Economical,stable,and corrosion-resistant catalytic electrodes are still urgently needed for the oxygen evolution reaction(OER)in water and seawater.Herein,a mild electroless plating strategy is used to achieve large-...Economical,stable,and corrosion-resistant catalytic electrodes are still urgently needed for the oxygen evolution reaction(OER)in water and seawater.Herein,a mild electroless plating strategy is used to achieve large-scale preparation of the“integrated”phosphorus-based precatalyst(FeP-NiP)on nickel foam(NF),which is in situ reconstructed into a highly active and corrosion-resistant(Fe)NiOOH phase for OER.The interaction between phosphate anions(PO_(x)^(y-))and iron ions(Fe^(3+))tunes the electronic structure of the catalytic phase to further enhance OER kinetics.The integrated FeP-NiP@NF electrode exhibits low overpotentials for OER in alkaline water/seawater,requiring only 275/289,320/336,and 349/358 mV to reach 0.1,0.5,and 1.0 A cm^(−2),respectively.The in situ reconstructed PO_(x)^(y-)anion electrostatically repels Cl−in seawater electrolytes,allowing stable operation for over 7 days at 1.0 A cm^(−2) in extreme electrolytes(1.0 M KOH+seawater and 6.0 M KOH+seawater),demonstrating industrial-level stability.This study overcomes the complex synthesis limitations of P-based materials through innovative material design,opening new avenues for electrochemical energy conversion.展开更多
Cu-based metal-organic frameworks(MOFs)are widely employed in CO_(2)reduction reactions(CO_(2)RR).Mostly,the in-situ reconstructed derivatives such as Cu or Cu oxides during CO_(2)RR are regarded as the catalytic acti...Cu-based metal-organic frameworks(MOFs)are widely employed in CO_(2)reduction reactions(CO_(2)RR).Mostly,the in-situ reconstructed derivatives such as Cu or Cu oxides during CO_(2)RR are regarded as the catalytic active center for the formation of catalytic products.However,in many cases,the pristine MOFs still exist during the catalytic process,the key role of these pristine MOFs is often ignored in revealing the catalytic mechanism.Here,we designed two Cu(imidazole)with different coordination environments,namely CuN_(2)and Cu_(2)N_(4)for CO_(2)RR.The structures of the two MOFs were still remained after the catalytic reaction.We discovered that the pristine MOFs served as activation catalysts for converting CO_(2)into CO.Sequentially,the Cu-based derivatives,in the two cases,Cu(111)converted the CO into C_(2+)products.The CuN_(2)with more exposed Cu-N centers showed a higher FE_(CO)and a higher final FEC_(2+)than Cu_(2)N_(4).This auto-tandem catalytic mechanism was supported by electrocatalytic performance,TPD-CO,HRTEM,SAED,XPS,in-situ XANES and XES and DFT computation.The auto-tandem catalytic mechanism provides a new route to design Cu-based MOF electrocatalysts for high product selectivity in CO_(2)RR.展开更多
Accurate segmentation of camouflage objects in aerial imagery is vital for improving the efficiency of UAV-based reconnaissance and rescue missions.However,camouflage object segmentation is increasingly challenging du...Accurate segmentation of camouflage objects in aerial imagery is vital for improving the efficiency of UAV-based reconnaissance and rescue missions.However,camouflage object segmentation is increasingly challenging due to advances in both camouflage materials and biological mimicry.Although multispectral-RGB based technology shows promise,conventional dual-aperture multispectral-RGB imaging systems are constrained by imprecise and time-consuming registration and fusion across different modalities,limiting their performance.Here,we propose the Reconstructed Multispectral-RGB Fusion Network(RMRF-Net),which reconstructs RGB images into multispectral ones,enabling efficient multimodal segmentation using only an RGB camera.Specifically,RMRF-Net employs a divergentsimilarity feature correction strategy to minimize reconstruction errors and includes an efficient boundary-aware decoder to enhance object contours.Notably,we establish the first real-world aerial multispectral-RGB semantic segmentation of camouflage objects dataset,including 11 object categories.Experimental results demonstrate that RMRF-Net outperforms existing methods,achieving 17.38 FPS on the NVIDIA Jetson AGX Orin,with only a 0.96%drop in mIoU compared to the RTX 3090,showing its practical applicability in multimodal remote sensing.展开更多
Reconstruction during the oxygen evolution reaction(OER)significantly transforms the geometric structure of transition metal compounds,leading to enhanced catalytic performance.However,the resulting structural disorde...Reconstruction during the oxygen evolution reaction(OER)significantly transforms the geometric structure of transition metal compounds,leading to enhanced catalytic performance.However,the resulting structural disorder complicates the development of accurate theoretical models.In this study,CoS2 is used as a model system to establish a framework for rationally modeling reconstructed OER catalysts based on density functional theory(DFT).In the reconstruction process,sulfur atoms are likely to be substituted by oxygen atoms,leading to the formation of the CoOOH phase.Based on the difference in reconstruction degree,we constructed three types of models:doping,heterostructure,and fully reconstructed,representing the reconstruction degree from minimal to full phase transition,respectively.Fully reconstructed models,which account for strain and vacancy effects,effectively simulate the unique coordination environments of reconstructed catalysts.Model e-CoOOH achieves a theoretical overpotential of 0.38 V,outperforming pristine CoOOH(0.56 V),demonstrating that the unique structural features resulting from reconstruction improve OER performance.The doping model and the heterostructure model are helpful to explain the electronic structure and performance transformation of the reconstruction process.This work provides a rational theoretical modeling approach,which is conducive to improving the reliability of the theoretical OER performance of the reconstructed catalyst.展开更多
Hydrogen peroxide(H_(2)O_(2))electrosynthesis via two-electron oxygen reduction reaction(2e-ORR)is a promising alternative for the energy-intensive anthraquinone process.However,the instability of the catalytic metal ...Hydrogen peroxide(H_(2)O_(2))electrosynthesis via two-electron oxygen reduction reaction(2e-ORR)is a promising alternative for the energy-intensive anthraquinone process.However,the instability of the catalytic metal sites in the state-of-the-art metal single-atom catalysts(M-SACs)hinders their further industrial applications,and the high potential and valueless oxygen product of the conventional anodic oxygen evolution reaction(OER)further limit the economic efficiency of this technology.To address this,a dynamically local structure reconstruction strategy is proposed to in situ transfer the active sites from unstable metal sites to the stable surrounding carbon sites for efficient and durable 2e^(-)ORR electrocatalysis.For the as-designed Mn-N_(3)O-C catalyst,by reconstructing Mn sites into Mn(^(*)OH),the Mn sites were passivated and carbon sites adjacent to the O atom were verified to be the actual active sites by in situ characterization and theoretical calculation.Consequently,Mn-N_(3)O-C exhibited>80%Faradaic efficiency and superior long-term durability over 100 h for H_(2)O_(2)electrosynthesis at~120 mA cm^(-2).In addition,coupling anodic ethylene glycol oxidation reaction(EGOR)further improves the efficiency and economic viability of the H_(2)O_(2)electrosynthesis system.This two-pronged strategy thus opens up a new opportunity for the development of stable H_(2)O_(2)electrosynthesis with low energy consumption and superior economic performance.展开更多
基金funding support from Natural Science Foundation of Shanghai(Grant No.23ZR1443900)the National Natural Science Foundation of China(Grant Nos.22178309,22476131 and 22176127)。
文摘Economical,stable,and corrosion-resistant catalytic electrodes are still urgently needed for the oxygen evolution reaction(OER)in water and seawater.Herein,a mild electroless plating strategy is used to achieve large-scale preparation of the“integrated”phosphorus-based precatalyst(FeP-NiP)on nickel foam(NF),which is in situ reconstructed into a highly active and corrosion-resistant(Fe)NiOOH phase for OER.The interaction between phosphate anions(PO_(x)^(y-))and iron ions(Fe^(3+))tunes the electronic structure of the catalytic phase to further enhance OER kinetics.The integrated FeP-NiP@NF electrode exhibits low overpotentials for OER in alkaline water/seawater,requiring only 275/289,320/336,and 349/358 mV to reach 0.1,0.5,and 1.0 A cm^(−2),respectively.The in situ reconstructed PO_(x)^(y-)anion electrostatically repels Cl−in seawater electrolytes,allowing stable operation for over 7 days at 1.0 A cm^(−2) in extreme electrolytes(1.0 M KOH+seawater and 6.0 M KOH+seawater),demonstrating industrial-level stability.This study overcomes the complex synthesis limitations of P-based materials through innovative material design,opening new avenues for electrochemical energy conversion.
基金supported by the National Natural Science Foundation of China(Nos.22174067 and 22204078)the Natural Science Foundation of Jiangsu Province of China(No.BK20220370)+2 种基金Jiangsu Provincial Department of Education(No.22KJB150009)State Key Laboratory of Analytical Chemistry for Life Science(No.SKLACLS2218)the Priority Academic Program Development of Jiangsu Higher Education Institutions。
文摘Cu-based metal-organic frameworks(MOFs)are widely employed in CO_(2)reduction reactions(CO_(2)RR).Mostly,the in-situ reconstructed derivatives such as Cu or Cu oxides during CO_(2)RR are regarded as the catalytic active center for the formation of catalytic products.However,in many cases,the pristine MOFs still exist during the catalytic process,the key role of these pristine MOFs is often ignored in revealing the catalytic mechanism.Here,we designed two Cu(imidazole)with different coordination environments,namely CuN_(2)and Cu_(2)N_(4)for CO_(2)RR.The structures of the two MOFs were still remained after the catalytic reaction.We discovered that the pristine MOFs served as activation catalysts for converting CO_(2)into CO.Sequentially,the Cu-based derivatives,in the two cases,Cu(111)converted the CO into C_(2+)products.The CuN_(2)with more exposed Cu-N centers showed a higher FE_(CO)and a higher final FEC_(2+)than Cu_(2)N_(4).This auto-tandem catalytic mechanism was supported by electrocatalytic performance,TPD-CO,HRTEM,SAED,XPS,in-situ XANES and XES and DFT computation.The auto-tandem catalytic mechanism provides a new route to design Cu-based MOF electrocatalysts for high product selectivity in CO_(2)RR.
基金National Natural Science Foundation of China(Grant Nos.62005049 and 62072110)Natural Science Foundation of Fujian Province(Grant No.2020J01451).
文摘Accurate segmentation of camouflage objects in aerial imagery is vital for improving the efficiency of UAV-based reconnaissance and rescue missions.However,camouflage object segmentation is increasingly challenging due to advances in both camouflage materials and biological mimicry.Although multispectral-RGB based technology shows promise,conventional dual-aperture multispectral-RGB imaging systems are constrained by imprecise and time-consuming registration and fusion across different modalities,limiting their performance.Here,we propose the Reconstructed Multispectral-RGB Fusion Network(RMRF-Net),which reconstructs RGB images into multispectral ones,enabling efficient multimodal segmentation using only an RGB camera.Specifically,RMRF-Net employs a divergentsimilarity feature correction strategy to minimize reconstruction errors and includes an efficient boundary-aware decoder to enhance object contours.Notably,we establish the first real-world aerial multispectral-RGB semantic segmentation of camouflage objects dataset,including 11 object categories.Experimental results demonstrate that RMRF-Net outperforms existing methods,achieving 17.38 FPS on the NVIDIA Jetson AGX Orin,with only a 0.96%drop in mIoU compared to the RTX 3090,showing its practical applicability in multimodal remote sensing.
基金supported by the National Key Research and Development program(2022YFA1504000)the National Natural Science Foundation of China(22302101)+4 种基金the Fundamental Research Funds for the Central Universities(63185015)Shenzhen Science and Technology Program(JCYJ20210324121002007,JCYJ20230807151503007)Yunnan Provincial Science and Technology Project at Southwest United Graduate School(202402AO370001)China Postdoctoral Science Foundation(2022M721699)Guangdong Basic and Applied Basic Research Foundation(2024A1515010347).
文摘Reconstruction during the oxygen evolution reaction(OER)significantly transforms the geometric structure of transition metal compounds,leading to enhanced catalytic performance.However,the resulting structural disorder complicates the development of accurate theoretical models.In this study,CoS2 is used as a model system to establish a framework for rationally modeling reconstructed OER catalysts based on density functional theory(DFT).In the reconstruction process,sulfur atoms are likely to be substituted by oxygen atoms,leading to the formation of the CoOOH phase.Based on the difference in reconstruction degree,we constructed three types of models:doping,heterostructure,and fully reconstructed,representing the reconstruction degree from minimal to full phase transition,respectively.Fully reconstructed models,which account for strain and vacancy effects,effectively simulate the unique coordination environments of reconstructed catalysts.Model e-CoOOH achieves a theoretical overpotential of 0.38 V,outperforming pristine CoOOH(0.56 V),demonstrating that the unique structural features resulting from reconstruction improve OER performance.The doping model and the heterostructure model are helpful to explain the electronic structure and performance transformation of the reconstruction process.This work provides a rational theoretical modeling approach,which is conducive to improving the reliability of the theoretical OER performance of the reconstructed catalyst.
基金supported by the National Natural Science Foundation of China(22379111 and 22179093)。
文摘Hydrogen peroxide(H_(2)O_(2))electrosynthesis via two-electron oxygen reduction reaction(2e-ORR)is a promising alternative for the energy-intensive anthraquinone process.However,the instability of the catalytic metal sites in the state-of-the-art metal single-atom catalysts(M-SACs)hinders their further industrial applications,and the high potential and valueless oxygen product of the conventional anodic oxygen evolution reaction(OER)further limit the economic efficiency of this technology.To address this,a dynamically local structure reconstruction strategy is proposed to in situ transfer the active sites from unstable metal sites to the stable surrounding carbon sites for efficient and durable 2e^(-)ORR electrocatalysis.For the as-designed Mn-N_(3)O-C catalyst,by reconstructing Mn sites into Mn(^(*)OH),the Mn sites were passivated and carbon sites adjacent to the O atom were verified to be the actual active sites by in situ characterization and theoretical calculation.Consequently,Mn-N_(3)O-C exhibited>80%Faradaic efficiency and superior long-term durability over 100 h for H_(2)O_(2)electrosynthesis at~120 mA cm^(-2).In addition,coupling anodic ethylene glycol oxidation reaction(EGOR)further improves the efficiency and economic viability of the H_(2)O_(2)electrosynthesis system.This two-pronged strategy thus opens up a new opportunity for the development of stable H_(2)O_(2)electrosynthesis with low energy consumption and superior economic performance.
