence of hole shape and location on the dynamic responses was analyzed to reveal the rocks' dynamic strengths and cracking characteristics. We used the ResNet18 (convolutional neural network-based) network to recognize crack types using high-speed photographs. Moreover, a prediction model for the stress-strain response of rocks with different openings was established using Deep Neural Network (DNN). The results show that the dynamic strengths of the granite with EL and ES holes are the highest and lowest, respectively. The strength-weakening coefficient decreases first and then increases with an increase of thickness-span ratio (h/L). The weakening of the granite with ES holes is the most obvious. The ResNet18 network can improve the analyzing efficiency of the cracking mechanism, and the trained model's recognition accuracy reaches 99%. Finally, the dynamic stress-strain prediction model can predict the complete stress-strain curve well, with an accuracy above 85%.展开更多
Aiming at assessing the ecological stress of land urbanization comprehensively,three perspectives are considered and combined,i.e.the amount effect with the proportion of construction lands as the indicator,the intens...Aiming at assessing the ecological stress of land urbanization comprehensively,three perspectives are considered and combined,i.e.the amount effect with the proportion of construction lands as the indicator,the intensity effect per the density of environmental pollutant emissions,and the location effect based on their spatial distribution in the heterogeneous landscape.The quantitative results of Southern Jiangsu case in Eastern China show the single-perspective ecological stress are spatially different;the proportion effect is higher in city propers which are more densely populated and industrialized.However,the intensity effect is more significant for units along the Yangtze river where heavy industries are gathered,while the location effect is higher in“ecologically suitable”regions.As the integration of proportion,intensity,and location effects,the comprehensive stress differs across Southern Jiangsu and are also different with the single-perspective results.Dominant stressors of each unit are spatially distinct,which benefits policymakers in targeting their objectives as per primary influencing factors.It is concluded that the comprehensive assessment could efficiently reveal the spatial differentiation of the ecological effects of land urbanization and also the differentiated role of different factors for each unit.展开更多
基金the National Key Research and Development Program on Nano Science and Technology of the Ministry of Science and Technology of China(No.2016YFA0200602 and No.2018YFA0208702)the National Natural Science Foundation of China(No.21573211 and No.21633007)the Anhui Initiative in Quantum Information Technologies(No.AHY090200)。
文摘We constructed two types of copper-doped metal-organic framework(MOF),i.e.,Cu@UiO-66-NH2 and Cu-UiO-66-NH2.In the former,Cu2+ions are impregnated in the pore space of the amine-functionalized,Zr-based UiO-66-NH2;while in the latter,Cu^2+ions are incorporated to form a bimetal-center MOF,with Zr^4+being partially replaced by Cu2+in the Zr-O oxo-clusters.Ultrafast spectroscopy revealed that the photoinduced relaxation kinetics associated with the ligand-to-cluster charge-transfer state is promoted for both Cudoped MOFs relative to undoped one,but in a sequence of Cu-UiO-66-NH2>Cu@UiO-66-NH2>UiO-66-NH2.Such a sequence turned to be in line with the trend observed in the visible-light photocatalytic hydrogen evolution activity tests on the three MOFs.These findings highlighted the subtle effect of copper-doping location in this Zr-based MOF system,further suggesting that rational engineering of the specific metal-doping location in alike MOF systems to promote the photoinduced charge separation and hence suppress the detrimental charge recombination therein is beneficial for achieving improved performances in MOF-based photocatalysis.
基金funding support from the National Natural Science Foundation of China(Grant No.52374119)the opening fund of State Key Laboratory of Coal Mine Disaster Dynamics and Control(Grant No.2011DA105827-FW202209)the opening fund of State Key Laboratory of Performance Monitoring and Protecting of Rail Transit Infrastructure,East China Jiaotong University(Grant No.HJGZ2023103).
文摘Understanding the dynamic responses of hard rocks is crucial during deep mining and tunneling activities and when constructing nuclear waste repositories. However, the response of deep massive rocks with openings of different shapes and orientations to dynamic loading is not well understood. Therefore, this study investigates the dynamic responses of hard rocks of deep underground excavation activities. Split Hopkins Pressure Bar (SHPB) tests on granite with holes of different shapes (rectangle, circle, vertical ellipse (elliptical short (ES) axis parallel to the impact load direction), and horizontal ellipse (elliptical long (EL) axis parallel to the impact load direction)) were carried out. The influence of hole shape and location on the dynamic responses was analyzed to reveal the rocks' dynamic strengths and cracking characteristics. We used the ResNet18 (convolutional neural network-based) network to recognize crack types using high-speed photographs. Moreover, a prediction model for the stress-strain response of rocks with different openings was established using Deep Neural Network (DNN). The results show that the dynamic strengths of the granite with EL and ES holes are the highest and lowest, respectively. The strength-weakening coefficient decreases first and then increases with an increase of thickness-span ratio (h/L). The weakening of the granite with ES holes is the most obvious. The ResNet18 network can improve the analyzing efficiency of the cracking mechanism, and the trained model's recognition accuracy reaches 99%. Finally, the dynamic stress-strain prediction model can predict the complete stress-strain curve well, with an accuracy above 85%.
基金The work was sponsored by the National Natural Science Foundation of China(41871209,41701193 and 41401187).
文摘Aiming at assessing the ecological stress of land urbanization comprehensively,three perspectives are considered and combined,i.e.the amount effect with the proportion of construction lands as the indicator,the intensity effect per the density of environmental pollutant emissions,and the location effect based on their spatial distribution in the heterogeneous landscape.The quantitative results of Southern Jiangsu case in Eastern China show the single-perspective ecological stress are spatially different;the proportion effect is higher in city propers which are more densely populated and industrialized.However,the intensity effect is more significant for units along the Yangtze river where heavy industries are gathered,while the location effect is higher in“ecologically suitable”regions.As the integration of proportion,intensity,and location effects,the comprehensive stress differs across Southern Jiangsu and are also different with the single-perspective results.Dominant stressors of each unit are spatially distinct,which benefits policymakers in targeting their objectives as per primary influencing factors.It is concluded that the comprehensive assessment could efficiently reveal the spatial differentiation of the ecological effects of land urbanization and also the differentiated role of different factors for each unit.
