Palladium(Pd)has long been constrained as a potential catalyst for CO2reduction reactions(CO2RR)due to significant deactivation caused by strongly adsorbed carbonaceous intermediates on its surface,severely limi...Palladium(Pd)has long been constrained as a potential catalyst for CO2reduction reactions(CO2RR)due to significant deactivation caused by strongly adsorbed carbonaceous intermediates on its surface,severely limiting its catalytic activity and stability.To address this critical bottleneck,this study proposes and implements a synergistic regulation strategy combining alloying and spatial confinement effects.This approach designs a composite catalyst by encapsulating boron-silver co-doped palladium alloy nanoparticles(B-Ag4Pd6)within hollow porous resin carbon spheres(HPRCS).In an H-cell,this catalyst achieved a CO Faradaic efficiency of 96.19%at jCO=24.8 mA/cm2 and maintained stable performance for 80 h.Even under flow cell conditions,it sustained 91.23%CO selectivity at jCO=157.86 mA/cm2 over 60 h.Experimental comparisons confirmed the significant promoting effect of spatial confinement on CO2RR.Furthermore,in situ ATR-FTIR spectroscopy and density functional theory(DFT)calculations reveal that B/Ag alloying downshifts the Pd d-band center,optimizes(*)^COOH and(*)^CO adsorption,and the confined Hmicroenvironment accelerates CO formation while suppressing hydrogen evolution.This study not only successfully addressed the issue of carbon intermediate poisoning on Pd surfaces through alloying and microenvironmental regulation,but also provides novel insights and approaches for designing high-performance CO2RR catalysts that integrate electronic structure control with microenvironmental engineering.展开更多
The Ecological-living-productive land(ELPL)classification system was proposed in an effort to steer China's land pattern to an ecological-centered path,with the development model shifting from a single function in...The Ecological-living-productive land(ELPL)classification system was proposed in an effort to steer China's land pattern to an ecological-centered path,with the development model shifting from a single function into more integrated multifunction land use.The focus is coordinating the man-land contradictions and developing an intensive,efficient and sustainable land use policy in an increasingly tense relationship between humans and nature.Driven by socioeconomic change and rapid population growth,many cities are undergoing urban sprawl,which involves the consumption of cropland and ecological land and threatens the ecological balance.This paper aims to quantitatively analyze the critical effects of ELPL changes on eco-environmental quality according to land use classification based on leading function of ecology,living and production from 1990 to 2015 with a case study of Xining City.Also,four future land use scenarios were simulated for 2030 using the Future Land Use Simulation(FLUS)model that couples human and natural effects.Our results show a decrease in productive land(PL)and an increase in ecological land(EL)and living land(LL)in Xining City.Forestry ecological land(FEL)covered the top largest proportion;agriculture productive land(APL)showed the greatest reduction and urban and rural living land(U-RLL)presented a dramatic increase.The eco-environmental quality improved in 1990-2010,mainly affected by the conversion of APL to FEL and GEL.However,the encroachment of U-RLL into APL,other ecological land(OEL)and FEL was the main contributor to the decline in eco-environmental quality in 2010-2015 as well as the primary reason for the increase area of lower-quality.The Harmonious Development(HD)-Scenario,characterized by a rational allocation of LL and PL and a better eco-environment,would have implications for planning and monitoring future management of ELPL,and may represent a valuable reference for local policy-makers.展开更多
Class imbalance can substantially affect classification tasks using traditional classifiers,especially when identifying instances of minority categories.In addition to class imbalance,other challenges can also hinder ...Class imbalance can substantially affect classification tasks using traditional classifiers,especially when identifying instances of minority categories.In addition to class imbalance,other challenges can also hinder accurate classification.Researchers have explored various approaches to mitigate the effects of class imbalance.However,most studies focus only on processing correlations within a single category of samples.This paper introduces an ensemble framework called Inter-and Intra-Class Overlapping Ensemble(llCOE),which incorporates two sampling methods.The first method,which is based on classification hardness undersampling,targets majority category samples by using simple samples as the foundation for classification and improving performance by focusing on samples near classification boundaries.The second method addresses the issue of overfitting minority category samples in undersampling and ensemble learning.To mitigate this,an adaptive augment hybrid sampling method is proposed,which enhances the classification boundary of samples and reduces overfitting.This paper conducts multiple experiments on 15 public datasets and concludes that the IlCOE ensemble framework outperforms other ensemble learning algorithms in classifying imbalanced data.展开更多
基金financial support from the National Natural Science Foundation of China(72088101,22474157)the Major Program from Xiangjiang Laboratory(23XJ01010,23XJ01011)+2 种基金the Natural Science Foundation of Hunan Province(2024JJ5417)the Innovation-Driven Project of Central South University(2023CXQD048)the Changsha Natural Science Foundation Project(kq2402199)。
摘要Palladium(Pd)has long been constrained as a potential catalyst for CO2reduction reactions(CO2RR)due to significant deactivation caused by strongly adsorbed carbonaceous intermediates on its surface,severely limiting its catalytic activity and stability.To address this critical bottleneck,this study proposes and implements a synergistic regulation strategy combining alloying and spatial confinement effects.This approach designs a composite catalyst by encapsulating boron-silver co-doped palladium alloy nanoparticles(B-Ag4Pd6)within hollow porous resin carbon spheres(HPRCS).In an H-cell,this catalyst achieved a CO Faradaic efficiency of 96.19%at jCO=24.8 mA/cm2 and maintained stable performance for 80 h.Even under flow cell conditions,it sustained 91.23%CO selectivity at jCO=157.86 mA/cm2 over 60 h.Experimental comparisons confirmed the significant promoting effect of spatial confinement on CO2RR.Furthermore,in situ ATR-FTIR spectroscopy and density functional theory(DFT)calculations reveal that B/Ag alloying downshifts the Pd d-band center,optimizes(*)^COOH and(*)^CO adsorption,and the confined Hmicroenvironment accelerates CO formation while suppressing hydrogen evolution.This study not only successfully addressed the issue of carbon intermediate poisoning on Pd surfaces through alloying and microenvironmental regulation,but also provides novel insights and approaches for designing high-performance CO2RR catalysts that integrate electronic structure control with microenvironmental engineering.
基金the support of the National Natural Science Foundation of China(No.41661038)Soft Science Research Project of Science and Technology Department of Qinghai province(No.2015-ZJ-602)
摘要The Ecological-living-productive land(ELPL)classification system was proposed in an effort to steer China's land pattern to an ecological-centered path,with the development model shifting from a single function into more integrated multifunction land use.The focus is coordinating the man-land contradictions and developing an intensive,efficient and sustainable land use policy in an increasingly tense relationship between humans and nature.Driven by socioeconomic change and rapid population growth,many cities are undergoing urban sprawl,which involves the consumption of cropland and ecological land and threatens the ecological balance.This paper aims to quantitatively analyze the critical effects of ELPL changes on eco-environmental quality according to land use classification based on leading function of ecology,living and production from 1990 to 2015 with a case study of Xining City.Also,four future land use scenarios were simulated for 2030 using the Future Land Use Simulation(FLUS)model that couples human and natural effects.Our results show a decrease in productive land(PL)and an increase in ecological land(EL)and living land(LL)in Xining City.Forestry ecological land(FEL)covered the top largest proportion;agriculture productive land(APL)showed the greatest reduction and urban and rural living land(U-RLL)presented a dramatic increase.The eco-environmental quality improved in 1990-2010,mainly affected by the conversion of APL to FEL and GEL.However,the encroachment of U-RLL into APL,other ecological land(OEL)and FEL was the main contributor to the decline in eco-environmental quality in 2010-2015 as well as the primary reason for the increase area of lower-quality.The Harmonious Development(HD)-Scenario,characterized by a rational allocation of LL and PL and a better eco-environment,would have implications for planning and monitoring future management of ELPL,and may represent a valuable reference for local policy-makers.
基金supported by the National Natural Science Foundation of China(No.62173158)the National Key Research and Development Program of China(No.2019YFC0119600)the Major Science and Technology Program of Hainan Province(No.ZDKJ202004).
摘要Class imbalance can substantially affect classification tasks using traditional classifiers,especially when identifying instances of minority categories.In addition to class imbalance,other challenges can also hinder accurate classification.Researchers have explored various approaches to mitigate the effects of class imbalance.However,most studies focus only on processing correlations within a single category of samples.This paper introduces an ensemble framework called Inter-and Intra-Class Overlapping Ensemble(llCOE),which incorporates two sampling methods.The first method,which is based on classification hardness undersampling,targets majority category samples by using simple samples as the foundation for classification and improving performance by focusing on samples near classification boundaries.The second method addresses the issue of overfitting minority category samples in undersampling and ensemble learning.To mitigate this,an adaptive augment hybrid sampling method is proposed,which enhances the classification boundary of samples and reduces overfitting.This paper conducts multiple experiments on 15 public datasets and concludes that the IlCOE ensemble framework outperforms other ensemble learning algorithms in classifying imbalanced data.