Identifying active sites and catalytic mechanism of the oxygen reduction reaction under anhydrous conditions are crucial for the development of next generation proton exchange membrane fuel cells(PEMFCs)operated at a ...Identifying active sites and catalytic mechanism of the oxygen reduction reaction under anhydrous conditions are crucial for the development of next generation proton exchange membrane fuel cells(PEMFCs)operated at a temperature>100℃.Here,by employing density functional theory calculations,we studied ORR on flat and stepped Pt(111)surfaces with both(110)and(100)type of steps.We found that,in contrast to ORR under hydrous conditions,(111)terrace sites are not active for ORR under anhydrous conditions,because of weakened binding of ORR intermediates induced by O*accumulation on the surface.On the other hand,step edges,which are generally not active for ORR under hydrous conditions,are predicted to be the active sites for ORR under anhydrous conditions.Among them,(110)type step edge with a unique configuration of accumulated O stabilizes O_(2)adsorption and facilitates O_(2)dissociation,which lead an overpotential<0.4 V.To improve ORR catalysts in high-temperature PEMFCs,it is desirable to maximize(110)step edge sites that present between two(111)facets of nanoparticles.展开更多
Knowledge about the spatial and temporal scales of both habitat use and the functional significance of different adaptations is essential for an understanding of the population dynamics of invertebrate assemblages. Th...Knowledge about the spatial and temporal scales of both habitat use and the functional significance of different adaptations is essential for an understanding of the population dynamics of invertebrate assemblages. This fundamental knowledge is not only interesting from an academic point of view, but is sorely lacking and needed in the field of restoration ecology. Many species are threatened due to degradation. Knowing what environmental conditions are needed dtLring the life cycle of these species is important in the design of restoration measures which aim to lift existing bottlenecks for threatened species. To assess the relative importance of water type and microhabitat in structuring the invertebrate assemblage during different seasons, invertebrates were sampled in three water bodies differing in trophic level and acidity. Different parts within a water body （microhabitats） were sampled separately and each water body was sampled in all four seasons. Results show that water body is an important factor structuring the invertebrate assemblage early in the season, whereas microhabitat became more important later in the season. Structural complexity of microhabitats was related to the type of locomotion employed by invertebrates. Seasonal differences could be related to population dynamics （reproduction, mortality）. Moreover, fluctuations in resource availability were expected to differ between the water bodies, with highest fluctuations in the eutrophic water body and with fluctuations becoming less predictable later in the season. This was confirmed by the data： species synchronization to pulses in food availability was strongest in the eutrophic water body. Moreover, synchronization was strongest in summer, while in autumn waters were invaded by dispersive species. Based on these results a synthesis is presented on the functioning of the different waters during the different seasons.展开更多
基金supported through the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical, Biological, and Geosciences Division under DE-SC0010379the support from an ECS Toyota Young Investigator Fellowship
文摘Identifying active sites and catalytic mechanism of the oxygen reduction reaction under anhydrous conditions are crucial for the development of next generation proton exchange membrane fuel cells(PEMFCs)operated at a temperature>100℃.Here,by employing density functional theory calculations,we studied ORR on flat and stepped Pt(111)surfaces with both(110)and(100)type of steps.We found that,in contrast to ORR under hydrous conditions,(111)terrace sites are not active for ORR under anhydrous conditions,because of weakened binding of ORR intermediates induced by O*accumulation on the surface.On the other hand,step edges,which are generally not active for ORR under hydrous conditions,are predicted to be the active sites for ORR under anhydrous conditions.Among them,(110)type step edge with a unique configuration of accumulated O stabilizes O_(2)adsorption and facilitates O_(2)dissociation,which lead an overpotential<0.4 V.To improve ORR catalysts in high-temperature PEMFCs,it is desirable to maximize(110)step edge sites that present between two(111)facets of nanoparticles.
文摘Knowledge about the spatial and temporal scales of both habitat use and the functional significance of different adaptations is essential for an understanding of the population dynamics of invertebrate assemblages. This fundamental knowledge is not only interesting from an academic point of view, but is sorely lacking and needed in the field of restoration ecology. Many species are threatened due to degradation. Knowing what environmental conditions are needed dtLring the life cycle of these species is important in the design of restoration measures which aim to lift existing bottlenecks for threatened species. To assess the relative importance of water type and microhabitat in structuring the invertebrate assemblage during different seasons, invertebrates were sampled in three water bodies differing in trophic level and acidity. Different parts within a water body （microhabitats） were sampled separately and each water body was sampled in all four seasons. Results show that water body is an important factor structuring the invertebrate assemblage early in the season, whereas microhabitat became more important later in the season. Structural complexity of microhabitats was related to the type of locomotion employed by invertebrates. Seasonal differences could be related to population dynamics （reproduction, mortality）. Moreover, fluctuations in resource availability were expected to differ between the water bodies, with highest fluctuations in the eutrophic water body and with fluctuations becoming less predictable later in the season. This was confirmed by the data： species synchronization to pulses in food availability was strongest in the eutrophic water body. Moreover, synchronization was strongest in summer, while in autumn waters were invaded by dispersive species. Based on these results a synthesis is presented on the functioning of the different waters during the different seasons.
