Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the...Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the use of Ca_(2)MnO_(4)-layered perovskites modified with NaNO_(3) dopants,serving as redox catalysts(also known as oxygen carriers),for the CL-ODH of ethane within a temperature range of 700-780℃.Our findings revealed that the incorporation of NaNO_(3) as a modifier significantly-nhanced the selectivity for-thylene generation from Ca_(2)MnO_(4).At 750℃and a gas hourly space velocity of 1300 h^(-1),we achieved an-thane conversion up to 68.17%,accompanied by a corresponding-thylene yield of 57.39%.X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO_(3) onto Ca_(2)MnO_(4) not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox catalyst.Furthermore,formation of NaNO_(3) shell on the surface of Ca_(2)MnO_(4) led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise manner.This modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO_(3)-doped Ca_(2)MnO_(4) catalyst.These findings provide compelling evidence for the potential of Ca_(2)MnO_(4)-layered perovskites as promising redox catalysts in the context of CL-ODH reactions.展开更多
The maximum velocity of a mobile vortex in movement is generally limited by the phenomenon of flux-flow instability(FFI),which necessitates weak vortex pinning and fast heat removal from non-equilibrium electrons.We h...The maximum velocity of a mobile vortex in movement is generally limited by the phenomenon of flux-flow instability(FFI),which necessitates weak vortex pinning and fast heat removal from non-equilibrium electrons.We here demonstrate exfoliations and nano-fabrications of Bi_(2)Sr_(2)Ca_(2)Cu_(3)O_(10+δ) crystalline nanostrips,which possess a rather weak pinning volume of vortices,relatively low resistivity,and large normal electron diffusion coefficient.The deduced vortex velocity in Bi_(2)Sr_(2)Ca_(2)Cu_(3)O_(10+δ) crystalline nanostrips can be up to 300 km/s near the superconducting transition temperature,well above the speed of sound.The observed vortex velocity is an order of magnitude faster than that of conventional superconducting systems,representing a perfect platform for exploration of ultra-fast vortex matter and a good candidate for fabrications of superconducting nanowire single photon detectors or superconducting THz modulator.展开更多
基金support of National Natural Science Foundation of China(22179027)gratefully acknowledged.This work was also supported by the Natural Science Foundation of Guangxi Province(2021GXNSFAA075063,2018GXNSFDA281005)+1 种基金the National Key Research and Development Program of China(2017YFE0105500)Science&Technology Research Project of Guangdong Province(2017A020216009).
文摘Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the use of Ca_(2)MnO_(4)-layered perovskites modified with NaNO_(3) dopants,serving as redox catalysts(also known as oxygen carriers),for the CL-ODH of ethane within a temperature range of 700-780℃.Our findings revealed that the incorporation of NaNO_(3) as a modifier significantly-nhanced the selectivity for-thylene generation from Ca_(2)MnO_(4).At 750℃and a gas hourly space velocity of 1300 h^(-1),we achieved an-thane conversion up to 68.17%,accompanied by a corresponding-thylene yield of 57.39%.X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO_(3) onto Ca_(2)MnO_(4) not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox catalyst.Furthermore,formation of NaNO_(3) shell on the surface of Ca_(2)MnO_(4) led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise manner.This modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO_(3)-doped Ca_(2)MnO_(4) catalyst.These findings provide compelling evidence for the potential of Ca_(2)MnO_(4)-layered perovskites as promising redox catalysts in the context of CL-ODH reactions.
基金supporting high quality of post growth treatment Bi_(2)Sr_(2)Ca_(2)Cu_(3)O_(10+δ)single crystalssupported by the National Key Research and Development Program of China(Grant No.2017YFA0304000)+4 种基金the National Natural Science Foundation of China(Grant Nos.61971408 and 61827823)Shanghai Municipal Science and Technology Major Project(Grant No.2019SHZDZX01)Shanghai Rising-Star Program(Grant No.20QA1410900)the Youth Innovation Promotion Association of Chinese Academy of Sciences(Grant Nos.2020241 and 2021230)the Natural Science Foundation of Shanghai(Grant No.19ZR1467400)。
文摘The maximum velocity of a mobile vortex in movement is generally limited by the phenomenon of flux-flow instability(FFI),which necessitates weak vortex pinning and fast heat removal from non-equilibrium electrons.We here demonstrate exfoliations and nano-fabrications of Bi_(2)Sr_(2)Ca_(2)Cu_(3)O_(10+δ) crystalline nanostrips,which possess a rather weak pinning volume of vortices,relatively low resistivity,and large normal electron diffusion coefficient.The deduced vortex velocity in Bi_(2)Sr_(2)Ca_(2)Cu_(3)O_(10+δ) crystalline nanostrips can be up to 300 km/s near the superconducting transition temperature,well above the speed of sound.The observed vortex velocity is an order of magnitude faster than that of conventional superconducting systems,representing a perfect platform for exploration of ultra-fast vortex matter and a good candidate for fabrications of superconducting nanowire single photon detectors or superconducting THz modulator.