The metal–support interactions induced by high-temperature hydrogen reduction have a strong influence on the catalytic performance of ceria-supported Ru catalysts. However, the appearance of the strong metal–support...The metal–support interactions induced by high-temperature hydrogen reduction have a strong influence on the catalytic performance of ceria-supported Ru catalysts. However, the appearance of the strong metal–support interaction leads to covering of the Ru species by Ce suboxides, which is detrimental to the ammonia synthesis reaction that requires metallic species as active sites. In the present work, the interaction between Ru and ceria in the Ru/CeO_(2) catalyst was induced by NaBH_(4) treatment. NaBH_(4) treatment enhanced the fraction of metallic Ru, proportion of Ce^(3+), content of exposed Ru species, and amount of surface oxygen species. As a result, a larger amount of hydrogen species would desorb by the H_(2)-formation pathway and the strength of hydrogen adsorption would be weaker, weakening the inhibition effect of the hydrogen species on ammonia synthesis. In addition, the strong electronic metal–support interaction aids in nitrogen dissociation. Consequently, Ru/CeO_(2) with NaBH_(4) treatment showed higher ammonia synthesis rates than that with only hydrogen reduction.展开更多
Creating a man-made life in the laboratory is one of life science's most intriguing yet challenging problems.Advances in synthetic biology and related theories,particularly those related to the origin of life,have...Creating a man-made life in the laboratory is one of life science's most intriguing yet challenging problems.Advances in synthetic biology and related theories,particularly those related to the origin of life,have laid the groundwork for further exploration and understanding in this field of artificial life or man-made life.But there remains a wealth of quantitative mathematical models and tools that have yet to be applied to this area.In this paper,we review the two main approaches often employed in the field of man-made life:the top-down approach that reduces the complexity of extant and existing living systems and the bottom-up approach that integrates welldefined components,by introducing the theoretical basis,recent advances,and their limitations.We then argue for another possible approach,namely"bottom-up from the origin of life":Starting with the establishment of autocatalytic chemical reaction networks that employ physical boundaries as the initial compartments,then designing directed evolutionary systems,with the expectation that independent compartments will eventually emerge so that the system becomes free-living.This approach is actually analogous to the process of how life originated.With this paper,we aim to stimulate the interest of synthetic biologists and experimentalists to consider a more theoretical perspective,and to promote the communication between the origin of life community and the synthetic man-made life community.展开更多
基金financially supported by the National Science Foundation of China (Nos. 21776047, 21825801, 21978051)the Program for Qishan Scholar of Fuzhou University (Grant XRC18033)。
文摘The metal–support interactions induced by high-temperature hydrogen reduction have a strong influence on the catalytic performance of ceria-supported Ru catalysts. However, the appearance of the strong metal–support interaction leads to covering of the Ru species by Ce suboxides, which is detrimental to the ammonia synthesis reaction that requires metallic species as active sites. In the present work, the interaction between Ru and ceria in the Ru/CeO_(2) catalyst was induced by NaBH_(4) treatment. NaBH_(4) treatment enhanced the fraction of metallic Ru, proportion of Ce^(3+), content of exposed Ru species, and amount of surface oxygen species. As a result, a larger amount of hydrogen species would desorb by the H_(2)-formation pathway and the strength of hydrogen adsorption would be weaker, weakening the inhibition effect of the hydrogen species on ammonia synthesis. In addition, the strong electronic metal–support interaction aids in nitrogen dissociation. Consequently, Ru/CeO_(2) with NaBH_(4) treatment showed higher ammonia synthesis rates than that with only hydrogen reduction.
基金National Natural Science Foundation of China,Grant/Award Numbers:12205012,71731002Beijing Normal University via the Youth Talent Strategic Program,Grant/Award Number:28705-310432106Atlas Project of bio-archae by Swarma Research。
文摘Creating a man-made life in the laboratory is one of life science's most intriguing yet challenging problems.Advances in synthetic biology and related theories,particularly those related to the origin of life,have laid the groundwork for further exploration and understanding in this field of artificial life or man-made life.But there remains a wealth of quantitative mathematical models and tools that have yet to be applied to this area.In this paper,we review the two main approaches often employed in the field of man-made life:the top-down approach that reduces the complexity of extant and existing living systems and the bottom-up approach that integrates welldefined components,by introducing the theoretical basis,recent advances,and their limitations.We then argue for another possible approach,namely"bottom-up from the origin of life":Starting with the establishment of autocatalytic chemical reaction networks that employ physical boundaries as the initial compartments,then designing directed evolutionary systems,with the expectation that independent compartments will eventually emerge so that the system becomes free-living.This approach is actually analogous to the process of how life originated.With this paper,we aim to stimulate the interest of synthetic biologists and experimentalists to consider a more theoretical perspective,and to promote the communication between the origin of life community and the synthetic man-made life community.