Machine learning(ML)integrated with density functional theory(DFT)calculations have recently been used to accelerate the design and discovery of single-atom catalysts(SACs)by establishing deep structure–activity rela...Machine learning(ML)integrated with density functional theory(DFT)calculations have recently been used to accelerate the design and discovery of single-atom catalysts(SACs)by establishing deep structure–activity relationships.The traditional ML models are always difficult to identify the structural differences among the single-atom systems with different modification methods,leading to the limitation of the potential application range.Aiming to the structural properties of several typical two-dimensional MA_(2)Z_(4)-based single-atom systems(bare MA_(2)Z_(4) and metal single-atom doped/supported MA_(2)Z_(4)),an improved crystal graph convolutional neural network(CGCNN)classification model was employed,instead of the traditional machine learning regression model,to address the challenge of incompatibility in the studied systems.The CGCNN model was optimized using crystal graph representation in which the geometric configuration was divided into active layer,surface layer,and bulk layer(ASB-GCNN).Through ML and DFT calculations,five potential single-atom hydrogen evolution reaction(HER)catalysts were screened from chemical space of 600 MA_(2)Z_(4)-based materials,especially V_(1)/HfSn_(2)N_(4)(S)with high stability and activity(Δ_(GH*)is 0.06 eV).Further projected density of states(pDOS)analysis in combination with the wave function analysis of the SAC-H bond revealed that the SAC-dz^(2)orbital coincided with the H-s orbital around the energy level of−2.50 eV,and orbital analysis confirmed the formation ofσbonds.This study provides an efficient multistep screening design framework of metal single-atom catalyst for HER systems with similar two-dimensional supports but different geometric configurations.展开更多
A large number of loose piles formed by mountain hazards are highly susceptible to hydraulic erosion under rainfall conditions.The use of ecological substrate materials for erosion control and ecological restoration o...A large number of loose piles formed by mountain hazards are highly susceptible to hydraulic erosion under rainfall conditions.The use of ecological substrate materials for erosion control and ecological restoration of gravel soil slopes has become a current research hotspot and the study difficulty.The post-earthquake slump accumulation gravel soil in Jiuzhaigou was selected as the research object,and the self-developed modified glutinous rice-based material was used to reinforce the gravel soil.The variable slope flume erosion test and rainfall simulation test were carried out to study the water erosion resistance of the material reconstructed soil under the influence of runoff erosion and raindrop splash erosion.The results show that:As the material content reached 12.5%,the reconstructed soil did not disintegrate after 24 hours of immersion,the internal friction angle was increased by 42.26%,and the cohesion was increased by 235.5%,which played a significant reinforcement effect.In the process of slope erosion,the soil rill erodibility parameter Kr was only 3‰ of the gravel soil control group,the critical shear force τ increased by 272%,and the soil erosion resistance was significantly improved.In the process of rainfall and rainfall on the slope,the runoff intensity of the reconstructed soil was stable,and the ability to resist runoff erosion and raindrop splash erosion was enhanced.The maximum value of soil loss rate on different slope slopes is 0.02-0.10 g·m^(-2)s^(-1),which is significantly lower than that of the control group and has better erosion reduction effect.展开更多
In this work,uniform reduced graphene oxide（RGO） films were formed on poly-（ethylene terephthalate）（PET） substrates using a simple drop-casting method.We investigated four types of substrates：unmodified PET,pol...In this work,uniform reduced graphene oxide（RGO） films were formed on poly-（ethylene terephthalate）（PET） substrates using a simple drop-casting method.We investigated four types of substrates：unmodified PET,polydopamine-coated PET.carboxyl-group-modified PET,and alkyl-group-modified PET.Upon water evaporation,the surface of the polydopamine-modified PET substrates can interact with the reduced graphene oxide sheets to form flattened and continuous RGO films,which exhibit a sheet resistance of 21.75 kΩ/sq at 82% transmittance.The result indicates that the properties of the surface groups determined whether uniform and flattened RGO films could be formed on the substrates.Hence,we proposed a simple and effective way to produce transparent and conductive films in which the catechol unit exhibits a great effect on the deposition of uniform RGO films on PET substrates.展开更多
基金supported by the National Key R&D Program of China(2021YFA1500900)National Natural Science Foundation of China(U21A20298,22141001).
文摘Machine learning(ML)integrated with density functional theory(DFT)calculations have recently been used to accelerate the design and discovery of single-atom catalysts(SACs)by establishing deep structure–activity relationships.The traditional ML models are always difficult to identify the structural differences among the single-atom systems with different modification methods,leading to the limitation of the potential application range.Aiming to the structural properties of several typical two-dimensional MA_(2)Z_(4)-based single-atom systems(bare MA_(2)Z_(4) and metal single-atom doped/supported MA_(2)Z_(4)),an improved crystal graph convolutional neural network(CGCNN)classification model was employed,instead of the traditional machine learning regression model,to address the challenge of incompatibility in the studied systems.The CGCNN model was optimized using crystal graph representation in which the geometric configuration was divided into active layer,surface layer,and bulk layer(ASB-GCNN).Through ML and DFT calculations,five potential single-atom hydrogen evolution reaction(HER)catalysts were screened from chemical space of 600 MA_(2)Z_(4)-based materials,especially V_(1)/HfSn_(2)N_(4)(S)with high stability and activity(Δ_(GH*)is 0.06 eV).Further projected density of states(pDOS)analysis in combination with the wave function analysis of the SAC-H bond revealed that the SAC-dz^(2)orbital coincided with the H-s orbital around the energy level of−2.50 eV,and orbital analysis confirmed the formation ofσbonds.This study provides an efficient multistep screening design framework of metal single-atom catalyst for HER systems with similar two-dimensional supports but different geometric configurations.
基金jointly funded by the Sichuan Provincial Natural Science Foundation of China (Grant No.2023NSFSC0378)the Jiuzhaigou Lake Swamp and River Ecological Restoration Research Project (N5132112022000246)。
文摘A large number of loose piles formed by mountain hazards are highly susceptible to hydraulic erosion under rainfall conditions.The use of ecological substrate materials for erosion control and ecological restoration of gravel soil slopes has become a current research hotspot and the study difficulty.The post-earthquake slump accumulation gravel soil in Jiuzhaigou was selected as the research object,and the self-developed modified glutinous rice-based material was used to reinforce the gravel soil.The variable slope flume erosion test and rainfall simulation test were carried out to study the water erosion resistance of the material reconstructed soil under the influence of runoff erosion and raindrop splash erosion.The results show that:As the material content reached 12.5%,the reconstructed soil did not disintegrate after 24 hours of immersion,the internal friction angle was increased by 42.26%,and the cohesion was increased by 235.5%,which played a significant reinforcement effect.In the process of slope erosion,the soil rill erodibility parameter Kr was only 3‰ of the gravel soil control group,the critical shear force τ increased by 272%,and the soil erosion resistance was significantly improved.In the process of rainfall and rainfall on the slope,the runoff intensity of the reconstructed soil was stable,and the ability to resist runoff erosion and raindrop splash erosion was enhanced.The maximum value of soil loss rate on different slope slopes is 0.02-0.10 g·m^(-2)s^(-1),which is significantly lower than that of the control group and has better erosion reduction effect.
基金supported by the National Basic Research Program of China(973 Program)with no.2011CB706900the National Nature Science Foundation of China(nos.50872149 and 50502003)+1 种基金the Scientific Research Foundation for Returned Scholars within the Ministry of Education of Chinathe Presidential Foundation of the Graduate University of the Chinese Academy of Sciences
文摘In this work,uniform reduced graphene oxide（RGO） films were formed on poly-（ethylene terephthalate）（PET） substrates using a simple drop-casting method.We investigated four types of substrates：unmodified PET,polydopamine-coated PET.carboxyl-group-modified PET,and alkyl-group-modified PET.Upon water evaporation,the surface of the polydopamine-modified PET substrates can interact with the reduced graphene oxide sheets to form flattened and continuous RGO films,which exhibit a sheet resistance of 21.75 kΩ/sq at 82% transmittance.The result indicates that the properties of the surface groups determined whether uniform and flattened RGO films could be formed on the substrates.Hence,we proposed a simple and effective way to produce transparent and conductive films in which the catechol unit exhibits a great effect on the deposition of uniform RGO films on PET substrates.
