Atmospheric ammonia(NH_(3)) is a chemically active trace gas that plays an important role in the atmospheric environment and climate change. Satellite remote sensing is a powerful technique to monitor NH_(3) concentra...Atmospheric ammonia(NH_(3)) is a chemically active trace gas that plays an important role in the atmospheric environment and climate change. Satellite remote sensing is a powerful technique to monitor NH_(3) concentration based on the absorption lines of NH_(3) in the thermal infrared region. In this study, we establish a retrieval algorithm to derive the NH_(3)column from the Hyperspectral Infrared Atmospheric Sounder(HIRAS) onboard the Chinese Feng Yun(FY)-3D satellite and present the first atmospheric NH_(3) column global map observed by the HIRAS instrument. The HIRAS observations can well capture NH_(3) hotspots around the world, e.g., India, West Africa, and East China, where large NH_(3) emissions exist. The HIRAS NH_(3) columns are also compared to the space-based Infrared Atmospheric Sounding Interferometer(IASI)measurements, and we find that the two instruments observe a consistent NH_(3) global distribution, with correlation coefficient(R) values of 0.28–0.73. Finally, some remaining issues about the HIRAS NH_(3) retrieval are discussed.展开更多
Focusing on revealing the origin of high ammonia yield rate on Cu via nitrate reduction(NO3RR),we herein applied constant potential method via grand-canonical density functional theory(GC-DFT)with implicit continuum s...Focusing on revealing the origin of high ammonia yield rate on Cu via nitrate reduction(NO3RR),we herein applied constant potential method via grand-canonical density functional theory(GC-DFT)with implicit continuum solvation model to predict the reaction energetics of NO3RR on pure copper surface in alkaline media.The potential-dependent mechanism on the most prevailing Cu(111)and the minor(100)and(110)facets were established,in consideration of NO_(2)_(−),NO,NH_(3),NH_(2)OH,N_(2),and N_(2)O as the main products.The computational results show that the major Cu(111)is the ideal surface to produce ammonia with the highest onset potential at 0.06 V(until−0.37 V)and the highest optimal potential at−0.31 V for ammonia production without kinetic obstacles in activation energies at critical steps.For other minor facets,the secondary Cu(100)shows activity to ammonia from−0.03 to−0.54 V with the ideal potential at−0.50 V,which requires larger overpotential to overcome kinetic activation energy barriers.The least Cu(110)possesses the longest potential range for ammonia yield from−0.27 to−1.12 V due to the higher adsorption coverage of nitrate,but also with higher tendency to generate di-nitrogen species.Experimental evaluations on commercial Cu/C electrocatalyst validated the accuracy of our proposed mechanism.The most influential(111)surface with highest percentage in electrocatalyst determined the trend of ammonia production.In specific,the onset potential of ammonia production at 0.1 V and emergence of yield rate peak at−0.3 V in experiments precisely located in the predicted potentials on Cu(111).Four critical factors for the high ammonia yield and selectivity on Cu surface via NO3RR are summarized,including high NO3RR activity towards ammonia on the dominant Cu(111)facet,more possibilities to produce ammonia along different pathways on each facet,excellent ability for HER inhibition and suitable surface size to suppress di-nitrogen species formation at high nitrate coverage.Overall,our work provides comprehensive potential-dependent insights into the reaction details of NO3RR to ammonia,which can serve as references for the future development of NO3RR electrocatalysts,achieving higher activity and selectivity by maximizing these characteristics of copper-based materials.展开更多
Elemental information carried by phytoliths plays a crucial indicative role in geochemical research.For instance,it serves as an indicator of the carbon pool effect in phytoliths and aids in the elucidation of silicon...Elemental information carried by phytoliths plays a crucial indicative role in geochemical research.For instance,it serves as an indicator of the carbon pool effect in phytoliths and aids in the elucidation of silicon sources.However,early extraction methods for soil phytoliths primarily focused on obtaining their morphological and quantitative information,lacking efficient techniques for quantitative elemental analysis.In this study,we aimed to extract Si/Al information from soil phytoliths.Considering the need for complete extraction of phytolith,six extraction methods were developed and further by alkaline dissolution to determine Si/Al.Six methods were compared in terms of enrichment capacity,the weight of extracted phytoliths,and Si/Al differences.The results indicated that the addition of Ammonia-Catechol in the commonly used heavy liquid flotation method effectively improved phytolith extraction capability and the accuracy of Si/Al results.Additionally,the inclusion of an acetic acid step before alkaline dissolution further removed surface-adsorbed impurities and enhanced the analytical quality of Si/Al in phytolith.The comparison of the data in this study with other published data shows that our method is relatively robust.The improved method proposed in this study can provide a new idea for the quantitative analysis of other elements in soil phytoliths.展开更多
基金supported by the Feng Yun Application Pioneering Project (FY-APP-2022.0502)the National Natural Science Foundation of China (Grant No. 42205140)。
文摘Atmospheric ammonia(NH_(3)) is a chemically active trace gas that plays an important role in the atmospheric environment and climate change. Satellite remote sensing is a powerful technique to monitor NH_(3) concentration based on the absorption lines of NH_(3) in the thermal infrared region. In this study, we establish a retrieval algorithm to derive the NH_(3)column from the Hyperspectral Infrared Atmospheric Sounder(HIRAS) onboard the Chinese Feng Yun(FY)-3D satellite and present the first atmospheric NH_(3) column global map observed by the HIRAS instrument. The HIRAS observations can well capture NH_(3) hotspots around the world, e.g., India, West Africa, and East China, where large NH_(3) emissions exist. The HIRAS NH_(3) columns are also compared to the space-based Infrared Atmospheric Sounding Interferometer(IASI)measurements, and we find that the two instruments observe a consistent NH_(3) global distribution, with correlation coefficient(R) values of 0.28–0.73. Finally, some remaining issues about the HIRAS NH_(3) retrieval are discussed.
基金supported by is supported by the Shanghai Municipal Science and Technology Major Projectthe support from Shanghai Super Postdoctoral Incentive Program
文摘Focusing on revealing the origin of high ammonia yield rate on Cu via nitrate reduction(NO3RR),we herein applied constant potential method via grand-canonical density functional theory(GC-DFT)with implicit continuum solvation model to predict the reaction energetics of NO3RR on pure copper surface in alkaline media.The potential-dependent mechanism on the most prevailing Cu(111)and the minor(100)and(110)facets were established,in consideration of NO_(2)_(−),NO,NH_(3),NH_(2)OH,N_(2),and N_(2)O as the main products.The computational results show that the major Cu(111)is the ideal surface to produce ammonia with the highest onset potential at 0.06 V(until−0.37 V)and the highest optimal potential at−0.31 V for ammonia production without kinetic obstacles in activation energies at critical steps.For other minor facets,the secondary Cu(100)shows activity to ammonia from−0.03 to−0.54 V with the ideal potential at−0.50 V,which requires larger overpotential to overcome kinetic activation energy barriers.The least Cu(110)possesses the longest potential range for ammonia yield from−0.27 to−1.12 V due to the higher adsorption coverage of nitrate,but also with higher tendency to generate di-nitrogen species.Experimental evaluations on commercial Cu/C electrocatalyst validated the accuracy of our proposed mechanism.The most influential(111)surface with highest percentage in electrocatalyst determined the trend of ammonia production.In specific,the onset potential of ammonia production at 0.1 V and emergence of yield rate peak at−0.3 V in experiments precisely located in the predicted potentials on Cu(111).Four critical factors for the high ammonia yield and selectivity on Cu surface via NO3RR are summarized,including high NO3RR activity towards ammonia on the dominant Cu(111)facet,more possibilities to produce ammonia along different pathways on each facet,excellent ability for HER inhibition and suitable surface size to suppress di-nitrogen species formation at high nitrate coverage.Overall,our work provides comprehensive potential-dependent insights into the reaction details of NO3RR to ammonia,which can serve as references for the future development of NO3RR electrocatalysts,achieving higher activity and selectivity by maximizing these characteristics of copper-based materials.
基金financial support from the National Natural Science Foundation of China(42273055)。
文摘Elemental information carried by phytoliths plays a crucial indicative role in geochemical research.For instance,it serves as an indicator of the carbon pool effect in phytoliths and aids in the elucidation of silicon sources.However,early extraction methods for soil phytoliths primarily focused on obtaining their morphological and quantitative information,lacking efficient techniques for quantitative elemental analysis.In this study,we aimed to extract Si/Al information from soil phytoliths.Considering the need for complete extraction of phytolith,six extraction methods were developed and further by alkaline dissolution to determine Si/Al.Six methods were compared in terms of enrichment capacity,the weight of extracted phytoliths,and Si/Al differences.The results indicated that the addition of Ammonia-Catechol in the commonly used heavy liquid flotation method effectively improved phytolith extraction capability and the accuracy of Si/Al results.Additionally,the inclusion of an acetic acid step before alkaline dissolution further removed surface-adsorbed impurities and enhanced the analytical quality of Si/Al in phytolith.The comparison of the data in this study with other published data shows that our method is relatively robust.The improved method proposed in this study can provide a new idea for the quantitative analysis of other elements in soil phytoliths.
